生物质流化床气化机理与工业应用研究
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摘要
作为生物质热化学转化技术中的一种，生物质气化的目标是尽可能多地得到高品质燃气。在各种气化反应器中，由于流化床具有气固两相接触充分，传热传质强烈，床层温度均匀，易于放大等特性而特别受到重视。生物质流化床气化反应器被认为是最具开发前景的生物质气化反应装置之一。目前，生物质流化床气化主要面临的问题有：燃气中焦油含量偏高且净化困难：燃气热值偏低(特别是空气气化)；仍然缺乏一个系统完整的气化装置放大准则；模型模拟结果与试验结果相差较大等，这些存在的问题直接影响了生物质气化技术的推广和应用。
为此，在国家‘863’基金资助下，围绕生物质流化床气化应用过程中的关键问题，从工程应用角度出发，本文对冷态实验条件下生物质颗粒在流化床中的流体力学特性、实验室规模生物质流化床气化特性、木炭床焦油高温催化裂解特性进行了研究，论文还针对工业规模生物质流化床气化发电系统的运行特性进行了分析，并基于得到的大量实验数据建立了关于生物质流化床气化特性的人工神经网络模型。
通过对冷态实验条件下，多种生物质原料在不同尺寸流化床中的流化特性研究发现：1)纯生物质(如木屑、稻壳)也是可以实现良好流化的。2)不同生物质原料流化特性有着显著区别，木屑的流化质量较好，当气速超过充分流化速度，可以观察到典型的‘鼓泡’流化状态。稻壳的流化质量稍差，比较容易出现‘沟流’现象。3)床层尺寸和料层高度对生物质颗粒的流化也有重要影响。当流化床直径小于100mm时，‘壁面效应’会比较明显，流化床尺寸增大有利于改善流化质量。料层高度与床径比(H／D)超过3.0，容易出现‘节涌’现象。4)对处于快速流态化下的生物质循环流化床速度分布和空隙率分布的考察表明：在生物质循环流化床中也存在着典型的‘环—核’流动结构。速度在径向呈‘抛物线’型分布，空隙率沿径向分布则比较均匀。改变操作气速和循环流率都对速度分布和空隙率分布有明显影响。5)对生物质颗粒在Loop seal型返料器中的流动特性研究表明：改变提升管的运行风速U_g对循环流率G_s影响不大；通过Loop seal的颗粒循环流率G_s随输送风量Q1和侧吹风量Q2增加而增大；改变侧吹风量Q2对循环流率的影响要比改变Q1的影响大得多。根据王擎实验关联式得到的
As one kind of biomass thermal chemistry conversion technology, biomass gasification has attracted more and more attentions in recent years. Its aim is attaining more possible combustible gases (such as H_2, CO, CH_4 et al.). Due to advantages of excellent gas-solid mixing, uniform bed temperature, intensive mass and heat transfer and easy scale-up, fluidized bed gasifier is thought as the most promising reactor among all kinds of biomass gasifier. At present, the main problems of biomass gasification in fluidized bed are the followings: the tar content in the product gas is rather high and tar conversion or removal is rather difficult; the product gas heating value is low when air was used as gasification agency; the scale-up rule of fluidized bed gasifier hasn't be built up until now; the simulation results of modeling of biomass gasification in fluidized bed is very poor, these problems directly and significantly hinder the application of biomass gasification technology.
To solve these problems, Funded by the National High Technology Research and Development Program of China (the '863' Program), the hydrodynamic characteristics of biomass particles in a cold fluidized bed and a cold circulating fluidized bed, the characteristics of biomass gasification in a lab-scale fluidized bed gasifier, the characteristics of high temperature tar cracking in a carbon furnace and the operation performances of industrial biomass gasification and power generation systems were studied in the present paper.
The fluidization hydrodynamics of different biomass particles were firstly investigated at room temperature in different diameter fluidized beds in the thesis. The experimental results have shown: 1) The pure biomass particles (such as sawdust /rice husk et al.) also could be fluidized. 2) The different biomass particles showed different characteristics of fluidization. Sawdust particles more easily achieved good fluidization than rice husk particles. When the gas velocity exceeded the complete fluidization velocity U_(cf), bubbling fluidization was observed when sawdust was used as bed material, however channeling was often observed when rice husk was fluidized.3) the diameter of bed and the height of bed material also had significant effects on fluidization quality. The 'wall effect' couldn't be ignored when the diameter of bed was less than 0.1 m, the bigger diameter facilitated to improve fluidization
为此，在国家‘863’基金资助下，围绕生物质流化床气化应用过程中的关键问题，从工程应用角度出发，本文对冷态实验条件下生物质颗粒在流化床中的流体力学特性、实验室规模生物质流化床气化特性、木炭床焦油高温催化裂解特性进行了研究，论文还针对工业规模生物质流化床气化发电系统的运行特性进行了分析，并基于得到的大量实验数据建立了关于生物质流化床气化特性的人工神经网络模型。
通过对冷态实验条件下，多种生物质原料在不同尺寸流化床中的流化特性研究发现：1)纯生物质(如木屑、稻壳)也是可以实现良好流化的。2)不同生物质原料流化特性有着显著区别，木屑的流化质量较好，当气速超过充分流化速度，可以观察到典型的‘鼓泡’流化状态。稻壳的流化质量稍差，比较容易出现‘沟流’现象。3)床层尺寸和料层高度对生物质颗粒的流化也有重要影响。当流化床直径小于100mm时，‘壁面效应’会比较明显，流化床尺寸增大有利于改善流化质量。料层高度与床径比(H／D)超过3.0，容易出现‘节涌’现象。4)对处于快速流态化下的生物质循环流化床速度分布和空隙率分布的考察表明：在生物质循环流化床中也存在着典型的‘环—核’流动结构。速度在径向呈‘抛物线’型分布，空隙率沿径向分布则比较均匀。改变操作气速和循环流率都对速度分布和空隙率分布有明显影响。5)对生物质颗粒在Loop seal型返料器中的流动特性研究表明：改变提升管的运行风速U_g对循环流率G_s影响不大；通过Loop seal的颗粒循环流率G_s随输送风量Q1和侧吹风量Q2增加而增大；改变侧吹风量Q2对循环流率的影响要比改变Q1的影响大得多。根据王擎实验关联式得到的
As one kind of biomass thermal chemistry conversion technology, biomass gasification has attracted more and more attentions in recent years. Its aim is attaining more possible combustible gases (such as H_2, CO, CH_4 et al.). Due to advantages of excellent gas-solid mixing, uniform bed temperature, intensive mass and heat transfer and easy scale-up, fluidized bed gasifier is thought as the most promising reactor among all kinds of biomass gasifier. At present, the main problems of biomass gasification in fluidized bed are the followings: the tar content in the product gas is rather high and tar conversion or removal is rather difficult; the product gas heating value is low when air was used as gasification agency; the scale-up rule of fluidized bed gasifier hasn't be built up until now; the simulation results of modeling of biomass gasification in fluidized bed is very poor, these problems directly and significantly hinder the application of biomass gasification technology.
To solve these problems, Funded by the National High Technology Research and Development Program of China (the '863' Program), the hydrodynamic characteristics of biomass particles in a cold fluidized bed and a cold circulating fluidized bed, the characteristics of biomass gasification in a lab-scale fluidized bed gasifier, the characteristics of high temperature tar cracking in a carbon furnace and the operation performances of industrial biomass gasification and power generation systems were studied in the present paper.
The fluidization hydrodynamics of different biomass particles were firstly investigated at room temperature in different diameter fluidized beds in the thesis. The experimental results have shown: 1) The pure biomass particles (such as sawdust /rice husk et al.) also could be fluidized. 2) The different biomass particles showed different characteristics of fluidization. Sawdust particles more easily achieved good fluidization than rice husk particles. When the gas velocity exceeded the complete fluidization velocity U_(cf), bubbling fluidization was observed when sawdust was used as bed material, however channeling was often observed when rice husk was fluidized.3) the diameter of bed and the height of bed material also had significant effects on fluidization quality. The 'wall effect' couldn't be ignored when the diameter of bed was less than 0.1 m, the bigger diameter facilitated to improve fluidization
引文
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1. K.G. Mansaray, A. E. Ghaly, A. M. Al-Taweel et al. Air gasification of rice husk in a dual distributor type fluidized bed gasifier. Biomass and Bioenergy, 1999, 17(4): 315-332.
2. A.A. Boateng, W. P. Walawender, L. T. Fan et al. Fluidized-bed steam gasification of rice hull. Bioresource Technology, 1992, 40 (3): 235-239.
3. Hongming Jiang and R. Vance Morey. Pyrolysis of corncobs at fluidization bed. Biomass and Bioenergy, 1992, 3(2): 81-85.
4. Hongming Jiang and R. Vance Morey. Air-gasification of corncobs at fluidization. Biomass and Bioenergy, 1992,3 (2): 87-92.
5. Paolo De Filippis, Carlo Borgianni, Martino Paolucci et al. Gasification process of Cuban bagasse in a two-stage reactor. Biomass and Bioenergy, 2004, 27(3): 247-252.
6. A. Ergudenler and A. E. Ghaly. Quality of gas produced from wheat straw in a dual-distributor type fluidized bed gasifier. Biomass and Bioenergy, 1992, 3(6): 419-430.
7. I. Narvaez, Alberto Orio, Maria P. Aznar et al. Biomass gasification with air in an Atmospheric bubbling fluidized bed .Effects of six operation variable on the quality of the Produced raw gas. Ind.eng.chem.res. 1996, 35, 2110-2120.
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32 T. R. McLendon et al. High-pressure co-gasification of coal and biomass in a fluidized bed: Biomass and Bioenergy, 2004, 26, (4): 377-388
33 Pinto, F. et al. Effect of experimental conditions on co-gasification of coal, biomass and plastics wastes with air/steam mixtures in a fluidized bed system [J]. Fuel, 2003, 82: 15-17.
34 Y. G. Pan, E. Velo, X. Roca, J. J. Manya. Fluidized-bed co-gasification of residual biomass/poor coal blends for fuel gas production. Fuel, 2000, 79 (11): 1317-1326.
35 K. Sjostrom, G. Chen, Q. Yu et al. Promoted reactivity of char in co-gasification of biomass and coal: synergies in the thermochemical process. Fuel, 1999,78(10): 1189-1194.
36 A. G. Collot, Y. Zhuo, D. R. Dugwell. Co-pyrolysis and co-gasification of coal and biomass in bench-scale fixed-bed and fluidised bed reactors. Fuel, 1999, 78(6):667-679.
37 M. Asadullah. et al. a comparison of Rh/CeO2/SiO2 catalysts with steam reforming catalysts, dolomite and inert materials as bed materials in low throughput fluidized bed gasification systems. Biomass and Bioenergy, 2004, 26, (3 ): 269-279.
38 M. Asadullah, Tomohisa Miyazawa, Shin-ichi Ito et al. Gasification of different biomasses in a dual-bed gasifier system combined with novel catalysts with high energy efficiency. Applied Catalysis A: General, 2004,267 (1-2): 95-102.
39 M. Asadullah, Tomohisa Miyazawa, Shin-ichi Ito et al. Catalyst development for the gasification of biomass in the dual-bed gasifier[j]. Applied Catalysis A: General, 2003, 255(2): 169-180.
40 M. Asadullah, Tomohisa Miyazawa, Shin-ichi Ito et al. Demonstration of real biomass gasification drastically promoted by effective catalyst. Applied Catalysis A: General, 2003, 246 (l):103-116.
41 M. Asadullah, Shin-ichi Ito, Kimio Kunimori et al. Biomass Gasification to Hydrogen and Syngas at Low Temperature: Novel Catalytic System Using Fluidized-Bed Reactor.Journal of Catalysis, 2002, 208(2):255-259.
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43 R.Q. Zhang, R. C. Brown, A. Suby et al. Catalytic destruction of tar in biomass derived producer gas [J]. Energy Conversion and Management, 2004, 45(7-8): 995-1014.
44 Min-Hon Rei, S. J. Yang and C. H. Hong.Catalytic gasification of rice hull and other biomass. The general effect of catalyst. Agricultural Wastes, 1986, 18(4): 269-281.
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49 Biomass IGCC at Varnamo Sweden. GCEP Energy Workshop, April 27, 2004.
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53 A. Sanz and J. Corella.Modeling circulating fluidized bed biomass gasifiers. Results from a pseudo-rigorous 1-dimensional model for stationary state [J].Fuel Processing Technology, 2006, 87(3): 247-258.
54 J. Corella and A. Sanz. Modeling circulating fluidized bed biomass gasifiers. A pseudo-rigorous model for stationary state [J]. Fuel Processing Technology,2005,86(9): 1021-1053.
55 G. Schuster, G. L6ffier, K. Weigl and H. Hofbauer. Biomass steam gasification - an extensive parametric modeling study. Bioresource Technology, 2001, 77(1): 71-79.
56 B, Guo, D.K. Li, C.M. Cheng et al. Simulation ofbiomass gasification with a hybrid neural network model. Bioresource Technology, 2001, 76(2): 77-83.
57 S. S. Sadaka, A. E. Ghaly and M. A. Sabbah. Two-phase biomass air-steam gasification model for fluidized bed reactors: Part Ⅲ—model validation.Biomass and Bioenergy, 2002, 22(6): 479-487.
58 D. Fiaschi and M. Michelini. A two-phase one-dimensional biomass gasification kinetics model. Biomass and Bioenergy, 2001, 21 (2): 121-132.
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