High-throughput screening of single-atom catalysts confined in monolayer black phosphorus for efficient nitrogen reduction reaction  

作　　者：Xiao-Yan Li Manyi Duan Pengfei Ou 

机构地区：[1]Department of Electrical and Computer Engineering,University of Toronto,Toronto,Ontario M5S 1A4,Canada [2]School of Physics and Electronic Engineering,Sichuan Normal University,Chengdu 610101,China [3]Department of Chemistry,Northwestern University,Evanston,IL 60208,USA

出　　处：《Nano Research》2024年第4期2360-2367,共8页纳米研究（英文版）

基　　金：support from the National Natural Science Foundation of China(No.11404230);the Foundation of Science and Technology Bureau of Sichuan Province(No.2013JY0085).

摘　　要：The discovery of metal-nitrogen centers as the active sites for electrolysis has aroused significant interest in utilizing single-atom catalysts for nitrogen reduction reaction(NRR).Properly designed nanostructured catalysts that strongly interact with nitrogen molecules(N_(2))can promote adsorption and activation,thereby resulting in efficient catalysts with high stability,activity,and selectivity.In this study,using density functional theory calculations,we selected monolayer black phosphorus(BP)as the substrate and screened a series of single-atom transition metals confined in tri-coordinated and tetra-coordinated active centers(without and with N dopants)to electro-catalyze NRR.As a result,we have identified two promising candidates(Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4)),which exhibit not only low overpotentials of 0.56 and 0.49 V but also high thermodynamic and electrochemical stability,as well as good selectivity towards NRR over the competing hydrogen evolution reaction.We also demonstrate the ability of Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4) to activate and hydrogenate N_(2) by donating electrons and regulating charge transfer.This study not only predicts new BP-based promising catalysts but also provides guidance for the rational design of high-performance NRR electrocatalysts under ambient conditions.

关 键 词：N_(2) electroreduction reaction single-atom catalysts black phosphorus density functional theory high-throughput calculations 

分 类 号：O64[理学—物理化学]