局部应变诱导的CO2吸附几何形状和电化学还原路径的转移
Chuhao Liu1, Yifan Bu1, Yifei Xu1
1College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
National science review
|November 18, 2024
概括
-铜 (PdCu) 合金中的应变和几何结构显著改变了电化学二氧化碳减排 (CO2RR) 途径. 不同的局部菌株特征决定了CO2是否转化为一氧化碳 (CO) 或酸盐 (HCOO-).
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:
- 了解双金属合金上二氧化碳 (CO2RR) 的电化学降解对于开发高效的催化剂至关重要.
- 局部微环境变量,包括应变和几何效应,使对基于Cu和基于Pd的合金的CO2RR选择性的预测变得复杂.
研究的目的:
- 研究如何应变和几何效应影响PdCu合金上的CO2RR选择性.
- 阐明二氧化碳在PdCu纳米粒子和纳米 dendrites上的特定吸附几何和反应途径.
主要方法:
- 合成和PdCu纳米粒子和纳米的特征.
- 电化学实验以确定CO2RR的选择性.
- 现场光谱检测反应条件下的催化剂表面.
- 密度函数理论 (DFT) 计算以建模吸附能量和反应途径.
主要成果:
- 具有不同几何形状的PdCu合金 (纳米颗粒与纳米) 呈现出不同的局部菌株形状,尽管相似的阶段和方面.
- 在抗拉力区域,二氧化碳优先吸附于碳侧几何结构,有利于*COOH-CO路径.
- 在压力紧张的区域上,CO2采用氧侧几何,由于d频段中心向下移动,促进了*OCHO-HCOO路径.
- 具有两种吸附几何形状的催化剂都显示出一个主要的*OCHO-to-HCOO-路径.
结论:
- 在PdCu合金中的局部应变环境是CO2RR选择性的关键决定因素.
- 不同的几何形态导致不同的局部菌株,影响二氧化碳吸附和随后的反应途径.
- 这项工作为了解双金属合金微环境及其对CO2RR路径转移的影响提供了一个模型.
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