蜂窝催化剂中甲醇自热重整制氢反应的研究
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摘要
本论文以研发高效的氢源系统为目标,采用实验研究、理论分析和数值模拟相结合的方法对ZNO-CR2O3/CEO2-ZRO2整体催化剂上的甲醇自热重整制氢反应进行了系统的研究,解决了甲醇重整制氢过程中重整催化剂和反应器的优化设计以及放大过程涉及的反应工程问题。
通过正交实验系统研究了整体催化剂上甲醇自热重整制氢体系的反应动力学;利用方差分析得出反应温度、空速、水醇摩尔比和氧醇摩尔比都是影响甲醇的转化率、氢产率和CO选择性的重要因素,而且其影响的显著程度依次减弱。
采用平板式石英玻璃反应器测试了蜂窝催化剂内的轴向浓度分布,并据此对甲醇自热重整反应的反应路径进行了探讨。结果表明,甲醇水蒸气重整反应在整个催化剂床层上发生,而甲醇完全氧化反应和甲醇分解反应则主要在催化剂床层前段发生。
建立了蜂窝反应器内多反应耦合过程的三维数学模型,运用CFD软件对重整器内的温度分布、浓度分布进行了数值计算,模拟与实验结果吻合良好。对蜂窝反应器进行结构优化设计,分析了催化剂长度、高径比、开孔率和载体材质对反应特性的影响,得出此蜂窝反应器最优的结构参数。
采用多孔介质模型考察了反应器入口分布方式对75kW重整制氢系统反应效果的影响,并对放大后的反应器内的流场分布进行了数值模拟,结果表明该模型能够比较准确地预测反应器内的场分布。研究了反应器的入口扩张管对反应的影响规律,为反应器的最优化设计提供了理论指导。
This paper focused on developing a fuel processing system with high efficiency. The reaction of autothermal reforming of methanol (ATR) over ZnO-Cr2O3/CeO2-ZrO2 monolithic catalyst was investigated by the experimental and theoretical studies. The problems involved in the optimization and scale-up of monolithic catalyst and reactors were discussed.
Kinetics of ATR reaction over monolithic catalyst was studied by means of orthogonal experiment. A power-type rate expression was established, and its accuracy was proved by F-examination. Effects of different operating conditions on ATR reaction were investigated by analysis of variance. It was proved that the highly notable influence factors were reaction temperature and space velocity.
The concentration profiles of the monolithic catalyst were measured by novel flat-bed reactor and sliced catalyst. The reaction pathways for ATR were discussed according to the results of concentration distribution. It was proved that the steam reforming of methanol happened in the whole parts of the catalyst; whereas the reactions of methanol decomposition and total oxidation of methanol mainly occured in the initial stage of the catalyst.
A three-dimensional mathematical model was established to describe the ATR reaction process in monolithic reactor. Distribution of concentration in the reactor had been calculated. Effects of the mole ratio of water/methanol, oxygen/methanol, temperature and gas hourly space velocity (GHSV) on the performance of monolithic reactor had also been simulated by the model. Mathematical simulations of the concentration distribution in monolith reactor were in good agreement with the experiments. The effects of configuration parameters of monolithic reactor on reaction were investigated, such as the length of catalyst, the ratio of height/diameter of catalyst, the porosity of catalyst bed, and even the substrate materials of the catalyst. Optimal design of the monolithic reactor was achieved.
The effect of different distributors in 75kW reformer on the performance of ATR system was investigated. Porous media model was chosen to simulate the temperature distribution of the scale-up reactor. The computational results indicate that this model can predict the field distribution of monolithic reactor accurately. The effect of different expanding tubes on reaction performance was also discussed. The result indicates that 120o expanding tube should be chosen preferentially.
通过正交实验系统研究了整体催化剂上甲醇自热重整制氢体系的反应动力学;利用方差分析得出反应温度、空速、水醇摩尔比和氧醇摩尔比都是影响甲醇的转化率、氢产率和CO选择性的重要因素,而且其影响的显著程度依次减弱。
采用平板式石英玻璃反应器测试了蜂窝催化剂内的轴向浓度分布,并据此对甲醇自热重整反应的反应路径进行了探讨。结果表明,甲醇水蒸气重整反应在整个催化剂床层上发生,而甲醇完全氧化反应和甲醇分解反应则主要在催化剂床层前段发生。
建立了蜂窝反应器内多反应耦合过程的三维数学模型,运用CFD软件对重整器内的温度分布、浓度分布进行了数值计算,模拟与实验结果吻合良好。对蜂窝反应器进行结构优化设计,分析了催化剂长度、高径比、开孔率和载体材质对反应特性的影响,得出此蜂窝反应器最优的结构参数。
采用多孔介质模型考察了反应器入口分布方式对75kW重整制氢系统反应效果的影响,并对放大后的反应器内的流场分布进行了数值模拟,结果表明该模型能够比较准确地预测反应器内的场分布。研究了反应器的入口扩张管对反应的影响规律,为反应器的最优化设计提供了理论指导。
This paper focused on developing a fuel processing system with high efficiency. The reaction of autothermal reforming of methanol (ATR) over ZnO-Cr2O3/CeO2-ZrO2 monolithic catalyst was investigated by the experimental and theoretical studies. The problems involved in the optimization and scale-up of monolithic catalyst and reactors were discussed.
Kinetics of ATR reaction over monolithic catalyst was studied by means of orthogonal experiment. A power-type rate expression was established, and its accuracy was proved by F-examination. Effects of different operating conditions on ATR reaction were investigated by analysis of variance. It was proved that the highly notable influence factors were reaction temperature and space velocity.
The concentration profiles of the monolithic catalyst were measured by novel flat-bed reactor and sliced catalyst. The reaction pathways for ATR were discussed according to the results of concentration distribution. It was proved that the steam reforming of methanol happened in the whole parts of the catalyst; whereas the reactions of methanol decomposition and total oxidation of methanol mainly occured in the initial stage of the catalyst.
A three-dimensional mathematical model was established to describe the ATR reaction process in monolithic reactor. Distribution of concentration in the reactor had been calculated. Effects of the mole ratio of water/methanol, oxygen/methanol, temperature and gas hourly space velocity (GHSV) on the performance of monolithic reactor had also been simulated by the model. Mathematical simulations of the concentration distribution in monolith reactor were in good agreement with the experiments. The effects of configuration parameters of monolithic reactor on reaction were investigated, such as the length of catalyst, the ratio of height/diameter of catalyst, the porosity of catalyst bed, and even the substrate materials of the catalyst. Optimal design of the monolithic reactor was achieved.
The effect of different distributors in 75kW reformer on the performance of ATR system was investigated. Porous media model was chosen to simulate the temperature distribution of the scale-up reactor. The computational results indicate that this model can predict the field distribution of monolithic reactor accurately. The effect of different expanding tubes on reaction performance was also discussed. The result indicates that 120o expanding tube should be chosen preferentially.
引文
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[1] Jahn R, Snita D, Kubek M, Marek M. 3-D modeling of monolith reactors. Catalysis Today, 1997, 38: 39-46.
[2] Shuai S, Wang J,Unsteady temperature fields of monoliths in catalytic converters,Chemical Engineering Journal, 2004, 100: 95-107.
[3] Springmann S, Friedrich G, Himmen M, Eigenberger G. Isothermal kinetic measurements for hydrogen production from hydrocarbon fuels using a novel kinetic reactor concept, Applied Catalysis A: General, 2002, 235: 101–111.
[4] Maxim L, Subir R. Novel catalytic reactor for oxidative reforming of methanol. Applied Catalysis B-Environmental, 2004, 54: 203–215.
[5] Wanker R, Berg M, Raupenstrauch H, Staudinger G.Numerical Simulation of Monolithic Catalysts with a Heterogeneous Model and Comparison with Experimental Results from a Wood-fired Domestic Boiler. Chemical Engineering Technology, 2000, 23: 535-542.
[6] Peppley B A, Amphlett J C, Kearns L M, Mann R F. Methanol–steam reforming on Cu/ZnO/Al2O3. Part 1: the reaction network. Applied Catalysis A: General, 1999, 179: 21-29.
[1] Jahn R, Snita D, Kubek M, Marek M. 3-D modeling of monolith reactors. Catalysis Today, 1997, 38: 39-46.
[2] Kolaczkowski S T, David J. W, Modeling channel interactions in a non-adiabatic multichannel catalytic combustion reactor. Catalysis Today, 1995, 26: 275-282.
[3] Sugiura S,Ijuin K. A multi-dimensional numerical method for predicting warm-up characteristic of automobile catalytic converter systems. SAE Paper 952413.
[4] Jeong S,Kim T. CFD investigation of the 3-dimensional unsteady flow in the catalytic converter. SAE Paper 971025.
[5] Shi-Jin Shuai, Jian-Xin Wang, Unsteady temperature fields of monoliths in catalytic converters,Chemical Engineering Journal, 2004, 100: 95-107.
[6] Fluent software. FLUENT user’s guide. Fluent Incorporated. http://www.fluent.com
[7] 邵潜,龙军,贺振富.规整结构催化剂及反应器. 北京:化学工业出版社,2005. p26-28.
[8] 魏伟,史庆南.汽车催化净化器载体材料的研究进展.云南冶金,2002, 31: 46-48.
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[1] 刘娜,王树东,袁中山.甲醇自热重整制氢整体催化剂的制备.化工学报,2004,第55 卷增刊:90-94.
[2] Maxim L, Subir R. Novel catalytic reactor for oxidative reforming of methanol, Applied Catalysis B-Environmental, 2004, 54:203–215.
[3] Agrell J, Birgersson H, Boutonnet M, Fierro J L G. Production of hydrogen from methanol over Cu/ZnO catalysts promoted by ZrO2 and Al2O3. Journal of Catalysis, 2003, 219: 389-403.
[4] 亓爱笃,洪学伦,王树东. 甲醇氧化重整制氢反应动力学的研究. 天然气化工, 2000, 25: 18-21.
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[6] 王胜年,王树东,吴迪镛. Cr-Zn 催化剂上甲醇水蒸气转化反应动力学 ?.本征动力学. 石油化工. 2001, 30(4): 259-262
[7] 蒋元力,黄强,陈卫航. 甲醇POSR 制氢的反应网络热力学分析和有效因子的估算[J].燃料化学学报. 2003, 131(4) : 349-354.
[8] Peppley B A, Amphlett J C, Kearns L.M, et al. Methanol steam reforming on Cu/Zn/Al2O3. Part 2: A comprehensive kinetic model. Applied Catalysis A: General, 1999, 179: 31-49
[9] Jiang C J, Trimm D L and Wainwright M S, Kinetic study of steam reforming of methanol over copper-based catalysts, Applied Catalysis A: General, 1993, 93: 245-255.
[10] Reitz T L, Ahmed S, Krumpelt M, Kumar R, et al. Characterization of CuO/ZnO under oxidizing conditions for the oxidative methanol reforming reaction. Journal of Molecular Catalysis A: Chemical, 2000, 162 :275-285.
[11] Pakornphant C, Sumaeth C, Johannes S. Temperature programmed desorption of methanol and oxidation of methanol on Pt–Sn/Al2O3 catalysts. Chemical Engineering Journal, 2004, 97: 161–171.
[12] 潘亚明,朱鹤孙.化学与化工中的数学方法. 北京:北京理工大学出版社,1993. p350-358.
[13] Ahmed S, Krumpelt M. Hydrogen from hydrocarbon fuels for fuel cells, International Journal of Hydrogen Energy, 2001, 26:291-301.
[1] Jahn R, Snita D, Kubek M, Marek M. 3-D modeling of monolith reactors. Catalysis Today, 1997, 38: 39-46.
[2] Shuai S, Wang J,Unsteady temperature fields of monoliths in catalytic converters,Chemical Engineering Journal, 2004, 100: 95-107.
[3] Springmann S, Friedrich G, Himmen M, Eigenberger G. Isothermal kinetic measurements for hydrogen production from hydrocarbon fuels using a novel kinetic reactor concept, Applied Catalysis A: General, 2002, 235: 101–111.
[4] Maxim L, Subir R. Novel catalytic reactor for oxidative reforming of methanol. Applied Catalysis B-Environmental, 2004, 54: 203–215.
[5] Wanker R, Berg M, Raupenstrauch H, Staudinger G.Numerical Simulation of Monolithic Catalysts with a Heterogeneous Model and Comparison with Experimental Results from a Wood-fired Domestic Boiler. Chemical Engineering Technology, 2000, 23: 535-542.
[6] Peppley B A, Amphlett J C, Kearns L M, Mann R F. Methanol–steam reforming on Cu/ZnO/Al2O3. Part 1: the reaction network. Applied Catalysis A: General, 1999, 179: 21-29.
[1] Jahn R, Snita D, Kubek M, Marek M. 3-D modeling of monolith reactors. Catalysis Today, 1997, 38: 39-46.
[2] Kolaczkowski S T, David J. W, Modeling channel interactions in a non-adiabatic multichannel catalytic combustion reactor. Catalysis Today, 1995, 26: 275-282.
[3] Sugiura S,Ijuin K. A multi-dimensional numerical method for predicting warm-up characteristic of automobile catalytic converter systems. SAE Paper 952413.
[4] Jeong S,Kim T. CFD investigation of the 3-dimensional unsteady flow in the catalytic converter. SAE Paper 971025.
[5] Shi-Jin Shuai, Jian-Xin Wang, Unsteady temperature fields of monoliths in catalytic converters,Chemical Engineering Journal, 2004, 100: 95-107.
[6] Fluent software. FLUENT user’s guide. Fluent Incorporated. http://www.fluent.com
[7] 邵潜,龙军,贺振富.规整结构催化剂及反应器. 北京:化学工业出版社,2005. p26-28.
[8] 魏伟,史庆南.汽车催化净化器载体材料的研究进展.云南冶金,2002, 31: 46-48.
[1] 王安杰,周裕之,赵蓓. 化学反应工程学. 北京:化学工业出版社,2005. p5-6.
[2] Wendland D W. The segmented oxidating monolith catalystic converter. Theory and performance. Trans. ASME, 1980, 102:194-198.
[3] Wanker R, Berg M, Raupenstrauch H, Staudinger G. Numerical Simulation of Monolithic Catalysts with a Heterogeneous Model and Comparison with Experimental Results from a Wood-fired Domestic Boiler. Chem. Eng. Technol. 2000, 23:535-542.