Enhanced Oxygen Evolution Reaction Performance by Dynamic Adsorption of Intermediates on C_(2)N-Supported Single Atom Catalysts  

中间物种动态吸附提升C_(2)N负载单原子催化剂析氧反应性能的理论研究

作　　者：Chongchong Li Li Sheng Yanan Zhou Wenhua Zhang 李冲冲;圣利;周亚男;张文华(中国科学技术大学精准智能化学重点实验室,合肥230026;比利时根特大学化学技术实验室,根特B-9052;宁波大学材料科学与化学工程学院,宁波315211)

机构地区：[1]Key Laboratory of Precision and Intelligent Chemistry,University of Science and Technology of China,Hefei 230026,China [2]Laboratory for Chemical Technology,Ghent University,Ghent B-9052,Belgium [3]School of Material Science and Chemical Engineering,Ningbo University,Ningbo 315211,China

出　　处：《Chinese Journal of Chemical Physics》2024年第5期662-670,I0078-I0093,I0100,I0101,共27页化学物理学报（英文）

基　　金：This work is supported by the National Key Research and Development Program(No.2018YFA0208600);the National Natural Science Foundation of Chi-na(No.U19A2015,No.22102167);CAS Project for Young Scientists in Basic Research(YSBR-051);Wenhua Zhang is supported by USTC Tang Scholarship and State Scholarship Fund(202206345005);The calculations were performed at the Super-computing Center of University of Science and Technology of China(USTCSCC).

摘　　要：The dynamic adsorption of possible intermediates on single-atom catalysts(SACs)under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction(OER),and therefore the performance of the dynamic adsorption should be fully considered in the theoretical screening of potential SACs.Based on density functional theory calculations,the OER performance of 27 types of C_(2)N-supported single transition metal atoms(TM@C_(2)N)is systematically investigated without and with considering the dynamic adsorption of possible intermediates.Without considering dynamic adsorption,only Rh@C_(2)N and Ni@C_(2)N are screened out as good catalysts.However,by further considering the dynamic adsorption configurations of possible intermediates,more promising TM@C_(2)N SACs including Fe(Co,Ni,Ru,Rh,Ir)@C_(2)N toward the OER are screened out.The presence of the intermediates(*HO,*O)on SACs could shift their d band center toward lower energy level,which makes the interaction between the adsorbate and SACs moderate and thus enhances their OER performance.The present work is instructive for further screening and designing of efficient single-atom catalysts for the oxygen evolution reaction.工况条件下可能的中间物种在原子催化剂上的动态吸附对其电催化析氧反应有着重要影响,因此在理论筛选高电催化析氧反应活性的原子催化剂时应充分考虑动态吸附的影响.本文基于密度泛函理论计算,系统研究了27种C_(2)N负载的过渡金属单原子(TM@C_(2)N)催化剂的电催化析氧反应性能.在不考虑中间物种动态吸附时,仅可筛选出Rh@C_(2)N和Ni@C_(2)N作为潜在的电催化析氧反应催化剂.而当进一步考虑可能的中间物种动态吸附时,可筛选出Fe(Co,Ni,Ru,Rh,Ir)@C_(2)N作为潜在的电催化析氧反应催化剂.电子结构分析表明中间物种(*OH,*O)的存在使金属原子的d带中心向较低能级移动,调控了吸附物和金属原子之间的相互作用,从而提高了电催化析氧反应性能。本工作对进一步筛选和设计高效电催化析氧反应单原子催化剂具有指导意义.

关 键 词：Density functional theory Single-atom catalyst Oxygen evolution reaction Dynamic adsorption 

分 类 号：O64[理学—物理化学]