Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products

Jiaqi Feng; Libing Zhang; Shoujie Liu; Liang Xu; Xiaodong Ma; Xingxing Tan; Limin Wu; Qingli Qian; Tianbin Wu; Jianling Zhang; Xiaofu Sun; Buxing Han

doi:10.1038/s41467-023-40412-9

Modulating adsorbed hydrogen drives electrochemical CO₂-to-C₂ products

Nat Commun. 2023 Aug 1;14(1):4615. doi: 10.1038/s41467-023-40412-9.

Authors

Jiaqi Feng¹, Libing Zhang^{1

2}, Shoujie Liu³, Liang Xu¹, Xiaodong Ma^{1

2}, Xingxing Tan^{1

2}, Limin Wu^{1

2}, Qingli Qian^{1

2}, Tianbin Wu^{1

2}, Jianling Zhang^{1

2}, Xiaofu Sun^{4

5}, Buxing Han^{6

7

8}

Affiliations

¹ 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.
² School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
³ School of Materials Science and Engineering, Anhui University, Hefei, 230601, China.
⁴ 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. sunxiaofu@iccas.ac.cn.
⁵ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China. sunxiaofu@iccas.ac.cn.
⁶ 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. hanbx@iccas.ac.cn.
⁷ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China. hanbx@iccas.ac.cn.
⁸ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China. hanbx@iccas.ac.cn.

Abstract

Electrocatalytic CO₂ reduction is a typical reaction involving two reactants (CO₂ and H₂O). However, the role of H₂O dissociation, which provides active *H species to multiple protonation steps, is usually overlooked. Herein, we construct a dual-active sites catalyst comprising atomic Cu sites and Cu nanoparticles supported on N-doped carbon matrix. Efficient electrosynthesis of multi-carbon products is achieved with Faradaic efficiency approaching 75.4% with a partial current density of 289.2 mA cm^-2 at -0.6 V. Experimental and theoretical studies reveal that Cu nanoparticles facilitate the C-C coupling step through *CHO dimerization, while the atomic Cu sites boost H₂O dissociation to form *H. The generated *H migrate to Cu nanoparticles and modulate the *H coverage on Cu NPs, and thus promote *CO-to-*CHO. The dual-active sites effect of Cu single-sites and Cu nanoparticles gives rise to the catalytic performance.

Abstract

Grants and funding