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

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

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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(N2)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(Hf1-N1P2-1 and Tc1-N4),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 Hf1-N1P2-1 and Tc1-N4 to activate and hydrogenate N2 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.

N2 electroreduction reactionsingle-atom catalystsblack phosphorusdensity functional theoryhigh-throughput calculations

Xiao-Yan Li、Manyi Duan、Pengfei Ou

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Department of Electrical and Computer Engineering,University of Toronto,Toronto,Ontario M5S1A4,Canada

School of Physics and Electronic Engineering,Sichuan Normal University,Chengdu 610101,China

Department of Chemistry,Northwestern University,Evanston,IL 60208,USA

National Natural Science Foundation of ChinaFoundation of Science and Technology Bureau of Sichuan ProvinceNiagara supercomputer at the SciNet HPC ConsortiumCanada Foundation for InnovationGovernment of OntarioOntario Research Fund-Research ExcellenceUniversity of Torontocomputing resources from the High-Performance Computing Center of Sichuan Normal University

114042302013JY0085

2024

10.1007/s12274-023-6068-1

纳米研究(英文版)

纳米研究(英文版)

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ISSN：
年,卷(期)：2024.17(4)
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