高密度分散可控碳基单原子钴催化过硫酸盐去除水中抗生素机理研究

鉴于抗生素在天然环境中的不断检出给水污染控制带来了新的挑战，迫切需要研究水中抗生素去除的深度处理工艺，控制工业、生活和医药废水中抗生素的排放，对保护水环境具有重要意义。本课题以水中典型抗生素的去除为出发点，开发催化性能优异的高密度分散可控生物炭基单原子钴催化剂（Co-HSACs），以实现抗生素的高效去除。结合理论计算、材料表征及催化性能，探究吸附法合成条件对Co-HSACs形貌、 结构、组成、原子分散性和性质的影响。应用最优材料，全面研究该材料催化激发过硫酸盐去除典型抗生素（以β-内酰胺类为代表）的行为；并基于密度泛函理论（DFT）的分子动力学和量子化学计算，建立抗生素受活性氧物种攻击的降解模型，预测材料的催化位点以及抗生素的活性反应位点，以此揭示Co-HSACs、过硫酸盐与抗生素的三者之间的界面反应机理。项目旨在为功能材料加成高级氧化技术净化水中有机污染物的应用提供理论依据和技术支撑。

In view of the continuous detection of antibiotics in natural environment, which has brought new challenges for the water pollution control, there is an urgent need to develop advanced treatment technologies for the removal of antibiotics to eliminate the discharge of antibiotics from industrial, domestic and medical wastewater, and to protect the water environment. In this work, we will develop high-density and high-dispersion single-Co atom catalysts based on biochar (Co-HSACs) with excellent performance for the efficient removal of antibiotics. The key properties of Co-HSACs will be investigated, i.e., morphology, structure, composition based on the theoretical calculation, dispersion of single-atom, characterizations, and catalytic experiments. In addition, β-lactam antibiotics are selected as the model pharmaceutically active compounds. The radicals including hydroxyl and sulfate generation via activation of peroxymonosulfate (PMS) by Co-HSACs will be evaluated. Furthermore, mechanism of radical attacking, the active sites of antibiotics, and quantitative structure-activity relationship (QSAR) will be clarified based on the ab-initio molecular dynamics and density functional theory (DFT). Then the mechanism of interface reaction among Co-HSACs, sulfate radicals and antibiotics will be proposed. The overall objective of this research is to provide theoretical and technical supports to materials enhanced PMS-involved advanced oxidation process for antibiotics removal in water purification area.