Zhong Dazhong, Zhao Zhi-Jian, Zhao Qiang, Cheng Dongfang, Liu Bin, Zhang Gong, Deng Wanyu, Dong Hao, Zhang Lei, Li Jingkun, Li Jinping, Gong Jinlong
Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Weijin Road 92, Tianjin, 300072, China.
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Yingze West Street 79, Taiyuan, 030024, Shanxi, China.
Angew Chem Int Ed Engl. 2021 Feb 23;60(9):4879-4885. doi: 10.1002/anie.202015159. Epub 2021 Jan 15.
Copper can efficiently electro-catalyze carbon dioxide reduction to C products (C H , C H OH, n-propanol). However, the correlation between the activity and active sites remains ambiguous, impeding further improvements in their performance. The facet effect of copper crystals to promote CO adsorption and C-C coupling and consequently yield a superior selectivity for C products is described. We achieve a high Faradaic efficiency (FE) of 87 % and a large partial current density of 217 mA cm toward C products on Cu(OH) -D at only -0.54 V versus the reversible hydrogen electrode in a flow-cell electrolyzer. With further coupled to a Si solar cell, record-high solar conversion efficiencies of 4.47 % and 6.4 % are achieved for C H and C products, respectively. This study provides an in-depth understanding of the selective formation of C products on Cu and paves the way for the practical application of electrocatalytic or solar-driven CO reduction.
铜能够高效地将二氧化碳电催化还原为含碳产物（C₂H₄、C₂H₅OH、正丙醇）。然而，活性与活性位点之间的关联仍不明确，这阻碍了其性能的进一步提升。阐述了铜晶体的晶面效应，该效应可促进CO吸附和C-C偶联，进而对含碳产物产生卓越的选择性。在流动电解槽中，相对于可逆氢电极，在仅为-0.54 V的电位下，我们在Cu(OH)₂-D上实现了对含碳产物87%的高法拉第效率（FE）和217 mA cm⁻²的大分电流密度。进一步与硅太阳能电池耦合后，对于C₂H₄和含碳产物，分别实现了创纪录的4.47%和6.4%的高太阳能转换效率。本研究深入理解了在铜上选择性形成含碳产物的过程，并为电催化或太阳能驱动的CO₂还原的实际应用铺平了道路。
