在酸盐电还原中切换N-N与N-H合,使用CuPd表面原子图案
Keying Wu1, Wei Wu1, Siyuan Liu1
1Research Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, China.
Angewandte Chemie (International ed. in English)
|February 11, 2026
概括
这项研究揭示了铜 (CuPd) 催化剂中的原子结构如何决定酸盐电还原 (NO3-RR) 结果. 有序的CuPd有利于 (N2) 生产,而相分离的CuPd则产生氨 (NH3).
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 酸盐电还原反应 (NO3-RR) 对于减轻酸盐污染和合成像氨这样的有价值化学物质至关重要.
- 双金属催化剂,特别是CuPd,对NO3-RR有希望,但对产品选择性的精确控制仍然是一个挑战.
- 了解原子级表面结构对反应路径的影响,是设计高效催化剂的关键.
研究的目的:
- 阐明酸盐电还原的CuPd双金属催化剂的结构性能关系.
- 调查有序 (o-CuPd) 与分相 (p-CuPd) 架构如何影响反应通路和产品选择性.
- 为脱和氨电合成催化剂的合理设计提供见解.
主要方法:
- 顺序 (o-CuPd) 和相分离 (p-CuPd) 双金属催化剂的合成和表征.
- 电化学评估催化性能,包括电流密度和对NO3-RR的法拉第效率.
- 现场光谱研究和密度函数理论 (DFT) 计算以探测反应中间体和结合强度.
主要成果:
- 订制的CuPd (o-CuPd) 选择性地产生了具有高电流密度 (200 mA cm-2) 和法拉第效率 (~95%) 的二 (N2).
- 阶段分离的CuPd (p-CuPd) 有效地产生了具有可比电流密度 (195 mA cm-2) 和法拉代效率 (~84%) 的氨 (NH3).
- DFT计算显示,受表面图案 (Cu-Pd与Cu-Cu/Pd-Pd) 影响的*NO和*N中间体的结合强度决定了N-N或N-H合路径.
结论:
- 原子层面的表面结构,特别是Cu-Pd异构基因与同构基因的存在,对NO3-RR产品的选择性进行了关键控制.
- 反应中间体 (*NO, *N) 的结合强度是线性的,在确定最终产品方面起着关键作用.
- 这项研究为设计针对性酸盐转换的先进双金属催化剂提供了基本的见解.
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