Zhang Renjie, Zhang Jianling, Song Yi, Yang Yisen, Li Meiling, Zhao Yingzhe, Teng Yunan, Han Buxing, Chen Zhongjun
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2025 Jul 28;64(31):e202501554. doi: 10.1002/anie.202501554. Epub 2025 Jul 1.
The efficient electrochemical CO reduction into value-added multi-carbon products is of great importance and remains challenging. Here, we demonstrate the highly selective, active, and long-term durable electrocatalytic production of ethylene from CO by constructing a CuO nano-homojunction, which is composed of CuO nanocubes in size of ≈100 nm and the surface-adhered CuO nanodots in size of ≈12 nm, as electrocatalyst. The maximum Faradaic efficiency of ethylene can reach 73.7% at -1.4 V versus reversible hydrogen electrode in H-type cell, with partial current density to ethylene of 38.2 mA cm. Moreover, it can work stably for more than 200 h at 0.31 A cm in membrane electrode assembly. The mechanism for the high selectivity, activity and stability for CO-to-ethylene conversion was investigated by in situ experiments and theoretical calculations. The results reveal that such a catalyst is efficient in adsorbing CO, stabilizing the key intermediate CO, and facilitating both the CO protonation to form CHO and the subsequent CO-CHO coupling for ethylene formation.
将电化学CO高效还原为增值多碳产物具有重要意义,但仍具有挑战性。在此,我们通过构建一种由尺寸约为100 nm的CuO纳米立方体和尺寸约为12 nm的表面附着CuO纳米点组成的CuO纳米同质结作为电催化剂,展示了从CO中高选择性、活性和长期耐用的乙烯电催化生产。在H型电池中,相对于可逆氢电极,在-1.4 V时乙烯的最大法拉第效率可达73.7%,乙烯的分电流密度为38.2 mA cm。此外,在膜电极组件中,它在0.31 A cm下可稳定工作超过200小时。通过原位实验和理论计算研究了CO转化为乙烯的高选择性、活性和稳定性的机制。结果表明,这种催化剂在吸附CO、稳定关键中间体CO以及促进CO质子化形成CHO和随后的CO-CHO偶联以形成乙烯方面是有效的。