Liu Xinzheng, Wang Wenwen, Wan Li, Hu Yubin, Xia Chenghui, Cao Lixin, Dong Bohua
School of Materials Science and Engineering, Ocean University of China, 1299 Sansha Road, Qingdao, Shandong Province, 266400, P. R. China.
Institute of Marine Science and Technology, Shandong University, 72 Coastal Highway, Qingdao, 266237, P. R. China.
Small. 2024 Dec;20(51):e2406012. doi: 10.1002/smll.202406012. Epub 2024 Oct 12.
The application of thermodynamically more favorable sulfur oxidation reaction (SOR) to replace oxygen evolution reaction (OER) in electrocatalytic water electrolysis is an appealing strategy to achieve low-energy hydrogen production while removing toxic sulfur ions from wastewater. However, the study of SOR catalysts with both activity and stability still faces great challenges. Herein, this study prepares partially amorphous Ru-doped CoSe (pa-Ru-CoSe) nanoparticles for SOR. The doping of Ru keeps Co in an electron-deficient state, which enhances the adsorption of SOR intermediates and improves the catalytic activity. Meanwhile, the partially amorphous selenide possesses great corrosion resistance to sulfur species, thus ensuring stability in long-term SOR. In addition, the pa-Ru-CoSe requires only 0.566 V to reach a current density of 100 mA cm in the SOR-HER coupled system and remains stable for 200 h. This work provides a promising partially amorphous strategy for SOR catalysts with both catalytic activity and long-term stability, enabling hydrogen production with low energy consumption and simultaneous sulfur production.
在电催化水电解中应用热力学上更有利的硫氧化反应（SOR）来替代析氧反应（OER），是一种在从废水中去除有毒硫离子的同时实现低能耗制氢的有吸引力的策略。然而，开发兼具活性和稳定性的SOR催化剂仍面临巨大挑战。在此，本研究制备了用于SOR的部分非晶态Ru掺杂CoSe（pa-Ru-CoSe）纳米颗粒。Ru的掺杂使Co处于缺电子状态，增强了SOR中间体的吸附并提高了催化活性。同时，部分非晶态硒化物对硫物种具有很强的耐腐蚀性，从而确保了长期SOR过程中的稳定性。此外，在SOR-析氢反应（HER）耦合系统中，pa-Ru-CoSe达到100 mA cm的电流密度仅需0.566 V，并且能保持200 h的稳定性。这项工作为兼具催化活性和长期稳定性的SOR催化剂提供了一种有前景的部分非晶态策略，实现了低能耗制氢并同时生成硫磺。
