在Cu-N-C中协调和氧化状态的潜在驱动演变提供了高效和选择性的乙半化
Wenying Li1, Jun Li1, Hai Xiao1
1Department of Chemistry, Tsinghua University, Beijing 100084, China.
Journal of the American Chemical Society
|March 6, 2026
概括
铜单原子催化剂 (Cu SAC) 通过电催化乙烯半化 (eASH) 实现可持续的乙烯净化. 应用潜力驱动Cu-N-C催化剂的结构变化,揭示了高选择性至关重要的活性Cu (I) -化物位点.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
背景情况:
- 电催化乙半化 (eASH) 是可持续乙烯净化的关键.
- 在N-化碳 (Cu-N-C) 上的铜单原子催化剂 (SAC) 显示出高的eASH性能.
- 在运行条件下确定Cu-N-C SAC的活跃地点是具有挑战性的.
研究的目的:
- 在eASH期间阐明Cu-N-C SACs在潜在驱动的结构演变.
- 在不同的电化学潜力下识别活性位点和反应机制.
- 为eASH设计先进的SAC提供见解.
主要方法:
- 大法典集合密度函数理论 (DFT) 的计算.
- 构建一个表面Pourbaix图表来绘制活点热力学图.
- 对潜在依赖反应机制和质子转移通路的分析.
主要成果:
- -N-C SAC 经历潜在驱动的结构转变,从 (II) N4 变为 (I) - 化物种.
- 生成的Cu (I) - 化物位点表现出高的化学选择性,有利于乙烯吸附和抑制副作用.
- 反应机制从以水为媒介的转移到具有增加潜力的分子内质子穿通道.
结论:
- 应用潜力从根本上决定了Cu-N-C SACs的协调几何学,氧化状态和催化活性.
- 运算生成的Cu (I) - 化物种是选择性eASH的关键活性位点.
- 这项研究为设计高效的eASH电催化剂建立了一个统一的机制范式.
更多相关视频
相关概念视频
Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation
9.2K
Introduction
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
9.2K
Reduction of Alkenes: Catalytic Hydrogenation
14.6K
Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
14.6K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
4.0K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
4.0K
Reduction of Benzene to Cyclohexane: Catalytic Hydrogenation
6.2K
Unlike the easy catalytic hydrogenation of an alkene double bond, hydrogenation of a benzene double bond under similar reaction conditions does not take place easily. For example, in the reduction of stilbene, the benzene ring remains unaffected while the alkene bond gets reduced. Hydrogenation of an alkene double bond is exothermic and a favorable process. In contrast, to hydrogenate the first unsaturated bond of benzene, an energy input is needed; that is, the process is endothermic. This is...
6.2K
Catalysis
31.4K
The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
31.4K
[3,3] Sigmatropic Rearrangement of 1,5-Dienes: Cope Rearrangement
3.5K
The Cope rearrangement is classified as a [3,3] sigmatropic shift in 1,5-dienes, leading to a more stable, isomeric 1,5-diene. The reaction involves a concerted movement of six electrons, four from two π bonds and two from a σ bond, via an energetically favorable chair-like transition state.
3.5K


