在具有高转化率的晶面选择性铜膜上实现高效的CO电还原。

Efficient CO electroreduction on facet-selective copper films with high conversion rate.

作者信息

Zhang Gong, Zhao Zhi-Jian, Cheng Dongfang, Li Huimin, Yu Jia, Wang Qingzhen, Gao Hui, Guo Jinyu, Wang Huaiyuan, Ozin Geoffrey A, Wang Tuo, Gong Jinlong

机构信息

School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.

Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin, 300072, China.

出版信息

Nat Commun. 2021 Sep 30;12(1):5745. doi: 10.1038/s41467-021-26053-w.

Tuning the facet exposure of Cu could promote the multi-carbon (C2+) products formation in electrocatalytic CO reduction. Here we report the design and realization of a dynamic deposition-etch-bombardment method for Cu(100) facets control without using capping agents and polymer binders. The synthesized Cu(100)-rich films lead to a high Faradaic efficiency of 86.5% and a full-cell electricity conversion efficiency of 36.5% towards C2+ products in a flow cell. By further scaling up the electrode into a 25 cm membrane electrode assembly system, the overall current can ramp up to 12 A while achieving a single-pass yield of 13.2% for C2+ products. An insight into the influence of Cu facets exposure on intermediates is provided by in situ spectroscopic methods supported by theoretical calculations. The collected information will enable the precise design of CO reduction reactions to obtain desired products, a step towards future industrial CO refineries.

调节铜的晶面暴露可以促进电催化CO还原中多碳（C2+）产物的形成。在此，我们报告了一种动态沉积-蚀刻-轰击方法的设计与实现，该方法无需使用封端剂和聚合物粘合剂即可控制Cu(100)晶面。合成的富含Cu(100)的薄膜在流动池中对C2+产物的法拉第效率高达86.5%，全电池电转换效率为36.5%。通过将电极进一步扩大到25平方厘米的膜电极组件系统，总电流可以增加到12 A，同时C2+产物的单程产率达到13.2%。理论计算支持的原位光谱方法揭示了铜晶面暴露对中间体的影响。所收集的信息将有助于精确设计CO还原反应以获得所需产物，这是迈向未来工业CO精炼厂的一步。