CoMo@SBA-15活化PMS去除双氯芬酸的性能与机理研究
- Performance and Mechanism Study of CoMo@SBA-15 Activated PMS for the Removal of Diclofenac
- 基金项目：“海洋环境安全与保障与岛礁可持续发展”重点专项(2021-01)
- 摘要：双氯芬酸（DCF）的广泛使用，严重威胁了水生态环境的健康发展。采用原位自燃法制备出钴钼双金属掺杂的复合催化剂材料（CoMo@SBA-15），通过TEM、BET、XRD、FT-IR等方法对催化剂进行表征，探究钴钼活性成分的负载情况，并考察其活化过一硫酸盐（PMS）降解 DCF的性能和影响因素。结果表明，CoMo@SBA-15/PMS体系对DCF具有较佳的降解效率，能在CoMo@SBA-15=0.075 g·L-1、PMS=0.5 mmol·L-1、pH=6~7、T=25 ℃的条件下，30 min内完全降解30mg·L-1的DCF。EPR、XPS和淬灭试验结果表明，硫酸根自由基SO4·- 和单线态氧1O2是起主要作用的活性物质，钼的引入显著提升了催化剂对PMS的催化性能。CoMo@SBA-15/PMS体系在循环试验和对其他有机染料和抗生素的实验中也展现出较好的稳定性和普适性，为进一步开发用于去除水中DCF的高级氧化技术提供了参考。
- Abstract：The widespread application of diclofenac (DCF) has caused severely adverse effects on aquatic ecosystems. A new cobalt-molybdenum doped CoMo@SBA-15 composite catalyst was synthesized by using an in-situ self-ignition method. The catalyst was characterized by using TEM, BET, XRD and FT-IR techniques, and the loading of cobalt and molybdenum active components in the catalyst were investigated. The performance and influencing factors of the catalyst in activating persulfate (PMS) for the degradation of DCF were then assessed. The results demonstrated that the CoMo@SBA-15/PMS system has exhibited optimal degradation efficiency towards DCF, achieving complete degradation of 30 mg·L-1 DCF within 30 minutes under conditions of 0.075 g·L-1 catalyst, 0.5 mmol·L-1PMS, 6.0~7.0 pH and 25°C temperature. Moreover, the results of EPR and XPS tests and quenching experiments indicated that sulfate radicals (SO4·-) and singlet oxygen (1O2) were the primary reactive matters, and the introduction of molybdenum could significantly enhance the catalyst's performance towards PMS. The CoMo@SBA-15/PMS system also showed good stability and universality in recycling tests and experiments of removing other organic dyes and antibiotics, which could be taking reference for further developing advanced oxidation technologies to remove DCF from wastewater.
