Tremendous efforts have been made in developing highly selective catalysts for electrochemical CO 2 conversion to formate. However, the rapid deactivation resulting from structural reconstruction and phase transition poses considerable challenges to the system's durability, particularly at industrially relevant current densities. In this study, we develop a stable hexagonal phase ( g-In 2 S 3 ) catalyst, demonstrating exceptional selectivity toward formate production with a Faradaic efficiency exceeding 90% across a broad current range from - 100 to - 1,300 mA cm - 2 . Theoretical calculations suggest that the formation of sulfur (S) vacancy in g-In 2 S 3 is impeded under CO 2 reduction conditions, thereby contributing to enhanced electrode stability during electrolysis. Further mechanism studies reveal that the persistence of the S atom enables electron -enriched indium (In) -active sites, likely modifying the adsorption/desorption of the key intermediates for formate production. When coupled with a commercial GaInP/GaAs/Ge triple -junction solar cell, the solar -assisted CO 2 electrolysis reaches a benchmark solar -to -formate conversion efficiency of 14.3% under standard illumination.
WOS:001243654700001
2024-05-15
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Funder | Grant Number |
National Key Research and Development Program of China | 2021YFF0500503 |
Joint Funds of the National Natural Science Foundation of China | U21A2072 |
National Natural Science Foundation of China | 62274099 |
Overseas Expertise Introduction Project for Discipline Innovation of Higher Education of China | B16027 |
Tianjin Science and Technology Project | 18ZXJMTG00220 |
Key R&D Program of Hebei Province | 19214301D |
Natural Science Foundation of Tianjin | 20JCQNJC02070 |
Haihe Laboratory of Sustainable Chemical Transformations | |
Fundamental Research Funds for the Central Universities, Nankai University | |