The performance of Fe-based heterogeneous Fenton catalysts is apparently affected by the electron density of Fe active site. Herein, we modulate the active site electronic density of the FeC-based catalyst by surface sulfidation to improve HO activation property. After sulfidation, the removal of acetaminophen (APAP) increased from 27.1% to 100%, and the degradation rate constant of APAP increased 5.44-fold. Sulfidation enhances the utilization of HO and improves the generation of active species. Theoretical calculations demonstrated that sulfidation increases the electron density of Fe sites and lowers the band gap between the d-band center and Fermi energy level, facilitating electron transfer and HO activation. The change in cleavage position of HO from O-H to O-O after sulfidation provides additional evidence for the increased generation of •OH. These results elucidate the promoting effect of sulfidation on heterogeneous Fenton catalysts and provide a strategy for improving the performance of catalyst and contaminant removal.

中文翻译：

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通过表面硫化调节 Fe3C 基催化剂的电子结构以促进 H2O2 活化


Fe基多相Fenton催化剂的性能明显受到Fe活性位点电子密度的影响。在此，我们通过表面硫化来调节FeC基催化剂的活性位点电子密度，以提高H2O活化性能。硫化后，对乙酰氨基酚（APAP）的去除率从27.1%提高到100%，APAP的降解速率常数提高5.44倍。硫化提高了 H2O 的利用率并提高了活性物质的生成。理论计算表明，硫化增加了Fe位点的电子密度，降低了d带中心和费米能级之间的带隙，有利于电子转移和H2O活化。硫化后H2O裂解位置从O-H变为O-O的变化为•OH的生成增加提供了额外的证据。这些结果阐明了硫化对非均相芬顿催化剂的促进作用，并为提高催化剂性能和污染物去除提供了策略。