Two-dimensional(2D)materials have exhibited great potential for replacing costly Pt for oxygen reduction reaction(ORR)because of their distinctive structural features and high pre-site activity.However,their performance is generally hindered by the limited density of active sites(e.g.,at the layer edges).Although they feature a high exposure of surface sites,these sites are typically inert for ORR.Herein,through density functional theory calculations,we propose a promising ORR catalyst candidate,a 2D TaTe2 nanosheet,which has an intrinsic high basal-plane activity.Both of the thermodynamic and kinetic processes are explored,which demonstrates that the basal-plane Te sites of the TaTe2 nanosheet have great potential for facilitating ORR.Specifically,we construct a microkinetic model of ORR pro-ceeding on TaTe2,which unveils its dynamic intermediate coverage under different electrode potentials and identifies the dominating associative pathway.The theoretical half-wave potential of TaTe2 is predicted to be 0.87 V,which exceeds those of the well-established Pt(111)and Fe-N-C single-atom catalysts computed at the same level.This study not only presents the first 2D,non-Pt ORR catalyst candidate with an intrinsic basal-plane activity but also offers a rational methodology for unveiling the mechanism/activity of ORR and other electrochemical reactions.

Yu Wang;Kun Zhou

Environmental Process Modelling Centre,Nanyang Environment and Water Research Institute,Nanyang Technological University,1 CleanTech Loop,637141,Singapore;School of Mechanical and Aerospace Engineering,Nanyang Technological University,50 Nanyang Avenue,639798,Singapore

绿色能源与环境（英文）

[1]Yu Wang;Kun Zhou-.Two-dimensional metallic tantalum ditelluride with an intrinsic basal-plane activity for oxygen reduction:A microkinetic modeling study)[J].绿色能源与环境（英文）,2022(03):525-532

ditelluride,TaTe2,ceeding

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