Jia-Xing Guo , Shao-Yi Wu , Chun-Yu Yao , Rong-Gang Tian , Shun-Ping Shi
{"title":"Theoretical screening of single transition-metal atoms anchored Janus MoSSe monolayers as efficient electrocatalysts for nitrogen fixation","authors":"Jia-Xing Guo , Shao-Yi Wu , Chun-Yu Yao , Rong-Gang Tian , Shun-Ping Shi","doi":"10.1016/j.fuel.2024.132474","DOIUrl":null,"url":null,"abstract":"<div><p>Designing efficient nitrogen reduction reaction (NRR) electrocatalysts for ammonia (NH<sub>3</sub>) synthesis under mild conditions is an attracting and challenging theme in energy electrocatalysis. Herein, the catalytic activity of a series of 3d (Cr, Mn, Fe, Co, Ni), 4d (Mo, Tc, Ru, Rh, Pd) and 5d (W, Re, Os, Ir, Pt) transition-metal (TM) atoms anchored Janus MoSSe monolayers for NRR is systematically explored by means of the first-principles calculations. A four-step NRR screening strategy (ΔG(*N<sub>2</sub>) < 0 eV, ΔG(*N<sub>2</sub> → *NNH) < 0.50 eV, ΔG(*NH<sub>2</sub> → *NH<sub>3</sub>) < 0.50 eV and ΔG(*N<sub>2</sub>) < ΔG(*H)) is designed and applied to 15 TM-MoSSe systems, and only the Mo-, Re- and Os-MoSSe stand out. The reaction mechanisms of NRR on Mo-, Re- and Os-MoSSe are all via the distal pathway and exhibit excellent catalytic activity (with the limiting potentials of −0.49, −0.39 and −0.49 V, respectively), especially the Re-MoSSe. The high NRR activity of the Mo-, Re- and Os-MoSSe can originate mainly from the effective activation of N<sub>2</sub>, high built-in electrical field and superior electrical conductivity. Present findings may suggest a reliable and effective NRR screening strategy for the design of NRR electrocatalysts and promote the further exploration and development of novel NRR electrocatalysts.</p></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":null,"pages":null},"PeriodicalIF":6.7000,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0016236124016223","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0
Abstract
Designing efficient nitrogen reduction reaction (NRR) electrocatalysts for ammonia (NH3) synthesis under mild conditions is an attracting and challenging theme in energy electrocatalysis. Herein, the catalytic activity of a series of 3d (Cr, Mn, Fe, Co, Ni), 4d (Mo, Tc, Ru, Rh, Pd) and 5d (W, Re, Os, Ir, Pt) transition-metal (TM) atoms anchored Janus MoSSe monolayers for NRR is systematically explored by means of the first-principles calculations. A four-step NRR screening strategy (ΔG(*N2) < 0 eV, ΔG(*N2 → *NNH) < 0.50 eV, ΔG(*NH2 → *NH3) < 0.50 eV and ΔG(*N2) < ΔG(*H)) is designed and applied to 15 TM-MoSSe systems, and only the Mo-, Re- and Os-MoSSe stand out. The reaction mechanisms of NRR on Mo-, Re- and Os-MoSSe are all via the distal pathway and exhibit excellent catalytic activity (with the limiting potentials of −0.49, −0.39 and −0.49 V, respectively), especially the Re-MoSSe. The high NRR activity of the Mo-, Re- and Os-MoSSe can originate mainly from the effective activation of N2, high built-in electrical field and superior electrical conductivity. Present findings may suggest a reliable and effective NRR screening strategy for the design of NRR electrocatalysts and promote the further exploration and development of novel NRR electrocatalysts.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.