原位铜刻面可实现高效的一氧化碳/二氧化碳电解。
In situ copper faceting enables efficient CO/CO electrolysis.
作者信息
Yao Kaili, Li Jun, Ozden Adnan, Wang Haibin, Sun Ning, Liu Pengyu, Zhong Wen, Zhou Wei, Zhou Jieshu, Wang Xi, Liu Hanqi, Liu Yongchang, Chen Songhua, Hu Yongfeng, Wang Ziyun, Sinton David, Liang Hongyan
机构信息
School of Materials Science and Engineering, Tianjin University, Tianjin, 300350, China.
Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
出版信息
Nat Commun. 2024 Feb 26;15(1):1749. doi: 10.1038/s41467-024-45538-y.
The copper (Cu)-catalyzed electrochemical CO reduction provides a route for the synthesis of multicarbon (C) products. However, the thermodynamically favorable Cu surface (i.e. Cu(111)) energetically favors single-carbon production, leading to low energy efficiency and low production rates for C products. Here we introduce in situ copper faceting from electrochemical reduction to enable preferential exposure of Cu(100) facets. During the precatalyst evolution, a phosphate ligand slows the reduction of Cu and assists the generation and co-adsorption of CO and hydroxide ions, steering the surface reconstruction to Cu (100). The resulting Cu catalyst enables current densities of > 500 mA cm and Faradaic efficiencies of >83% towards C products from both CO reduction and CO reduction. When run at 500 mA cm for 150 hours, the catalyst maintains a 37% full-cell energy efficiency and a 95% single-pass carbon efficiency throughout.
铜（Cu）催化的电化学CO还原为多碳（C）产物的合成提供了一条途径。然而，热力学上有利的Cu表面（即Cu(111)）在能量上有利于单碳产物的生成，导致C产物的能量效率低和生产率低。在这里，我们引入了从电化学还原开始的原位铜刻面，以实现Cu(100)晶面的优先暴露。在预催化剂演化过程中，磷酸配体减缓了Cu的还原，并协助CO和氢氧根离子的生成和共吸附，引导表面重构为Cu(100)。所得的Cu催化剂对于CO还原和CO₂还原生成C产物的电流密度>500 mA cm⁻²，法拉第效率>83%。当在500 mA cm⁻²下运行150小时时，该催化剂始终保持37%的全电池能量效率和95%的单程碳效率。
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