以铜粒边界指导催化CO2降解为乙醇
Dongfang Cheng1,2, Gong Zhang1,2, Lulu Li1,2
1Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University Tianjin 300072 China jlgong@tju.edu.cn.
Chemical science
|July 28, 2023
概括
铜电催化剂中的颗粒边界 (GB) 是二氧化碳电还原到乙醇的关键. 这些GBs通过促进关键的中间吸附和降低反应障碍来增强乙醇选择性.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 铜 (Cu) 电催化剂中的颗粒边界 (GB) 是二氧化碳电还原到乙醇的建议活性场所.
- GBs影响这种反应的确切机制尚不清楚.
研究的目的:
- 阐明GBs在调整CO2转化为乙醇的铜电催化剂活性和选择性的作用.
- 为了研究两个代表的Cu-GB模型:Cu3/(111) GB和Cu5/(100) GB.
主要方法:
- 联合应用第一原则计算和实验验证.
- 动力学分析以了解反应障碍.
- 使用膜电极组装系统进行电化学测试.
主要成果:
- 独特的GB结构促进了关键中间体 (*COOH, *CHO) 和较低的CO-CHO合障碍物的吸附.
- 在Cu (100) 中引入GBs将选择性从乙烯转移到乙醇.
- GBs稳定*CH3CHO,并呈现不利的*O吸附点,促进乙醇的生产.
- 在扩大规模的系统中实现了12.5A电流和5.18%的单通转换以乙醇.
结论:
- 谷物边界通过优化中间吸附和反应途径,显著提高了二氧化碳电还原到乙醇的水平.
- 这些发现为设计针对性C2+产品合成的高效铜电催化剂提供了一种机制的理解.
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