@misc{10481/88138,
year = {2018},
month = {8},
url = {https://hdl.handle.net/10481/88138},
abstract = {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.},
organization = {The Spanish Ministry of Economy and Competitivity and UE Feder Program (project CTQ2014-53486R and CTQ2017-84692-R), Japan Society for the Promotion of Science [EB, Invitation Fellowship (Long-Term) L-14529], University of Granada (CRM, Reincorporación Plan Propio), and COST action CM1105 are gratefully acknowledged for generous funding. This study was partially supported by the “Unidad de Excelencia de Química aplicada a biomedicina y medioambiente” (University of Granada). The authors thank Proterris (Portugal) Lda for providing ALF794 and H. Jeremias for preparing it. The NMR data were acquired at CERMAX, ITQB-NOVA, Oeiras, Portugal. The authors thank iCeMS Analysis Centers for access to the experimental facilities. Structural analyses were supported by the 3DEMNATUR project from the Knut and Alice Wallenberg Foundation (KAW) and the MATsynCELL project through Röntgen-Ångström Cluster, the Swedish Research Council (VR).},
publisher = {ACS},
keywords = {carbon monoxide metal−organic framework solid-state materials guest inclusion},
title = {Coordination Modulation Method To Prepare New Metal–Organic Framework-Based CO-Releasing Materials},
doi = {https://doi.org/10.1021/acsami.8b11758},
author = {Carmona Fernández, Francisco Jesús and Rodríguez Maldonado, Carmen and Ikemura, Shuya and Romão, Carlos C. and Huang, Zhehao and Xu, Hongyi and Zou, Xiaodong and Kitagawa, Susumu and Furukawa, Shuhei and Barea Martínez, Elisa María},
}