浙江大学张兵团队报道了高熵硫化物催化剂促进硫代硫酸盐的节能电化学增值与制氢。相关研究成果于2024年7月31日发表在国际知名学术期刊《德国应用化学》。

电化学亚砜氧化反应（SOR）为富硫废水处理提供了一种可持续的策略，可以与阴极析氢反应（HER）结合，实现节能制氢。然而，硫物种的腐蚀和钝化导致催化SOR性能较差，氧化产物多硫化物需要进一步酸化以回收廉价的元素硫。

该文中，研究人员报道了一种用于SOR的CuCoNiMnCrSx纳米片在泡沫镍（CuCoNiMn CrSx/NF）上原位生长的非晶态高熵硫化物催化剂，该催化剂实现了0.25 V的超低电势，可提供100 mA cm^-2，并在高达1 A cm^-2的条件下稳定电解100小时。这些是由Cu⁺位点周围的操纵化学环境和构建的“软酸”到“硬酸”吸附/解吸位点赋予的，能够协同促进SOR过程中硫物种的吸附/解吸过程。此外，研究人员开发了一种电化学化学串联工艺，将亚砜转化为增值硫代硫酸盐，为同时利用废水和生产氢气提供了良好的选择。

附：英文原文

Title: High-entropy Sulfide Catalyst Boosts Energy-saving Electrochemical Sulfion Upgrading to Thiosulfate Coupled with Hydrogen Production

Author: Yuhou Pei, Di Li, Chuntian Qiu, Liang Yan, Zongmiao Li, Zexin Yu, Wenzhang Fang, Yingying Lu, Bing Zhang

Issue&Volume: 2024-07-31

Abstract: Electrochemical sulfion oxidation reaction (SOR) offers a sustainable strategy for sulfion-rich wastewater treatment, which can couple with cathodic hydrogen evolution reaction (HER) for energy-saving hydrogen production. However, the corrosion and passivation of sulfur species render the inferior catalytic SOR performance, and the oxidation product, polysulfide, requires further acidification to recover cheap elementary sulfur. Here, we reported an amorphous high-entropy sulfide catalyst of CuCoNiMnCrSx nanosheets in-situ growth on the nickel foam (CuCoNiMnCrSx/NF) for SOR, which achieved an ultra-low potential of 0.25 V to afford 100 mA cm-2, and stable electrolysis at as high as 1 A cm-2 for 100 h. These were endowed by the manipulated chemical environments surrounding Cu+ sites and the constructed “soft-acid” to “hard-acid” adsorption/desorption sites, enabling synergistically boosted adsorption/desorption process of sulfur species during SOR. Moreover, we developed an electrochemical-chemical tandem process to convert sulfions to value-added thiosulfate, providing a good choice for simultaneous wastewater utilization and hydrogen production.

DOI: 10.1002/anie.202411977

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202411977