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    Research Article

    Coordination Modulation Method To Prepare New Metal–Organic Framework-Based CO-Releasing Materials
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    • Francisco J. Carmona
      Francisco J. Carmona
      Department of Inorganic Chemistry, University of Granada, Av. Fuentenueva S/N, 18071 Granada, Spain
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    • Carmen R. Maldonado
      Carmen R. Maldonado
      Department of Inorganic Chemistry, University of Granada, Av. Fuentenueva S/N, 18071 Granada, Spain
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      Orcidhttp://orcid.org/0000-0002-4958-6052
    • Shuya Ikemura
      Shuya Ikemura
      Institute for Integrated Cell-Material Sciences (WPI-iCEMs), Kyoto University, Yoshida, Sakyo-ku, Kyoto 606-8501, Japan
      Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Carlos C. Romão
      Carlos C. Romão
      Instituto de Tecnologia Química e Biológica, Universidade Nova de Lisboa, Av. da República, EAN, 2780-157 Oeiras, Portugal
      Proterris (Portugal), Instituto de Biologia Experimental e Tecnológica, Av. da República, EAN, 2780-157 Oeiras, Portugal
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    • Zhehao Huang
      Zhehao Huang
      Department of Materials and Environmental Chemistry, Berzelii Centre EXSELENT on Porous Materials, and Inorganic and Structural Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden
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    • Hongyi Xu
      Hongyi Xu
      Department of Materials and Environmental Chemistry, Berzelii Centre EXSELENT on Porous Materials, and Inorganic and Structural Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden
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    • Xiaodong Zou*
      Xiaodong Zou
      Department of Materials and Environmental Chemistry, Berzelii Centre EXSELENT on Porous Materials, and Inorganic and Structural Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden
      *E-mail: [email protected] (X.Z.).
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      Orcidhttp://orcid.org/0000-0001-6748-6656
    • Susumu Kitagawa
      Susumu Kitagawa
      Institute for Integrated Cell-Material Sciences (WPI-iCEMs), Kyoto University, Yoshida, Sakyo-ku, Kyoto 606-8501, Japan
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    • Shuhei Furukawa*
      Shuhei Furukawa
      Institute for Integrated Cell-Material Sciences (WPI-iCEMs), Kyoto University, Yoshida, Sakyo-ku, Kyoto 606-8501, Japan
      Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan
      *E-mail: [email protected] (S.F.).
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      Orcidhttp://orcid.org/0000-0003-3849-8038
    • Elisa Barea*
      Elisa Barea
      Department of Inorganic Chemistry, University of Granada, Av. Fuentenueva S/N, 18071 Granada, Spain
      *E-mail: [email protected] (E.B.).
      More by Elisa Barea
      Orcidhttp://orcid.org/0000-0001-9895-1047
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2018, 10, 37, 31158–31167
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    https://doi.org/10.1021/acsami.8b11758
    Published August 28, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Aluminum-based metal–organic frameworks (MOFs), [Al(OH)(SDC)]n, (H2SDC: 4,4′-stilbenedicarboxylic acid), also known as CYCU-3, were prepared by means of the coordination modulation method to produce materials with different crystal size and morphology. In particular, we screened several reagent concentrations (20–60 mM) and modulator/ligand ratios (0–50), leading to 20 CYCU x_y materials (x: reagent concentration, y = modulator/ligand ratio) with different particle size and morphology. Noteworthy, the use of high modulator/ligand ratio gives rise to a new phase of CYCU-3 (CYCU-3′ x_50 series), which was structurally analyzed. Afterward, to test the potential of these materials as CO-prodrug carriers, we selected three of them to adsorb the photo- and bioactive CO-releasing molecule (CORM) ALF794 [Mo(CNCMe2CO2H)3(CO)3] (CNCMe2CO2H = 2-isocyano-2-methyl propionic acid): (i) CYCU-3 20_0, particles in the nanometric range; (ii) CYCU-3 50_5, bar-type particles with heterogeneous size, and (iii) CYCU-3′ 50_50, a new phase analogous to pristine CYCU-3. The corresponding hybrid materials were fully characterized, revealing that CYCU-3 20_0 with the smallest particle size was not stable under the drug loading conditions. Regarding the other two materials, similar ALF794 loadings were found (0.20 and 0.19 CORM/MOF molar ratios for ALF794@CYCU-3 50_5 and ALF794@CYCU-3′ 50_50, respectively). In addition, these hybrid systems behave as CO-releasing materials (CORMAs), retaining the photoactive properties of the pristine CORM in both phosphate saline solution and solid state. Finally, the metal leaching studies in solution confirmed that ALF794@CYCU-3′ 50_50 shows a good retention capacity toward the potentially toxic molybdenum fragments (75% of retention after 72 h), which is the lowest value reported for a MOF-based CORMA to date.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.8b11758.

    • SEM and TEM images, powder X-ray diffractograms, additional structural data, TGA, infrared spectra, N2 adsorption isotherms and pore size distribution, CO delivery assays in solution, and Mo leaching studies (PDF)

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    Cited By

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2018, 10, 37, 31158–31167
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.8b11758
    Published August 28, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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