A green and efficient Fe/N/S co-doped carbon catalysts (ITC-X-800) was successfully prepared from Fe/N-rich salvaged cyanobacteria and thiourea for catalyzing peroxymonosulfate (PMS) to degradate hydroxychloroquine (HCQ). Characterization tests confirmed that defect degree, electron transfer capability, and the content of main functional groups like π-π*, Fe-N_X, graphitic N and thiophene S etc. in ITC-X-800 was firstly increased and then decreased with the increasing doping S, indicating the critical role of S for regulating functional sites containing Fe/N on the carbon nanosheets. Optimized ITC-2-800 with appropriate S showed suitable HCQ adsorption ability, lowest resistance and more PMS activation sites. Almost 100% of HCQ could be removed via ITC-2-800/PMS system in 60 min within 0.5 mM PMS and 0.1 g/L ITC-2-800, whose HCQ degradation kinetic constant was 2.5 times that of Fe/N doped carbon catalyst. Based on the basic strong electron transfer ability and HCQ adsorption affinity of π-π*, the high PMS adsorption and catalyzing capacity of Fe-N_X, and the extra enhanced carbon skeleton activation of thiophene S, the synergistic effect of these groups in ITC-2-800 was proved to play a more important role in enhanced PMS activation and HCQ degradation. Ascribed to the synergistic effect of Fe/N/S, non-radical pathway based on ¹O₂ and high-valent iron-oxo species played a dominant role in HCQ degradation. Furthermore, ITC-2-800 showed high universality, stability, reusability and potential practicability during comprehensive test. This study provided deeper insights for the resourceful treatment of algae mud and the synergistic mechanism of heteroatoms in carbon-based catalysts for PMS activation.

中文翻译：

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铁/氮/硫共掺杂蓝藻衍生的碳复合材料在过氧一硫酸盐基 fenton 样系统中通过初级非自由基途径增强羟氯喹降解


以富Fe/N回收的蓝藻和硫脲为原料，成功制备了绿色高效的Fe/N/S共掺杂碳催化剂（ITC-X-800），用于催化过氧一硫酸盐（PMS）降解羟氯喹（HCQ）。表征测试证实，ITC-X-800 中的缺陷程度、电子传递能力以及 π-π*、Fe-N _X 、石墨 N 和噻吩 S 等主要官能团的含量随着掺杂 S 的增加而先增加后降低，表明 S 在调控碳纳米片上含有 Fe/N 的功能位点中起着关键作用。具有适当 S 的优化 ITC-2-800 显示出合适的 HCQ 吸附能力、最低的电阻和更多的 PMS 激活位点。在 0.5 mM PMS 和 0.1 g/L ITC-2-800 中，通过 ITC-2-800/PMS 系统可在 60 分钟内去除几乎 100% 的 HCQ，其 HCQ 降解动力学常数是 Fe/N 掺杂碳催化剂的 2.5 倍。基于π-π*的基本强电子转移能力和HCQ吸附亲和力、Fe-N _X 的高PMS吸附和催化能力，以及噻吩S额外增强的碳骨架活化，这些基团在ITC-2-800中的协同作用被证明在增强PMS活化和HCQ降解中发挥了更重要的作用。归因于 Fe/N/S 的协同作用，基于 ¹ O ₂ 和高价铁-氧代物种的非自由基途径在 HCQ 降解中起主导作用。此外，ITC-2-800 在综合测试中表现出较高的通用性、稳定性、可重用性和潜在实用性。本研究为藻泥的资源处理和碳基催化剂中杂原子的协同机制用于 PMS 活化提供了更深入的见解。