Huang Xuewei, Li Xinwei, Yan Shuhao, Wang Dawei, Long Chang, Ying Yue, An Pengfei, Guo Zhiyu, Li Qun, Yang Caoyu, Chen Sheng, Han Jianyu, Chang Lin, Lu Siyu, Tang Zhiyong
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, P. R. China.
Department of Criminal Science and Technology, Henan Police College, Zhengzhou 450046, P. R. China.
Sci Adv. 2025 Sep 12;11(37):eads0609. doi: 10.1126/sciadv.ads0609.
Electrocatalytic carbon dioxide (CO) reduction holds the great potential to convert excess emissions of carbon footprint into high value-added chemicals, but its activity, selectivity, stability, and reproducibility are still far away from satisfactory. The molecular catalysts with precise structures are unique platform to decipher the electrocatalytic mechanism, but they usually suffer from low performance. Herein, we report a strain-optimized dual copper complex immobilized in mesoporous carbon, which exhibits remarkable ethylene (CH) Faradaic efficiency (FE) up to 49.9% along with a multicarbon (C) product's FE up to 65.2% at -1.19 volts versus reversible hydrogen electrode. Concurrently, the catalyst displays considerable stability for 15 hours at a full cell potential of -3.1 volts. The density functional theory calculation reveals that the strain effect imposed by mesoporous carbon regulates the neighboring dual copper sites in the electrocatalyst to decrease the energy barrier of rate-determining step (*COCO → *COCOH), thus significantly promoting ethylene production.
电催化二氧化碳(CO)还原具有将过量的碳足迹排放转化为高附加值化学品的巨大潜力,但其活性、选择性、稳定性和重现性仍远不能令人满意。具有精确结构的分子催化剂是解读电催化机理的独特平台,但它们通常性能较低。在此,我们报道了一种固定在介孔碳中的应变优化双铜配合物,在相对于可逆氢电极-1.19伏的电位下,其乙烯(CH)法拉第效率(FE)高达49.9%,多碳(C)产物的FE高达65.2%。同时,该催化剂在-3.1伏的全电池电位下显示出15小时的可观稳定性。密度泛函理论计算表明,介孔碳施加的应变效应调节了电催化剂中相邻的双铜位点,降低了速率决定步骤(*COCO → *COCOH)的能垒,从而显著促进了乙烯的生成。