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Deciphering the high-carbonization-temperature triggered enzymatic activity of wool-derived N,S-co-doped carbon nanosheets

查看全文 作　　者：Jiachen [1]Zhao;Deshuai [1]Yu;Jianmin [2,4]Chen;Shihao [3]Lin;Yonghua [1]Tang;Chaoyu [1]Fan;Dongfang [3]Zhou;Youhui [1]Lin 高影响力作者 机构地区：[1]Department of Physics,Research Institute for Biomimetics and Soft Matter,Fujian Provincial Key Laboratory for Soft Functional Materials Research,Xiamen University,Xiamen 361005,China;[2]School of Pharmacy and Medical Technology,Putian University,Putian 351100,China;[3]Key Laboratory of Mental Health of the Ministry of Education,NMPA Key Laboratory for Research and Evaluation of Drug Metabolism&Guangdong Provincial Key Laboratory of New Drug Screening,School of Pharmaceutical Sciences,Southern Medical University,Guangzhou 510515,China;[4]Key Laboratory of Pharmaceutical Analysis and Laboratory Medicine(Putian University),Fujian Province University,Putian 351100,China高影响力机构 出　　处：《Chinese Chemical Letters》索引2024年第35卷第3期,共7页高影响力期刊 基　　金：funded by the National Natural Science Foundation of China(Nos.12274356,22275081);Key Laboratory of Pharmaceutical Analysis and Laboratory Medicine(Putian University)(No.PALM 202206);Fujian Province University,the Fundamental Research Funds for the Central Universities(No.20720220022);the 111 Project(No.B16029)。 摘　　要：It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design of nanomaterials as enzyme mimics.Hereby,N,S-rich carbonized wool nanosheets(CWs)were synthesized at different pyrolysis temperatures.As expected,only CWs treated with high-temperature possess intrinsic oxidase-and peroxidase-like activities.Meanwhile,density functional theory(DFT)calculations demonstrate that graphitic nitrogen and the co-existence of nitrogen and sulfur in the carbon matrix serve as the active sites for the enzyme-like process.More importantly,combining theoretical calculations and experimental observations,the high-temperature triggered catalytic mechanism can be ascribed to the fact that an appropriate high-temperature maximizes the graphitization degree to a certain extent,at which most of the catalytic active sites are well retained rather than evaporating.Moreover,coupling with excellent photothermal conversion efficiency and catalytic performance,CWs can be applied to photothermal-catalytic cancer therapy under near-infrared region(NIR)light irradiation.We believe this work will contribute to understanding the catalytic mechanism of carbon-based nanozymes and promote the development of new biomedical and pharmaceutical applications. 关 键 词：Carbon-based nanozyme Catalytic mechanism Density functional theory High-temperature carbonization
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