氨基酸修饰的MOF-808催化降解神经毒剂的模拟酶性质研究  

Study on the mimic enzymatic performance of amino acid modified MOF-808 for nerve agents decontamination

作　　者：刘克清 崔燕 于琼 陈立坤 郑永超 乔智威 郑禾 LIU Keqing;CUI Yan;YU Qiong;CHEN Likun;ZHENG Yongchao;QIAO Zhiwei;ZHENG He(Guangzhou Key Laboratory for New Energy and Green Catalysis,College of Chemistry and Chemical Engineering,Guangzhou University,Guangzhou 510006,Guangdong,China;State Key Laboratory of NBC Protection for Civilian,Beijing 102205,China)

机构地区：[1]广州大学化学化工学院,能源与催化研究所,广东广州510006 [2]国民核生化灾害防护国家重点实验室,北京102205

出　　处：《化工学报》2024年第2期616-625,共10页CIESC Journal

基　　金：国家自然科学基金项目(21978058,21676094);广东省自然科学基金项目(2022A1515011446)。

摘　　要：通过后合成修饰方法制备了一系列不同氨基酸(amino acid,AA)接枝的MOF-808-AA催化剂,研究了孔结构和孔道微环境对神经毒剂模拟剂催化性能的影响,探索了MOF-808和MOF-808-AA的模拟酶性质。结果表明:氨基酸修饰造成MOF-808的孔结构和孔道微环境发生变化,从而影响催化剂对模拟剂的催化性能。其中,氨基酸侧链提供的氢键以及疏水作用使得MOF-808-AA对模拟剂的亲和力有所提升;氨基酸接枝后,MOF-808原始结构中的活性金属位点数量减少造成了降解速率的降低;氨基酸侧链官能团的酸碱性会导致孔道微环境差异,当侧链为氨基等碱性官能团时,催化效率明显提高,而当侧链为羧基时,催化效率则明显降低。A series of MOF-808-AA catalysts grafted with different amino acids were prepared by post-synthesis modification method.The effects of pore structure and pore microenvironment on the catalytic performance of nerve agent simulant were studied,and the mimic enzyme properties of MOF-808 and MOF-808-AA were further explored.The results showed that amino acid modification caused changes in the pore structure and pore microenvironment of MOF-808,thereby affecting the catalytic performance of the catalyst against the mimic agent.Among them,the hydrogen bond and hydrophobic interaction provided by the amino acid side chain improve the affinity of MOF-808-AA to the simulant.After amino acid grafting,the number of active metal sites in the original structure of MOF-808 decreased,resulting in the decrease in the degradation rate.The acidity and alkalinity of the amino acid side chain groups could lead to differences of the pore microenvironment.When the side chain is a basic group such as amino,the catalytic efficiency of the simulant decontamination is significantly improved.However,when the side chain is a carboxyl group,the catalytic efficiency is significantly reduced.

关 键 词：MOF-808 氨基酸 后合成修饰 神经毒剂模拟剂 

分 类 号：O643.322[理学—物理化学]