首页|"Capture-activation-recapture"mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction

"Capture-activation-recapture"mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction

扫码查看
原文链接
  • NETL
  • NSTL
  • 万方数据
Compared with the traditional industrial nitrogen fixation,electrocatalytic methods,especially those uti-lizing double-atom catalysts containing nonmetals,can give good consideration to the economy and environmental protection.However,the existing"acceptance-donation"mechanism is only applicable to bimetallic catalysts and nonmetallic double-atom catalysts containing boron atoms.Herein,a novel"capture-activation-recapture"mechanism for metal-nonmetal double-atom catalyst is proposed to solve the problem by adjusting the coordination environments of nonmetallic atoms and utilizing the activation effect of metal atoms on nitrogen.Based on this mechanism,the nitrogen reduction reaction(NRR)activity of 48 structures is calculated by density functional theory calculation,and four candidates are selected as outstanding electrocatalytic nitrogen reduction catalysts:Si-Fe@NG(UL=-0.14 V),Si-Co@NG(UL=-0.15 V),Si-Mo@BP1(UL=0 V),and Si-Re@BP1(UL=-0.02 V).The analyses of electronic properties further confirm"capture-activation-recapture"mechanism and suggest that the difference in valence electron distribution between metal and Si atoms triggers the activation of N≡N bonds.In addition,a machine learning approach is utilized to generate an expression and an intrinsic descriptor that considers the coordination environment to predict the limiting potential.This study offers profound insight into the synergistic mechanism of TM and Si for NRR and guidance in the design of novel double-atom nitrogen fixation catalysts.

"Capture-activation-recapture"mechanismDouble-atom catalystNitrogen reduction reactionDensity functional theory

Cheng He、Shiqi Yan、Wenxue Zhang

展开 >

State Key Laboratory for Mechanical Behavior of Materials,School of Materials Science and Engineering,Xi'an Jiaotong University,Xi'an 710049,Shaanxi,China

School of Materials Science and Engineering,Chang'an University,Xi'an 710064,Shaanxi,China

National Natural Science Foundation of ChinaNatural Science Foundation of Shaanxi Province,ChinaFundamental Research Funds for the Central UniversitiesHPC platform,Xi'an Jiaotong University

522711132020JM 218CHD300102311405

2024

10.1016/j.jechem.2024.04.047

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.96(9)