新型Fe基材料高效高选择性还原废水中NO3-为N2的研究
批准号:
52070136
项目类别:
面上项目
资助金额:
59.0 万元
负责人:
刘咏
依托单位:
学科分类:
工业水处理与回用
结题年份:
2024
批准年份:
2020
项目状态:
已结题
项目参与者:
刘咏
中文摘要
废水中NO3-去除对于控制总氮排放至关重要。Fe0还原NO3-,操作简单、条件温和,但还原产物主要为NH4+,如何高效、高选择性地将NO3-还原为N2,是亟待解决的难题。本项目拟制备一种新型Fe基材料(Fe0-Cu0-CuFe2O4@CNTs),将NO3-高效还原为NO2-;再利用CuFe2O4光催化活化甲酸产生二氧化碳自由基(CO2•−),将NO2-高选择性还原为N2,以实现NO3-的高效、高选择性还原。研究内容包括:(1)制备新型Fe基材料并探讨其高效还原NO3-为NO2-的调控机制;(2)探讨CuFe2O4光催化活化甲酸形成CO2•−的作用机制,揭示CO2•−高选择性还原NO2-为N2的机理;(3)联合利用新型Fe基材料与CO2•−,高效、高选择性还原NO3-为N2,揭示协同作用机制;(4)探讨焦化废水、垃圾渗滤液中NO3-的去除特性。研究成果将为废水中NO3-的去除提供新方法。
英文摘要
The removal of nitrate plays a key role in controlling the discharge of total nitrogen in wastewater. Zero valent iron (Fe0) is often used to reduce nitrate in wastewater due to its simple operation and mild reaction condition. However, the main reduction product is ammonia,which limits its practical application. The project will develop a novel Fe based materials(Fe0-Cu0-CuFe2O4@CNTs),which can be obtained by a chemical replacement combined with oxidation process for the modification of Fe0 surface. The reduction of nitrate into nitrogen with high efficiency and high selectivity will be realized by the following processes: firstly, nitrate is reduced into nitrite by Fe0-Cu0-CuFe2O4@CNTs with rational structure under suitable reaction conditions; then, nitrite is further reduced into nitrogen by the carbon dioxide radicals (CO2•−), which can be produced by photo-activation of formic acid (HCOOH)with the help of CuFe2O4. The as-prepared Fe0-Cu0-CuFe2O4@CNTs will be applied for the removal of nitrate from simulated and practical wastewater, such as coking wastewater and landfill leachate. This project will mainly investigated the regulation mechanism of selective reduction of nitrate into nitrite by Fe0-Cu0-CuFe2O4@CNTs , the formation mechanism of CO2•− from the photocatalytic activation of formic acid by CuFe2O4 and the reduction mechanism of nitrite into nitrogen by CO2•−, the coupling mechanism and specific synergistic mode of Fe0-Cu0-CuFe2O4@CNTs and CO2•− in the denitrification process.The results of this project will provide a technical support for developing a new technology for the removal of nitrate from wastewater.
废水中NO3-去除对于控制总氮排放至关重要。化学还原法还原NO3-,操作简单、反应速度快、条件温和,但还原产物主要为NH4+,如何高效、高选择性地将NO3-还原为N2、减少NH4+的生成,是亟待解决的难题。本项目设计合成了两种新型铁基材料(Fe0-Cu0-CuFe2O4和Cu0@Fe0-CuFe2O4-x),结合光活化小分子有机酸,通过两步法实现了NO3-还原产物的高N2选择性(N2可达96.3%)。结合DFT理论计算、电化学测试和EPR测试等手段,深入解析了体系中CO2•−、光电子等活性物种的产生及还原NO3-的作用机制:新型铁基材料含Fe0、Cu0和CuFe2O4(或CuFe2O4-x)等成分,Fe0和CuFe2O4(或CuFe2O4-x)的光生电子是电子供给源,Cu0是电子富集中心使NO3-选择性还原为NO2-,体系中产生的铁离子可促进小分子有机酸活化为CO2•−,从而使NO2-高选择性还原为N2;接着采用廉价易得的铁基材料(天然黄铁矿和亚硫酸铁),通过一步法光还原NO3-,还原产物的N2选择性高达98%;进一步构建了一系列脱氮体系,用于垃圾渗滤液二级出水、城市生活污水二级出水等实际废水中NO3-的去除,取得了良好的效果。针对试验研究过程中发现NH4+浓度有时会降低的现象,进一步构建了几种高级氧化体系,其NH4+氧化为N2的选择性高达96%,并解析了其作用机制。该研究具有拓展性和普适性,为设计合理的非贵金属铁基材料用于废水处理提供了新思路,也为废水中无机氮的化学转化去除提供理论依据和技术支撑。相关研究成果已在ACS ES&T Engineering等期刊上发表论文22篇,其中SCI一区论文8篇,高被引1篇;授权发明专利2项;基于化学脱氮的研究成果获得“挑战杯”大学生创业计划竞赛省级金奖,培养硕士生9名,其硕士毕业论文教育部盲审优秀率62.5%、良好率100%。
新型零价铁基材料活化O2降解垃圾渗滤液污染地下水中抗生素及抗性基因的研究
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批准号:42577058
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项目类别:面上项目
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资助金额:49.00万元
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批准年份:2025
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负责人:刘咏
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依托单位:
原位产生并利用H2O2的新型类Fenton催化剂及去除废水中抗生素的机制
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批准号:51878427
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项目类别:面上项目
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资助金额:61.0万元
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批准年份:2018
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负责人:刘咏
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依托单位:
国内基金
海外基金