Insights into the effect of substrate adsorption behavior over hemelike Fe_(1)/AC single-atom catalyst

作     者：Jianglin Duan Yanan Zhou Yujing Ren Dan Feng Jinlong Shang Huibin Ge Jie Gao Jinlong Yang Yong Qin Jianglin Duan;Yanan Zhou;Yujing Ren;Dan Feng;Jinlong Shang;Huibin Ge;Jie Gao;Jinlong Yang;Yong Qin

作者机构：Interdisciplinary Research Center of Biology&CatalysisSchool of Life SciencesNorthwestern Polytechnical UniversityXi’an 710072China Hefei National Laboratory for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Analytical&Testing CenterNorthwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Coal ConversionInstitute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2022年第15卷第7期

页      面：5970-5976页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：The authors wish to acknowledge the support of National Natural Science Foundation of China(NSFC,Nos.21802094,22002118,22172119,and 22102167) Postdoctoral Research Foundation of China(Nos.2020TQ0245 and 2021M693060) Natural Science Basic Research Plan in Shaanxi Province of China(No.2021JM047) 

主　　题：single-atom catalysts heme-like carboxyl group substrate adsorption behavior peroxidase-like activity 

摘      要：Unraveling the substrate adsorption structure–performance relationship is pivotal for heterogeneous carbon supported metal single-atom catalysts(M_(1)/C SACs).However,due to the complexity of the functional groups on carbon material surface,it is still a great ***,inspired by structure of enzymes,we used activated carbon(AC),which has adjustable surface oxygen functional groups(OFGs),supported atomically dispersed Fe-N_(4) sites as heme-like *** based on a combination of scanning transmission electron microscopy(STEM),X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),Mössbauer spectroscopy,Fourier transform infrared(FT-IR)characterizations,kinetics experiments and density functional theory(DFT)calculations,we revealed the effect of substrate adsorption behavior on AC support surface,that is,with the increase of carboxyl group in OFGs,the adsorbed 3,3 ,5,5 -tetramethylbenzidine(TMB)molecular increased,and consequently the substrate enriched on AC *** carboxyl group as well as Fe-N_(4) active sites synergistically realized high-efficiency peroxidase-like activity,just like the *** work suggests that simultaneously constructing metal single-atom active sites and specific functional groups on carbon support surface may open an avenue for engineering metal-support synergistic catalysis in M_(1)/C SACs,which can further improve catalytic performance.