Wang Min, Li Xiaoyao, Ma Xia, Wang Jie, Jin Xixiong, Zhang Lingxia, Shi Jianlin
Institution Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding-xi Road, Shanghai, 200050, P.R. China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, No. 19 A Yuquan Road, Beijing, 100049, P.R. China.
ChemSusChem. 2023 Dec 19;16(24):e202300879. doi: 10.1002/cssc.202300879. Epub 2023 Oct 9.
CO electroreduction into liquid fuels is of broad interest and benefits reducing the energy crisis and environment burdens. CuS has been reported to be a desirable candidate for CO electroreduction into formate; however, its formate selectivity and stability are still far from the demands of practical application. Herein, we report CuS nanoparticles exhibiting good Faradaic efficiency of formate (about 98 %) in CO electroreduction and its deactivation mechanism during the reaction. The deactivation of CuS was found to be associated with the reconstruction and S loss of CuS, which deteriorates the Faradaic efficiency of formate. Combined with ionic and gas analyses, the S atom in CuS was lost in the form of H S, SO , and SO , followed by the reconstruction of CuS into copper oxides. Such a catalyst reconstruction facilitates electroreductions of CO and H O, respectively, into CO and H , etc., resulting in the degradation of catalytical performance of CO electroreduction into formate. This work reveals the important role of S loss and reconstruction of metal sulfide catalysts during the electroreduction reaction, which may benefit the further development of CuS-based electro-catalyst for CO electroreduction.
将CO电还原为液体燃料备受关注，有利于缓解能源危机和减轻环境负担。据报道，CuS是将CO电还原为甲酸盐的理想候选材料；然而，其甲酸盐选择性和稳定性仍远未达到实际应用的要求。在此，我们报道了在CO电还原过程中表现出良好甲酸盐法拉第效率（约98%）的CuS纳米颗粒及其反应过程中的失活机制。发现CuS的失活与CuS的重构和硫损失有关，这会降低甲酸盐的法拉第效率。结合离子和气体分析，CuS中的硫原子以H₂S、SO₂和SO₃的形式损失，随后CuS重构为铜氧化物。这种催化剂重构分别促进了CO和H₂O向CO和H₂等的电还原，导致CO电还原为甲酸盐的催化性能下降。这项工作揭示了硫损失和金属硫化物催化剂重构在电还原反应中的重要作用，这可能有利于基于CuS的CO电还原电催化剂的进一步发展。
