State Key Laboratory of Environmental Criteria and Risk Assessment, State Environmental Protection Key Laboratory of Drinking Water Source Protection, Research Centre of Lak Environment, National Engineering Laboratory for Lake Pollution Control and Ecological Restoration, Chinese Research Academy of Environmental Sciences, Beijing 100012, China; School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China.
College of Civil Engineering, Zhejiang University of Technology, Hangzhou 310023, China.
Environ Res. 2024 Sep 15;257:119348. doi: 10.1016/j.envres.2024.119348. Epub 2024 Jun 4.
In this study, a UV-driven photocatalytic activation of peroxymonosulfate (PMS) system was constructed using bimetallic metal-organic frameworks to degrade pharmaceuticals and personal care products (PPCPs). Mn-MIL-53(Fe) was successfully synthesised by adjusting the doping ratio of Mn using solvothermal method. The removal of ibuprofen (IBP) by UV/Mn-MIL-53(Fe)/PMS process was as high as 79.7% in 30 min with a Mn doping ratio of 1.0 (molar ratio of Mn to Fe), and the reaction rate constant was 26.9% higher than undoped. Mn-MIL-53(Fe) had been systematically characterized in terms of its physical structure, microscopic morphology, surface functional groups and photoelectric properties. The mechanism investigation revealed that the cycling of Mn and Fe accelerated the rate of electron transfer in the system, which significantly increased the activation efficacy of PMS to generate more hydroxyl and sulfate radicals for IBP degradation. A total of 13 transformation products were detected during the degradation of IBP by the UV/Mn-MIL-53(Fe)/PMS process. Theoretical calculations were used to predict the sites on the IBP molecule that were vulnerable to attack, and four possible degradation pathways were deduced. The excellent stability and efficient catalytic properties of Mn-MIL-53(Fe) provided a promising solution to the problem of water treatment contaminated with PPCPs.
在这项研究中,使用双金属金属有机骨架构建了一种光催化过一硫酸盐(PMS)体系,用于降解药品和个人护理产品(PPCPs)。通过溶剂热法调整 Mn 的掺杂比例成功合成了 Mn-MIL-53(Fe)。在 Mn 掺杂比为 1.0(Mn 与 Fe 的摩尔比)时,UV/Mn-MIL-53(Fe)/PMS 工艺在 30 分钟内可将布洛芬(IBP)的去除率高达 79.7%,反应速率常数比未掺杂时高 26.9%。从物理结构、微观形貌、表面官能团和光电性能等方面对 Mn-MIL-53(Fe)进行了系统的表征。机理研究表明,Mn 和 Fe 的循环加速了体系中电子转移的速率,这显著提高了 PMS 的活化效率,生成更多的羟基和硫酸根自由基用于 IBP 的降解。在 UV/Mn-MIL-53(Fe)/PMS 工艺降解 IBP 的过程中,共检测到 13 种转化产物。理论计算用于预测 IBP 分子上易受攻击的位点,并推断出四条可能的降解途径。Mn-MIL-53(Fe) 的优异稳定性和高效催化性能为处理受 PPCPs 污染的水提供了一种有前途的解决方案。