Peng Chen, Zhu Xiaorong, Xu Zikai, Yan Shuai, Chang Lo Yueh, Wang Zhiqiang, Zhang Junbo, Chen Menghuan, Sham Tsun-Kong, Li Yafei, Zheng Gengfeng
Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai, 200438, China.
Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.
Small. 2022 Feb;18(8):e2106433. doi: 10.1002/smll.202106433. Epub 2021 Dec 12.
Electrochemical CO reduction to valuable multi-carbon (C ) products is attractive but with poor selectivity and activity due to the low-efficient CC coupling. Herein, a lithium vacancy-tuned Li CuO with square-planar [CuO ] layers is developed via an electrochemical delithiation strategy. Density functional theory calculations reveal that the lithium vacancies (V ) lead to a shorter distance between adjacent [CuO ] layers and reduce the coordination number of Li around each Cu, featuring with a lower energy barrier for COCO coupling than pristine Li CuO without V . With the V percentage of ≈1.6%, the Li CuO catalyst exhibits a high Faradaic efficiency of 90.6 ± 7.6% for C at -0.85 V versus reversible hydrogen electrode without iR correction, and an outstanding partial current density of -706 ± 32 mA cm . This work suggests an attractive approach to create controllable alkali metal vacancy-tuned Cu catalytic sites toward C products in electrochemical CO reduction.
通过电化学CO还原制备有价值的多碳（C）产物很有吸引力，但由于CC耦合效率低，其选择性和活性较差。在此，通过电化学脱锂策略开发了一种具有平面正方形[CuO ]层的锂空位调谐Li CuO。密度泛函理论计算表明，锂空位（V ）导致相邻[CuO ]层之间的距离缩短，并降低了每个Cu周围Li的配位数，与没有V 的原始Li CuO相比，其COCO耦合的能垒更低。在V 百分比约为1.6%时，Li CuO催化剂在相对于可逆氢电极-0.85 V且无iR校正的条件下，对C的法拉第效率高达90.6 ± 7.6%，并且具有-706 ± 32 mA cm 的出色分电流密度。这项工作提出了一种有吸引力的方法，即在电化学CO还原中创造可控的碱金属空位调谐Cu催化位点以制备C产物。
