Abstract
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 Ti2-xMnxCO2 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-VO-Ti0.89Mn1.11CO2 displays the lowest overpo-tential(ηORR/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 components,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.
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