FeSeS@C cage-in-cage superlattices for peroxymonosulfate activation: Surface acidity regulates Fe spin state

Applied Catalysis B: Environment and Energy Pub Date : 2024-08-26 DOI:10.1016/j.apcatb.2024.124539

Qiang Zhong, Yan Xue, Zihao Qi, Yue Sun, Leliang Wu, Dunyu Sun, Chenmin Xu, Kwangchol Ri, Shaogui Yang, Jiandong Zhu, Qiuyi Ji, Yazi Liu, Shiyin Li, Huan He

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Abstract

Two-dimensional cage-in-cage carbon-coated FeSeS superlattices with varying degrees of sulfidation (FeSeS@C) are developed for activating peroxymonosulfate (PMS) to effectively degrade diatrizoic acid (DTZ), and the intrinsic origin that govern the activity of FeSeS@C are deeply elucidated. Experimental and theoretical analyses manifested that proper sulfidation led to increased surface acidity of FeSeS@C. The high surface acidity can optimize the exposure and spin state of Fe sites for FeSeS@C-4, a high spin state of Fe (6.27 μ) not only regulating PMS adsorption for enhancing the charge density, but also expediting interfacial charge deliver to trigger the efficient PMS activation. Therefore, among FeSeS@C, FeSeS@C-4 exhibited the best degradation performance for DTZ, with first-order kinetic rate constants (k) of 0.232 min and degradation rate of 100 %. This study demonstrates a novel application of cage-in-cage superlattices in environmental remediation and offers new insights into the mechanism of PMS activation by sulfur modification Fe-based catalysts.

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用于过氧化单硫酸盐活化的笼中笼超晶格 FeSeS@C：表面酸度调节铁的自旋态

实验和理论分析表明，适当的硫化可提高 FeSeS@C 的表面酸度。高表面酸度可以优化 FeSeS@C-4 的铁位点暴露和自旋态，高自旋态的铁位点（6.27 μ）不仅可以调节 PMS 的吸附以提高电荷密度，还可以加速界面电荷的传递，从而引发 PMS 的高效活化。因此，在 FeSeS@C 中，FeSeS@C-4 对 DTZ 的降解性能最好，一阶动力学速率常数（k）为 0.232 分钟，降解率为 100%。这项研究展示了笼中笼超晶格在环境修复中的新应用，并为硫改性铁基催化剂活化 PMS 的机理提供了新的见解。

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Applied Catalysis B: Environment and Energy

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