环隙流化床中纳米颗粒聚团流态化/光催化降解VOCs的研究
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摘要
可挥发性有机污染物(Volatile Organic Compouds, VOCs)是指沸点范围在50～260℃之间,室温下饱和蒸气压超过133.32 Pa,以蒸气形式存在于空气中的一类有机物,主要来源于室内装饰装修材料、吸烟、外界动力机械尾气排放和燃料燃烧残余组分等。人们长时间滞留于室内,其危害是十分严重的。在VOCs的控制技术方面,半导体光催化氧化技术(Photocatalytic Oxidation,PCO)具有明显的优势。本文提出多相流颗粒动理学耦合光催化氧化技术的思想,依托环隙流化床光催化反应器,对光催化降解气态环己烷和苯进行了系统研究。
采用实验、数值模拟和理论分析相结合的方法研究了纳米P25颗粒聚团在环隙流化床中的流态化特征。建立了符合环隙流化床纳米P25颗粒聚团流态化的最小流化速度模型;得到摩擦因子、初始流态化的床层空隙率的参数值、沉降颗粒尺寸与操作气速的关系;建立了不同区域床层空隙率的的关联式,揭示了床层平均空隙率随流化物料量和操作气速的变化规律。
通过修订聚团颗粒的曳力、碰撞力和粘附力,得到了环隙流化床中P25颗粒聚团流态化模型。模型分析表明,P25颗粒聚团在局限的环隙区间内实现流态化时,颗粒与环隙壁面的壁面效应不可忽视,只有当环隙尺寸大于0.075m后壁效应方可忽略;两碰撞颗粒的尺寸比例ξ<0.298时,两个聚团可能产生团聚;两碰撞颗粒的尺寸比例ξ>0.298时,两个聚团可能产生分离或破碎;随着操作气速的增大,聚团尺寸逐渐减小,与实验测定的结果一致。
建立了气固两相分配动力学模型,揭示了环己烷/苯的初始浓度、操作气速、相对湿度与饱和吸附值的关系;通过修正langmuir吸附模型,得到了苯和环己烷的吸附平衡常数,并通过线性自由能关联吸附能量控制模型的验证,结果表明,修订模型更具有合理性。
环隙流化床中光催化降解苯和环己烷的实验表明,光催化降解效率是环己烷/苯的初始浓度、操作气速和系统相对湿度的函数。通过构建的P25颗粒聚团光催化反应的动力学模型分析,揭示了苯和环己烷的光催化降解半衰期与初始浓度的关系;验证了流化数1.62和1.8分别为环己烷和苯的最佳操作气速条件;揭示了湿度与浓度在光催化降解反应中的关系为C_(H_2O)=(1+K_AC_M)/2K_H。
基于光催化降解中间产物的FTIR、GC-MS和UV光谱信息,推断出环己烷/苯光催化降解的主要中间产物、光催化降解反应可能的历程、光催化剂失活的主要原因;通过光催化剂的循环使用和再生实验发现,该催化剂具有较好的循环使用效果和再生性能。
根据光催化降解VOCs反应过程分析,建立了光催化降解VOCs反应动力学模型,揭示了光催化反应过程中水分子与VOCs目标分子的关系,以及反应过程中水的促进/抑制作用机理。
Volatile organic compounds (VOCs) belongs to the organic chemicals with boiling point at 50-260℃and saturated vapor pressure at 133.32 Pa, which released or diffused from building materials, indoor furnishings, smoking, automobile exhaust and fuels combustion. Due to people stayed indoors for long time, some of VOCs may have short- and long-term adverse health effects on humsn beings. Photocatalytic oxidation (PCO) technology using semiconductors has some advantages over other VOCs controlling processes. The multiphase flow of photocatalyst particles coupling with PCO technology was put forward in this paper, and the photocatalytic degradation of gaseous benzene and cyclohexane in an annular fluidized bed reactor designed was investigated in details.
The fluidization characterization of nano-titania (P25) agglomerates in the dedigned annular fluidized bed reactor was investigated by experimental data, numerical simulation, and theoretical analyses. The model of minimum fluidization velocity related to fluidization materials and reactor structure was developed based on the modified traditional models. For initial fluidization stage, the bed voidage and friction coefficient between agglomerates and reactor walls were determined using linear-fitting method, respectively. In addition, the average dimension values of elutriation agglomerates were evaluated by Navier-Stokes equation. Finally, the bed voidage distribution model considering bed diameter was developed.
The model of nano-titania agglomerates in the annular fluidized bed was also presented considering the friction effect between agglomerates and reactor walls. According to the model, the following conclusions were given. (1) The friction between agglomerates and reactor walls should be considered unless the distance between the inner and outer wall is larger than 0.075 m; (2) If an agglomerate collides with other whose diameter is 0.298 times less than or equal to the former, the two agglomerates may coalesce. The dimensionless diameter coefficient exceeds 0.298, the two agglomerates may separate. Using the above-mentioned model, the relationship of diameter of agglomerate and gas velocity is explored.
The adsorption experiments of benzene and cyclohexane in the annular fluidized bed indicated that (1) their adsorption efficiencies were a degressive function of concentration at the fixed gas velocity and RH; that (2) adsorption active sites were a function of gas velocity based on the analyses of kinetic data, and the maximum value of adsorption active sites for cyclohexane was 2.71×10-4 mmol g~(-1) at fluidization number of 2.11 and the minimum value of adsorption active sites for benzene was 0.81×10-4 mmol g~(-1) at fluidization number of 1.37, respectively; and that (3) the adsorption efficiencies of benzene and cyclohexane were decreaed with increasing RH, which was explained by the variation of adsorbate structure and adsorption active sites.
Photocatalytic degradation of benzene and cyclohexane gave the following conclusions. Firstly, the concentration of target has obvious influences on photocatalytic degradation efficiency, and the degradation efficiency decreased with increasing concentration. Secondly, the photocatalytic degradation efficiency was approximated to the maximum values at the optimal fluidization numbers 1.62 and 1.8 for cyclohexane and benzene respectively. Thirdly, the influences of RH on photocatalytic degradation of cyclohexane and benzene were similar, and there was an inflexion point corresponding to the maximum degradation efficiency at variation of concentrations. Fourthly, the relationship of RH and target concentration was explored asC_(H_2O)=(1+K_AC_M)/2K_Hwithout consideration of adsorption of the products and intermediates yielded in photocatalysis.
Using FTIR, GC-MS, and UV-Spectrum, the intermediates yielded in photocatalytic degradation of cyclohexane were cyclohexanol, cyclohexanone and 2-cyclohexen~(-1)-one, while the intermediates for benzene were phenol and carboxylic acid. We can infer the photocatalytic degradation mechanisms of benzene and cyclohexane and the causes of photocatalyst deactivation. Based on the adsorption active sites occupied by intermediates, the regeneration and recycling experiments were performed, suggesting that the photocatalyst can be regenerated and recycled over three times.
Photocatalysis kinetic models based on the elementary reactions explores the roles of water molecule in this process.
采用实验、数值模拟和理论分析相结合的方法研究了纳米P25颗粒聚团在环隙流化床中的流态化特征。建立了符合环隙流化床纳米P25颗粒聚团流态化的最小流化速度模型;得到摩擦因子、初始流态化的床层空隙率的参数值、沉降颗粒尺寸与操作气速的关系;建立了不同区域床层空隙率的的关联式,揭示了床层平均空隙率随流化物料量和操作气速的变化规律。
通过修订聚团颗粒的曳力、碰撞力和粘附力,得到了环隙流化床中P25颗粒聚团流态化模型。模型分析表明,P25颗粒聚团在局限的环隙区间内实现流态化时,颗粒与环隙壁面的壁面效应不可忽视,只有当环隙尺寸大于0.075m后壁效应方可忽略;两碰撞颗粒的尺寸比例ξ<0.298时,两个聚团可能产生团聚;两碰撞颗粒的尺寸比例ξ>0.298时,两个聚团可能产生分离或破碎;随着操作气速的增大,聚团尺寸逐渐减小,与实验测定的结果一致。
建立了气固两相分配动力学模型,揭示了环己烷/苯的初始浓度、操作气速、相对湿度与饱和吸附值的关系;通过修正langmuir吸附模型,得到了苯和环己烷的吸附平衡常数,并通过线性自由能关联吸附能量控制模型的验证,结果表明,修订模型更具有合理性。
环隙流化床中光催化降解苯和环己烷的实验表明,光催化降解效率是环己烷/苯的初始浓度、操作气速和系统相对湿度的函数。通过构建的P25颗粒聚团光催化反应的动力学模型分析,揭示了苯和环己烷的光催化降解半衰期与初始浓度的关系;验证了流化数1.62和1.8分别为环己烷和苯的最佳操作气速条件;揭示了湿度与浓度在光催化降解反应中的关系为C_(H_2O)=(1+K_AC_M)/2K_H。
基于光催化降解中间产物的FTIR、GC-MS和UV光谱信息,推断出环己烷/苯光催化降解的主要中间产物、光催化降解反应可能的历程、光催化剂失活的主要原因;通过光催化剂的循环使用和再生实验发现,该催化剂具有较好的循环使用效果和再生性能。
根据光催化降解VOCs反应过程分析,建立了光催化降解VOCs反应动力学模型,揭示了光催化反应过程中水分子与VOCs目标分子的关系,以及反应过程中水的促进/抑制作用机理。
Volatile organic compounds (VOCs) belongs to the organic chemicals with boiling point at 50-260℃and saturated vapor pressure at 133.32 Pa, which released or diffused from building materials, indoor furnishings, smoking, automobile exhaust and fuels combustion. Due to people stayed indoors for long time, some of VOCs may have short- and long-term adverse health effects on humsn beings. Photocatalytic oxidation (PCO) technology using semiconductors has some advantages over other VOCs controlling processes. The multiphase flow of photocatalyst particles coupling with PCO technology was put forward in this paper, and the photocatalytic degradation of gaseous benzene and cyclohexane in an annular fluidized bed reactor designed was investigated in details.
The fluidization characterization of nano-titania (P25) agglomerates in the dedigned annular fluidized bed reactor was investigated by experimental data, numerical simulation, and theoretical analyses. The model of minimum fluidization velocity related to fluidization materials and reactor structure was developed based on the modified traditional models. For initial fluidization stage, the bed voidage and friction coefficient between agglomerates and reactor walls were determined using linear-fitting method, respectively. In addition, the average dimension values of elutriation agglomerates were evaluated by Navier-Stokes equation. Finally, the bed voidage distribution model considering bed diameter was developed.
The model of nano-titania agglomerates in the annular fluidized bed was also presented considering the friction effect between agglomerates and reactor walls. According to the model, the following conclusions were given. (1) The friction between agglomerates and reactor walls should be considered unless the distance between the inner and outer wall is larger than 0.075 m; (2) If an agglomerate collides with other whose diameter is 0.298 times less than or equal to the former, the two agglomerates may coalesce. The dimensionless diameter coefficient exceeds 0.298, the two agglomerates may separate. Using the above-mentioned model, the relationship of diameter of agglomerate and gas velocity is explored.
The adsorption experiments of benzene and cyclohexane in the annular fluidized bed indicated that (1) their adsorption efficiencies were a degressive function of concentration at the fixed gas velocity and RH; that (2) adsorption active sites were a function of gas velocity based on the analyses of kinetic data, and the maximum value of adsorption active sites for cyclohexane was 2.71×10-4 mmol g~(-1) at fluidization number of 2.11 and the minimum value of adsorption active sites for benzene was 0.81×10-4 mmol g~(-1) at fluidization number of 1.37, respectively; and that (3) the adsorption efficiencies of benzene and cyclohexane were decreaed with increasing RH, which was explained by the variation of adsorbate structure and adsorption active sites.
Photocatalytic degradation of benzene and cyclohexane gave the following conclusions. Firstly, the concentration of target has obvious influences on photocatalytic degradation efficiency, and the degradation efficiency decreased with increasing concentration. Secondly, the photocatalytic degradation efficiency was approximated to the maximum values at the optimal fluidization numbers 1.62 and 1.8 for cyclohexane and benzene respectively. Thirdly, the influences of RH on photocatalytic degradation of cyclohexane and benzene were similar, and there was an inflexion point corresponding to the maximum degradation efficiency at variation of concentrations. Fourthly, the relationship of RH and target concentration was explored asC_(H_2O)=(1+K_AC_M)/2K_Hwithout consideration of adsorption of the products and intermediates yielded in photocatalysis.
Using FTIR, GC-MS, and UV-Spectrum, the intermediates yielded in photocatalytic degradation of cyclohexane were cyclohexanol, cyclohexanone and 2-cyclohexen~(-1)-one, while the intermediates for benzene were phenol and carboxylic acid. We can infer the photocatalytic degradation mechanisms of benzene and cyclohexane and the causes of photocatalyst deactivation. Based on the adsorption active sites occupied by intermediates, the regeneration and recycling experiments were performed, suggesting that the photocatalyst can be regenerated and recycled over three times.
Photocatalysis kinetic models based on the elementary reactions explores the roles of water molecule in this process.
引文
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