Cu_(1)-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO_(2)electroreduction
作者机构：Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of EducationAnhui University of TechnologyMaanshan 243002China Anhui Laboratory of Clean Catalytic EngineeringSchool of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China Institute of Clean Energy and Advanced Nanocatalysis(iClean)School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Chemistry and Chemical Engineering Guangdong LaboratoryShantou 515063China Institute of Molecular PlusTianjin UniversityTianjin 300072China School of Chemistry and Chemical EngineeringAnqing Normal UniversityAnqing 246001China Jiangxi Province Engineering Research Center of Ecological Chemical IndustryJiujiang UniversityJiujiang 332005China College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China
出 版 物：《Nano Research》 (纳米研究（英文版）)
年 卷 期：2023年第16卷第4期
页 面：4582-4588页
核心收录：
学科分类：07[理学] 070304[理学-物理化学(含∶化学物理)] 0703[理学-化学] 0702[理学-物理学]
基 金：supported by the National Natural Science Foundation of China(Nos.51902003,22002085,21771003,21501004) the University Synergy Innovation Program of Anhui Province(No.GXXT-2021-020) the Anhui Province Natural Science Foundation(Nos.2108085QB71 and 2008085QB53) the Natural Science Research Project of Anhui Province Education Department(No.KJ2019A0581) the Open Project of Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of Education(No.JKF21-03) the Open Foundation of Anhui Laboratory of Clean Catalytic Engineering(No.LCCE-01) the Open Research Funds of Jiangxi Province Engineering Research Center of Ecological Chemical Industry(STKF2109).
主 题：dual-active sites single-atom catalysis porous carbon dehydrogenative coupling
摘 要：Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(99%)and selectivity(99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.
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