在CO电还原过程中对Cu基催化剂的重组:证据表明表面缺陷在C2+产品选择性上的主导作用
Floriane A Rollier1, Valery Muravev1, Alexander Parastaev1
1Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, Eindhoven 5600 MB, The Netherlands.
氧化铜 (CuO) 前体颗粒的大小会影响CO电还原到C2+产品. 较小的CuO粒子导致更多的,而中型的CuO粒子由于表面缺陷而产生更高的C2+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:
- 铜 (Cu) 催化对于将二氧化碳 (CO2) 电降解为有价值的C-C结合产品至关重要.
- 一氧化碳 (CO) 是这一过程中的关键中间体,其电还原 (CORR) 选择性至关重要.
研究的目的:
- 研究铜氧化物 (CuO) 前体的颗粒大小如何影响CO (CORR) 到C2+产品的直接电还原.
- 确定前体颗粒大小,由此产生的金属铜 (Cu) 颗粒特性和产品选择性之间的关系.
主要方法:
- 准备的CuO纳米粒子 (4-30纳米) 使用火焰喷雾热解.
- 使用现场同步广角X射线散射 (WAXS),准现场X射线光电子光谱和传输电子显微镜.
- 通过循环电量计 (CV) 与WAXS结合分析了电化学氧化.
主要成果:
- 不管CuO的初始大小,CuO前体转化为~30nm金属Cu粒子,具有~17nm晶体域,不论CuO的初始大小.
- 从10-20纳米 CuO 前体中获得的Cu显示出最高的C2+选择性 (60%法拉第效率).
- 从<10nm CuO前体中衍生出的Cu有利于的演化,这归因于较高密度的低协调表面缺陷.
结论:
- 电化学降解CuO前体导致显著重组到类似大小的Cu颗粒.
- 在CORR中的性能差异与表面缺陷类型和度在产生的Cu粒子上的变化有关.
- 表面结构在确定二氧化碳二元化 (C2+产物) 和演变之间的竞争中起着至关重要的作用.
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