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Full reaction mechanism of hydrogen peroxide catalyzed by reductive CoP nanoparticles:the enzyme-like activity

Science China Chemistry 2023年第4期66卷 1221-1227页

作者： Kaiwei Wan Chang Long Bing Jiang Minmin Liang Zhiyong Tang Hui Wang Xinghua Shi Laboratory of Theoretical and Computational Nanoscience CAS Key Laboratory of Nanosystem and Hierarchical FabricationCAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Molecular Electrochemistry Laboratory Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 610054China Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

The hydrogen peroxide(H2O2)catalyzed by nanoparticles(NPs)demonstrates potential broad applications in the field of biomedicine and environmental protection.However,a systematic understanding of the catalytic mechanism severely limited the rational design of NPs with better enzyme-like activity and selectivity.Here,compared with the widely concerned Fe3O4NPs,the decomposition process of H_(2)O_(2) on reductive Co P NPs and p H-regulated peroxidase-and catalase-like activities with 3,3′,5,5′-tetramethylbenzidine(TMB)as reductive substrates were explored.All results show that OH·radical intermediates generated from the decomposition of H2O2*/OOH*at acidic conditions and complexed with TMB via H-bonds(complexed OH·)are the principal oxidant of TMB rather than free OH·as reported.Besides,the produced O*/OH*on Co P NPs shows negligible oxidation activity due to the strong reducibility of catalysts.The high coverage of O*/OH*from the dissociation of H2O2(H2O)at neutral(alkaline)p H conditions on Co P NPs enhances the dehydrogenation of H_(2)O_(2) to O2,leading to the transition between peroxidase-and catalase-like activities.

关键词： CoP nanoparticle peroxidase,catalase DFT calculations heterogeneous catalysis

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