Theoretical regulating the M-site composition of Janus MXenes enables the tailoring design for highly active bifunctional ORR/OER catalysts  

作　　者：Shuang Luo Ninggui Ma Jun Zhao Yuhang Wang Yaqin Zhang Yu Xiong Jun Fan 

机构地区：[1]Department of Materials Science and Engineering,City University of Hong Kong,Hong Kong 999077,China [2]Department of Mechanical Engineering,City University of Hong Kong,Hong Kong 999077,China [3]Center for Advanced Nuclear Safety and Sustainable Development,City University of Hong Kong 999077,Hong Kong,China

出　　处：《Journal of Materials Science & Technology》2024年第32期145-155,共11页材料科学技术(英文版)

基　　金：supported by the Research Grants Council of Hong Kong(Nos.CityU 11305919 and 11308620);the NSFC/RGC Joint Research Scheme(No.N_CityU104/19);Hong Kong Re-search Grant Council Collaborative Research Fund(Nos.C1002-21 G and C1017-22 G);This research made use of the comput-ing resources of the X-GPU cluster supported by the Hong Kong Research Grant Council Collaborative Research Fund(No.C6021-19EF).

摘　　要：Rechargeable metal-air batteries generally require efficient,durable,and safe bifunctional electrocatalysts to simultaneously support oxygen reduction/evolution reactions(ORR/OER).Herein,we employed first-principles calculations to explore the structure-activity relationship between the composition control of metal atoms and the catalytic activity of Pt-doped Ti_(2-x) Mn_(x) CO_(2) single-atom catalysts(SACs).The research found a clear linear relationship between the proportion of Mn and bifunctional performance,which can effectively modulate catalytic activity.Additionally,it shows excellent bifunctional catalytic activity at medium concentrations,among which the catalyst of Pt-V_(O)-Ti_(0.89) Mn_(1.11) CO_(2) displays the lowest overpo-tential(η^(ORR/OER)=0.26/0.28 V).Attributed to the modulation of the average magnetism of Mn and the d-band center of Pt by different com ponents,the bonding strength of the active center of Pt to adsorption intermediates is changed,resulting in the enhancement of the catalyst activity.Crucially,the molecular orbital-level bonding between the active site Pt and the adsorbed intermediate OH is clarified,shedding light on the involvement of the partially occupied antibonding state of Pt’s d orbital in the activation process.The research extensively explores the control of catalyst activity through composition,offering strong support for designing and optimizing highly active Janus MXene-supported SACs.

关 键 词：DFT Janus-MXene-based SACs Composition regulation STRUCTURE-ACTIVITY 

分 类 号：O64[理学—物理化学]