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

Release Time:2025-04-30  Hits:

• Date:2025-04-30
• Title of Paper:‘‘Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction
• Journal:Journal of Energy Chemistry
• Summary: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.
• Co-author:Cheng He , Shiqi Yan , Wenxue Zhang*
• Volume:2024, 96, 437-447
• Page Number:2024, 96, 437-447
• Translation or Not:No
• Date of Publication:2024-06-05