Laboratory of Environmental Technology, INET, Tsinghua University, Beijing 100084, PR China.
Laboratory of Environmental Technology, INET, Tsinghua University, Beijing 100084, PR China; Beijing Key Laboratory of Radioactive Wastes Treatment, Tsinghua University, Beijing 100084, PR China.
Sci Total Environ. 2022 Jun 25;827:154379. doi: 10.1016/j.scitotenv.2022.154379. Epub 2022 Mar 6.
In this study cobalt sulfides (CoS) coated on the nitrogen and sulfur co-doped graphene (CoS@S-N-RG) was firstly prepared and used for degradation of antibiotic sulfamethoxazole (SMX). The results showed that SMX could be completely degraded by CoS@S-N-RG-activated peroxymonosulfate (PMS) within 20 min with its mineralization efficiency of 38.7%. The SMX degradation rate followed pseudo first-order kinetics with kinetic constant of 0.377 min that was higher than that induced by CoS, N-RG, S-N-RG and CoS@S-RG, indicating CoS@S-N-RG had superior catalytic activity. CoS@S-N-RG can activate PMS to produce sulfate radicals and hydroxyl radicals, while sulfate radicals played major role. CoS participated in PMS activation in which Co was involved in sulfate radicals formation, while sulfur species facilitated the conversion of Co to Co. In addition, carbon defects, CO, pyridinic N and pyrrolic N also contributed to PMS activation.The superior catalytic activity was attributed to the synergistic effect of CoS and S-N-RG. This study could provide an efficient and stable PMS activator, and insight into the PMS activation mechanism by CoS@S-N-RG.
在这项研究中,首次制备了钴硫化物(CoS)包覆在氮硫共掺杂石墨烯(CoS@S-N-RG)上,并将其用于降解抗生素磺胺甲恶唑(SMX)。结果表明,CoS@S-N-RG 活化过一硫酸盐(PMS)可在 20 分钟内完全降解 SMX,其矿化效率为 38.7%。SMX 的降解速率遵循拟一级动力学,动力学常数为 0.377 min,高于 CoS、N-RG、S-N-RG 和 CoS@S-RG 诱导的动力学常数,表明 CoS@S-N-RG 具有较高的催化活性。CoS@S-N-RG 可以活化 PMS 生成硫酸根自由基和羟基自由基,而硫酸根自由基起主要作用。CoS 参与 PMS 活化,其中 Co 参与硫酸根自由基的形成,而硫物种促进 Co 向 Co 的转化。此外,碳缺陷、CO、吡啶氮和吡咯氮也有助于 PMS 的活化。优异的催化活性归因于 CoS 和 S-N-RG 的协同作用。本研究可为高效稳定的 PMS 活化剂提供参考,并深入了解 CoS@S-N-RG 活化 PMS 的机制。