太阳能固定膜光催化氧化去除饮用水中污染物研究
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摘要
本研究以结构简单、光能利用率高的复合抛物面采光板为采光元件，采用溶胶-凝胶法在比表面积大、化学性质稳定的玻璃纤维网上制备高活性TiO_2固定催化剂作为催化组件，并用长寿命冷阴极低压汞灯作为人工辅助光源，研制成功一种新型中试规模太阳光固定膜光催化反应器。
以草酸铁钾化学光量计曝光试验对新型太阳光催化反应器的光学性能进行了评价，其光子采集效率φ_(ef)约为0.759。本装置降解苯酚表观量子产率可以达到悬浆催化体系的1／2。固定在玻璃纤维网上的光催化剂，可在较长期内重复使用。装置对水中苯酚、甲酸等低浓度有机物具有较高处理效率；由于采用电光源作为太阳光的补充，装置对天气具有良好的适应性，能够实现全天候稳定运行。
以苯酚为模型污染物的研究表明，新装置具有良好的传质作用，在循环流量大于5L／min时即可消除传质限制作用。在苯酚初始浓度在1.8～7.5mg／L范围内时，苯酚的太阳光催化降解呈表观一级反应，表观动力学常数随着初始浓度的增加而变小。在太阳光强介于12.4～25.9W／m~2时，苯酚降解的表观反应速率常数和光强呈线性关系。采用电光源时，苯酚的降解是光催化和直接光分解综合作用的结果。
对蒸馏水中大肠杆菌的灭活特性研究表明，太阳光固定膜光催化灭菌是光催化灭菌和阳光直接灭菌协同作用的结果，光催化杀菌效果优于阳光直接杀菌作用。环境扫描电镜分析(ESEM)表明光催化对菌体产生了致命性破坏。光催化灭菌速率和循环流速、光强存在正相关性。光催化灭菌还具有良好的持久性，灭菌处理8h后，没有出现明显复活再生现象。
对双酚A(BPA)光催化降解特性的研究表明，BPA的降解受不同光源影响显著。BPA在阳光照射下很难光解；在较低浓度下，BPA的太阳光光催化降解呈现表观一级反应，反应速率常数随初始浓度增大而减小；在光强介于5.7～23.5W／m~2时，表观反应速率常数和光强呈线性关系。在UV254下，BPA存在明显光解作用，一级表观反应速率常数随初始浓度增大而增大。太阳光催化对BPA具有良好的矿化作用，但和短波紫外光下光催化矿化过程存在很大差异。通过BSTFA衍生和GC／MS分析，在不同光源下均检测到多种BPA降解中间产物。
新装置在不同光源下对自来水中半挥发性有机污染物均具有良好的净化效果。在本研究中太阳光催化条件下，自来水中可通过GC／MS较准确定性的23种微量半挥发性有机物中的18种物质去除率在50％以上，其中16种物质在处理后水中已经降到仪器检测限以下。装置对自来水中常见的有机污染物如三氯甲烷、苯酚和双酚A具有良好的去除效果；另外，装置在去除自来水中有机污染物同时，还对自来水中细菌具有一定的杀灭效果。太阳光固定膜光催化具有良好的实际应用前景。
A novel pilot-scale solar photocatalytic reactor with immobilized catalyst wasdeveloped, where low concentrating compound parabolic concentrator was applied assolar collecting component, and immobilized TiO_2 membrane supported on glassfiber mesh with sol-gel method used as catalyst and cold cathode low-pressuremercury lamps used as assisting artificial UV source.
The photonic collection efficiency factorφ_(ef) was estimated to be about 0.759 bypotassium ferrioxalate actinometries. And apparent quantum yield of phenoldegradation can reach up to 1/2 of that of slurry system. The photocatalyst supportedon glass fiber net can be reused in a rather long time. The new reactor, which treatedphenol and formic acid with high efficiency, can make all-weather stable operationwith good compatibility to different weathers.
Phenol was used as model pollutant to evaluating the device performance. Thelimitation of mass transfer was diminished when the circular flux exceeded 5L/min.When initial concentration ranged from 1.8 to 7.5mg/L, the solar photocatalyticreaction followed apparent first-order kinetics, and the apparent kinetic constantsdecreased with the increase of initial concentration. The linear dependence betweenapparent reaction rate and radiation density flux was also found from 12.4 to 25.9W/m~2. Phenol removal under artificial UV radiation was the combined effects ofphotocatalysis as well as photolytic degradation.
Inactivation characteristics of Escherichia coli were also studied by the newsolar photocatalytic reactor. Photocatalytic deactivation of Escherichia coli was aconsequence of the synergistic effect of the oxidant species generated by supportedTiO_2 and solar UV irradiation, and the disinfection efficiency of photocatalysis washigher than sunlight deactivation. Increasing flow rate and light intensity had positiveeffects on disinfection rate. ESEM examination indicated that bacteria cell waslethally destroyed by solar photocatalysis. No significant recovery or multiplicationwas observed during 8 hatter solar photocatalysis treatment.
Photocatalytic degradation characteristics of bisphenol A (BPA) were explored.And experiment results indicated that BPA degradation was influenced significantlyby different light sources. BPA underwent insignificant photolysis under solarirradiation. At low initial concentrations, the apparent reaction kinetics was first orderwith respect to the concentration and the apparent kinetic constants decreased withthe increase of initial concentrations. Linear dependence between apparent reactionrate and radiation density flux was also found from 5.7 to 23.5 W/m~2. While underUV254, BPA underwent significant photolysis and the first-order kinetic constantsincreased with the increase of initial concentration. Solar photocatalysis couldmineralize BPA well, but the mineralization process differs greatly from that undershort wavelength UV. Several intermediates were detected by GC/MS analysis afterBSTFA-derivatization of intermediate samples.
Semi-volatile organic pollutants in tap water could be purified well by the newphotocatalytic reactor under different irradiation. Under solar photocatalysiscondition, 18 trace semi-volatile organics among those 23 ones which were identifiedby GC/MS analysis were removed more than 50％, and 16 of them were evenlowered below detection limits. Common pollutants such as chloroform, phenol andBPA could also be removed well. Furthermore, bacteria in tap water were inactivatedsuccessfully while organic pollutants were removed. Solar photocatalysis techniquewith immobilized catalyst is promising in tap water purification.
以草酸铁钾化学光量计曝光试验对新型太阳光催化反应器的光学性能进行了评价，其光子采集效率φ_(ef)约为0.759。本装置降解苯酚表观量子产率可以达到悬浆催化体系的1／2。固定在玻璃纤维网上的光催化剂，可在较长期内重复使用。装置对水中苯酚、甲酸等低浓度有机物具有较高处理效率；由于采用电光源作为太阳光的补充，装置对天气具有良好的适应性，能够实现全天候稳定运行。
以苯酚为模型污染物的研究表明，新装置具有良好的传质作用，在循环流量大于5L／min时即可消除传质限制作用。在苯酚初始浓度在1.8～7.5mg／L范围内时，苯酚的太阳光催化降解呈表观一级反应，表观动力学常数随着初始浓度的增加而变小。在太阳光强介于12.4～25.9W／m~2时，苯酚降解的表观反应速率常数和光强呈线性关系。采用电光源时，苯酚的降解是光催化和直接光分解综合作用的结果。
对蒸馏水中大肠杆菌的灭活特性研究表明，太阳光固定膜光催化灭菌是光催化灭菌和阳光直接灭菌协同作用的结果，光催化杀菌效果优于阳光直接杀菌作用。环境扫描电镜分析(ESEM)表明光催化对菌体产生了致命性破坏。光催化灭菌速率和循环流速、光强存在正相关性。光催化灭菌还具有良好的持久性，灭菌处理8h后，没有出现明显复活再生现象。
对双酚A(BPA)光催化降解特性的研究表明，BPA的降解受不同光源影响显著。BPA在阳光照射下很难光解；在较低浓度下，BPA的太阳光光催化降解呈现表观一级反应，反应速率常数随初始浓度增大而减小；在光强介于5.7～23.5W／m~2时，表观反应速率常数和光强呈线性关系。在UV254下，BPA存在明显光解作用，一级表观反应速率常数随初始浓度增大而增大。太阳光催化对BPA具有良好的矿化作用，但和短波紫外光下光催化矿化过程存在很大差异。通过BSTFA衍生和GC／MS分析，在不同光源下均检测到多种BPA降解中间产物。
新装置在不同光源下对自来水中半挥发性有机污染物均具有良好的净化效果。在本研究中太阳光催化条件下，自来水中可通过GC／MS较准确定性的23种微量半挥发性有机物中的18种物质去除率在50％以上，其中16种物质在处理后水中已经降到仪器检测限以下。装置对自来水中常见的有机污染物如三氯甲烷、苯酚和双酚A具有良好的去除效果；另外，装置在去除自来水中有机污染物同时，还对自来水中细菌具有一定的杀灭效果。太阳光固定膜光催化具有良好的实际应用前景。
A novel pilot-scale solar photocatalytic reactor with immobilized catalyst wasdeveloped, where low concentrating compound parabolic concentrator was applied assolar collecting component, and immobilized TiO_2 membrane supported on glassfiber mesh with sol-gel method used as catalyst and cold cathode low-pressuremercury lamps used as assisting artificial UV source.
The photonic collection efficiency factorφ_(ef) was estimated to be about 0.759 bypotassium ferrioxalate actinometries. And apparent quantum yield of phenoldegradation can reach up to 1/2 of that of slurry system. The photocatalyst supportedon glass fiber net can be reused in a rather long time. The new reactor, which treatedphenol and formic acid with high efficiency, can make all-weather stable operationwith good compatibility to different weathers.
Phenol was used as model pollutant to evaluating the device performance. Thelimitation of mass transfer was diminished when the circular flux exceeded 5L/min.When initial concentration ranged from 1.8 to 7.5mg/L, the solar photocatalyticreaction followed apparent first-order kinetics, and the apparent kinetic constantsdecreased with the increase of initial concentration. The linear dependence betweenapparent reaction rate and radiation density flux was also found from 12.4 to 25.9W/m~2. Phenol removal under artificial UV radiation was the combined effects ofphotocatalysis as well as photolytic degradation.
Inactivation characteristics of Escherichia coli were also studied by the newsolar photocatalytic reactor. Photocatalytic deactivation of Escherichia coli was aconsequence of the synergistic effect of the oxidant species generated by supportedTiO_2 and solar UV irradiation, and the disinfection efficiency of photocatalysis washigher than sunlight deactivation. Increasing flow rate and light intensity had positiveeffects on disinfection rate. ESEM examination indicated that bacteria cell waslethally destroyed by solar photocatalysis. No significant recovery or multiplicationwas observed during 8 hatter solar photocatalysis treatment.
Photocatalytic degradation characteristics of bisphenol A (BPA) were explored.And experiment results indicated that BPA degradation was influenced significantlyby different light sources. BPA underwent insignificant photolysis under solarirradiation. At low initial concentrations, the apparent reaction kinetics was first orderwith respect to the concentration and the apparent kinetic constants decreased withthe increase of initial concentrations. Linear dependence between apparent reactionrate and radiation density flux was also found from 5.7 to 23.5 W/m~2. While underUV254, BPA underwent significant photolysis and the first-order kinetic constantsincreased with the increase of initial concentration. Solar photocatalysis couldmineralize BPA well, but the mineralization process differs greatly from that undershort wavelength UV. Several intermediates were detected by GC/MS analysis afterBSTFA-derivatization of intermediate samples.
Semi-volatile organic pollutants in tap water could be purified well by the newphotocatalytic reactor under different irradiation. Under solar photocatalysiscondition, 18 trace semi-volatile organics among those 23 ones which were identifiedby GC/MS analysis were removed more than 50％, and 16 of them were evenlowered below detection limits. Common pollutants such as chloroform, phenol andBPA could also be removed well. Furthermore, bacteria in tap water were inactivatedsuccessfully while organic pollutants were removed. Solar photocatalysis techniquewith immobilized catalyst is promising in tap water purification.
引文
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