协调环境金属中心的工程协调聚合物用于选择性二氧化碳电还原向多碳产品的聚合物
Juan Wang1, Mingzi Sun2, Hongming Xu1,3
1Department of Chemistry, City University of Hong Kong, Hong Kong 999077, China.
ACS nano
|February 22, 2024
概括
工程铜协调聚合物有效地将二氧化碳 (CO2) 转化为有价值的多碳产品. 修改铜活性位点的协调环境可以提高C2+产品对酸的选择性.
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:
- 电催化二氧化碳还原反应 (CO2RR) 对可持续能源至关重要.
- 控制有效的CO2RR转化为多碳 (C2+) 产品的催化剂活性位点仍然具有挑战性.
- 协调环境工程提供了一个调整催化剂性能的途径.
研究的目的:
- 设计用于CO2RR的协调聚合物中的金属中心的协调环境.
- 为了在中性条件下实现CO2到C2+产品的高效电降解.
- 调查协调结构与产品选择性之间的关系.
主要方法:
- 合成和表征具有不同协调配置 (Cu-N2S2和Cu-I2S2) 的铜协调聚合物.
- 电化学评估CO2RR性能,包括法拉第效率和产品选择性.
- 现场光谱研究和理论计算 (DFT) 以了解反应机制和电子性质.
主要成果:
- Cu-N2S2协调聚合物 (Cu-N-S) 在乙烯 (61.2%) 和C2+产品 (82.2%) 中实现了高法拉达效率.
- Cu-I2S2协调聚合物 (Cu-I-S) 选择性地产生了酸.
- Cu-N-S通过平衡的*CO中间体促进了C-C合,而Cu-I-S抑制了C2+通路.
结论:
- 活性地点的协调环境工程显著影响CO2RR选择性.
- Cu-N2S2配置通过向上移动Cu d带中心并促进C-C合,有利于C2+产品生成.
- 本研究展示了一种设计有效催化剂的策略,以实现可持续的二氧化碳转化.
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