Dual-Site Activation for Efficient Acidic CO2 Electroreduction at Industrial-Level Current Densities

Shanshan Wu; Shuhui Li; Zhuoyue Hou; Yang Hu; Zhuang Zhang; Jiamin Zhu; Shaowen Xu; Rui Wang; Nan Zhang; Li An; Pinxian Xi; Chun-Hua Yan

doi:10.1002/adma.202503772

Dual-Site Activation for Efficient Acidic CO₂ Electroreduction at Industrial-Level Current Densities

Adv Mater. 2025 Jun 26:e2503772. doi: 10.1002/adma.202503772. Online ahead of print.

Authors

Shanshan Wu¹, Shuhui Li¹, Zhuoyue Hou¹, Yang Hu¹, Zhuang Zhang¹, Jiamin Zhu¹, Shaowen Xu¹, Rui Wang¹, Nan Zhang¹, Li An¹, Pinxian Xi^{1

2}, Chun-Hua Yan^{1

3}

Affiliations

¹ State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, P. R. China.
² State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou Research Institute of Rare Earths, Baotou, 014030, P. R. China.
³ Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.

PMID: 40574408
DOI: 10.1002/adma.202503772

Abstract

Electroreduction of CO₂ to formic acid in acidic media offers a promising approach for value-added CO₂ utilization. However, achieving high selectivity for formic acid in acidic electrolytes remains challenging due to the competitive hydrogen evolution reaction (HER), particularly at industrially relevant current densities. Herein, a charge redistribution modulation strategy is demonstrated by constructing the CuS /SnS₂ Mott-Schottky catalyst to enhance formic acid selectivity. Experiments and calculation results reveal the broadening of Sn orbitals and reduced orbital symmetry of Sn orbitals contribute to enhanced CO₂ adsorption, while the modulated Cu sites with a stronger Lewis acid character stabilize ^*OCHO intermediates more effectively. This enables dual-site activation for efficient CO₂ electroreduction into formic acid synthesis. Consequently, the optimized CuS/SnS₂ catalysts achieve a maximum formic acid Faradaic efficiency (FE) of 99% in acidic electrolytes and maintain selectivity above 80% at a current density of 1 A cm^-2, significantly surpassing the performance of CuS and SnS₂ alone. Moreover, the excellent selectivity across pH-universal electrolytes demonstrates that dual-site activation is a promising strategy for designing highly efficient CO₂ reduction reaction catalysts.

Keywords: CO2 reduction reaction; dual‐site; interface structure; sulfides.

Abstract

Grants and funding