基于铁卟啉衍生的多级孔Fe-N-C阴极/电芬顿体系用于河流水体中PAEs污染修复的行为机理研究
批准号:
52100183
项目类别:
青年科学基金项目(C类)
资助金额:
30.0 万元
负责人:
秦蕾
依托单位:
学科分类:
环境污染治理与修复
结题年份:
2024
批准年份:
2021
项目状态:
已结题
项目参与者:
秦蕾
中文摘要
湘江流域工农业发达且水体环境复杂,水体中邻苯二甲酸酯(PAEs)污染会威胁水生态环境和人类健康。非均相电芬顿技术是一种能有效用于水体中PAEs污染修复的环境友好型方法,但催化效率受阴极对氧气利用率低、Fe(II)再生效率低的限制,影响了其在实际复杂环境条件下的修复效果。因此,本项目针对湘江流域PAEs污染关键问题,拟制备铁卟啉衍生的多级孔Fe-N-C材料作为阴极构建非均相电芬顿体系用于湘江水体中PAEs污染修复。优化阴极关键制备参数,采用单因素实验优化应用过程,探知PAEs的去除效能;采用现代化表征手段结合单因素实验结果,探求体系对PAEs的去除机制及中间产物演变规律;考察关键环境因子对PAEs降解效能的影响,分析降解过程中间产物的毒性演变规律,综合评价修复水体进一步利用的安全性和可行性。以期为发展新型催化剂构建的电芬顿体系安全高效用于PAEs污染河流水体修复提供重要的理论依据和技术支撑。
英文摘要
The industry and agriculture in Xiangjiang River Valley developed very fast, which makes the complex water environment. And the pollution of phthalate esters (PAEs) in Xiangjiang River possesses a threat to water ecological environment and human health. The heterogeneous electro-Fenton technique is an environmentally friendly method that can be used for the remediation of PAEs from river water. However, the catalytic efficiency is limited by the low oxygen utilization of cathode and low Fe(II) regeneration efficiency, which affects the remediation performance under complex conditions. Concerning on the key problems of PAEs pollution, in this project, a ferriporphyrin-derived hierarchical porous Fe-N-C catalyst will be prepared as cathode material and used to structure a heterogeneous electro-Fenton system for the removal of PAEs from Xiangjiang River. Firstly, the key preparation parameters of Fe-N-C catalyst will be optimized, and the single factor experiment will be carried out to optimize the application process and further ascertain the removal efficiency of PAEs. Secondly, the mechanism and intermediates of PAEs degradation will be investigated by the combination of some characterization techniques and single factor experiment results. Besides, the effects on the degradation efficiency by key environmental factors and the toxic effects on degradation intermediates to microbes and plants will be also studied to comprehensively evaluate the security and feasibility for further utilization of river water after remediation. This project is expected to provide important theoretical basis and technical support for the development of new catalyst-based electro-Fenton oxidation system and its safe and efficient remediation of PAEs polluted river water.
非均相电芬顿技术是一种能有效用于水体中有机污染物处理的环境友好型方法,但它的催化效率受阴极对氧气的利用率低、Fe(II)再生效率低的限制,影响了其在实际复杂条件下的处理效果。因此,选择合适的非均相芬顿催化剂对克服上述问题具有十分重要的意义。本项目首先制备了一系列铁卟啉衍生的多级孔Fe-N-C催化剂并构建非均相电芬顿体系,用于水体中环丙沙星(CIP)的降解。700℃下煅烧得到的材料(Fe-N-C-700)呈现出丰富的三维多孔结构,内部存在碳层包裹的铁氮颗粒。BET和Raman表明Fe-N-C-700存在丰富的活性位点,XPS表明Fe-N-C-700中FeNx和氮物种活性位点的存在。催化实验表明,在CIP浓度为20mg/L、pH为3,催化剂浓度为0.1g/L,空气流速为0.5L/min,Na2SO4电解质浓度为0.05M的反应条件下,Fe-N-C-700在90 min内对CIP降解率为99.5%,矿化率为88.87%。循环实验表明Fe-N-C-700具有很好的稳定性和重复利用性,体系中铁的浸出量仅为49.17 μg/ L。该体系在实际水体中也具有较好的实际应用潜力,并通过计算得到该体系具有较低的能耗消耗。进一步地,本项目还制备了一系列磺酸基金属有机框架(UiO-66-SO3H)衍生的铁掺杂碳催化剂,并构建非均相电芬顿体系用于水体中四环素(TC)的降解。表征结果表明,UiO-66-SO3H/Fe(1:1)-800具有中空的八面体结构,表面粗糙。EDS元素映射图表明Zr、Fe、O、C、N和S元素均匀地分散在碳骨架中。BET结果则表明UiO-66-SO3H/Fe(1:1)-800中存在丰富的孔结构,这些孔结构有利于活性位点的暴露,提高电芬顿的催化效率。此外,材料比为1:1(w/w)的复合材料,在800℃煅烧下,外加电流密度为200 mA,pH为7时,对TC的降解率在90min内能达90.1%,矿化率在120 min内达到42.94%,能耗低至4.39 kWh/kg/TOC。重复8次后铁离子的浸出量低于1 μg/L,在实际水体中仍具有较好的TC去除效率,且一些常见的共存物质对其降解效率影响较小,进一步表明该体系具有较好的重复利用性和实际应用性能。本项目为发展新型催化剂构建的非均相电芬顿体系安全高效用于有机污染水体修复提供了重要的理论依据和技术支撑。
生物炭粒子电极协同3D电化学体系活化PS的调控机制及氧化降解CPs的机理
-
批准号:2026JJ50483
-
项目类别:省市级项目
-
资助金额:0.0万元
-
批准年份:2026
-
负责人:秦蕾
-
依托单位:
稳定化超薄水滑石/非均相SR-AOPs体系氧化修复抗生素污染水体的效能与机制研究
-
批准号:2023JJ30145
-
项目类别:省市级项目
-
资助金额:0.0万元
-
批准年份:2023
-
负责人:秦蕾
-
依托单位:
国内基金
海外基金