A DFT study of two-dimensional P_2Si monolayer modified by single transition metal(Sc-Cu)atoms for efficient electrocatalytic CO_(2)reduction  

作　　者：Chaozheng He Houyong Yang Xi Fu Xiaoli Cheng Jiyuan Guo Ling Fu 

机构地区：[1]Institute of Environmental and Energy Catalysis,Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices,School of Materials Science and Chemical Engineering,Xi'an Technological University,Xi'an 710021,China [2]College of Science,Hunan University of Science and Engineering,Yongzhou 425199,China [3]Department of Physics,Jishou University,Jishou 416000,China [4]School of Science,Jiangsu University of Science and Technology,Zhenjiang 212003,China [5]College of Resources and Environmental Engineering,Tianshui Normal University,Tianshui 741001,China

出　　处：《Chinese Chemical Letters》2023年第5期580-586,共7页中国化学快报（英文版）

基　　金：funded by the Natural Science Foundation of China(Nos.21603109,11304128);the Henan Joint Fund of the National Natural Science Foundation of China(No.U1404216);the Science and Technology Program of Henan Department of Science and Technology,China(No.182102310609);the Construct Program of Applied Characteristic Discipline in Hunan University of Science and Engineering(Mathematics,Education and Electronic Science and Technology)。

摘　　要：In the present work,a stable two-dimensional(2D)P_(2)Si monolayer was predicted.The monolayer is semimetallic/metallic under the PBE/HSE06 functional and is mechanically isotropic.The stability of the P_(2)Si monolayer has been proved via cohesive energy,mechanical criteria,molecular dynamics simulation,and phonon dispersion respectively,and the monolayer possesses high carrier mobility which is three times that of Mo S_(2).On the other hand,the catalytic performance of the P_(2)Si monolayer modified with a single transition metals(M=Sc-Cu)atom for the electrochemical reduction of CO_(2)was investigated,and the monolayer can catalyze CO_(2)with three constraints:stable molecular dynamics,high migration potential of metal atoms,and suitable band gap for electrocatalyst after metal doping exhibiting excellent catalytic stabilization activity and CRR selectivity.In addition,the reduction product of V@P_(2)Si is HCOOH with an overpotential as low as 0.75 V,and the most suitable reaction path is^(*)CO_(2)→^(*)CHOO→O^(*)CHOH→^(*)+HCOOH with the final reduction product HCOOH obtained.As a whole,the above results endow the P_(2)Si monolayer to be a good 2D material holding great promises for applications in nanoelectronics and CO_(2)reduction catalysts.

关 键 词：First-principles calculation Global optimization method CO_(2)electrochemical reduction reaction Single-atom catalysts Phosphorus silicon compound 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]