Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, China.
Sci Total Environ. 2012 Nov 1;438:201-9. doi: 10.1016/j.scitotenv.2012.08.081. Epub 2012 Sep 19.
Concentrations of 13 gaseous intermediates in photocatalytic oxidation (PCO) of toluene in indoor air were determined in real-time by proton transfer reaction mass spectrometry and desorption intensities of 7 adsorbed intermediates on the surface of photocatalysts were detected by temperature-programmed desorption-mass spectrometry. Effects of relative humidity (RH), photocatalysts, and vacuum ultraviolet (VUV) irradiation on the distribution and category of the intermediates and health risk influence index (η) were investigated. RH enhances the formation rate of hydroxide radicals, leading to more intermediates with higher oxidation states in gas phase. N doping promotes the separation of photo-generated electrons and holes and enhances PCO activity accordingly. VUV irradiation results in higher mineralization rate and more intermediates with higher oxidation states and lower toxicity e.g. carboxylic acids. Health risk analysis indicates that higher RH, N doping of TiO(2), and VUV lead to "greener" intermediates and smaller η. Finally, a conceptual diagram was proposed to exhibit the scenario of η varied with extent of mineralization for various toxicities of inlet pollutants.
采用质子转移反应质谱实时测定了室内空气中甲苯光催化氧化(PCO)过程中 13 种气态中间产物的浓度,采用程序升温脱附-质谱法检测了 7 种吸附在光催化剂表面的中间产物的脱附强度。考察了相对湿度(RH)、光催化剂和真空紫外(VUV)辐照对中间产物的分布和种类以及健康风险影响指数(η)的影响。RH 会促进氢氧自由基的生成速率,导致气相中具有更高氧化态的中间产物增多。N 掺杂可以促进光生电子和空穴的分离,从而提高 PCO 活性。VUV 辐照会导致更高的矿化率以及更多具有更高氧化态和更低毒性(如羧酸)的中间产物。健康风险分析表明,较高的 RH、TiO2 的 N 掺杂和 VUV 辐照会产生“更环保”的中间产物,η 值更小。最后,提出了一个概念图来展示各种毒性的入口污染物的矿化程度与 η 值变化的情况。