CN106006929B - 一种光电催化膜耦合微生物燃料电池全天候处理污水的方法 - Google Patents
一种光电催化膜耦合微生物燃料电池全天候处理污水的方法 Download PDFInfo
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Abstract
本发明提供了一种光电催化膜耦合微生物燃料电池全天候处理污水的方法,属于污水处理与能源回收及利用技术领域。Ag/RGO/BiVO4经硅溶胶稳定涂覆在不锈钢网上形成导电复合膜,与微生物阳极经外电阻构成双室MFC‑PFC耦合膜过滤系统。在光电催化及膜组件辅助膜分离作用下,系统连续进出水,调控停留时间和工艺,弥补单独MFC和PFC的不足。非膜过滤方式下,系统仍全天侯条件下净化处理水并产电。在120min内,MFC‑PFC处理TC溶液去除率达87%,无光照时,仍有68%的TC去除率。在10h内,MFC‑PFC耦合系统连续式处理受污染的景观水,阳极室微生物降解水中有机物去除率51%;阴极室去除率达63%。
Description
技术领域
本发明属于污水处理与能源利用领域,涉及Ag/RGO/BiVO4纳米复合催化剂、及光电催化功能膜组件的制备,及其作为微生物燃料电池阴极,耦合微生物和光电催化协同作用,降解污染物且产生电能,同时出水经过阴极膜过滤或截留作用,以更低能耗实现了污染物的高效降解,提高了出水水质及其安全性。
背景技术
膜技术是一种高效低耗的水处理技术。然而经常发生膜污染,其污染导致分离效率下降,膜清洗致使能耗上升。通过外加电场排斥污染物,膜的功能化改性,结合光催化及光电催化,或者臭氧氧化催化作用可以实现有效控制膜污染。但是这些方法大多需要外加化学药剂或者电场,成本及能耗较高。一般的微滤或超滤,不能截留小分子的污染物,不能解决水中毒性难降解污染物的去除问题。一般需要将高级氧化技术(臭氧氧化,光催化,光电催化,电催化)与膜技术结合。目前,将Ag/RGO/BiVO4光电催化过滤分离功能膜作为阴极与燃料电池耦合进行水处理的报道还未出现。
为了节能,人们发明了燃料电池水处理技术。该技术既可降解污染物又能产电。其中,光催化燃料电池(Photocatalytic fuel call,PFC),由负载型光催化剂作为电极材料,它利用光能降解污染物,弥补了分散型光催化剂难回收再利用的缺点,且极大提高了光催化(Photocatalytic,PC)降解污染物效率,同时产电。微生物燃料电池(Microbial fuelcell,MFC)利用微生物将水中的污染物中的化学能直接转化成电能,降解底物同时也可提供能量。
燃料电池水处理研究中,着重解决两方面的问题,其一是PFC的光催化剂作为阳极催化剂,贵金属Pt作为阴极,价格昂贵,难以运用于实际废水处理工艺。其二是MFC在污水处理及资源化系统中,微生物对生物毒性物质(例如,抗生素等)难以降解。因此将MFC与PFC两系统“合二为一”,可以实现功能最大化,并且实现阴极膜催化降解和过滤多功能,关于该耦合系统(MFC-PFC),目前很少有人研究。
BiVO4,带隙宽度2.4–2.9eV,与被研究最早、最广泛的光催化剂TiO2(3.0-3.2ev)相比,有较强的可见光响应能力,化学物理性质稳定,目前得到广泛关注。研究表明,纳米复合催化剂可以有效抑制光生电子-空穴的结合,增强材料可见光响应能力,较单独材料有更好的光催化性能,例如,BiVO4/RGO,BiVO4/Ag2O,BiVO4/Graphene/TiO2等。本申请选取Ag/RGO/BiVO4作为实验催化剂,希望提高BiVO4基材料的导电性及光催化性能,并制作成光电催化分离膜,实现了燃料电池产电和阴极催化膜过滤出水方式下的水处理。
发明内容
本发明设计了Ag/RGO/BiVO4光电催化多功能膜,成功构建了MFC-PFC耦合膜过滤水处理系统。该膜不仅可以用作电极,还兼具过滤和光催化作用,整体处理效率高,能耗较低,出水水质更好更安全。该系统理论上可降解所有污染物,扩展了负载型光催化剂的应用,在光电催化膜组件的辅助作用下,可实现系统连续进水操作,弥补了单独MFC和PFC的不足。
本发明的技术方案:
一种光电催化膜耦合微生物燃料电池全天候处理污水的方法,将光电催化膜组件用于微生物燃料电池阴极,处理污水。步骤如下:
(1)制备纳米xAg/yRGO/BiVO4系列复合物:分别配制等物质的量浓度的Bi(NO3)3稀硝酸溶液和NH4VO3氢氧化钠溶液;在磁力搅拌下,按CTAB与Bi(NO3)3质量比为0.08,将CTAB的悬浊液逐滴加入到Bi(NO3)3的稀硝酸溶液里,得到A液;继续向A液中添加氧化石墨烯的悬浊液,得到B液;最后,将与Bi(NO3)3稀硝酸溶液等体积的NH4VO3氢氧化钠溶液逐滴滴进B液中,得到含BiVO4的C液;用NaOH调C液PH=6,再加入AgNO3,继续搅拌10min,转入反应釜,240℃反应2h;沉淀经50%无水乙醇溶液多次洗涤,离心,80℃烘干,研磨,获得纳米xAg/yRGO/BiVO4系列复合物,x为Ag与BiVO4的质量比,y为RGO与BiVO4的质量比,其中x不大于6%,y不大于3%;
(2)光电催化膜组件制备:向步骤(1)制备得到的纳米xAg/yRGO/BiVO4系列复合物中添加硅溶胶,超声均匀,将其涂抹于不锈钢网片上,每平方厘米面 积上纳米xAg/yRGO/BiVO4系列复合物的负载量为5mg,室温晾干,将膜固定在组装的膜组件上;
(3)MFC-PFC膜催化过滤系统构建:MFC-PFC膜催化过滤系统通过质子交换膜分为两室,一室中放置负载有产电微生物的活性炭颗粒,碳棒阳极插入活性炭颗粒中;另一室中放置光电催化膜组件阴极和受污染的水样(污水/河水/景观水/或四环素溶液),底部有曝气装置,两极经铜导线和外电阻连接,形成电路,钨卤灯垂直照射膜电极,模拟太阳光。
本发明的有益效果:该系统集成了生物降解和催化降解作用,降解去除水中污染物为小分子,尤其生物难降解及毒性污染物;作为水处理的预处理或后处理,在光催化剂光电催化及膜组件辅助膜分离作用下,通过调控停留时间和工艺,系统实现连续进出水操作且出水水质和安全性达到要求,非膜过滤方式下,系统仍全天侯条件下净化处理水并产电。
附图说明
图1是光催化(PC)、电催化(MFC-EC)、光电催化(MFC-PFC)和光催化燃料电池(PFC)四中不同方式阴极室内处理四环素溶液的效果对比图。图中,横坐标为时间,纵坐标为Ct/C0。
图2是MFC-PFC耦合系统间歇式处理受污染的景观水效果图。纵坐标为10小时内系统阴极室对景观水中COD及NH4 +-N的去除率。
图3是MFC-PFC耦合系统连续式处理受污染的景观水效果图。图中曲线分别代表系统阳极及阴极室内景观水中COD量随反应时间的变化。
具体实施方式
以下结合技术方案和附图详细叙述本发明的具体实施方式。
实施例一:MFC-PFC耦合系统处理四环素溶液
膜组件放入反应器右室,量取200ml50mg/l已配制的四环素溶液,加入分析纯Na2SO4固体,配制0.1MNa2SO4电解液,倒入系统右室,鳄鱼夹一端夹住膜电极上方,另一端由铜导线连接。另捞取约80g负载产电微生物的活性炭颗粒,装入左室,量取200ml配制好的微生物营养液于左室,插入碳棒阳极,阳阴极 之间连接360Ω电阻,反应时启动50w220v钨素灯和曝气装置。反应前断开电路,系统静置30min,一方面微生物适应营养液环境,另一方面,实现四环素底物在膜催化剂和溶液中吸附脱附平衡。反应开始后,每隔30min取样3ml,共反应两小时,用高效液相测四环素去除率,TOC测定仪测TOC去出率,同时,数据采集卡监测记录电阻两端电压电流变化。
图1表明:在120min内,MFC-PFC去除TC效果最好,达87%,该效果明显优于PC(30%),MFC-EC(68%)和MFC(50%);此外,未光照时,在微生物提供的外电场作用下的电化学催化(MFC-EC)降解四环素效果也不错。这些数据证明了MFC和PFC之间的协同作用,及该系统在有无光情况下均可作业的可能性。
实施例二:MFC-PFC耦合系统间歇式处理受污染的景观水
系统左室放微生物约130mg、河流景观水200ml和碳棒电极,右室放300ml校园河流景观水,膜组件,鳄鱼夹一端夹住膜上方,两极之间连接361欧姆电阻形成电路。蠕动泵以3ml/min流速从膜组件上端抽取溶液回流至反应器内原溶液中来模拟间歇式污水处理工艺。反应前需静置30min,反应时,启动曝气、光源、蠕动泵和数据采集卡装置。反应时长10小时,每隔2h取膜组件出口处溶液4ml,测量其NH4 +-N和COD。其中氨氮测定采用纳氏试剂紫外可见分光光度计法,COD使用COD快速测定仪测定。
图2中,COD的去除率达75%,NH4 +-N去除率为63%。
实施例三:MFC-PFC耦合系统连续式处理受污染的景观水
系统左室放微生物约130mg、河流景观水200ml和碳棒电极,右室放300ml校园河流景观水,膜组件,鳄鱼夹一端夹住膜上方,两极之间连接361欧姆电阻形成电路。蠕动泵以3ml/min流速从膜组件上端抽取溶液至烧杯,另一蠕动以3ml/min流速抽取原水样流进反应器,模拟连续式污水处理工艺。反应前需静置30min,反应时,启动曝气、光源、蠕动泵和数据采集卡装置。反应时长10小时,每隔2h取膜组件出口处溶液4ml,使用COD快速测定仪测定其COD。附图3中结果说明在10h内阳极室微生物降解水中有机物去除率为51%,阴极 室模拟连续式污水处理工艺,污染去除率达63%。
Claims (2)
1.一种光电催化膜耦合微生物燃料电池全天候处理污水的方法,其特征在于,步骤如下:
(1)制备纳米xAg/yRGO/BiVO4系列复合物:分别配制等物质的量浓度的Bi(NO3)3稀硝酸溶液和NH4VO3氢氧化钠溶液;在磁力搅拌下,按CTAB与Bi(NO3)3质量比为0.08,将CTAB的悬浊液逐滴加入到Bi(NO3)3的稀硝酸溶液里,得到A液;继续向A液中添加氧化石墨烯的悬浊液,得到B液;最后,将与Bi(NO3)3稀硝酸溶液等体积的NH4VO3氢氧化钠溶液逐滴滴进B液中,得到含BiVO4的C液;用NaOH调C液pH=6,再加入AgNO3,继续搅拌10min,转入反应釜,240℃反应2h;沉淀经50%无水乙醇溶液多次洗涤,离心,80℃烘干,研磨,获得纳米xAg/yRGO/BiVO4系列复合物,x为Ag与BiVO4的质量比,y为RGO与BiVO4的质量比,其中x不大于6%,y不大于3%;
(2)光电催化膜组件制备:向步骤(1)制备得到的纳米xAg/yRGO/BiVO4系列复合物中添加硅溶胶,超声均匀,将其涂抹于不锈钢网片上,每平方厘米面积上纳米xAg/yRGO/BiVO4系列复合物的负载量为5mg,室温晾干,将膜固定在组装的膜组件上;
(3)MFC-PFC膜催化过滤系统构建:MFC-PFC膜催化过滤系统通过质子交换膜分为两室,一室中放置负载有产电微生物的活性炭颗粒,碳棒阳极插入活性炭颗粒中;另一室中放置光电催化膜组件阴极和受污染的水样,底部有曝气装置,两极经铜导线和外电阻连接,形成电路,钨卤灯垂直照射膜电极,模拟太阳光。
2.根据权利要求1所述的方法,其特征在于,所述的受污染的水样为污水、河水、景观水或四环素溶液。
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