锰-铜双金属层状硅酸盐纳米酶的构筑及类酶活性

Construction of Mn-Cu Bimetal Containing Phyllosilicate Nanozyme and Evaluation of the Enzyme-like Properties

采用一步溶胶凝胶法,在室温下合成了一种含有锰、铜的双金属层状硅酸盐(AMCP),并探究了其类漆酶和类过氧化物酶活性.结果表明, AMCP具有与天然黏土类似的层状结构,且结构中多价态的锰和铜使其具有优异的类漆酶和类过氧化物酶活性.此外,与天然酶相比, AMCP在极端温度和pH值下具有更强的耐受性,当温度高于70℃后,天然酶完全失活,而AMCP仍保留了80%以上的活性,而在pH=3~9条件下AMCP依然保持90%左右的催化活性.随后,进一步探究了其类酶活性机理,证实了锰、铜之间的电子传导可加速活性位点中铜电对的循环,从而促进活性氧的产生,提高其类酶催化活性.本研究为高效多酶活性纳米酶的构筑提供了参考,也可为双金属层状硅酸盐在生物传感、疾病诊疗及环境修复等领域的应用奠定了基础.

A Mn-Cu containing bimetallic phyllosilicate(AMCP)was prepared by one-pot sol-gel method,which was verified to present intrinsic laccase-like and peroxidase-like performance.The results indicated that AMCP pre⁃sented a well confined 2-dimentional layered structure,and the varied valence states arose from Mn and Cu endow it with excellent enzyme-mimetic activities.Moreover,it exhibits superior pH and temperature tolerance comparing with natural analogue,when the temperature was higher than 70℃,AMCP retained above 80%activity while natural enzyme was completely deactivated.Besides,it also remained around 90%activity under pH value of 3-9.Finally,the catalytic mechanism indicated the electron transfer between Mn and Cu accelerated the cycle of Cu2+and Cu+,which could promote the production of ROS and facilitate the catalytic performance of AMCP.This work provides a novel strategy and direction for the customization of high performance,multi-enzyme mimetic nanozyme,which has a potential application prospect on biosensing,disease therapy and environmental remediation.