‘‘Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction
发布时间：2025-04-30
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- 发布时间：
- 2025-04-30
- 论文名称：
- ‘‘Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction
- 发表刊物：
- Journal of Energy Chemistry
- 摘要：
- 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.
- 合写作者：
- Cheng He , Shiqi Yan , Wenxue Zhang*
- 卷号：
- 2024, 96, 437-447
- 页面范围：
- 2024, 96, 437-447
- 是否译文：
- 否
- 发表时间：
- 2024-06-05