The role of in situ generated morphological motifs and Cu(i) species in C2+ product selectivity during CO2 pulsed electroreduction
The role of in situ generated morphological motifs and Cu(i) species in C2+ product selectivity during CO2 pulsed electroreduction
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DOI：
10.1038/s41560-020-0594-9
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发表时间：
2020-03-30
期刊：
影响因子：
56.7
通讯作者：
Roldan Cuenya, Beatriz
中科院分区：
文献类型：
--
作者：
Aran-Ais, Rosa M.;Scholten, Fabian;Roldan Cuenya, Beatriz
使用铜催化剂可以将二氧化碳电催化还原为燃料，但决定这些材料对特定产品的选择性的关键特征仍然不确定。Aran-Ais等人使用原位方法探索了形态和氧化态对铜催化剂性能的影响。CO2的高效电化学转化为燃料和原料提供了一条途径。众所周知，铜催化剂对多碳产物具有选择性，但其表面结构和氧化物的存在所起的作用还不完全清楚。在这里，我们报告了通过脉冲CO2电解调整铜催化剂的形态和氧化态来提高乙醇的效率。我们建立了C2+产物（76%乙烯、乙醇和正丙醇在-1.0 V下相对于可逆氢电极）的增强的产生与Cu（100）上的（100）阶地、Cu 2 O和缺陷的存在之间的相关性。我们通过循环伏安曲线和非原位原子力显微镜数据分析监测催化剂形态的演变，而表面的化学状态通过准原位X射线光电子能谱检查。我们发现，缺陷和Cu（i）物种的连续再生协同有利于C-C耦合途径。
Carbon dioxide can be reduced electrocatalytically to fuels using copper catalysts, but the key features that determine the selectivity of these materials to specific products remains uncertain. Here Aran-Ais et al. use in situ methods to explore the influence of morphology and oxidation state on the performance of copper catalysts.The efficient electrochemical conversion of CO2 provides a route to fuels and feedstocks. Copper catalysts are well-known to be selective to multicarbon products, although the role played by the surface architecture and the presence of oxides is not fully understood. Here we report improved efficiency towards ethanol by tuning the morphology and oxidation state of the copper catalysts through pulsed CO2 electrolysis. We establish a correlation between the enhanced production of C2+ products (76% ethylene, ethanol and n-propanol at -1.0 V versus the reversible hydrogen electrode) and the presence of (100) terraces, Cu2O and defects on Cu(100). We monitored the evolution of the catalyst morphology by analysis of cyclic voltammetry curves and ex situ atomic force microscopy data, whereas the chemical state of the surface was examined via quasi in situ X-ray photoelectron spectroscopy. We show that the continuous regeneration of defects and Cu(i) species synergistically favours C-C coupling pathways.