Yan Xupeng, Chen Chunjun, Wu Yahui, Liu Shoujie, Chen Yizhen, Feng Rongjuan, Zhang Jing, Han Buxing
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 P. R. China
University of Chinese Academy of Sciences Beijing 100049 China.
Chem Sci. 2021 Mar 30;12(19):6638-6645. doi: 10.1039/d1sc01117k.
Electrocatalytic reduction of CO into multicarbon (C) products powered by renewable electricity offers one promising method for CO utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO/CuO) and showed an outstanding catalytic performance for C products. The faradaic efficiency of the C products could reach 75.2% with a current density of 1.21 A cm. experiments and density functional theory (DFT) calculations demonstrated that the interface between CeO and Cu and the subsurface CuO coexisted in CeO/CuO during CORR and two competing pathways for C-C coupling were promoted separately, of which hydrogenation of *CO to *CHO is energetically favoured. In addition, the introduction of CeO also enhanced water activation, which could accelerate the formation rate of *CHO. Thus, the selectivity and activity for C products over CeO/CuO can be improved simultaneously.
由可再生电力驱动的将CO电催化还原为多碳（C）产物为CO的利用提供了一种有前景的方法，并促进了环境条件下可再生能源的存储。然而，在制造有价值的C产物时，在平衡选择性和活性之间仍然存在两难困境。在这项工作中，氧化铈与CuO结合（CeO/CuO），并对C产物表现出出色的催化性能。C产物的法拉第效率在电流密度为1.21 A cm时可达到75.2%。实验和密度泛函理论（DFT）计算表明，在CO还原反应（CORR）过程中，CeO与Cu之间的界面和次表面CuO在CeO/CuO中共存，并且分别促进了两种C-C偶联的竞争途径，其中CO加氢生成CHO在能量上更有利。此外，CeO的引入还增强了水的活化，这可以加速*CHO的形成速率。因此，CeO/CuO对C产物的选择性和活性可以同时提高。
