Copper nanowire with enriched high-index facets for highly selective CO2 reduction
Copper nanowire with enriched high-index facets for highly selective CO2 reduction
复制标题
具有富集高折射率面的铜纳米线，用于高选择性二氧化碳减排
DOI：
10.1002/smm2.1082
复制
发表时间：
2022-03-01
期刊：
影响因子：
20.4
通讯作者：
Sun, Xiaoming
中科院分区：
文献类型：
--
作者：
Han, Lu;Tian, Benqiang;Sun, Xiaoming
将二氧化碳电还原为可再生能源燃料和原料是减少碳排放和解决能源危机的一条有吸引力的途径。然而，如何提高高价值多碳产品的选择性仍然是一个挑战。本研究证明，通过对铜纳米线进行简单的方波电位处理，可以设计和获得高折射率的铜晶体表面，这有利于提高多碳产物的选择性，特别是对乙烯的反应路线。C2+产物的法拉第效率可达近60%，氢气可抑制到20%以下。密度泛函理论（DFT）计算表明，（311）高指数facet可以有效激活CO2，促进*COCOH中间体在铜上吸附乙烯，从而提高乙烯的选择性，抑制竞争性析氢反应。该方法可推广到其他催化体系的设计中，对其他电化学催化反应有一定的启示。
Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis. However, how to improve the selectivity of high-value multicarbon products is still challenging. Here, we demonstrate that the high-index crystalline surface of copper could be designed and obtained through a simple square-wave potential treatment on copper nanowires, which is beneficial to improve the selectivity of multi-carbon products, especially the reaction route towards ethylene. The Faradaic efficiency of C2+ products can reach nearly 60%, and hydrogen can be suppressed to below 20%. Density functional theory (DFT) calculations reveal that (311) high-index facet can activate CO2 effectively and promote adsorption of the *COCOH intermediate on copper for ethylene formation, therefore improves the selectivity of ethylene and inhibits the competing hydrogen evolution reaction. This method can be extended to the design of other catalytic systems and has inspirations for other electrochemical catalytic reactions.