新型Mn基材料催化去除水中抗生素抗性基因定量构效关系与微观机制

Aiming at addressing the issue that conventional sewage purification technologies can hardly eliminate antibiotic resistance genes (ARGs), the applicant provides a span-new proposal as to novel Mn-based materials (NMCs) for catalyzing peroxides to form reactive oxygen species with high oxidation abilities towards removing ARGs from wastewaters based on the principle that breaking or decomposing gene fragments can remove ARGs. This project will study the effects of the micro-structures/properties of NMCs, the types of ARGs and the water quality parameters on the removal of ARGs and the key factors controlling their removal. The quantitative structure-activity relationships (with respect to the micro-structures/properties of NMCs and the types of ARGs) regarding the removal of ARGs by NMCs-catalyzed peroxides will be established, followed by providing the kinetic models for describing the removal of ARGs under different processes. The interface processes and mechanisms on the removal of ARGs by NMCs-catalyzed peroxides will be probed, and the qualitative/quantitative relationships between the changes of the types/contents of ARGs and the changes of the amounts of microorganisms and 16S rRNA/rDNA in wastewaters will also be pinpointed with the intention of providing strategies against controlling the antibiotic resistance. The results of this study are expected to document the difficult issue of eliminating ARGs over the sewage deep purification processes, and meanwhile, the close links between the disciplines of novel materials for environmental catalysis, wastewater treatments, environmental microorganisms, and so on, will be established, which will undoubtedly provide scientific foundations and new perspectives for improving and innovating the principles and processes of sewage treatments for removing ARGs.

针对常规污水净化技术难以去除抗生素抗性基因（ARGs）的问题，申请者从破碎/降解基因片段去除ARGs的原理出发，提出新型Mn基材料（NMCs）催化过氧化物形成强氧化性的活性氧物种去除污水中ARGs新思路。项目将研究NMCs微结构性能、ARGs类型和水质条件对ARGs去除过程的影响规律及关键因子，建立“NMCs微结构性能和ARGs类型”响应的NMCs催化过氧化物去除ARGs定量构效关系以及反映ARGs不同去除过程的动力学模型，探明NMCs催化过氧化物去除ARGs界面过程与机制，明确污水中ARGs类型/含量与微生物总量和16S rRNA/rDNA之间定性/定量变化关系并提出抗性控制策略。研究结果可解决污水深度净化过程中ARGs难去除的问题，同时将在新型环境催化材料、污水处理、环境微生物等领域之间建立起密切关系，为完善和创新ARGs污水处理工艺与原理提供科学依据和新视角。

针对污水中新污染物（如抗生素抗性基因、抗生素、耐药菌等）难去除问题，开发一种新型高效类Fenton催化氧化体系具有明显的现实意义和技术需求。本项目开展了新型Mn基磁性材料、金属有机框架衍生毫米级铝基尖晶石微球和碳纳米管（CNTs）负载空间分隔型位点的量子点复合材料催化去除抗性素、抗性菌和抗性基因效能与机制的研究。首先，本项目利用各种合成工艺设计了具有不同结构性能的催化剂，具体如下：1）利用溶剂热耦合高温热解过程制备了具有不同微结构性能的棒状磁性Mn-Fe碳氧化物（mMFC），2）借助液相原位生长在γ-Al2O3活性载体上的ZIF-67，直接高温煅烧形成了毫米级CoAl2O4/Co2AlO4@Al2O3复合催化剂，3）以廉价、低毒溶剂甲酰胺作为氮源和金属离子螯合剂、CNTs为碳载体，通过一步聚合反应构建了具有空间分隔型位点的MnNx-CNTs、CoNx-CNTs和FeNx-CNTs量子点复合材料。.本项目完成的研究目标如下：1）探明了具有金属位点和非金属位点mMFC催化/激活过一硫酸盐（PMS）同时产生O2•‒、1O2、SO4•‒和•OH机制及其降解新污染相对贡献，2）系统探究了CoAl2O4/Co2AlO4@Al2O3毫米球催化PMS去除抗生素的构效关系、灭活抗性菌和去除抗性基因效能、及其相关机制，同时明确了CoAl2O4/Co2AlO4@Al2O3活性再生工艺，3）构建了新型MnNx-CNTs、CoNx-CNTs和FeNx-CNTs量子点复合材料介导的非自由基氧化体系，并研究了其去除有机新污染物、抗性菌和抗性基因的效能与机理。如上有关新型催化剂的设计与催化去除抗生素、耐药菌和抗性基因的研究工作可为污水中新污染物去除技术的革新提供理论支撑。.项目实施后，在具有国际影响力期刊发表SCI论文7篇，申请发明专利2项（其中1项已授权），邀请了抗性基因、环境催化理论计算、类Fenton无机助剂等研究领域同行进行学术交流报告3人次，协助培养博士生和硕士生各1名。