材料科学
电催化剂
乙醇
还原(数学)
乙醇燃料
无机化学
化学工程
纳米技术
电化学
电极
物理化学
有机化学
几何学
数学
工程类
化学
作者
Ting Wang,Xinyi Duan,Rui Bai,Haoyang Li,Qin Chen,Jian Zhang,Zhiyao Duan,Kai‐Jie Chen,Fuping Pan
标识
DOI:10.1002/adma.202410125
摘要
Abstract The electroreduction of CO 2 offers a sustainable route to generate synthetic fuels. Cu‐based catalysts have been developed to produce value‐added C 2+ alcohols; however, the limited understanding of complex C−C coupling and reaction pathway hinders the development of efficient CO 2 ‐to‐C 2+ alcohols catalysts. Herein, a Cu‐free, highly mesoporous NiO catalyst, derived from the microphase separation of a block copolymer, is reported, which achieves selective CO 2 reduction toward ethanol with a Faradaic efficiency of 75.2% at −0.6 V versus RHE. The dense mesopores create a favorable local reaction environment with CO 2 ‐rich and H 2 O‐deficient interfaces, suppressing hydrogen evolution and maximizing catalytic activity of NiO for CO 2 reduction. Importantly, the C 1 ‐feeding experiments, in situ spectroscopy, and theoretical calculations consistently show that the direct coupling of *CO 2 and *COOH is responsible for C−C bond formation on NiO, and subsequent reduction of *CO 2 ‐COOH to ethanol is energetically facile through the *COCOH and *OC 2 H 5 pathway. The unconventional C−C coupling mechanism on NiO, in contrast to the *CO dimerization on Cu, is triggered by strong CO 2 adsorption on the polarized Ni 2+ ‐O 2− sites. The work not only demonstrates a highly selective Cu‐free Ni‐based alternative for CO 2 ‐to‐C 2+ alcohols transformation but also provides a new perspective on C−C coupling toward C 2+ synthesis.
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