在CO2过程中激活铜上的C-C合RR:合金催化剂的电荷控制设计
Wei Wang1, Mattia Salomone1, Michele Re Fiorentin1
1Department of Applied Science and Technology, Politecnico di Torino, 10129 Turin, Italy.
将铜与等p块金属合金增强二氧化碳电还原. 电子捐赠稳定了中间体,促进了碳-碳合,以有效地形成多碳产品.
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
- 计算化学的计算化学
背景情况:
- 将二氧化碳 (CO2) 电还原为多碳 (C2+) 产品对于可持续化学至关重要.
- 基于铜 (Cu) 的催化剂对二氧化碳二极化具有独特的活性,这是一个关键的C2+形成阶段.
- 合金是一种增强二氧化碳电还原的有希望的策略,但机制尚不清楚.
研究的目的:
- 系统地使用计算方法对稀释CuM(100) 合金上的CO二分化进行研究.
- 了解p块金属合金在改善二氧化碳电还原活性和选择性方面的作用.
- 确定用于预测催化剂性能的实用描述符.
主要方法:
- 用机器学习对稀释CuM100) 合金进行选.
- 恒定电位密度函数理论 (DFT) 模拟.
- 分析反应能量,激活障碍和表面电荷.
主要成果:
- 与纯相比,p-块金属,特别是Al和Ga,显著降低了激活障碍,并增加了CO二分化的外热性.
- 在研究的合金中, (Al) 具有最高的催化活性.
- 异原子的电子捐赠稳定了CO二极体中间体,促进了C-C合.
- 在固定电位的反应能量和过量的表面电荷之间发现了强烈的线性相关性.
结论:
- 过多的表面电荷作为二氧化碳电还原反应 (CO2RR) 活动的强有力的描述符,整合了共振和静电效应.
- 这个描述符可以指导先进电催化剂的合理设计,以实现高效的C-C合.
- 将Cu与特定的p块元素合金为提高CO2RR性能提供了一条可行的途径.
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