Feng Jiaqi, Wu Limin, Song Xinning, Zhang Libing, Jia Shunhan, Ma Xiaodong, Tan Xingxing, Kang Xinchen, Zhu Qinggong, Sun Xiaofu, Han Buxing
Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
College of Chemical Engineering and Environment, China University of Petroleum (Beijing), Beijing, 102249, China.
Nat Commun. 2024 Jun 6;15(1):4821. doi: 10.1038/s41467-024-49308-8.
Achieving satisfactory multi-carbon (C) products selectivity and current density under acidic condition is a key issue for practical application of electrochemical CO reduction reaction (CORR), but is challenging. Herein, we demonstrate that combining microenvironment modulation by porous channel structure and intrinsic catalytic activity enhancement via doping effect could promote efficient CORR toward C products in acidic electrolyte (pH ≤ 1). The La-doped Cu hollow sphere with channels exhibits a C products Faradaic efficiency (FE) of 86.2% with a partial current density of -775.8 mA cm. CO single-pass conversion efficiency for C products can reach 52.8% at -900 mA cm. Moreover, the catalyst still maintains a high C FE of 81.3% at -1 A cm. The channel structure plays a crucial role in accumulating K and OH species near the catalyst surface and within the channels, which effectively suppresses the undesired hydrogen evolution and promotes C-C coupling. Additionally, the La doping enhances the generation of *CO intermediate, and also facilitates C products formation.
在酸性条件下实现令人满意的多碳（C）产物选择性和电流密度是电化学CO还原反应（CORR）实际应用中的关键问题，但具有挑战性。在此，我们证明，通过多孔通道结构进行微环境调控与通过掺杂效应增强本征催化活性相结合，可以促进在酸性电解质（pH≤1）中高效地将CORR转化为C产物。具有通道的La掺杂Cu空心球表现出86.2%的C产物法拉第效率（FE），部分电流密度为-775.8 mA cm。在-900 mA cm下，C产物的CO单程转化效率可达52.8%。此外，该催化剂在-1 A cm下仍保持81.3%的高C FE。通道结构在催化剂表面和通道内积累K和OH物种方面起着关键作用，有效抑制了不希望的析氢反应并促进了C-C偶联。此外，La掺杂增强了*CO中间体的生成，也促进了C产物的形成。
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