Jia-Xing Guo , Shao-Yi Wu , Chun-Yu Yao , Rong-Gang Tian , Shun-Ping Shi
{"title":"锚定单过渡金属原子的 Janus MoSSe 单层作为高效固氮电催化剂的理论筛选","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":"{\"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}","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}
Theoretical screening of single transition-metal atoms anchored Janus MoSSe monolayers as efficient electrocatalysts for nitrogen fixation
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.