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Bright, Magnetic NIR-II Quantum Dot Probe for Sensitive Dual-Modality Imaging and Intensive Combination Therapy of Cancer

  • Yingying Li
    Yingying Li
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
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  • Peisen Zhang
    Peisen Zhang
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
    More by Peisen Zhang
  • Wen Tang
    Wen Tang
    South China Advanced Institute for Soft Matter Science and Technology, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, China
    More by Wen Tang
  • Kevin J. McHugh
    Kevin J. McHugh
    Department of Bioengineering, Rice University, 6100 Main Street, MS-142, Houston, Texas 77005, United States
  • Stephen V. Kershaw
    Stephen V. Kershaw
    Department of Materials Science and Engineering & Centre for Functional Photonics, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon 99077, Hong Kong SAR, China
  • Mingxia Jiao
    Mingxia Jiao
    Key Laboratory of Optic-Electric Sensing and Analytical Chemistry for Life Science, MOE, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
    More by Mingxia Jiao
  • Xiaodan Huang
    Xiaodan Huang
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
  • Sergii Kalytchuk
    Sergii Kalytchuk
    Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacký University Olomouc, Olomouc 783 71, Czech Republic
  • Collin F. Perkinson
    Collin F. Perkinson
    Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
  • Saisai Yue
    Saisai Yue
    College of Life Science and Technology, Beijing University of Chemical Technology, Beijing 100029, China
    More by Saisai Yue
  • Yuanyuan Qiao
    Yuanyuan Qiao
    College of Life Science and Technology, Beijing University of Chemical Technology, Beijing 100029, China
  • Lichong Zhu
    Lichong Zhu
    College of Life Science and Technology, Beijing University of Chemical Technology, Beijing 100029, China
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  • Lihong Jing*
    Lihong Jing
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
    *L. Jing. Email: [email protected]. Tel: +86 10 8236 2540.
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  • Mingyuan Gao
    Mingyuan Gao
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
    State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China
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  • , and 
  • Buxing Han
    Buxing Han
    CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China
    More by Buxing Han
Cite this: ACS Nano 2022, 16, 5, 8076–8094
Publication Date (Web):April 20, 2022
https://doi.org/10.1021/acsnano.2c01153
Copyright © 2022 American Chemical Society

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    Abstract

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    Improving the effectiveness of cancer therapy will require tools that enable more specific cancer targeting and improved tumor visualization. Theranostics have the potential for improving cancer care because of their ability to serve as both diagnostics and therapeutics; however, their diagnostic potential is often limited by tissue-associated light absorption and scattering. Herein, we develop CuInSe2@ZnS:Mn quantum dots (QDs) with intrinsic multifunctionality that both enable the accurate localization of small metastases and act as potent tumor ablation agents. By leveraging the growth kinetics of a ZnS shell on a biocompatible CuInSe2 core, Mn doping, and folic acid functionalization, we produce biocompatible QDs with high near-infrared (NIR)-II fluorescence efficiency up to 31.2%, high contrast on magnetic resonance imaging (MRI), and preferential distribution in 4T1 breast cancer tumors. MRI-enabled contrast of these nanoprobes is sufficient to timely identify small metastases in the lungs, which is critically important for preventing cancer spreading and recurrence. Further, exciting tumor-resident QDs with NIR light produces both fluorescence for tumor visualization through radiative recombination pathways as well as heat and radicals through nonradiative recombination pathways that kill cancer cells and initiate an anticancer immune response, which eliminates tumor and prevents tumor regrowth in 80% of mice.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.2c01153.

    • (1) Temporal evolutions of PL emission peak maxima, fluorescence intensity, and PL fwhm/peak for the CISe core QDs; (2) PL spectra of QDs grown under similar condition as for the CISe core QDs while in the absence of Se precursors; (3) fluorescence spectra and normalized PL fwhm of CISe@ZnS QDs recorded during shell growth; (4) thermal gravimetry curves of ZnSt2 and MnSt2; (5) temporal evolutions of PL emission peak maxima, PL fwhm/peak for the QDs during the Mn doping; (6) PL spectra of the CISe@MnS QDs; (7) radiative and apparent nonradiative recombination rates for CIS QDs during 3 h of ZnS shell growth and subsequent 2 h of Mn doping; (8) selected area electron diffraction patterns; (9) XPS spectra; (10) EPR spectra; (11) experimentally determined T1 relaxation rates of water protons against the molar concentration of QD particles; (12) FTIR spectra and hydrodynamic size distribution; (13) calculation of the PCE of QD-FA probe; (14) variation of fluorescence intensity of the cross section in NIR-II fluorescence imaging in vivo; (15) tumor-to-background ratio against postinjection time; (16) FR expression of 4T1 tumor cells; (17) T2-weighted MR images of lung metastasis tumors; (18) photographs of mice bearing 4T1 tumors receiving different treatments; (19) immunofluorometric images of tumor tissue slices showing the staining of M1-phenotype macrophage marker; (20) percentage of TNF-α-positive cells and Ki 67-positive cells for tumor treated with different groups; (21) molar ratios of cations determined from ICP-AES analysis; (22) multiexponential fitting parameters for PL decay curves (PDF)

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    Cited By

    This article is cited by 16 publications.

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