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作者机构:School of Engineering and Applied Sciences Harvard University CambridgeMA02138 United States School of Chemistry Chemical Engineering and Life Science State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China State Key Laboratory of Biocatalysis and Enzyme Engineering Environmental Microbial Technology Center of Hubei Province School of Life Sciences Hubei University Hubei Wuhan430062 China
出 版 物:《SSRN》
年 卷 期:2022年
核心收录:
摘 要:Benefiting from unique properties including faster mass transfer, more exposed active sites and large molecule recognition, hierarchically porous metal-organic frameworks (HP-MOFs), in the form of ultrasmall nanoparticles (NPs) and having self-assembled interparticle mesopores, have garnered greater attention in recent years that given to typical MOFs. However, the controllable synthesis of HP-MOFs on the nanoscale remains a significant challenge. Herein, we describe the results of a study that led to the development of the first, facile top-down acid etching method for preparing the nanosized (~15 nm) mesoporous MOF, HP-UiO-66-NH2(Hf). The sizes of mesopores in this material can be effectively tuned by simply controlling the concentration of propionic acid (PA) utilized in the preparation solution. Remarkably, the mesoporous structure of HP-UiO-66-NH2(Hf) exhibits excellent chemical stability under acid/base conditions and it can be readily constructed by using at least 4 times recycled PA etching solution. In addition, HP-UiO-66-NH2(Hf) displays high size-selectivity for adsorption of enzymes. Moreover, the nanocomposite generated by complexation with glucose oxidase (GOD), GOD@HP-UiO-66-NH2(Hf) has a higher catalytic activity and a significantly enhanced stability (recycled for at least 7 times) in promoting oxidation of glucose compared to its MOF counterpart, GOD@UiO-66-NH2(Hf) and native GOD. This study provides a potentially general strategy to design and construct stable nanosized HP-MOFs which have applications to large molecule encapsulation and catalysis. © 2022, The Authors. All rights reserved.