Temoporfin-Conjugated PEGylated Poly(N,N-dimethylacrylamide)-Coated Upconversion Colloid for NIR-Induced Photodynamic Therapy of Pancreatic Cancer

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This article references 70 other publications.

1. 1

   Halbrook, C. J.; Lyssiotis, C. A.; Pasca di Magliano, M.; Maitra, A. Pancreatic cancer: Advances and challenges. Cell 2023, 186, 1729– 1754,  DOI: 10.1016/j.cell.2023.02.014

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   Pancreatic cancer advances and challenge

   Halbrook, Christopher J.; Lyssiotis, Costas A.; Pasca di Magliano, Marina; Maitra, Anirban

   Cell (Cambridge, MA, United States) (2023), 186 (8), 1729-1754CODEN: CELLB5; ISSN:0092-8674. (Cell Press)

   A review. Pancreatic ductal adenocarcinoma (PDAC) remains one of the deadliest cancers. Significant efforts have largely defined major genetic factors driving PDAC pathogenesis and progression. Pancreatic tumors are characterized by a complex microenvironment that orchestrates metabolic alterations and supports a milieu of interactions among various cell types within this niche. In this review, we highlight the foundational studies that have driven our understanding of these processes. We further discuss the recent technol. advances that continue to expand our understanding of PDAC complexity. We posit that the clin. translation of these research endeavors will enhance the currently dismal survival rate of this recalcitrant disease.

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2. 2

   Rawla, P.; Sunkara, T.; Gaduputi, V. Epidemiology of pancreatic cancer: Global trends, etiology and risk factors. World J. Oncol. 2019, 10, 10– 27,  DOI: 10.14740/wjon1166

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   Epidemiology of Pancreatic Cancer: Global Trends, Etiology and Risk Factors

   Rawla Prashanth; Sunkara Tagore; Gaduputi Vinaya

   World journal of oncology (2019), 10 (1), 10-27 ISSN:.

   Pancreatic cancer is the seventh leading cause of cancer-related deaths worldwide. However, its toll is higher in more developed countries. Reasons for vast differences in mortality rates of pancreatic cancer are not completely clear yet, but it may be due to lack of appropriate diagnosis, treatment and cataloging of cancer cases. Because patients seldom exhibit symptoms until an advanced stage of the disease, pancreatic cancer remains one of the most lethal malignant neoplasms that caused 432,242 new deaths in 2018 (GLOBOCAN 2018 estimates). Globally, 458,918 new cases of pancreatic cancer have been reported in 2018, and 355,317 new cases are estimated to occur until 2040. Despite advancements in the detection and management of pancreatic cancer, the 5-year survival rate still stands at 9% only. To date, the causes of pancreatic carcinoma are still insufficiently known, although certain risk factors have been identified, such as tobacco smoking, diabetes mellitus, obesity, dietary factors, alcohol abuse, age, ethnicity, family history and genetic factors, Helicobacter pylori infection, non-O blood group and chronic pancreatitis. In general population, screening of large groups is not considered useful to detect the disease at its early stage, although newer techniques and the screening of tightly targeted groups (especially of those with family history), are being evaluated. Primary prevention is considered of utmost importance. Up-to-date statistics on pancreatic cancer occurrence and outcome along with a better understanding of the etiology and identifying the causative risk factors are essential for the primary prevention of this disease.

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3. 3

   Park, W.; Chawla, A.; O’Reilly, E. M. Pancreatic cancer: A review. JAMA 2021, 326, 851– 862,  DOI: 10.1001/jama.2021.13027

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   3

   Pancreatic cancer: a review

   Park, Wungki; Chawla, Akhil; O'Reilly, Eileen M.

   JAMA, the Journal of the American Medical Association (2021), 326 (9), 851-862CODEN: JAMAAP; ISSN:1538-3598. (American Medical Association)

   A review. Pancreatic ductal adenocarcinoma (PDAC) is a relatively uncommon cancer, with approx. 60 430 new diagnoses expected in 2021 in the US. The incidence of PDAC is increasing by 0.5%to 1.0%per year, and it is projected to become the second-leading cause of cancer-related mortality by 2030. observations Effective screening is not available for PDAC, and most patients present with locally advanced (30%-35%) or metastatic (50%-55%) disease at diagnosis. A multidisciplinary management approach is recommended. Localized pancreas cancer includes resectable, borderline resectable (localized and involving major vascular structures), and locally advanced (unresectable) disease based on the degree of arterial and venous involvement by tumor, typically of the superior mesenteric vessels. For patients with resectable disease at presentation (10%-15%), surgery followed by adjuvant chemotherapy with FOLFIRINOX (fluorouracil, irinotecan, leucovorin, oxaliplatin) represents a std. therapeutic approach with an anticipated median overall survival of 54.4 mo, compared with 35 mo for single-agent gemcitabine (stratified hazard ratio for death, 0.64 [95%CI, 0.48-0.86]; P = .003). Neoadjuvant systemic therapy with or without radiation followed by evaluation for surgery is an accepted treatment approach for resectable and borderline resectable disease. For patients with locally advanced and unresectable disease due to extensive vascular involvement, systemic therapy followed by radiation is an option for definitive locoregional disease control. For patients with advanced (locally advanced and metastatic) PDAC, multiagent chemotherapy regimens, including FOLFIRINOX, gemcitabine/nab-paclitaxel, and nanoliposomal irinotecan/fluorouracil, all have a survival benefit of 2 to 6 mo compared with a single-agent gemcitabine. For the 5%to 7%of patients with a BRCA pathogenic germline variant and metastatic PDAC, olaparib, a poly (ADP [ADB]-ribose) polymerase inhibitor, is a maintenance option that improves progression-free survival following initial platinum-based therapy. conclusions and relevance Approx. 60 000 new cases of PDAC are diagnosed per yr, and approx. 50% of patients have advanced disease at diagnosis. The incidence of PDAC is increasing. Currently available cytotoxic therapies for advanced disease are modestly effective. For all patients, multidisciplinary management, comprehensive germline testing, and integrated supportive care are recommended.

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4. 4

   Adekolujo, O. S.; Wahab, A.; Akanbi, M. O.; Oyasiji, T.; Hrinczenko, B.; Alese, O. B. Isolated pulmonary metastases in pancreatic ductal adenocarcinoma: A review of current evidence. Cancer Biol. Ther. 2023, 24, 2198479,  DOI: 10.1080/15384047.2023.2198479

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5. 5

   Grossberg, A. J.; Chu, L. C.; Deig, C. R.; Fishman, E. K.; Hwang, W. L.; Maitra, A.; Marks, D. L.; Mehta, A.; Nabavizadeh, N.; Simeone, D. M.; Weekes, C. D.; Thomas, C. R. Multidisciplinary standards of care and recent progress in pancreatic ductal adenocarcinoma. Ca-Cancer J. Clin. 2020, 70, 375– 403,  DOI: 10.3322/caac.21626

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6. 6

   Vetvicka, D.; Sivak, L.; Jogdeo, C. M.; Kumar, R.; Khan, R.; Hang, Y.; Oupický, D. Gene silencing delivery systems for the treatment of pancreatic cancer: Where and what to target next?. J. Controlled Release 2021, 331, 246– 259,  DOI: 10.1016/j.jconrel.2021.01.020

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   Gene silencing delivery systems for the treatment of pancreatic cancer: Where and what to target next?

   Vetvicka, David; Sivak, Ladislav; Jogdeo, Chinmay M.; Kumar, Raj; Khan, Rubayat; Hang, Yu; Oupicky, David

   Journal of Controlled Release (2021), 331 (), 246-259CODEN: JCREEC; ISSN:0168-3659. (Elsevier B.V.)

   A review. Despite intensive research efforts and development of numerous new anticancer drugs and treatment strategies over the past decades, there has been only very limited improvement in overall patient survival and in effective treatment options for pancreatic cancer. Current chemotherapy improves survival in terms of months and death rates in pancreatic cancer patients are almost equiv. to incidence rates. It is imperative to develop new therapeutic approaches. Among them, gene silencing shows promise of effectiveness in both tumor cells and stromal cells by inhibiting tumor-promoting genes. This review summarizes potential targets for gene silencing in both pancreatic cancer cells and abundant stromal cells focusing on non-viral delivery systems for small RNAs and discusses the potential immunol. implications. The review concludes with the importance of multifactorial therapy of pancreatic cancer.

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7. 7

   Olajubutu, O.; Ogundipe, O. D.; Adebayo, A.; Adesina, S. K. Drug delivery strategies for the treatment of pancreatic cancer. Pharmaceutics 2023, 15, 1318,  DOI: 10.3390/pharmaceutics15051318

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8. 8

   Huang, H. C.; Mallidi, S.; Liu, J.; Chiang, C. T.; Mai, Z.; Goldschmidt, R.; Ebrahim-Zadeh, N.; Rizvi, I.; Hasan, T. Photodynamic therapy synergizes with irinotecan to overcome compensatory mechanisms and improve treatment outcomes in pancreatic cancer. Cancer Res. 2016, 76, 1066– 1077,  DOI: 10.1158/0008-5472.CAN-15-0391

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   Photodynamic Therapy Synergizes with Irinotecan to Overcome Compensatory Mechanisms and Improve Treatment Outcomes in Pancreatic Cancer

   Huang, Huang-Chiao; Mallidi, Srivalleesha; Liu, Joyce; Chiang, Chun-Te; Mai, Zhiming; Goldschmidt, Ruth; Ebrahim-Zadeh, Neema; Rizvi, Imran; Hasan, Tayyaba

   Cancer Research (2016), 76 (5), 1066-1077CODEN: CNREA8; ISSN:0008-5472. (American Association for Cancer Research)

   The ability of tumor cells to adapt to therapeutic regimens by activating alternative survival and growth pathways remains a major challenge in cancer therapy. Nanoliposomal irinotecan is approved by the FDA for gemcitabine-refractory metastatic pancreatic cancer. However, the full potential of irinotecan treatment is hindered by several cancer cell survival mechanisms, including ATP-binding cassette G2 (ABCG2) transporter-mediated irinotecan efflux from cells. Here, we demonstrate that benzoporphyrin deriv.-based photodynamic therapy (PDT), a photochem. cytotoxic modality that activates the apoptotic pathway, reduced ABCG2 expression to increase intracellular irinotecan levels in pancreatic cancer. Moreover, we show that PDT inhibited survivin expression. Although PDT potentiated irinotecan treatment, we also demonstrate that irinotecan reduced the tumoral expression of monocarboxylate transporter 4, which was upregulated by PDT. Notably, using orthotopic xenograft models, we demonstrate that combination of single low-dose PDT and a subclin. dose of nanoliposomal irinotecan synergistically inhibited tumor growth by 70% for 3 wk compared with 25% redn. after either monotherapies. Our findings offer new opportunities for the clin. translation of PDT and irinotecan combination therapy for effective pancreatic cancer treatment.

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9. 9

   Broadwater, D.; Medeiros, H. C. D.; Lunt, R. R.; Lunt, S. Y. Current advances in photoactive agents for cancer imaging and therapy. Annu. Rev. Biomed. Eng. 2021, 23, 29– 60,  DOI: 10.1146/annurev-bioeng-122019-115833

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   Current Advances in Photoactive Agents for Cancer Imaging and Therapy

   Broadwater, Deanna; Medeiros, Hyllana C. D.; Lunt, Richard R.; Lunt, Sophia Y.

   Annual Review of Biomedical Engineering (2021), 23 (), 29-60CODEN: ARBEF7; ISSN:1523-9829. (Annual Reviews)

   A review. Photoactive agents are promising complements for both early diagnosis and targeted treatment of cancer. The dual combination of diagnostics and therapeutics is known as theranostics. Photoactive theranostic agents are activated by a specific wavelength of light and emit another wavelength, which can be detected for imaging tumors, used to generate reactive oxygen species for ablating tumors, or both. Photodynamic therapy (PDT) combines photosensitizer (PS) accumulation and site-directed light irradn. for simultaneous imaging diagnostics and spatially targeted therapy. Although utilized since the early 1900s, advances in the fields of cancer biol., materials science, and nanomedicine have expanded photoactive agents to modern medical treatments. In this review we summarize the origins of PDT and the subsequent generations of PSs and analyze seminal research contributions that have provided insight into rational PS design, such as photophysics, modes of cell death, tumor-targeting mechanisms, and light dosing regimens. We highlight optimizable parameters that, with further exploration, can expand clin. applications of photoactive agents to revolutionize cancer diagnostics and treatment.

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10. 10

    Dougherty, T. J.; Gomer, C. J.; Henderson, B. W.; Jori, G.; Kessel, D.; Korbelik, M.; Moan, J.; Peng, Q. Photodynamic therapy. J. Natl. Cancer Inst. 1998, 90, 889– 905,  DOI: 10.1093/jnci/90.12.889

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    Photodynamic therapy

    Dougherty, Thomas J.; Gomer, Charles J.; Henderson, Barbara W.; Jori, Giulio; Kessel, David; Korbelik, Mladen; Moan, Johan; Peng, Qian

    Journal of the National Cancer Institute (1998), 90 (12), 889-905CODEN: JNCIEQ; ISSN:0027-8874. (Oxford University Press)

    A review with 221 refs. Photodynamic therapy involves administration of a tumor-localizing photosensitizing agent, which may require metabolic synthesis (i.e., a prodrug), followed by activation of the agent by light of a specific wavelength. This therapy results in a sequence of photochem. and photobiol. processes that cause irreversible photodamage to tumor tissues. Results from preclin. and clin. studies conducted world-wide over a 25-yr period have established photodynamic therapy as a useful treatment approach for some cancers. Since 1993, regulatory approval for photodynamic therapy involving use of a partially purified, com. available hematoporphyrin deriv. compd. (Photofrin) in patients with early and advanced stage cancer of the lung, digestive tract, and genitourinary tract has been obtained in Canada, The Netherlands, France, Germany, Japan, and the United States. We have attempted to conduct and present a comprehensive review of this rapidly expanding field. Mechanisms of subcellular and tumor localization of photosensitizing agents, as well as of mol., cellular, and tumor responses assocd. with photodynamic therapy, are discussed. Tech. issues regarding light dosimetry are also considered.

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    Agostinis, P.; Berg, K.; Cengel, K. A.; Foster, T. H.; Girotti, A. W.; Gollnick, S. O.; Hahn, S. M.; Hamblin, M. R.; Juzeniene, A.; Kessel, D. Photodynamic therapy of cancer: An update. Ca-Cancer J. Clin. 2011, 61, 250– 281,  DOI: 10.3322/caac.20114

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    Photodynamic therapy of cancer: an update

    Agostinis Patrizia; Berg Kristian; Cengel Keith A; Foster Thomas H; Girotti Albert W; Gollnick Sandra O; Hahn Stephen M; Hamblin Michael R; Juzeniene Asta; Kessel David; Korbelik Mladen; Moan Johan; Mroz Pawel; Nowis Dominika; Piette Jacques; Wilson Brian C; Golab Jakub

    CA: a cancer journal for clinicians (2011), 61 (4), 250-81 ISSN:.

    Photodynamic therapy (PDT) is a clinically approved, minimally invasive therapeutic procedure that can exert a selective cytotoxic activity toward malignant cells. The procedure involves administration of a photosensitizing agent followed by irradiation at a wavelength corresponding to an absorbance band of the sensitizer. In the presence of oxygen, a series of events lead to direct tumor cell death, damage to the microvasculature, and induction of a local inflammatory reaction. Clinical studies revealed that PDT can be curative, particularly in early stage tumors. It can prolong survival in patients with inoperable cancers and significantly improve quality of life. Minimal normal tissue toxicity, negligible systemic effects, greatly reduced long-term morbidity, lack of intrinsic or acquired resistance mechanisms, and excellent cosmetic as well as organ function-sparing effects of this treatment make it a valuable therapeutic option for combination treatments. With a number of recent technological improvements, PDT has the potential to become integrated into the mainstream of cancer treatment.

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    Chatterjee, D. K.; Yong, Z. Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells. Nanomedicine 2008, 3, 73– 82,  DOI: 10.2217/17435889.3.1.73

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    Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells

    Chatterjee, Dev K.; Yong, Zhang

    Nanomedicine (London, United Kingdom) (2008), 3 (1), 73-82CODEN: NLUKAC; ISSN:1743-5889. (Future Medicine Ltd.)

    Background: Photodynamic therapy (PDT) involves killing of diseased cells by excitation of photosensitizer chems. with high-energy light to produce cytotoxic oxygen species from surrounding dissolved oxygen. However, poor tissue penetration of high-energy light and hydrophobic photosensitizers limits the effectiveness to superficial pathologies. Upconversion phosphor nanoparticles convert low-energy radiation to higher-energy emissions. Aim:To create upconverting nanotransducers' to enable PDT in deep tissues. Results: Monodisperse, 50 nm PEI/NaYF4:Yb3+,Er3+ nanoparticles producing green/red emission on near-IR (NIR) excitation were targeted to folate receptors on human colon cancer cells and imaged with high signal-to-background ratio. It was demonstrated that these particles could be excited after deep i.m. injection in rats. On NIR excitation, the particles, modified with zinc phthalocyanin photosensitizer, released singlet oxygen and, after targeted binding to cancer cells, resulted in significant cell destruction. Conclusion: Potential clin. use of these nanoparticles includes imaging and PDT of cancer in deep tissues.

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    Wang, H.; Han, R.-L.; Yang, L.-M.; Shi, J.-H.; Liu, Z.-J.; Hu, Y.; Wang, Y.; Liu, S.-J.; Gan, Y. Design and synthesis of core-shell-shell upconversion nanoparticles for NIR-induced drug release, photodynamic therapy, and cell imaging. ACS Appl. Mater. Interfaces 2016, 8, 4416– 4423,  DOI: 10.1021/acsami.5b11197

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    Design and Synthesis of Core-Shell-Shell Upconversion Nanoparticles for NIR-Induced Drug Release, Photodynamic Therapy, and Cell Imaging

    Wang, Hao; Han, Ren-lu; Yang, Li-ming; Shi, Jun-hui; Liu, Zong-jun; Hu, Yu; Wang, You; Liu, Shu-juan; Gan, Yang

    ACS Applied Materials & Interfaces (2016), 8 (7), 4416-4423CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)

    Novel core-shell-shell structured nanoparticles 75 nm in diam. with all-in-one "smart" functional capabilities for simultaneous photoresponsive drug release, photodynamic therapy, and cell imaging are designed and prepd. These nanoparticles consist of an upconversion (UC) emission core, a photosensitizer-embodied silica sandwich shell, and a β-cyclodextrin (β-CD) gated mesoporous silica outmost shell with drugs (Rhodamine B as a model) loaded inside. We show in this proof-of-concept demonstration that, under 980 nm near-IR irradn., UC 540 nm green light emissions were emitted for cell imaging, and 660 nm red light emissions were excited for activating photosensitizers to generate singlet oxygen, which could be exploited directly to kill cancer cells and simultaneously dissoc. β-CD gatekeeper to release drugs. The preliminary results reported here will shed new light on the future design and applications of multifunctional platforms for cancer therapy and diagnostic.

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    van Straten, D.; Mashayekhi, V.; de Bruijn, H.; Oliveira, S.; Robinson, D. Oncologic photodynamic therapy: Basic principles, current clinical status and future directions. Cancers 2017, 9, 19,  DOI: 10.3390/cancers9020019

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15. 15

    Huggett, M. T.; Jermyn, M.; Gillams, A.; Illing, R.; Mosse, S.; Novelli, M.; Kent, E.; Bown, S. G.; Hasan, T.; Pogue, B. W.; Pereira, S. P. Phase I/II study of verteporfin photodynamic therapy in locally advanced pancreatic cancer. Br. J. Cancer 2014, 110, 1698– 1704,  DOI: 10.1038/bjc.2014.95

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    Phase I/II study of verteporfin photodynamic therapy in locally advanced pancreatic cancer

    Huggett, M. T.; Jermyn, M.; Gillams, A.; Illing, R.; Mosse, S.; Novelli, M.; Kent, E.; Bown, S. G.; Hasan, T.; Pogue, B. W.; Pereira, S. P.

    British Journal of Cancer (2014), 110 (7), 1698-1704CODEN: BJCAAI; ISSN:0007-0920. (Nature Publishing Group)

    Background: Patients with pancreatic cancer have a poor prognosis apart from the few suitable for surgery. Photodynamic therapy (PDT) produces localized tissue necrosis but previous studies using the photosensitizer meso-tetrahydroxyphenylchlorin (mTHPC) caused prolonged skin photosensitivity. This study assessed a shorter acting photosensitizer, verteporfin. Methods: Fifteen inoperable patients with locally advanced cancers were sensitized with 0.4 mg kg-1 verteporfin. After 60-90 min, laser light (690 nm) was delivered via single (13 patients) or multiple (2 patients) fibers positioned percutaneously under computed tomog. (CT) guidance, the light dose escalating (initially 5 J, doubling after each three patients) until 12 mm of necrosis was achieved consistently. Results: In all, 12 mm lesions were seen consistently at 40 J, but with considerable variation in necrosis vol. (mean vol. 3.5 cm3 at 40 J). Minor, self-limiting extrapancreatic effects were seen in multifiber patients. No adverse interactions were seen in patients given chemotherapy or radiotherapy before or after PDT. After PDT, one patient underwent an R0 Whipple's pancreaticoduodenectomy. Conclusions: Verteporfin PDT-induced tumor necrosis in locally advanced pancreatic cancer is feasible and safe. It can be delivered with a much shorter drug light interval and with less photosensitivity than with older compds.

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    Lange, C.; Lehmann, C.; Mahler, M.; Bednarski, P. J. Comparison of cellular death pathways after mTHPC-mediated photodynamic therapy (PDT) in five human cancer cell lines. Cancers 2019, 11, E702  DOI: 10.3390/cancers11050702

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17. 17

    Senge, M. O.; Brandt, J. C. Temoporfin (Foscan, 5,10,15,20-tetra(m-hydroxyphenyl)chlorin) - A second-generation photosensitizer. Photochem. Photobiol. 2011, 87, 1240– 1296,  DOI: 10.1111/j.1751-1097.2011.00986.x

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    Temoporfin (foscan, 5,10,15,20-tetra(m-hydroxyphenyl)chlorin)-A second-generation photosensitizer

    Senge, Mathias O.; Brandt, Johan C.

    Photochemistry and Photobiology (2011), 87 (6), 1240-1296CODEN: PHCBAP; ISSN:0031-8655. (Wiley-Blackwell)

    This review traces the development and study of the second-generation photosensitizer 5,10,15,20-tetra(m-hydroxyphenyl)chlorin through to its acceptance and clin. use in modern photodynamic (cancer) therapy. The literature has been covered up to early 2011.

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18. 18

    Wiehe, A.; Senge, M. O. The photosensitizer temoporfin (mTHPC) – Chemical, pre-clinical and clinical developments in the last decade. Photochem. Photobiol. 2023, 99, 356– 419,  DOI: 10.1111/php.13730

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19. 19

    Bown, S. G.; Rogowska, A. Z.; Whitelaw, D. E.; Lees, W. R.; Lovat, L. B.; Ripley, P.; Jones, L.; Wyld, P.; Gillams, A.; Hatfield, A. W. R. Photodynamic therapy for cancer of the pancreas. Gut 2002, 50, 549– 557,  DOI: 10.1136/gut.50.4.549

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    19

    Photodynamic therapy for cancer of the pancreas

    Bown S G; Rogowska A Z; Whitelaw D E; Lees W R; Lovat L B; Ripley P; Jones L; Wyld P; Gillams A; Hatfield A W R

    Gut (2002), 50 (4), 549-57 ISSN:0017-5749.

    BACKGROUND: Few pancreatic cancers are suitable for surgery and few respond to chemoradiation. Photodynamic therapy produces local necrosis of tissue with light after prior administration of a photosensitising agent, and in experimental studies can be tolerated by the pancreas and surrounding normal tissue. AIMS: To undertake a phase I study of photodynamic therapy for cancer of the pancreas. PATIENTS: Sixteen patients with inoperable adenocarcinomas (2.5-6 cm in diameter) localised to the region of the head of the pancreas were studied. All presented with obstructive jaundice which was relieved by biliary stenting prior to further treatment. METHODS: Patients were photosensitised with 0.15 mg/kg meso-tetrahydroxyphenyl chlorin intravenously. Three days later, light was delivered to the cancer percutaneously using fibres positioned under computerised tomographic guidance. Three had subsequent chemotherapy. RESULTS: All patients had substantial tumour necrosis on scans after treatment. Fourteen of 16 left hospital within 10 days. Eleven had a Karnofsky performance status of 100 prior to treatment. In 10 it returned to 100 at one month. Two patients with tumour involving the gastroduodenal artery had significant gastrointestinal bleeds (controlled without surgery). Three patients developed duodenal obstruction during follow up that may have been related to treatment. There was no treatment related mortality. The median survival time after photodynamic therapy was 9.5 months (range 4-30). Seven of 16 patients (44%) were alive one year after photodynamic therapy. CONCLUSIONS: Photodynamic therapy can produce necrosis in pancreatic cancers with an acceptable morbidity although care is required for tumours invading the duodenal wall or involving the gastroduodenal artery. Further studies are indicated to assess its influence on the course of the disease, alone or in combination with chemoradiation.

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    Kiesslich, T.; Berlanda, J.; Plaetzer, K.; Krammer, B.; Berr, F. Comparative characterization of the efficiency and cellular pharmacokinetics of Foscan- and Foslip-based photodynamic treatment in human biliary tract cancer cell lines. Photochem. Photobiol. Sci. 2007, 6, 619– 627,  DOI: 10.1039/b617659c

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    Comparative characterization of the efficiency and cellular pharmacokinetics of Foscan- and Foslip-based photodynamic treatment in human biliary tract cancer cell lines

    Kiesslich, Tobias; Berlanda, Juergen; Plaetzer, Kristjan; Krammer, Barbara; Berr, Frieder

    Photochemical & Photobiological Sciences (2007), 6 (6), 619-627CODEN: PPSHCB; ISSN:1474-905X. (Royal Society of Chemistry)

    Due to the poor prognosis and limited management options for perihilar cholangiocarcinoma (CC) the development of alternatives for treatment is an important topic. Photodynamic therapy (PDT) with porfimer as palliative or neoadjuvant endoscopic treatment of non-resectable perihilar CC has improved quality of life and survival time, but cannot eradicate the primary tumors because of inadequate tumoricidal depth (4 mm only around the tumor stenoses). The use of meta-tetrahydroxyphenyl chlorin (mTHPC) and photoactivation at higher wavelengths (650-660 nm) provides high tumoricidal depth (10 mm) for PDT of pancreatic cancer and should yield similar tumoricidal depth in CC. This study investigates the photodynamic characteristics of mTHPC in solvent-based formulation (Foscan) and in liposomal (water sol.) formulation (Foslip) in an in vitro model system consisting of two biliary cancer cell lines (GBC, gall bladder cancer and BDC, bile duct cancer cells). Dark toxicity, photodynamic efficiency, time-dependent uptake and retention and intracellular localization of Foscan and Foslip were studied. The results prove mTHPC as a potent photosensitizing agent with high phototoxic potential in biliary cancer cells as a concn. of 600 ng ml-1 and irradn. with 1.5 J cm-2 (660 ± 10 nm) is sufficient for about 90% cell killing. Addn. of fetal bovine serum (FBS) to the incubation medium and anal. of the uptake and phototoxic properties reveals that both photosensitizer formulations bind to serum protein fractions, i.e. no difference between Foscan and Foslip can be found in the presence of FBS. Laser scanning fluorescence microscopy indicates a similar pattern of perinuclear localization of both sensitizers. This study demonstrates the potential of mTHPC for treatment of bile duct malignancies and provides evidence that Foslip is an equiv. water-sol. formulation of mTHPC that should ease i.v. application and thus clin. use of mTHPC.

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21. 21

    Dos Santos, A. F.; Arini, G. S.; de Almeida, D. R. Q.; Labriola, L. Nanophotosensitizers for cancer therapy: A promising technology?. J. Phys. Mater. 2021, 4, 032006,  DOI: 10.1088/2515-7639/abf7dd

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22. 22

    Saeed, M.; Ren, W.; Wu, A. Therapeutic applications of iron oxide based nanoparticles in cancer: Basic concepts and recent advances. Biomater. Sci. 2018, 6, 708– 725,  DOI: 10.1039/C7BM00999B

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    22

    Therapeutic applications of iron oxide based nanoparticles in cancer: basic concepts and recent advances

    Saeed, Madiha; Ren, Wenzhi; Wu, Aiguo

    Biomaterials Science (2018), 6 (4), 708-725CODEN: BSICCH; ISSN:2047-4849. (Royal Society of Chemistry)

    Nanotechnol. has introduced new techniques and phototherapy approaches to fabricate and utilize nanoparticles for cancer therapy. These phototherapy approaches, such as photothermal therapy (PTT) and photodynamic therapy (PDT), hold great promise to overcome the limitations of traditional treatment methods. In phototherapy, magnetic iron oxide nanoparticles (IONPs) are of paramount importance due to their wide range of biomedical applications. This review discusses the basic concepts, various therapy approaches (PTT, PDT, magnetic hyperthermia therapy (MHT), chemotherapy and immunotherapy), intrinsic properties, and mechanisms of cell death of IONPs; it also provides a brief overview of recent developments in IONPs, with focus on their therapeutic applications. Much attention is devoted to elaborating the various parameters, intracellular behaviors and limitations of MHT. Bimodal therapies which act alone or in combination with other modalities are also discussed. The review highlights some limitations in the explored research areas and suggests future directions to overcome these limitations.

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23. 23

    Yang, H.; Liu, R.; Xu, Y.; Qian, L.; Dai, Z. Photosensitizer nanoparticles boost photodynamic therapy for pancreatic cancer treatment. Nano-Micro Lett. 2021, 13, 35,  DOI: 10.1007/s40820-020-00561-8

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    23

    Photosensitizer Nanoparticles Boost Photodynamic Therapy for Pancreatic Cancer Treatment

    Yang Huanyu; Qian Linxue; Liu Renfa; Xu Yunxue; Dai Zhifei

    Nano-micro letters (2021), 13 (1), 35 ISSN:.

    Patients with pancreatic cancer (PCa) have a poor prognosis apart from the few suitable for surgery. Photodynamic therapy (PDT) is a minimally invasive treatment modality whose efficacy and safety in treating unresectable localized PCa have been corroborated in clinic. Yet, it suffers from certain limitations during clinical exploitation, including insufficient photosensitizers (PSs) delivery, tumor-oxygenation dependency, and treatment escape of aggressive tumors. To overcome these obstacles, an increasing number of researchers are currently on a quest to develop photosensitizer nanoparticles (NPs) by the use of a variety of nanocarrier systems to improve cellular uptake and biodistribution of photosensitizers. Encapsulation of PSs with NPs endows them significantly higher accumulation within PCa tumors due to the increased solubility and stability in blood circulation. A number of approaches have been explored to produce NPs co-delivering multi-agents affording PDT-based synergistic therapies for improved response rates and durability of response after treatment. This review provides an overview of available data regarding the design, methodology, and oncological outcome of the innovative NPs-based PDT of PCa.

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24. 24

    Yakavets, I.; Millard, M.; Zorin, V.; Lassalle, H.-P.; Bezdetnaya, L. Current state of the nanoscale delivery systems for temoporfin-based photodynamic therapy: Advanced delivery strategies. J. Controlled Release 2019, 304, 268– 287,  DOI: 10.1016/j.jconrel.2019.05.035

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    24

    Current state of the nanoscale delivery systems for temoporfin-based photodynamic therapy: Advanced delivery strategies

    Yakavets, Ilya; Millard, Marie; Zorin, Vladimir; Lassalle, Henri-Pierre; Bezdetnaya, Lina

    Journal of Controlled Release (2019), 304 (), 268-287CODEN: JCREEC; ISSN:0168-3659. (Elsevier B.V.)

    A review. Enthusiasm for photodynamic therapy (PDT) as a promising technique to eradicate various cancers has increased exponentially in recent decades. The majority of clin. approved photosensitizers are hydrophobic in nature, thus, the effective delivery of photosensitizers at the targeted site is the main hurdle assocd. with PDT. Temoporfin (mTHPC, medicinal product name: Foscan), is one of the most potent clin. approved photosensitizers, is not an exception. Successful temoporfin-PDT requires nanoscale delivery systems for selective delivery of photosensitizer. Over the last 25 years, the no. of papers on nanoplatforms developed for mTHPC delivery such as conjugates, host-guest inclusion complexes, lipid-and polymer-based nanoparticles and carbon nanotubes is burgeoning. However, none of them appeared to be "ultimate". The present review offers the description of different challenges and achievements in nanoparticle-based mTHPC delivery focusing on the synergetic combination of various nano-platforms to improve temoporfin delivery at all stages of biodistribution. Furthermore, the assocn. of different nanoparticles in one nanoplatform might be considered as an advanced strategy allowing the combination of several treatment modalities.

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25. 25

    Grahn, M. F.; Giger, A.; McGuinness, A.; de Jode, M. L.; Stewart, J. C.; Ris, H. B.; Altermatt, H. J.; Williams, N. S. mTHPC polymer conjugates: The in vivo photodynamic activity of four candidate compounds. Lasers Med. Sci. 1999, 14, 40– 46,  DOI: 10.1007/s101030050019

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    25

    mTHPC Polymer Conjugates: The In Vivo Photodynamic Activity of Four Candidate Compounds

    Grahn M F; Giger A; McGuinness A; de Jode M L; Stewart J C; Ris H B; Altermatt H J; Williams N S

    Lasers in medical science (1999), 14 (1), 40-6 ISSN:0268-8921.

    The in vivo photodynamic activities of four poly(ethylene glycol) (PEG) conjugates of the photosensitiser 5,10,15,20-tetrakis-(m-hydroxyphenyl)chlorin (mTHPC, temoporfin, Foscan(®)) were compared with that of mTHPC over a range of drug-light intervals using acute tumour necrosis and skeletal muscles swelling in a mouse model in order to ascertain the influence of linking group stability and PEG chain length on the photodynamic activity. The four compounds examined contained either PEG 2000 or PEG 5000 attached by carbonate or triazine linkages at the phenol hydroxyl groups of the mTHPC.All compounds tested caused tumour necrosis at drug-light intervals of between one and four days. mTHPC produced tumour necrosis of over 5 mm at drug-light intervals of 1 and 2 days with limited muscle damage at early drug-light intervals. The relatively labile carbonate-linked conjugates gave tumour necrosis similar to mTHPC but produced severe muscle and systemic phototoxicity on irradiation at 4-24 h after injection. The more stable triazine-linked conjugates produced no significant muscle damage at any of the drug-light intervals tested, but gave only limited tumour necrosis under the conditions tested. PEG chain length had relatively little effect on the patterns of bioactivity.It is concluded that both classes of mTHPC PEG conjugates may be suitable for photodynamic therapy if the problems of stability and early photosensitivity in the case of the carbonates and reduced potency in the case of the triazines can be overcome through improved formulations and PDT treatment regimens.

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26. 26

    Bautista-Sanchez, A.; Kasselouri, A.; Desroches, M.-C.; Blais, J.; Maillard, P.; de Oliveira, D. M.; Tedesco, A. C.; Prognon, P.; Delaire, J. Photophysical properties of glucoconjugated chlorins and porphyrins and their associations with cyclodextrins. J. Photochem. Photobiol., B 2005, 81, 154– 162,  DOI: 10.1016/j.jphotobiol.2005.05.013

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    26

    Photophysical properties of glucoconjugated chlorins and porphyrins and their associations with cyclodextrins

    Bautista-Sanchez, Antonia; Kasselouri, Athena; Desroches, Marie-Catherine; Blais, Jocelyne; Maillard, Philippe; Manfrim de Oliveira, Daniela; Tedesco, Antonio C.; Prognon, Patrice; Delaire, Jacques

    Journal of Photochemistry and Photobiology, B: Biology (2005), 81 (3), 154-162CODEN: JPPBEG; ISSN:1011-1344. (Elsevier B.V.)

    Glucoconjugated analogs of the meta-hydroxyphenyl porphyrin (m-THPP) and meta-hydroxyphenyl chlorin (m-THPC) has been recently synthesized. The characteristics of their triplet states have been detd. with regard to their involvement in the photodynamic (PDT) efficiency. In the case of porphyrin derivs., triplet quantum yields (ΦT) were ranging from 0.42 to 0.55 and triplet lifetimes (τT) from 1 to 5 μs. High reaction rate consts. (kq) with mol. oxygen (kq: 1.2-1.6 × 109 s-1) have been found. The triplet lifetimes of chlorin derivs. were about four times higher than those of porphyrins whereas the ΦT and kq values remained quite similar. Singlet oxygen yields of glucosylated and non-glucosylated porphyrins and chlorins were not significantly different within exptl. errors (ΦΔ(1O2): 0.41-0.58). Furthermore, it has been shown that glucoconjugated photosensitizers could undergo assocns. with the methyl-β-cyclodextrin (Me-β-CD) which exhibit high triplet lifetimes and singlet oxygen yields ranging from 0.27 to 0.48.

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27. 27

    Gravier, J.; Schneider, R.; Frochot, C.; Bastogne, T.; Schmitt, F.; Didelon, J.; Guillemin, F.; Barberi-Heyob, M. Improvement of meta-tetra(hydroxyphenyl)chlorin-like photosensitizer selectivity with folate-based targeted delivery, Synthesis and in vivo delivery studies. J. Med. Chem. 2008, 51, 3867– 3877,  DOI: 10.1021/jm800125a

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    27

    Improvement of meta-tetra(Hydroxyphenyl)chlorin-Like Photosensitizer Selectivity with Folate-Based Targeted Delivery. Synthesis and in Vivo Delivery Studies

    Gravier, Julien; Schneider, Raphael; Frochot, Celine; Bastogne, Thierry; Schmitt, Frederic; Didelon, Jacques; Guillemin, Francois; Barberi-Heyob, Muriel

    Journal of Medicinal Chemistry (2008), 51 (13), 3867-3877CODEN: JMCMAR; ISSN:0022-2623. (American Chemical Society)

    The cell membrane folate receptor (FR) is a mol. target for tumor-selective drug delivery, including delivery of photosensitizers for anticancer photodynamic therapy (PDT). Tumor selectivity of meta-tetra(hydroxyphenyl)chlorin (m-THPC), a photosensitizer used in PDT clin. trials, demonstrates a low tumor-to-normal epithelial uptake ratio. We report on the synthesis and on the photophys. properties of a m-THPC-like photosensitizer I conjugated to folic acid (compd. II). A comparative study of the accumulation of photosensitizers I and II is described. Nude mice were xenografted with FR-α-pos. KB or HT-29 cells lacking FR-α as a neg. control. Using optical fiber fluorimetry, we demonstrated that conjugate II exhibited enhanced accumulation in KB tumors compared to I 4 h after injection. No significant difference between KB and HT-29 tumors was obsd. in case of compd. I. Tumor-to-normal tissue ratio exhibited a very interesting selectivity for conjugate II (5:1) in KB tumors 4 h postinjection.

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28. 28

    Rogers, L.; Sergeeva, N. N.; Paszko, E.; Vaz, G. M.; Senge, M. O. Lead structures for applications in photodynamic therapy. 6. Temoporfin anti-inflammatory conjugates to target the tumor microenvironment for in vitro PDT. PLoS One 2015, 10, e0125372  DOI: 10.1371/journal.pone.0125372

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    There is no corresponding record for this reference.
29. 29

    Rezende, T. K. L.; Barbosa, H. P.; dos Santos, L. F.; Lima, K.; Alves de Matos, P.; Tsubone, T. M.; Gonçalves, R. R.; Ferrari, J. L. Upconversion rare earths nanomaterials applied to photodynamic therapy and bioimaging. Front. Chem. 2022, 10, 1035449,  DOI: 10.3389/fchem.2022.1035449

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    There is no corresponding record for this reference.
30. 30

    Kostiv, U.; Patsula, V.; Noculak, A.; Podhorodecki, A.; Větvička, D.; Poučková, P.; Sedláková, Z.; Horák, D. Phthalocyanine-conjugated upconversion NaYF₄:Yb³⁺/Er³⁺@SiO₂ nanospheres for NIR-triggered photodynamic therapy in a tumor mice model. ChemMedChem 2017, 12, 2066– 2073,  DOI: 10.1002/cmdc.201700508

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    30

    Phthalocyanine-conjugated upconversion NaYF4:Yb3+/Er3+@SiO2 nanospheres for NIR-triggered photodynamic therapy in a tumor mouse model

    Kostiv, Uliana; Patsula, Vitalii; Noculak, Agnieszka; Podhorodecki, Artur; Vetvicka, David; Pouckova, Pavla; Sedlakova, Zdenka; Horak, Daniel

    ChemMedChem (2017), 12 (24), 2066-2073CODEN: CHEMGX; ISSN:1860-7179. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Photodynamic therapy (PDT) has garnered immense attention as a minimally invasive clin. treatment modality for malignant cancers. However, its low penetration depth and photodamage of living tissues by UV and visible light, which activate a photosensitizer, limit the application of PDT. In this study, monodisperse NaYF4:Yb3+/Er3+ nanospheres 20 nm in diam., that serve as near-IR (NIR)-to-visible light converters and activators of a photosensitizer, were synthesized by high-temp. co-pptn. of lanthanide chlorides in a high-boiling org. solvent (octadec-1-ene). The nanoparticles were coated with a thin shell (≈3 nm) of homogenous silica via the hydrolysis and condensation of tetra-Me orthosilicate. The NaYF4:Yb3+/Er3+@SiO2 particles were further functionalized by methacrylate-terminated groups via 3-(trimethoxysilyl)propyl methacrylate. To introduce a large no. of reactive amino groups on the particle surface, methacrylate-terminated NaYF4:Yb3+/Er3+@SiO2 nanospheres were modified with a branched polyethyleneimine (PEI) via Michael addn. Aluminum carboxyphthalocyanine (Al Pc-COOH) was then conjugated to NaYF4:Yb3+/Er3+@SiO2-PEI nanospheres via carbodiimide chem. The resulting NaYF4:Yb3+/Er3+@SiO2-PEI-Pc particles were finally modified with succinimidyl ester of poly(ethylene glycol) (PEG) in order to alleviate their future uptake by the reticuloendothelial system. Upon 980 nm irradn., the intensive red emission of NaYF4:Yb3+/Er3+@SiO2-PEI-Pc-PEG nanoparticles completely vanished, indicating efficient energy transfer from the nanoparticles to Al Pc-COOH, which generates singlet oxygen (1O2). Last but not least, NaYF4:Yb3+/Er3+@SiO2-PEI-Pc-PEG nanospheres were intratumorally administered into mammary carcinoma MDA-MB-231 growing s.c. in athymic nude mice. Extensive necrosis developed at the tumor site of all mice 24-48 h after irradn. by laser at 980 nm wavelength. The results demonstrate that the NaYF4:Yb3+/Er3+@SiO2-PEI-Pc-PEG nanospheres have great potential as a novel NIR-triggered PDT nanoplatform for deep-tissue cancer therapy.

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31. 31

    Hamblin, M. R. Upconversion in photodynamic therapy: Plumbing the depths. Dalton Trans. 2018, 47, 8571– 8580,  DOI: 10.1039/C8DT00087E

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    31

    Upconversion in photodynamic therapy: plumbing the depths

    Hamblin, Michael R.

    Dalton Transactions (2018), 47 (26), 8571-8580CODEN: DTARAF; ISSN:1477-9226. (Royal Society of Chemistry)

    Photodynamic therapy (PDT) involves the combination of non-toxic dyes called photosensitizers (PS) and harmless visible light that interact with ambient oxygen to give reactive oxygen species (ROS) that can damage biomols. and kill cells. PDT has mostly been developed as a cancer therapy but can also be used as an antimicrobial approach against localized infections. However even the longest wavelength used for exciting PS (in the 700 nm region) has relatively poor tissue penetration, and many PS are much better excited by blue and green light. Therefore upconversion nanoparticles (UCNPs) have been investigated in order to allow deeper-penetrating near-IR light (980 nm or 810 nm) to be used for PDT. NaYF4 nanoparticles doped with Yb3+ and Er3+ or with Tm3+ and Er3+ have been attached to PS either by covalent conjugation, or by absorption to the coating or shell (used to render the UCNPs biocompatible). Forster resonance energy transfer to the PS then allows NIR light energy to be transduced into ROS leading to cell killing and tumor regression. Some studies have exptl. demonstrated the deep tissue advantage of UCNP-PDT. Recent advances have included dye-sensitized UCNPs and UCNPs coupled to PS, and other potentially synergistic drug mols. or techniques. A variety of bioimaging modalities have also been combined with upconversion PDT. Further studies are necessary to optimize the drug-delivery abilities of the UCNPs, improve the quantum yields, allow i.v. injection and tumor targeting, and ensure lack of toxicity at the required doses before potential clin. applications.

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32. 32

    Tsai, Y. C.; Vijayaraghavan, P.; Chiang, W. H.; Chen, H. H.; Liu, T. I.; Shen, M. Y.; Omoto, A.; Kamimura, M.; Soga, K.; Chiu, H. C. Targeted delivery of functionalized upconversion nanoparticles for externally triggered photothermal/photodynamic therapies of brain glioblastoma. Theranostics 2018, 8, 1435– 1448,  DOI: 10.7150/thno.22482

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    32

    Targeted delivery of functionalized upconversion nanoparticles for externally triggered photothermal/photodynamic therapies of brain glioblastoma

    Tsai, Yuan-Chung; Vijayaraghavan, Priya; Chiang, Wen-Hsuan; Chen, Hsin-Hung; Liu, Te-I.; Shen, Ming-Yin; Omoto, Ayumu; Kamimura, Masao; Soga, Kohei; Chiu, Hsin-Cheng

    Theranostics (2018), 8 (5), 1435-1448CODEN: THERDS; ISSN:1838-7640. (Ivyspring International Publisher)

    Therapeutic efficacy of glioblastoma multiforme (GBM) is often severely limited by poor penetration of therapeutics through blood-brain barrier (BBB) into brain tissues and lack of tumor targeting. In this regard, a functionalized upconversion nanoparticle (UCNP)-based delivery system which can target brain tumor and convert deep tissue-penetrating near-IR (NIR) light into visible light for precise phototherapies on brain tumor was developed in this work. Methods: The UCNP-based phototherapy delivery system was acquired by assembly of oleic acid-coated UCNPs with angiopep-2/cholesterol-conjugated poly(ethylene glycol) and the hydrophobic photosensitizers. The hybrid nanoparticles (ANG-IMNPs) were characterized by DLS, TEM, UV/vis and fluorescence spectrophotometer. Cellular uptake was examd. by laser scanning confocal microscopy and flow cytometry. The PDT/PTT effect of ANG-IMNPs was evaluated using MTT assay. Tumor accumulation of NPs was detd. by a non-invasive in vivo imaging system (IVIS). The in vivo anti-glioma effect of ANG-IMNPs was evaluated by immunohistochem. (IHC) examn. of tumor tissues and Kaplan-Meier survival anal. Results:In vitro data demonstrated enhanced uptake of ANG-IMNPs by murine astrocytoma cells (ALTS1C1) and pronounced cytotoxicity by combined NIR-triggered PDT and PTT. In consistence with the increased penetration of ANG-IMNPs through endothelial monolayer in vitro, the NPs have also shown significantly enhanced accumulation at brain tumor by IVIS. The IHC tissue examn. confirmed prominent apoptotic and necrotic effects on tumor cells in mice receiving targeted dual photo-based therapies, which also led to enhanced median survival (24 days) as compared to the NP treatment without angiopep-2 (14 days). Conclusion:In vitro and in vivo data strongly indicate that the ANG-IMNPs were capable of selectively delivering dual photosensitizers to brain astrocytoma tumors for effective PDT/PTT in conjugation with a substantially improved median survival. The therapeutic efficacy of ANG-IMNPs demonstrated in this study suggests their potential in overcoming BBB and establishing an effective treatment against GBM.

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33. 33

    Yu, Q.; Rodriguez, E. M.; Naccache, R.; Forgione, P.; Lamoureux, G.; Sanz-Rodriguez, F.; Scheglmann, D.; Capobianco, J. A. Chemical modification of temoporfin - a second generation photosensitizer activated using upconverting nanoparticles for singlet oxygen generation. Chem. Commun. 2014, 50, 12150– 12153,  DOI: 10.1039/C4CC05867D

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    Chemical modification of temoporfin - a second generation photosensitizer activated using upconverting nanoparticles for singlet oxygen generation

    Yu, Q.; Rodriguez, E. M.; Naccache, R.; Forgione, P.; Lamoureux, G.; Sanz-Rodriguez, F.; Scheglmann, D.; Capobianco, J. A.

    Chemical Communications (Cambridge, United Kingdom) (2014), 50 (81), 12150-12153CODEN: CHCOFS; ISSN:1359-7345. (Royal Society of Chemistry)

    LiYF4:Tm3+/Yb3+ upconverting nanoparticles (UCNPs) were functionalized with the second generation photosensitizer 5,10,15,20-tetra(m-hydroxyphenyl)chlorin (m-THPC, Temoporfin, Foscan). m-THPC was modified using 4-(bromomethyl)benzoic acid, which induced a bathochromic shift of the m-THPC blue absorption peak. The nanoconstruct causes up to 70% cell death under 980 nm irradn.

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34. 34

    Shapoval, O.; Větvička, D.; Patsula, V.; Engstová, H.; Kočková, O.; Konefał, M.; Kabešová, M.; Horák, D. Temoporfin-conjugated upconversion nanoparticles for NIR-induced photodynamic therapy: Studies with pancreatic adenocarcinoma cells in vitro and in vivo. Pharmaceutics 2023, 15, 2694,  DOI: 10.3390/pharmaceutics15122694

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35. 35

    Reschel, T.; Koňák, Č.; Oupický, D.; Seymour, L. W.; Ulbrich, K. Physical properties and in vitro transfection efficiency of gene delivery vectors based on complexes of DNA with synthetic polycations. J. Control. Release 2002, 81, 201– 217,  DOI: 10.1016/s0168-3659(02)00045-7

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36. 36

    Colombo, C.; Monhemius, A. J.; Plant, J. A. Platinum, palladium and rhodium release from vehicle exhaust catalysts and road dust exposed to simulated lung fluids. Ecotoxicol. Environ. Saf. 2008, 71, 722– 730,  DOI: 10.1016/j.ecoenv.2007.11.011

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    36

    Platinum, palladium and rhodium release from vehicle exhaust catalysts and road dust exposed to simulated lung fluids

    Colombo, Claudia; Monhemius, A. John; Plant, Jane A.

    Ecotoxicology and Environmental Safety (2008), 71 (3), 722-730CODEN: EESADV; ISSN:0147-6513. (Elsevier B.V.)

    The risk assocd. with the inhalation of platinum group element (PGE) emissions from vehicle exhaust catalysts (VECs) has been investigated by extg. road dust and milled auto catalyst with simulated lung fluids. Gamble's soln. (representative of the interstitial fluid of the deep lung) and artificial lysosomal fluid (ALF) (representative of the more acidic environment within the lung) were employed as extn. fluids. The highest PGE release was obsd. in ALF, implying that inhaled particles would have to be phagocytized before significant amts. of PGEs dissolve. The greatest percentage (up to 88%) of PGEs was released from road dust, possibly due to the presence of mobile PGE species formed in the roadside environment. Pt showed the highest abs. bioavailability, due to its greater concn. in the environmental samples. Pd and Rh had higher percentage of release, however, because of their more sol. nature. From the toxicol. perspective, the results demonstrate potential health risks due to the likely formation of PGE-chloride complexes in the respiratory tract, such species having well-known toxic and allergenic effects on human beings and living organisms.

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    Freinbichler, W.; Tipton, K. F.; Corte, L. D.; Linert, W. Mechanistic aspects of the Fenton reaction under conditions approximated to the extracellular fluid. J. Inorg. Biochem. 2009, 103, 28– 34,  DOI: 10.1016/j.jinorgbio.2008.08.014

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    Shapoval, O.; Brandmeier, J. C.; Nahorniak, M.; Oleksa, V.; Makhneva, E.; Gorris, H. H.; Farka, Z.; Horák, D. PMVEMA-coated upconverting nanoparticles for upconversion-linked immunoassay of cardiac troponin. Talanta 2022, 244, 123400,  DOI: 10.1016/j.talanta.2022.123400

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    There is no corresponding record for this reference.
39. 39

    Shapoval, O.; Sulimenko, V.; Klebanovych, A.; Rabyk, M.; Shapoval, P.; Kaman, O.; Rydvalová, E.; Filipová, M.; Dráberová, E.; Dráber, P.; Horák, D. Multimodal fluorescently labeled polymer-coated GdF₃ nanoparticles inhibit degranulation in mast cells. Nanoscale 2021, 13, 19023– 19037,  DOI: 10.1039/D1NR06127E

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    Luo, X.; Chen, Q.; Guo, H.; Zhang, H.; He, X.; Zhao, W. One-step hydrothermal synthesis of Cit-NaYbF₄:Er³⁺ nanocrystals with enhanced red upconversion emission for in vivo fluorescence molecular tomography. J. Rare Earths 2024, 42, 36– 45,  DOI: 10.1016/j.jre.2022.09.027

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    Gregori, M.; Bertani, D.; Cazzaniga, E.; Orlando, A.; Mauri, M.; Bianchi, A.; Re, F.; Sesana, S.; Minniti, S.; Francolini, M.; Cagnotto, A.; Salmona, M.; Nardo, L.; Salerno, D.; Mantegazza, F.; Masserini, M.; Simonutti, R. Investigation of functionalized poly(N,N-dimethylacrylamide)-block-polystyrene nanoparticles as novel drug delivery system to overcome the blood-brain barrier in vitro. Macromol. Biosci. 2015, 15, 1687– 1697,  DOI: 10.1002/mabi.201500172

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    Gualdesi, M. S.; Vara, J.; Aiassa, V.; Alvarez Igarzabal, C. I.; Ortiz, C. S. New poly(acrylamide) nanoparticles in the development of third generation photosensitizers. Dyes Pigments 2021, 184, 108856,  DOI: 10.1016/j.dyepig.2020.108856

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    New poly(acrylamide) nanoparticles in the development of third generation photosensitizers

    Gualdesi, M. S.; Vara, J.; Aiassa, V.; Alvarez Igarzabal, C. I.; Ortiz, C. S.

    Dyes and Pigments (2021), 184 (), 108856CODEN: DYPIDX; ISSN:0143-7208. (Elsevier Ltd.)

    There are promising data on the use of poly(acrylamide) nanoparticles (PAA-NPs) in the development of third generation photosensitizers for application in antimicrobial photodynamic therapy. These nanoparticle delivery systems are suitable for biol. applications and have potential for drug delivery due to their biocompatibility, chem. flexibility, easy prepn. and low cost. The objective of this work was to obtain new PAA-NPs for the vehiculization of the monobrominated derivs. of Azure B (AzBBr) and Neutral Red (NRBr). These two dyes were found to have promising properties as photosensitizers. However, the use of nanotechnol. was required to overcome difficulties in soly., aggregation and stability in order to optimize their photodynamic efficiency. The combination of different monomers and crosslinkers allowed us to develop two new PAA-NPs. These systems were loaded with AzBBr and NRBr and characterized according to their morphol., size, polydispersity index and zeta potential. The new third generation photosensitizers showed better photochem. reactivity, chem. stability and photodynamic efficacy against Gram-pos. and Gram-neg. bacteria than the free photosensitizers. The use of this vehiculization strategy improved the properties of the second generation photosensitizers (AzBBr and NRBr) studied. This improvement in their properties makes them good candidates for potential phototherapeutic applications against numerous pathologies.

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    Borah, B. M.; Cacaccio, J.; Watson, R.; Pandey, R. K. Phototriggered release of tumor-imaging and therapy agents from lyophilized multifunctional polyacrylamide nanoparticles. ACS Appl. Bio Mater. 2019, 2, 5663– 5675,  DOI: 10.1021/acsabm.9b00741

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    Awar, A. A.; Codd, M.; Pratt, N.; Scott, R. M. Involvement of amine protons in n-butylamine-cresol hydrogen bonding. J. Phys. Chem. 1983, 87, 1188– 1191,  DOI: 10.1021/j100230a019

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    Quiñones Vélez, G.; Carmona-Sarabia, L.; Rodríguez-Silva, W. A.; Rivera Raíces, A. A.; Feliciano-Cruz, L.; Hu, T.; Peterson, E. A.; Lopez-Mejias, V. Potentiating bisphosphonate-based coordination complexes to treat osteolytic metastases. J. Mater. Chem. B 2020, 8, 2155– 2168,  DOI: 10.1039/c9tb01857c

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    Potentiating bisphosphonate-based coordination complexes to treat osteolytic metastases

    Quinones Velez, Gabriel; Carmona-Sarabia, Lesly; Rodriguez-Silva, Waldemar A.; Rivera Raices, Alondra A.; Feliciano Cruz, Lorraine; Hu, Tony; Peterson, Esther; Lopez-Mejias, Vilmali

    Journal of Materials Chemistry B: Materials for Biology and Medicine (2020), 8 (10), 2155-2168CODEN: JMCBDV; ISSN:2050-7518. (Royal Society of Chemistry)

    The hydrothermal reaction between bioactive metal (Ca2+, Zn2+, and Mg2+) salts and a clin. utilized bisphosphonate, alendronate (ALEN), promotes the formation of several materials denominated as bisphosphonate-based coordination complexes (BPCCs). The systematic exploration of the effect of three variables, M2+/ALEN molar ratio, temp., and pH, on the reaction yielded an unprecedented no. of materials of enough crystal quality for structural elucidation. Five crystal structures were unveiled by single crystal X-ray diffraction (ALEN-Ca forms I and II, ALEN-Zn forms I and II, and ALEN-Mg) and their solid-state properties revealed in tandem with other techniques. The dissoln. of these BPCCs was tested and contrasted to that of the com. employed generic form of Fosamax Alendronate Sodium, using fasted-state simulated gastric fluid and phosphate-buffered saline soln. Quantification of ALEN content was performed by derivatization with Cu2+, which produced a sol. complex suitable for quantification. The results show that these materials present a pH-dependent degrdn. Moreover, a phase inversion temp. (PIT) nano-emulsion method was applied to the synthesis of ALEN-Ca form II. Size distribution anal. demonstrated the efficiency of the PIT-nano-emulsion method to decrease the particle size of this BPCC from ∼60 μm to ∼438 d nm. The cytotoxicity of ALEN, ALEN-Ca form II (bulk crystals), and nano-Ca@ALEN (nanocrystals) against the MDA-MB-231 cell line was investigated. Nano-Ca@ALEN form II presents higher cytotoxicity effects than ALEN and ALEN-Ca form II (bulk crystals), showing inhibition of cell proliferation at 7.5 μM. These results provide evidence of the structure, stability, dissoln. and cytotoxicity properties of ALEN-based BPCCs and pave the way for better formulation strategies for this drug through the design of nano-sized BPCCs for the treatment of bone-related diseases.

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46. 46

    Kostiv, U.; Janoušková, O.; Šlouf, M.; Kotov, N.; Engstová, H.; Smolková, K.; Ježek, P.; Horák, D. Silica-modified monodisperse hexagonal lanthanide nanocrystals: Synthesis and biological properties. Nanoscale 2015, 7, 18096– 18104,  DOI: 10.1039/C5NR05572E

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    Silica-modified monodisperse hexagonal lanthanide nanocrystals: synthesis and biological properties

    Kostiv, U.; Janouskova, O.; Slouf, M.; Kotov, N.; Engstova, H.; Smolkova, K.; Jezek, P.; Horak, D.

    Nanoscale (2015), 7 (43), 18096-18104CODEN: NANOHL; ISSN:2040-3372. (Royal Society of Chemistry)

    Oleic acid-stabilized hexagonal NaYF4:Yb3+/Er3+ nanocrystals, emitting green and red luminescence, were prepd. by the high-temp. co-pptn. of lanthanide chlorides. By varying the reaction time and the Ln3+/Na+ ratio, the nanocrystal size can be controlled within the range 16-270 nm. The max. upconversion quantum yield is achieved under 970 nm excitation. The reverse microemulsion technique using hydrolysis and condensation of tetraethoxysilane is a suitable method to coat the nanocrystal surface with a silica shell to make the particles dispersible and colloidally stable in aq. media. During the subsequent functionalization, (3-aminopropyl)trimethoxysilane introduced amino groups onto the silica to enable future bioconjugation with the target mols. All specimens were characterized by TEM microscopy, electron and X-ray diffraction, ATR FT-IR spectroscopy, and upconversion luminescence. Finally, in vitro cytotoxicity and intracellular nanoparticle uptake (using confocal microscopy) were detd. with human cervical carcinoma HeLa and mRoGFP HeLa cells, resp. From the investigated particles, amino-functionalized NaYF4:Yb3+/Er3+ nanocrystals internalized into the cells most efficiently. The nanoparticles proved to be nontoxic at moderate concns., which is important when considering their prospective application in biolabeling and luminescence imaging of various cell types.

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47. 47

    Patsula, V.; Mareková, D.; Jendelová, P.; Nahorniak, M.; Shapoval, O.; Matouš, P.; Oleksa, V.; Konefał, R.; Vosmanská, M.; Machová-Urdziková, L.; Horák, D. Polymer-coated hexagonal upconverting nanoparticles: Chemical stability and cytotoxicity. Front. Chem. 2023, 11, 1207984,  DOI: 10.3389/fchem.2023.1207984

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    Kostiv, U.; Kučka, J.; Lobaz, V.; Kotov, N.; Janoušková, O.; Šlouf, M.; Krajnik, B.; Podhorodecki, A.; Francová, P.; Šefc, L.; Jirák, D.; Horák, D. Highly colloidally stable trimodal ¹²⁵I-radiolabeled PEG-neridronate-coated upconversion/magnetic bioimaging nanoprobes. Sci. Rep. 2020, 10, 20016,  DOI: 10.1038/s41598-020-77112-z

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    Highly colloidally stable trimodal 125I-radiolabeled PEG-neridronate-coated upconversion/magnetic bioimaging nanoprobes

    Kostiv, Uliana; Kucka, Jan; Lobaz, Volodymyr; Kotov, Nikolay; Janouskova, Olga; Slouf, Miroslav; Krajnik, Bartosz; Podhorodecki, Artur; Francova, Pavla; Sefc, Ludek; Jirak, Daniel; Horak, Daniel

    Scientific Reports (2020), 10 (1), 20016CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)

    "All-in-one" multifunctional nanomaterials, which can be visualized simultaneously by several imaging techniques, are required for the efficient diagnosis and treatment of many serious diseases. This report addresses the design and synthesis of upconversion magnetic NaGdF4:Yb3+/Er3+(Tm3+) nanoparticles by an oleic acid-stabilized high-temp. copptn. of lanthanide precursors in octadec-1-ene. The nanoparticles, which emit visible or UV light under near-IR (NIR) irradn., were modified by inhouse synthesized PEG-neridronate to facilitate their dispersibility and colloidal stability in water and bioanalytically relevant phosphate buffered saline (PBS). The cytotoxicity of the nanoparticles was detd. using HeLa cells and human fibroblasts (HF). Subsequently, the particles were modified by Bolton-Hunter-neridronate and radiolabeled by 125I to monitor their biodistribution in mice using single-photon emission computed tomog. (SPECT). The upconversion and the paramagnetic properties of the NaGdF4:Yb3+/Er3+(Tm3+)@PEG nanoparticles were evaluated by photoluminescence, magnetic resonance (MR) relaxometry, and magnetic resonance imaging (MRI) with 1 T and 4.7 T preclin. scanners. MRI data were obtained on phantoms with different particle concns. and during pilot long-time in vivo observations of a mouse model. The biol. and physicochem. properties of the NaGdF4:Yb3+/Er3+(Tm3+) @PEG nanoparticles make them promising as a trimodal optical/MRI/SPECT bioimaging and theranostic nanoprobe for exptl. medicine.

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    Hanana, H.; Turcotte, P.; Dubé, M.; Gagnon, C.; Gagné, F. Response of the freshwater mussel, Dreissena polymorpha to sub-lethal concentrations of samarium and yttrium after chronic exposure. Ecotoxicol. Environ. Saf. 2018, 165, 662– 670,  DOI: 10.1016/j.ecoenv.2018.09.047

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    Andresen, E.; Würth, C.; Prinz, C.; Michaelis, M.; Resch-Genger, U. Time-resolved luminescence spectroscopy for monitoring the stability and dissolution behaviour of upconverting nanocrystals with different surface coatings. Nanoscale 2020, 12, 12589– 12601,  DOI: 10.1039/D0NR02931A

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    Lisjak, D.; Plohl, O.; Vidmar, J.; Majaron, B.; Ponikvar-Svet, M. Dissolution mechanism of upconverting AYF₄:Yb,Tm (A = Na or K) nanoparticles in aqueous media. Langmuir 2016, 32, 8222– 8229,  DOI: 10.1021/acs.langmuir.6b02675

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    51

    Dissolution Mechanism of Upconverting AYF4:Yb,Tm (A = Na or K) Nanoparticles in Aqueous Media

    Lisjak, Darja; Plohl, Olivija; Vidmar, Janja; Majaron, Boris; Ponikvar-Svet, Maja

    Langmuir (2016), 32 (32), 8222-8229CODEN: LANGD5; ISSN:0743-7463. (American Chemical Society)

    The dissoln. of upconverting AYF4:Yb,Tm (A = Na or K) nanoparticles (UCNPs) in aq. media was systematically studied. UCNPs with a cubic structure and sizes of between 10 and 33 nm were synthesized solvothermally in ethylene glycol at 200°. The UCNPs of both compns. showed an upconversion fluorescence emission characteristic of Tm3+. The effects of the A cation, the particle size, the temp., the pH, and the compn. of the aq. medium on the dissoln. of the UCNPs were evaluated. The degree of dissoln. was detd. from the fraction of dissolved fluoride (F-) using potentiometry. Unexpectedly, the compn. of aq. media had the most significant effect on the dissoln. of the UCNPs. The highest degree of dissoln. and rate were measured for the phosphate-buffered saline (PBS), which can be explained by the formation of stable lanthanide compds. with phosphates. The degree of dissoln. was much lower in water and in the phthalate buffer, which was attributed to the release of F- as a result of the hydrolysis of the UCNPs' surfaces.

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    Nahorniak, M.; Patsula, V.; Mareková, D.; Matouš, P.; Shapoval, O.; Oleksa, V.; Vosmanská, M.; Machová Urdzíková, L.; Jendelová, P.; Herynek, V.; Horák, D. Chemical and colloidal stability of polymer-coated NaYF₄:Yb,Er nanoparticles in aqueous media and viability of cells: The effect of a protective coating. Int. J. Mol. Sci. 2023, 24, 2724,  DOI: 10.3390/ijms24032724

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53. 53

    Saleh, M. I.; Rühle, B.; Wang, S.; Radnik, J.; You, Y.; Resch-Genger, U. Assessing the protective effects of different surface coatings on NaYF₄:Yb³⁺, Er³⁺ upconverting nanoparticles in buffer and DMEM. Sci. Rep. 2020, 10, 19318,  DOI: 10.1038/s41598-020-76116-z

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    53

    Assessing the protective effects of different surface coatings on NaYF4:Yb3+, Er3+ upconverting nanoparticles in buffer and DMEM

    Saleh, Maysoon I.; Ruehle, Bastian; Wang, Shu; Radnik, Joerg; You, Yi; Resch-Genger, Ute

    Scientific Reports (2020), 10 (1), 19318CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)

    We studied the dissoln. behavior of βNaYF4:Yb(20%), Er(2%) UCNP of two different sizes in biol. relevant media i.e., water (neutral pH), phosphate buffered saline (PBS), and Dulbecco ' s modified Eagle medium (DMEM) at different temps. and particle concns. Special emphasis was dedicated to assess the influence of different surface functionalizations, particularly the potential of mesoporous and microporous silica shells of different thicknesses for UCNP stabilization and protection. Dissoln. was quantified electrochem. using a fluoride ion selective electrode (ISE) and by inductively coupled plasma optical emission spectrometry (ICP OES). In addn., dissoln. was monitored fluorometrically. These expts. revealed that a thick microporous silica shell drastically decreased dissoln. Our results also underline the crit. influence of the chem. compn. of the aq. environment on UCNP dissoln. In DMEM, we obsd. the formation of a layer of adsorbed mols. on the UCNP surface that protected the UCNP from dissoln. and enhanced their fluorescence. Examn. of this layer by XPS and mass spectrometry (MS) suggested that mainly phenylalanine, lysine, and glucose are adsorbed from DMEM. These findings should be considered in the future for cellular toxicity studies with UCNP and other nanoparticles and the design of new biocompatible surface coatings.

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    Firsching, F. H.; Brune, S. N. Solubility products of the trivalent rare-earth phosphates. J. Chem. Eng. Data 1991, 36, 93– 95,  DOI: 10.1021/je00001a028

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    Solubility products of the trivalent rare-earth phosphates

    Firsching, F. Henry; Brune, Stephen N.

    Journal of Chemical and Engineering Data (1991), 36 (1), 93-5CODEN: JCEAAX; ISSN:0021-9568.

    The soly. and soly. products of 14 rare-earth phosphates in aq. soln. were detd. at 25 ± 1°. The most sol. compd. is Y phosphate (pK = 24.76). The least sol. ones are La phosphate (pK = 26.15) and Yb phosphate (pK = 26.17). The rare earth phosphates were prepd. by pptn. from homogeneous soln. Satd. solns. were analyzed for pH, the concns. of some rare-earth cations and the total concn. of phosphate. Activity products were calcd. from the exptl. data. The solubilities of the rare earth phosphates are so low that the soly. products and the activity products essentially have the same value. The rare earth phosphates are more insol. at higher temps. Lanthanum phosphate has a pK of 26.49 at 70°. Twelve values for the activity product of rare earth phosphates at elevated temps. were detd.

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    Boyer, J. C.; Manseau, M. P.; Murray, J. I.; van Veggel, F. C. J. M. Surface modification of upconverting NaYF₄ nanoparticles with PEG-phosphate ligands for NIR (800 nm) biolabeling within the biological window. Langmuir 2010, 26, 1157– 1164,  DOI: 10.1021/la902260j

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    Surface Modification of Upconverting NaYF4 Nanoparticles with PEG-Phosphate Ligands for NIR (800 nm) Biolabeling within the Biological Window

    Boyer, John-Christopher; Manseau, Marie-Pascale; Murray, Jill I.; van Veggel, Frank C. J. M.

    Langmuir (2010), 26 (2), 1157-1164CODEN: LANGD5; ISSN:0743-7463. (American Chemical Society)

    The authors present a technique for the replacement of oleate with a PEG-phosphate ligand [PEG = poly(ethylene glycol)] as an efficient method for the generation of water-dispersible NaYF4 nanoparticles (NPs). The PEG-phosphate ligands are shown to exchange with the original oleate ligands on the surface of the NPs, resulting in water-dispersible NPs. The upconversion intensity of the NPs in aq. environments was severely quenched when compared to the original NPs in org. solvents. This is attributed to an increase in the multiphonon relaxations of the lanthanide excited state in aq. environments due to high energy vibrational modes of water mols. This problem could be overcome partially by the synthesis of core/shell NPs which demonstrated improved photophys. properties in water over the original core NPs. The PEG-phosphate coated upconverting NPs were then used to image a line of ovarian cancer cells (CaOV3) to demonstrate their promise in biol. application.

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    Hu, P.; Wu, T.; Fan, W.; Chen, L.; Liu, Y.; Ni, D.; Bu, W.; Shi, J. Near infrared-assisted Fenton reaction for tumor-specific and mitochondrial DNA-targeted photochemotherapy. Biomaterials 2017, 141, 86– 95,  DOI: 10.1016/j.biomaterials.2017.06.035

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    Near infrared-assisted Fenton reaction for tumor-specific and mitochondrial DNA-targeted photochemotherapy

    Hu, Ping; Wu, Tong; Fan, Wenpei; Chen, Lei; Liu, Yanyan; Ni, Dalong; Bu, Wenbo; Shi, Jianlin

    Biomaterials (2017), 141 (), 86-95CODEN: BIMADU; ISSN:0142-9612. (Elsevier Ltd.)

    The strong dependence on oxygen level, low UV/visible (UV/vis) light penetration depth and the extremely short lifetime of reactive oxygen species (ROS) are the major challenges of photodynamic therapy (PDT) for tumors. Fenton reaction can produce abundant ROS such as reactive hydroxyl radicals (·OH) with significantly higher oxidn. performance than singlet oxygen (1O2), which, however, has been rarely used in biomedical fields due to strict reaction conditions (favorably in pH range of 3-4, mostly under UV/vis light catalysis). Herein we propose and demonstrate a photochemotherapy (PCT) strategy of cancer therapy using near-IR (NIR)-assisted tumor-specific Fenton reactions. NIR light-upconverted UV/vis light by upconversion nanoparticles (UCNPs) catalyze the intra-mitochondrial Fenton reaction between the delivered Fe2+ and H2O2 species over-expressed in cancer cell's mitochondria to in-situ kill the cancer cells. The intra-mitochondrial ROS generation of enabled by directly targeting the mitochondrial DNA (mtDNA) helix minimized the distance between the ROS and mtDNA mols., thus the present PCT strategy showed much enhanced and tumor-specific therapeutic efficacy, as demonstrated by the intratumoral-accelerated ·OH burst and elevated cytotoxicity. Following the direct intratumoral injection, the PCT revealed marked tumor regression effect in vivo. This constructed PCT-agent is the first paradigm of NIR-upconversion catalyzed intra-mitochondrial Fenton reaction in response to tumoral microenvironment, establishing a novel photochemotherapy strategy for efficient cancer therapy.

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    Larue, L.; Myrzakhmetov, B.; Ben-Mihoub, A.; Moussaron, A.; Thomas, N.; Arnoux, P.; Baros, F.; Vanderesse, R.; Acherar, S.; Frochot, C. Fighting hypoxia to improve PDT. Pharmaceuticals 2019, 12, 163,  DOI: 10.3390/ph12040163

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    Fighting hypoxia to improve PDT

    Larue, Ludivine; Myrzakhmetov, Bauyrzhan; Ben-Mihoub, Amina; Moussaron, Albert; Thomas, Noemie; Arnoux, Philippe; Baros, Francis; Vanderesse, Regis; Acherar, Samir; Frochot, Celine

    Pharmaceuticals (2019), 12 (4), 163CODEN: PHARH2; ISSN:1424-8247. (MDPI AG)

    A review. Photodynamic therapy (PDT) has drawn great interest in recent years mainly due to its low side effects and few drug resistances. Nevertheless, one of the issues of PDT is the need for oxygen to induce a photodynamic effect. Tumors often have low oxygen concns., related to the abnormal structure of the microvessels leading to an ineffective blood distribution. Moreover, PDT consumes O2. In order to improve the oxygenation of tumor or decrease hypoxia, different strategies are developed and are described in this review: (1) The use of O2 vehicle; (2) the modification of the tumor microenvironment (TME); (3) combining other therapies with PDT; (4) hypoxia-independent PDT; (5) hypoxia-dependent PDT and (6) fractional PDT.

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    Friedmann Angeli, J. P.; Krysko, D. V.; Conrad, M. Ferroptosis at the crossroads of cancer-acquired drug resistance and immune evasion. Nat. Rev. Cancer 2019, 19, 405– 414,  DOI: 10.1038/s41568-019-0149-1

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    Ferroptosis at the crossroads of cancer-acquired drug resistance and immune evasion

    Friedmann Angeli, Jose Pedro; Krysko, Dmitri V.; Conrad, Marcus

    Nature Reviews Cancer (2019), 19 (7), 405-414CODEN: NRCAC4; ISSN:1474-175X. (Nature Research)

    Ferroptosis is a recently recognized cell death modality that is morphol., biochem. and genetically distinct from other forms of cell death and that has emerged to play an important role in cancer biol. Recent discoveries have highlighted the metabolic plasticity of cancer cells and have provided intriguing insights into how metabolic rewiring is a crit. event for the persistence, dedifferentiation and expansion of cancer cells. In some cases, this metabolic reprogramming has been linked to an acquired sensitivity to ferroptosis, thus opening up new opportunities to treat therapy-insensitive tumors. However, it is not yet clear what metabolic determinants are crit. for therapeutic resistance and evasion of immune surveillance. Therefore, a better understanding of the processes that regulate ferroptosis sensitivity should ultimately aid in the discovery of novel therapeutic strategies to improve cancer treatment. In this Perspectives article, we provide an overview of the known mechanisms that regulate sensitivity to ferroptosis in cancer cells and how the modulation of metabolic pathways controlling ferroptosis might reshape the tumor niche, leading to an immunosuppressive microenvironment that promotes tumor growth and progression.

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    Chu, H.; Cao, T.; Dai, G.; Liu, B.; Duan, H.; Kong, C.; Tian, N.; Hou, D.; Sun, Z. Recent advances in functionalized upconversion nanoparticles for light-activated tumor therapy. RSC Adv. 2021, 11, 35472– 35488,  DOI: 10.1039/D1RA05638G

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    Recent advances in functionalized upconversion nanoparticles for light-activated tumor therapy

    Chu, Hongqian; Cao, Tingming; Dai, Guangming; Liu, Bei; Duan, Huijuan; Kong, Chengcheng; Tian, Na; Hou, Dailun; Sun, Zhaogang

    RSC Advances (2021), 11 (56), 35472-35488CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)

    A review. Upconversion nanoparticles (UCNPs) are a class of optical nanocrystals doped with lanthanide ions that offer great promise for applications in controllable tumor therapy. In recent years, UCNPs have become an important tool for studying the treatment of various malignant and nonmalignant cutaneous diseases. UCNPs convert near-IR (NIR) radiation into shorter-wavelength visible and UV radiation, which is much better than conventional UV activated tumor therapy as strong UV-light can be damaging to healthy surrounding tissue. Moreover, UV light generally does not penetrate deeply into the skin, an issue that UCNPs can now address. However, the current studies are still in the early stage of research, with a long way to go before clin. implementation. In this paper, we systematically analyzed recent advances in light-activated tumor therapy using functionalized UCNPs. We summarized the purpose and mechanism of UCNP-based photodynamic therapy (PDT), gene therapy, immunotherapy, chemo-therapy and integrated therapy. We believe the creation of functional materials based on UCNPs will offer superior performance and enable innovative applications, increasing the scope and opportunities for cancer therapy in the future.

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    Chen, C. W.; Chan, Y. C.; Hsiao, M.; Liu, R. S. Plasmon-enhanced photodynamic cancer therapy by upconversion nanoparticles conjugated with Au nanorods. ACS Appl. Mater. Interfaces 2016, 8, 32108– 32119,  DOI: 10.1021/acsami.6b07770

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    Plasmon-Enhanced Photodynamic Cancer Therapy by Upconversion Nanoparticles Conjugated with Au Nanorods

    Chen, Chieh-Wei; Chan, Yung-Chieh; Hsiao, Michael; Liu, Ru-Shi

    ACS Applied Materials & Interfaces (2016), 8 (47), 32108-32119CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)

    Photodynamic therapy (PDT) based on photosensitizers (PSs) constructed with nanomaterials has been widely applied to treat cancer. This therapy is characterized by an improved PS accumulation in tumor regions. However, challenges, such as short penetration depth of light and low extinction coeff. of PSs, limit PDT applications. In this study, a nanocomposite consisting of NaYF4:Yb/Er upconversion nanoparticles (UCPs) conjugated with gold nanorods (Au NRs) was developed to improve the therapeutic efficiency of PDT. Methylene blue (MB) was embedded in a silica shell for plasmon-enhanced PDT. UCPs served as a light converter from near-IR (NIR) to visible light to excite MB to generate reactive oxygen species (ROS). Au NRs could effectively enhance upconversion efficiency and ROS content through a localized surface plasmon resonance (SPR) effect. Silica shell thickness was adjusted to investigate the optimized MB loading amt., ROS prodn. capability, and efficient distance for plasmon-enhanced ROS prodn. The mechanism of plasmon-enhanced PDT was verified by enhancing UC luminescence intensity through the plasmonic field and by increasing the light-harvesting capability and absorption cross section of the system. This process improved the ROS generation by comparing the exchange of Au NRs to Au nanoparticles with different SPR bands. NIR-triggered nanocomposites of UCP@SiO2:MB-NRs were significantly confirmed by improving ROS generation and further modifying folic acid (FA) to develop an active component targeting OECM-1 oral cancer cells. Consequently, UCP@SiO2:MB-NRs-FA could highly produce ROS and undergo efficient PDT in vitro and in vivo. The mechanism of PDT treatment by UCP@SiO2:MB-NRs-FA was evaluated via the cell apoptosis pathway. The proposed process is a promising strategy to enhance ROS prodn. through plasmonic field enhancement and thus achieve high PDT therapeutic efficacy.

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    Zhou, A.; Wei, Y.; Chen, Q.; Xing, D. In vivo near-infrared photodynamic therapy based on targeted upconversion nanoparticles. J. Biomed. Nanotechnol. 2015, 11, 2003– 2010,  DOI: 10.1166/jbn.2015.2150

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62. 62

    Sharma, K. S.; Dubey, A. K.; Kumar, C.; Phadnis, P. P.; Sudarsan, V.; Vatsa, R. K. Mesoporous silica-coated upconversion nanoparticles assisted photodynamic therapy using 5-aminolevulinic acid: Mechanistic and in vivo studies. ACS Appl. Bio Mater. 2022, 5, 583– 597,  DOI: 10.1021/acsabm.1c01074

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    There is no corresponding record for this reference.
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    Punjabi, A.; Wu, X.; Tokatli-Apollon, A.; El-Rifai, M.; Lee, H.; Zhang, Y.; Wang, C.; Liu, Z.; Chan, E. M.; Duan, C.; Han, G. Amplifying the red-emission of upconverting nanoparticles for biocompatible clinically used prodrug-induced photodynamic therapy. ACS Nano 2014, 8, 10621– 10630,  DOI: 10.1021/nn505051d

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    Amplifying the Red-Emission of Upconverting Nanoparticles for Biocompatible Clinically Used Prodrug-Induced Photodynamic Therapy

    Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira; El-Rifai, Mahmoud; Lee, Hyungseok; Zhang, Yuanwei; Wang, Chao; Liu, Zhuang; Chan, Emory M.; Duan, Chunying; Han, Gang

    ACS Nano (2014), 8 (10), 10621-10630CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high abs. upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clin. used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power d. Furthermore, we show that our UCNP-PDT system with NIR irradn. outperforms clin. used red light irradn. in a deep tumor setting in vivo. This study marks a major step forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors. It also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.

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64. 64

    Wang, C.; Tao, H.; Cheng, L.; Liu, Z. Near-infrared light induced in vivo photodynamic therapy of cancer based on upconversion nanoparticles. Biomaterials 2011, 32, 6145– 6154,  DOI: 10.1016/j.biomaterials.2011.05.007

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    64

    Near-infrared light induced in vivo photodynamic therapy of cancer based on upconversion nanoparticles

    Wang, Chao; Tao, Huiquan; Cheng, Liang; Liu, Zhuang

    Biomaterials (2011), 32 (26), 6145-6154CODEN: BIMADU; ISSN:0142-9612. (Elsevier Ltd.)

    Upconversion nanoparticles (UCNPs) that emit high-energy photons upon excitation by the low-energy near-IR (NIR) light are emerging as new optical nano-probes useful in biomedicine. Herein, we load Chlorin e6 (Ce6), a photosensitizer, on polymer-coated UCNPs, forming a UCNP-Ce6 supramol. complex that produces singlet oxygen to kill cancer cells under NIR light. Excellent photodynamic therapy (PDT) efficacy is achieved in tumor-bearing mice upon intratumoral injection of UCNP-Ce6 and the followed NIR light exposure. It is further uncovered that UCNPs after PDT treatment are gradually cleared out from mouse organs, without rendering appreciable toxicity to the treated animals. Moreover, we demonstrate that the NIR-induced PDT based on UCNP-Ce6 exhibits a remarkably increased tissue penetration depth compared to the traditional PDT using visible excitation light, offering significantly improved treatment efficacy for tumors blocked by thick biol. tissues. Our work demonstrates NIR light-induced in vivo PDT treatment of cancer in animals, and highlights the promise of UCNPs for multifunctional in vivo cancer treatment and imaging.

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    Yang, S.; Li, N.; Liu, Z.; Sha, W.; Chen, D.; Xu, Q.; Lu, J. Amphiphilic copolymer coated upconversion nanoparticles for near-infrared light-triggered dual anticancer treatment. Nanoscale 2014, 6, 14903– 14910,  DOI: 10.1039/C4NR05305B

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    Amphiphilic copolymer coated upconversion nanoparticles for near-infrared light-triggered dual anticancer treatment

    Yang, Shun; Li, Najun; Liu, Zhuang; Sha, Wenwei; Chen, Dongyun; Xu, Qingfeng; Lu, Jianmei

    Nanoscale (2014), 6 (24), 14903-14910CODEN: NANOHL; ISSN:2040-3372. (Royal Society of Chemistry)

    The light-triggered controlled release of anticancer drugs accompanied with NIR-responsive photodynamic therapy was prepd. via a self-assembly process. Firstly, Mn2+-doped upconversion nanoparticles (UCNPs) were coated with a mesoporous silica shell and modified with photosensitizer (Chlorin e6) and long alkyl chains. And then the NIR light-responsive amphiphilic copolymer contg. 9,10-dialkoxyanthracene groups was synthesized and then coated as the outermost layer. Upon irradn. with a 980 nm laser, the CCUCNPs@PM would absorb and then convert the NIR light to higher-energy visible red light (660 nm) via the UCNPs-based core, which could excite Chlorin e6 (Ce-6) to produce singlet oxygen (1O2). Then the 1O2-sensitive dialkoxyanthracene group in the amphiphilic copolymer would be degraded and detach from the surface of the CCUCNPs@PM, followed by the controlled release of the pre-loaded drugs and the photodynamic therapy for cancer cells caused by the excess 1O2. In vitro and in vivo expts. also demonstrated that the drug-loaded CCUCNPs@PM possessed better therapeutic efficacy compared with vacant ones. Therefore, the NIR light-controlled chemotherapy and photodynamic therapy could be realized simultaneously by CCUCNPs@PM.

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66. 66

    Wang, C.; Cheng, L.; Liu, Y.; Wang, X.; Ma, X.; Deng, Z.; Li, Y.; Liu, Z. Imaging-guided pH-sensitive photodynamic therapy using charge reversible upconversion nanoparticles under near-infrared light. Adv. Funct. Mater. 2013, 23, 3077– 3086,  DOI: 10.1002/adfm.201202992

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    Imaging-Guided pH-Sensitive Photodynamic Therapy Using Charge Reversible Upconversion Nanoparticles under Near-Infrared Light

    Wang, Chao; Cheng, Liang; Liu, Yumeng; Wang, Xiaojing; Ma, Xinxing; Deng, Zhaoyi; Li, Yonggang; Liu, Zhuang

    Advanced Functional Materials (2013), 23 (24), 3077-3086CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Photodynamic therapy (PDT) based on upconversion nanoparticles (UCNPs) can effectively destroy cancer cells under tissue-penetrating near-IR light (NIR) light. Herein, we synthesize manganese (Mn2+)-doped UCNPs with strong red light emission at ca. 660 nm under 980 nm NIR excitation to activate Chlorin e6 (Ce6), producing singlet oxygen (1O2) to kill cancer cells. A layer-by-layer (LbL) self-assembly strategy is employed to load multiple layers of Ce6 conjugated polymers onto UCNPs via electrostatic interactions. UCNPs with two layers of Ce6 loading (UCNP@2xCe6) are found to be optimal in terms of Ce6 loading and 1O2 generation. By further coating UCNP@2xCe6 with an outer layer of charge-reversible polymer contg. dimethylmaleic acid (DMMA) groups and polyethylene glycol (PEG) chains, we obtain a UCNP@2xCe6-DMMA-PEG nanocomplex, the surface of which is neg. charged and PEG coated under pH 7.4; this could be converted to have a pos. charged naked surface at pH 6.8, significantly enhancing cell internalization of nanoparticles and increasing in vitro NIR-induced PDT efficacy. We then utilize the intrinsic optical and paramagnetic properties of Mn2+-doped UCNPs for in vivo dual modal imaging, and uncover an enhanced retention of UCNP@2xCe6-DMMA-PEG inside the tumor after intratumoral injection, owing to the slightly acidic tumor microenvironment. Consequently, a significantly improved in vivo PDT therapeutic effect is achieved using our charge-reversible UCNP@2xCe6-DMMA-PEG nanoparticles. Finally, we further demonstrate the remarkably enhanced tumor-homing of these pH-responsive charge-switchable nanoparticles in comparison to a control counterpart without pH sensitivity after systemic i.v. injection. Our results suggest that UCNPs with finely designed surface coatings could serve as smart pH-responsive PDT agents promising in cancer theranostics.

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    Liang, S.; Sun, C.; Yang, P.; Ma, P. A.; Huang, S.; Cheng, Z.; Yu, X.; Lin, J. Core-shell structured upconversion nanocrystal-dendrimer composite as a carrier for mitochondria targeting and catalase enhanced anti-cancer photodynamic therapy. Biomaterials 2020, 240, 119850,  DOI: 10.1016/j.biomaterials.2020.119850

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    67

    Core-shell structured upconversion nanocrystal-dendrimer composite as a carrier for mitochondria targeting and catalase enhanced anti-cancer photodynamic therapy

    Liang, Shuang; Sun, Chunqiang; Yang, Piaoping; Ma, Ping'an; Huang, Shanshan; Cheng, Ziyong; Yu, Xifei; Lin, Jun

    Biomaterials (2020), 240 (), 119850CODEN: BIMADU; ISSN:0142-9612. (Elsevier Ltd.)

    Recently, photodynamic therapy (PDT) has been deemed to be the most promising strategy for cancer treatment. To improve the efficacy for PDT, nanocarriers are expected to target mitochondria that are vulnerable to toxic reactive oxygen species (ROS). Moreover, overcoming tumor hypoxia is also conducive to enhance the PDT efficacy. Upconversion nanoparticles (UCNPs) can convert near IR (NIR) light to visible light, thus stimulating photosensitizers to effectively produce cytotoxic ROS and achieving a high tissue penetration depth. In this study, a multifunctional nanocarrier UCNPs@G4/Ce6/CAT-CTPP was synthesized by a novel thiol-ene and azide-acetylene click reaction route to connect the original oleic acid ligands and dendrimers. Interestingly, the constructed "hydrophobic and hydrophilic pockets" around one single upconversion nanoparticle can simultaneously load hydrophobic photosensitizer Chlorin e6 (Ce6) and hydrophilic catalase (CTA) for catalytic enhanced PDT activated by NIR laser. Also, the mitochondrial targeting mols. (3-carboxypropyl) triphenylphosphonium bromide (CTPP) were modified outside of the dendrimers to efficiently target mitochondria. Both the catalytic degrdn. of hydrogen peroxide (H2O2) by catalase to overcome tumor hypoxia and mitochondrial targeting greatly enhance the efficacy of PDT. More importantly, this system provides a new paradigm for designing inorg. nanocrystal core and dendrimer shell for cargo delivery.

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68. 68

    Park, Y. I.; Kim, H. M.; Kim, J. H.; Moon, K. C.; Yoo, B.; Lee, K. T.; Lee, N.; Choi, Y.; Park, W.; Ling, D.; Na, K.; Moon, W. K.; Choi, S. H.; Park, H. S.; Yoon, S. Y.; Suh, Y. D.; Lee, S. H.; Hyeon, T. Theranostic probe based on lanthanide-doped nanoparticles for simultaneous in vivo dual-modal imaging and photodynamic therapy. Adv. Mater. 2012, 24, 5755– 5761,  DOI: 10.1002/adma.201202433

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    Theranostic Probe Based on Lanthanide-Doped Nanoparticles for Simultaneous In Vivo Dual-Modal Imaging and Photodynamic Therapy

    Park, Yong Il; Kim, Hyung Min; Kim, Jeong Hyun; Moon, Kyung Chul; Yoo, Byeongjun; Lee, Kang Taek; Lee, Nohyun; Choi, Yoonseok; Park, Wooram; Ling, Daishun; Na, Kun; Moon, Woo Kyung; Choi, Seung Hong; Park, Hong Seok; Yoon, Soo-Young; Suh, Yung Doug; Lee, Sung Ho; Hyeon, Taeghwan

    Advanced Materials (Weinheim, Germany) (2012), 24 (42), 5755-5761CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Dual-mode in vivo tumor imaging and PDT were performed using photosensitizer-conjugated lanthanide-doped nanoparticles. Hexagonal phase NaYF4:Yb,Er/Na GdF4 core-shell UCNPs could be used for both in vivo luminescence imaging and MRI and conjugated with Ce6, a PDT drug. C26 nanoparticles were readily accumulated in tumor sites by the EPR effect. Cytotoxic singlet oxygen could be generated upon irradn. by a 980 nm laser.

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    Tang, X. L.; Wu, J.; Lin, B. L.; Cui, S.; Liu, H. M.; Yu, R. T.; Shen, X. D.; Wang, T. W.; Xia, W. Near-infrared light-activated red-emitting upconverting nanoplatform for T₁-weighted magnetic resonance imaging and photodynamic therapy. Acta Biomater. 2018, 74, 360– 373,  DOI: 10.1016/j.actbio.2018.05.017

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    69

    Near-infrared light-activated red-emitting upconverting nanoplatform for T1-weighted magnetic resonance imaging and photodynamic therapy

    Tang, Xiang-long; Wu, Jun; Lin, Ben-lan; Cui, Sheng; Liu, Hong-mei; Yu, Ru-tong; Shen, Xiao-dong; Wang, Ting-wei; Xia, Wei

    Acta Biomaterialia (2018), 74 (), 360-373CODEN: ABCICB; ISSN:1742-7061. (Elsevier Ltd.)

    Herein, to overcome the limited tissue penetration in traditional PDT, a novel near-IR (NIR) light-activated NaScF4: 40% Yb, 2% Er@CaF2 upconversion nanoparticle (rUCNP) is successfully designed and synthesized. Chlorin e6, a photosensitizer and a chelating agent for Mn2+, is loaded into human serum albumin (HSA) that further conjugates onto rUCNPs. To increase the ability to target glioma tumor, an acyclic Arg-Gly-Asp peptide (cRGDyK) is linked to rUCNPs@HSA(Ce6-Mn). This nanoplatform enables efficient adsorption and conversion of NIR light (980 nm) into bright red emission (660 nm), which can trigger the photosensitizer Ce6-Mn complex for PDT and T1-weighted magnetic resonance imaging (T1-weighted MRI) for glioma diagnosis. Our in vitro and in vivo expts. demonstrate that NIR light-activated and glioma tumor-targeted PDT can generate large amts. of intracellular ROS that induce U87 cell apoptosis and suppress glioma tumor growth owing to the deep tissue penetration of irradiated light and excellent tumor-targeting ability.

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    Hayashi, K.; Jiang, P.; Yamauchi, K.; Yamamoto, N.; Tsuchiya, H.; Tomita, K.; Moossa, A. R.; Bouvet, M.; Hoffman, R. M. Real-time imaging of tumor-cell shedding and trafficking in lymphatic channels. Cancer Res. 2007, 67, 8223– 8228,  DOI: 10.1158/0008-5472.CAN-07-1237

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