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Subsurface engineering for directional-selective CO₂-to-ethanol electrocatalysis at industrial-level
Ming-Zheng Gu1, Yuan Min2, Ling Jiang1
1Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Key Laboratory of Molecule-Based Materials, Anhui Engineering Research Center of Carbon Neutrality, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui, China.
A new subsurface cobalt-doped copper sulfide (Co-Sub-CuS) catalyst enhances selectivity for electroreduction of carbon dioxide (CO2) to ethanol. This catalyst improves intermediate conversion and C-C coupling for efficient and stable ethanol production.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
Background:
- Controlling selectivity in CO2 electroreduction to ethanol is challenging due to intermediate adsorption.
- The branching pathway following C-C coupling limits directed selectivity.
Purpose of the Study:
- To develop a catalyst for directed selectivity in CO2 electroreduction to ethanol.
- To elucidate the mechanism of subsurface doping in enhancing catalyst performance.
Main Methods:
- Synthesis of subsurface Co-doped CuS (Co-Sub-CuS) catalyst.
- Theoretical calculations and in-situ isotopic spectroscopy.
- Electrochemical testing in a membrane electrode assembly electrolyzer.
Main Results:
- Co-Sub-CuS exhibits directed selectivity toward ethanol.
- Subsurface doping enhances oxophilicity and facilitates intermediate conversion via surface-O bonds.
- Surface sulfur vacancies regulate dual-site distance for asymmetric C-C coupling.
- Achieved 78.7% ethanol Faradaic efficiency at 550.9 mA cm⁻² and 305 h stability at 700 mA cm⁻².
Conclusions:
- Subsurface doping provides a rational design strategy for selective CO2 electroreduction catalysts.
- The Co-Sub-CuS catalyst demonstrates high efficiency and stability for ethanol production.
- Understanding intermediate conversion pathways is crucial for catalyst development.
