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太阳能光催化气相降解正癸烷——使用涂覆有P25或溶胶-凝胶TiO₂薄膜的醋酸纤维素整体柱的对比研究。

Solar photocatalytic gas-phase degradation of n-decane--a comparative study using cellulose acetate monoliths coated with P25 or sol-gel TiO₂ films.

作者信息

Miranda Sandra M, Lopes Filipe V S, Rodrigues-Silva Caio, Martins Susana D S, Silva Adrián M T, Faria Joaquim L, Boaventura Rui A R, Vilar Vítor J P

机构信息

LSRE-Laboratory of Separation and Reaction Engineering, Associate Laboratory LSRE/LCM, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, Porto, 4200-465, Portugal.

出版信息

Environ Sci Pollut Res Int. 2015 Jan;22(2):820-32. doi: 10.1007/s11356-014-2952-2. Epub 2014 May 9.

Abstract

Cellulose acetate monoliths (CAM) were used as the substrate for the deposition of TiO2 films to produce honeycombed photoactive structures to fill a tubular photoreactor equipped with a compound parabolic collector. By using such a setup, an efficient single-pass gas-phase conversion was achieved in the degradation of n-decane, a model volatile organic compound. The CAM three-dimensional, gas-permeable transparent structure with a rugged surface enables a good adhesion of the catalytic coating. It also provides a rigid structure for packing the tubular photoreactor, and maximizing the illuminated catalyst surface. The efficiency of the photocatalytic oxidation (PCO) process on n-decane degradation was evaluated under different operating conditions, such as feeding concentration (73 and 146 ppm), gas stream flow rate (73, 150, and 300 mL min(-1)), relative humidity (3 and 25 %), and UV irradiance (18.9, 29.1, and 38.4 WUV m(-2)). The results show that n-decane degradation by neat photolysis is negligible, but mineralization efficiencies of 86 and 82 % were achieved with P25-CAM and SG-CAM, respectively, for parent pollutant conversions above 95 %, under steady-state conditions. A mass transfer model, considering the mass balance to the plug-flow packed photoreactor, and PCO reaction given by a Langmuir-Hinshelwood bimolecular non-competitive two types of sites equation, was able to predict well the PCO kinetics under steady-state conditions, considering all the operational parameters tested. Overall, the performance of P25-CAM was superior taking into account mineralization efficiency, cost of preparation, surface roughness, and robustness of the deposited film.

摘要

醋酸纤维素整体柱(CAM)被用作沉积TiO₂薄膜的基底,以制备蜂窝状光活性结构,用于填充配备复合抛物面聚光器的管式光反应器。通过使用这种装置,在降解作为挥发性有机化合物模型的正癸烷过程中实现了高效的单通道气相转化。具有粗糙表面的CAM三维透气透明结构能够使催化涂层良好附着。它还为填充管式光反应器提供了刚性结构,并使被光照的催化剂表面最大化。在不同操作条件下评估了光催化氧化(PCO)过程对正癸烷降解的效率,这些条件包括进料浓度(73和146 ppm)、气流流速(73、150和300 mL min⁻¹)、相对湿度(3%和25%)以及紫外线辐照度(18.9、29.1和38.4 WUV m⁻²)。结果表明,单纯光解对正癸烷的降解可忽略不计,但在稳态条件下,对于母体污染物转化率高于95%的情况,P25-CAM和SG-CAM分别实现了86%和82%的矿化效率。考虑到活塞流填充光反应器的质量平衡以及由Langmuir-Hinshelwood双分子非竞争性两类位点方程给出的PCO反应的传质模型,能够在考虑所有测试操作参数的情况下很好地预测稳态条件下的PCO动力学。总体而言,考虑到矿化效率、制备成本、表面粗糙度以及沉积膜的坚固性,P25-CAM的性能更优。

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