通过原子兰化物诱导的拉伸式CuO催化剂提高CO2到C2+产品的电还原效率
Jiaqi Feng1, Limin Wu1,2, Shoujie Liu3
1Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Journal of the American Chemical Society
|April 24, 2023
概括
加多 (Gd) 注使铜催化剂稳定,有效地减少二氧化碳反应 (CO2RR) 成为有价值的C2+产品,提高性能和选择性.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 铜 (Cu) 是通过二氧化碳还原反应 (CO2RR) 将二氧化碳 (CO2) 转化为高价值C2+产品的关键电催化剂.
- 活性Cu+物种对于C-C合至关重要,在反应条件下往往不稳定,限制了催化剂的性能.
- 了解原子剂对基于的催化剂的影响对于提高CO2RR效率至关重要.
研究的目的:
- 研究原子剂如何影响CO2RR的基于Cu的电催化剂的性能.
- 在理论和实验上设计和评估加氧化铜 (Gd-CuO) 催化剂,以增强二氧化碳的电减.
主要方法:
- 确定各种金属合Cu2O系统的热力学限制潜力和CO结合能量的第一原理计算.
- 基于理论预测的Gd化CuO (Gd1/CuO) 催化剂的合成
- 用于减少二氧化碳的Gd1/CuO催化剂的电化学评估,包括法拉迪效率和部分电流密度测量.
- 在现场实验和理论研究以阐明兴奋剂机制.
主要成果:
- 理论选确定了加多 (Gd) 作为改善基于Cu的CO2RR催化剂的有效补充剂.
- 在CuO (Gd1/CuO) 中的Gd注稳定了Cu+物种并诱导了拉伸应变,增强了催化活性.
- 对于C2+产品,Gd1/CuO催化剂实现了81.4%的法拉迪效率,其部分电流密度为444.3 mA cm-2在-0.8 V和RHE之间.
- Gd兴奋剂促进了二氧化碳的激活,稳定了O*CCO中间体,并降低了C-C合能障碍.
结论:
- 原子Gd注是一种可行的策略,可以提高基于Cu的CO2RR电催化剂的稳定性和性能.
- Gd1/CuO催化剂在从二氧化碳电还原中产生C2+产品方面表现出卓越的效率和选择性.
- 该研究提供了Gd兴奋剂机制的见解,强调其在稳定中间体和促进C-C合中的作用.
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