Liu Ying, Du Ningjie, Liu Xinru, Yao Ducheng, Wu Deli, Li Zhuo, Mao Shun
College of Environmental Science and Engineering, Biomedical Multidisciplinary Innovation Research Institute, Shanghai East Hospital, State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, 1239 Siping Road, Shanghai, 200092, China.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China.
Environ Sci Ecotechnol. 2023 Nov 11;19:100338. doi: 10.1016/j.ese.2023.100338. eCollection 2024 May.
Transition metal sulfides have garnered increasing attention for their role in persulfate activation, a crucial process in environmental remediation. However, the function of metal sulfides without reversible valence changes, such as ZnS, remains largely unexplored in this context. Here we report ZnS-embedded porous carbon (ZnS-C), synthesized through the pyrolysis of Zn-MOF-74 and dibenzyl disulfide. ZnS-C demonstrates remarkable activity in activating peroxydisulfate (PDS) across a wide pH range, enabling the efficient mineralization removal of bisphenol A (BPA). Through electrochemical investigation and theoretical simulations of charge density distributions, we unveil that the electron transfer from BPA to PDS mediated by the ZnS-C catalyst governs the reaction. This study, both in theory and experiment, demonstrates metal sulfide as electron pump that enhances electron transfer efficiency in PDS activation. These findings redefine the role of metal sulfide catalysts, shedding new light on their potential for regulating reaction pathways in PDS activation processes.
过渡金属硫化物因其在过硫酸盐活化中的作用而受到越来越多的关注,过硫酸盐活化是环境修复中的一个关键过程。然而,在这种情况下,诸如硫化锌等没有可逆价态变化的金属硫化物的功能在很大程度上仍未得到探索。在此,我们报道了通过热解锌基金属有机框架材料(Zn-MOF-74)和二苄基二硫合成的嵌入硫化锌的多孔碳(ZnS-C)。ZnS-C在很宽的pH范围内对过二硫酸盐(PDS)的活化表现出显著活性,能够高效矿化去除双酚A(BPA)。通过电化学研究和电荷密度分布的理论模拟,我们揭示了由ZnS-C催化剂介导的从BPA到PDS的电子转移控制着该反应。这项研究在理论和实验上均表明金属硫化物作为电子泵可提高PDS活化中的电子转移效率。这些发现重新定义了金属硫化物催化剂的作用,为其在PDS活化过程中调节反应途径的潜力提供了新的见解。