Hydrodynamics study and industrial applications of slurry reactors

doi:10.3969/j.issn.0438-1157.2014.07.007

Abstract

Abstract: The slurry reactor is an important type of gas-liquid-solid multiphase reactors. It has the advantages of simple construction, good mass and heat transfer performance, and feasibility of on-line addition or replacement of catalysts. It has received attentions from both academic and industrial circles. This paper reviews the study of hydrodynamics of slurry reactor, including flow regime, gas holdup, bubble behavior, and mass and heat transfer rates. The effects of temperature, pressure and liquid properties on the hydrodynamics are discussed. Novel slurry reactors, such as multi-stage slurry reactor and slurry reactors with internals are introduced. The industrial applications of slurry reactor on bulk chemical and fine chemical industries and environmental processes are summarized. Perspectives are given on the potential application and future research of slurry reactors.

Key words: multiphase reactor, hydrodynamics, transport processes, industrial application

摘要： 浆态床是一种重要的气-液-固三相反应器，具有结构简单，传热、传质性能好以及催化剂可在线补加和更换等优点，在学术研究和工业应用上备受关注。对浆态床反应器的流型、气含率、气泡行为、传质、传热等研究进行了总结，并对温度、压力、液体性质等参数对于流体力学性质的影响进行了分析。介绍了多级浆态床和构件式浆态床新型反应器，对浆态床在大化工、精细化工及环保等重要过程中的工业应用进行了总结，并对浆态床反应器的应用前景和研究趋势进行了展望。

关键词: 多相反应器, 流体动力学, 传递过程, 工业应用

CLC Number:

TQ021.1

GUO Kunyu, WANG Tiefeng, XING Chutian, WANG Jinfu. Hydrodynamics study and industrial applications of slurry reactors[J]. CIESC Journal, 2014, 65(7): 2454-2464.

郭坤宇, 王铁峰, 邢楚填, 王金福. 浆态床反应器流体力学行为研究及工业应用[J]. 化工学报, 2014, 65(7): 2454-2464.

References 90

[1]	Wang T F, Wang J F, Jin Y. Slurry reactors for gas-to-liquid processes: a review [J]. Ind. Eng. Chem. Res., 2007, 46 (18): 5824-5847
[2]	Deckwer W D, Field R W. Bubble Column Reactors [M]. New York: Wiley, 1992: 533
[3]	Zhang Tongwang (张同旺), He Guangxiang (何广湘), Jin Haibo (靳海波), Tong Zemin (佟泽民). Progress of hydrodynamics in slurry bubble column reactor [J]. J. Beijing Inst. Petro-chem. Technol. (北京石油化工学院学报), 2001, 9 (2): 47-53
[4]	Yang G Q, Luo X, Lau R, Fan L S. Heat-transfer characteristics in slurry bubble columns at elevated pressures and temperatures [J]. Ind. Eng. Chem. Res., 2000, 39 (7): 2568-2577
[5]	Chen Maotao (陈茂涛). Reference progress on technology of direct synthesizing dimethyl ether from syngas [J]. Appl. Chem. Ind. (应用化工), 2001, 30 (3): 1-3
[6]	Bai Liang (白亮), Liu Lijun (刘利军), Li Xiaobei (李小蓓), Zhang Zhixin (张志新), Xiang Hongwei (相宏伟), Li Yongwang (李永旺), Han Yizhuo (韩怡卓). Investigation on the adaptability of an industrial fixed-bed Fe-Cu-K catslyst to slurry reactor [J]. J. Fuel Chem. Technol. (燃料化学学报), 2005, 33 (2): 211-217
[7]	Ruthiya K C, Chilekar V P, Warnier M J F, van der Schaaf J, Kuster B F M, Schouten J C, van Ommen J R. Detecting regime transitions in slurry bubble columns using pressure time series [J]. AIChE J., 2005, 51 (7): 1951-1965
[8]	Camarasa E, Vial C, Poncin S, Wild G, Midoux N, Bouillard J. Influence of coalescence behaviour of the liquid and of gas sparging on hydrodynamics and bubble characteristics in a bubble column [J]. Chem. Eng. Process., 1999, 38 (4/5/6): 329-344
[9]	Song Wei (宋巍), Jing Ying (靖英), Yu Bo (于波). Research progress on the gas holdup of slurry bed reactor [J]. Tianjin Chem. Ind. (天津化工), 2009, 33 (1): 12-15
[10]	Degaleesan S, Dudukovic M, Pan Y. Experimental study of gas-induced liquid-flow structures in bubble columns [J]. AIChE J., 2001, 47 (9): 1913-1931
[11]	Wang Lijun (王丽军), Zhang Yu (张煜), Li Xi (李希). Studies on hydrodynamics of slurry turbulent bubble column (I): Gas holdup and its radial distribution [J]. Journal of Chemical Industry and Engineering (China) (化工学报), 2008, 59 (12): 2996-3002
[12]	Xing C T, Wang T F, Wang J F. Experimental study and numerical simulation with a coupled CFD-PBM model of the effect of liquid viscosity in a bubble column [J]. Chem. Eng. Sci., 2013, 95: 313-322
[13]	Yang J H, Yang J I, Kim H J, Chun D H, Lee H T, Jung H. Two regime transitions to pseudo-homogeneous and heterogeneous bubble flow for various liquid viscosities [J]. Chem. Eng. Process., 2010, 49 (10): 1044-1050
[14]	Mouza A A, Dalakoglou G K, Paras S V. Effect of liquid properties on the performance of bubble column reactors with fine pore spargers [J]. Chemical Engineering Science, 2005, 60 (5): 1465-1475
[15]	Krishna R, de Swart J W, Ellenberger J, Martina G B, Maretto C. Gas holdup in slurry bubble columns: effect of column diameter and slurry concentrations [J]. AIChE J., 1997, 43 (2): 311-316
[16]	Liu M L, Wang T F, Yu W, Wang J F. Hydrodynamics of a slurry airlift reactor at high solid concentrations [J]. Chem. Eng. Sci., 2007, 62 (24): 7098-7106
[17]	Lemoine R, Behkish A, Morsi B I. Hydrodynamic and mass-transfer characteristics in organic liquid mixtures in a large-scale bubble column reactor for the toluene oxidation process [J]. Ind. Eng. Chem. Res., 2004, 43 (19): 6195-6212
[18]	Soong Y, Harke F W, Gamwo I K, Schehl R R, Zarochak M F. Hydrodynamic study in a slurry-bubble-column reactor [J]. Catal. Today, 1997, 35 (4): 427-434
[19]	Gandhi B, Prakash A, Bergougnou M A. Hydrodynamic behavior of slurry bubble column at high solids concentrations [J]. Powder Technol., 1999, 103 (2): 80-94
[20]	Li H, Prakash A. Influence of slurry concentrations on bubble population and their rise velocities in a three-phase slurry bubble column [J]. Powder Technol., 2000, 113 (1/2): 158-167
[21]	Fazeli A, Fatemi S, Ganji E, Khakdaman H R. A statistical approach of heat transfer coefficient analysis in the slurry bubble column [J]. Chem. Eng. Res. Des., 2008, 86 (5A): 508-516
[22]	Behkish A, Men Z W, Inga J R, Morsi B I. Mass transfer characteristics in a large-scale slurry bubble column reactor with organic liquid mixtures [J]. Chem. Eng. Sci., 2002, 57 (16): 3307-3324
[23]	Vandu C O, Koop K, Krishna R. Volumetric mass transfer coefficient in a slurry bubble column operating in the heterogeneous flow regime [J]. Chem. Eng. Sci., 2004, 59 (22/23): 5417-5423
[24]	Akita K, Yoshida F. Gas holdup and volumetric mass transfer coefficient in bubble columns. Effects of liquid properties [J]. Industrial & Engineering Chemistry Process Design and Development, 1973, 12 (1): 76-80
[25]	Mena P, Ferreira A, Teixeira J, Rocha F. Effect of some solid properties on gas-liquid mass transfer in a bubble column [J]. Chemical Engineering and Processing: Process Intensification, 2011, 50 (2): 181-188
[26]	Saxena S, Rao N, Saxena A. Heat transfer and gas holdup studies in a bubble column: air-water-sand system [J]. The Canadian Journal of Chemical Engineering, 1992, 70 (1): 33-41
[27]	Hikita H, Asai S, Kikukawa H, Zaike T, Ohue M. Heat transfer coefficient in bubble columns [J]. Industrial & Engineering Chemistry Process Design and Development, 1981, 20 (3): 540-545
[28]	Saxena S, Rao N, Saxena A. Heat-transfer and gas-holdup studies in a bubble column: air-water-glass bead system [J]. Chemical Engineering Communications, 1990, 96 (1): 31-55
[29]	Jhawar A K, Prakash A. Heat transfer in a slurry bubble column reactor: a critical overview [J]. Ind. Eng. Chem. Res., 2012, 51 (4): 1464-1473
[30]	Li H, Prakash A. Analysis of bubble dynamics and local hydrodynamics based on instantaneous heat transfer measurements in a slurry bubble column [J]. Chem. Eng. Sci., 1999, 54 (21): 5265-5271
[31]	Deckwer W D. On the mechanism of heat-transfer in bubble column reactors [J]. Chem. Eng. Sci., 1980, 35 (6): 1341-1346
[32]	Wu C T, Al-Dahhan M H, Prakash A. Heat transfer coefficients in a high-pressure bubble column [J]. Chem. Eng. Sci., 2007, 62 (1/2): 140-147
[33]	Yu W, Wang T F, Liu M L, Wang Z W. Liquid backmixing and particle distribution in a novel multistage internal-loop airlift slurry reactor [J]. Ind. Eng. Chem. Res., 2008, 47 (11): 3974-3982
[34]	Yu W, Wang T F, Liu M L, Song F F. Investigation of operation regimes in a multistage internal-loop airlift reactor [J]. Ind. Eng. Chem. Res., 2010, 49 (22): 11752-11759
[35]	Yu W, Wang T F, Song F F, Wang Z W. Investigation of the gas layer height in a multistage internal-loop airlift reactor [J]. Ind. Eng. Chem. Res., 2009, 48 (20): 9278-9285
[36]	Zhang T W, Wang J F, Wang T F, Lin J, Jin Y. Effect of internal on the hydrodynamics in external-loop airlift reactors [J]. Chem. Eng. Process., 2005, 44 (1): 81-87
[37]	Lin J, Han M H, Wang T F, Zhang T W, Wang J F, Jin Y. Experimental study on the local hydrodynamic behavior of a three-phase external loop airlift reactor [J]. Ind. Eng. Chem. Res., 2004, 43 (18): 5432-5437
[38]	Withers H P, Eliezer K F, Mitchell J W. Slurry-phase Fischer-Tropsch synthesis and kinetic-studies over supported cobalt carbonyl derived catalysts [J]. Ind. Eng. Chem. Res., 1990, 29 (9): 1807-1814
[39]	Krishna R, Sie S T. Design and scale-up of the Fischer-Tropsch bubble column slurry reactor [J]. Fuel Process. Technol., 2000, 64 (1/2/3): 73-105
[40]	Espinoza R L, Steynberg A P, Jager B, Vosloo A C. Low temperature Fischer-Tropsch synthesis from a Sasol perspective [J]. Appl. Catal., A, 1999, 186 (1/2): 13-26
[41]	Shi Yong (石勇). Recent advances in reactor of Fischer-Tropsh synthesis [J]. Technol. Dev. Chem. Ind. (化工技术与开发), 2008, 37 (5): 31-38
[42]	Wu Y X, Gidaspow D. Hydrodynamic simulation of methanol synthesis in gas-liquid slurry bubble column reactors [J]. Chem. Eng. Sci., 2000, 55 (3): 573-587
[43]	Ledakowicz S, Stelmachowski M, Chacuk A, Deckwer W D. Methanol synthesis in bubble column slurry reactors [J]. Chem. Eng. Process., 1992, 31 (4): 213-219
[44]	Lee S Y, Gogate M R, Kulik C J. A novel single-step dimethyl ether (DME) synthesis in a 3-phase slurry reactor from co-rich syngas [J]. Chem. Eng. Sci., 1992, 47 (13/14): 3769-3776
[45]	Li Hansheng (黎汉生), Ren Fei (任飞), Wang Jinfu (王金福). Progress in development of direct mass production technique of dimethyl ether from synthesis gas in a slurry reactor [J]. Chem. Ind. Eng. Progress (化工进展), 2004, 23 (9): 921-924
[46]	Dautzenberg F M, Dedeken J C. Reactor developments in hydrotreating and conversion of residues [J]. Catal. Rev.: Sci. Eng., 1984, 26 (3/4): 421-444
[47]	Brito A, Borges M E, Arvelo R, Garcia F, Diaz M C, Otero N. Reuse of fried oil to obtain biodiesel: zeolites Y as a catalyst [J]. Int. J. Chem. Reactor Eng., 2007, 5 (1): A104
[48]	Liu X J, Piao X L, Wang Y J, Zhu S F. Calcium ethoxide as a solid base catalyst for the transesterification of soybean oil to biodiesel [J]. Energy Fuels, 2008, 22 (2): 1313-1317
[49]	Meng W J, Li J W, Chen B H, Li H B. Modeling and simulation of ethylene polymerization in industrial slurry reactor series [J]. Chinese J. Chem. Eng., 2013, 21 (8): 850-859
[50]	Ying Weiyong (应卫勇), Fang Dingye (房鼎业). Methanol carbonylation [J]. Coal Conversion (煤炭转化), 1994, 17 (4): 39-48
[51]	Zhang Qiumin (张秋民), Pan Qikun (潘琦琨), Guan Jun (关珺), He Demin (何德民), Zhao Shuchang (赵树昌). Synthesis of terephthalic acid by isomerization of coal acid in slurry reactor [J]. J. Fuel Chem. Technol. (燃料化学学报), 2008, 36 (2): 139-143
[52]	Li Xiuping (李秀平), Li Chunhu (李春虎). Study on hydrolysis of high-concentration COS in slurry bed system [J]. Adv. Fine Petrochemicals (精细石油化工进展), 2007, 8 (4): 26-28
[53]	Li Kejing (李克景), He Guangxiang (何广湘), Jin Haibo (靳海波), Zhao Zhen (赵震). Synthesis of 2,6-diisopropylnaphthalene with isopropylation of naphthalene in a slurry bubble column reactor [J]. Chinese J. Process Eng. (过程工程学报), 2008, 8 (3): 523-528
[54]	Holderich W F, Heitmann G. Synthesis of intermediate and fine chemicals on heterogeneous catalysts with respect to environmental protection [J]. Catal. Today, 1997, 38 (2): 227-233
[55]	Rajashekharam M V, Chaudhari R V. Kinetics of hydrogenation of p-isobutyl acetophenone using a supported Ni catalyst in a slurry reactor [J]. Chem. Eng. Sci., 1996, 51 (10): 1663-1672
[56]	de Jong K P, Mesters C, Peferoen D G R, van Brugge P T M, de Groot C. Paraffin alkylation using zeolite catalysts in a slurry reactor: chemical engineering principles to extend catalyst lifetime [J]. Chem. Eng. Sci., 1996, 51 (10): 2053-2060.
[57]	Toor A P, Verma A, Jotshi C K, Bajpai P K, Singh V. Photocatalytic degradation of Direct Yellow 12 dye using UV/TiO2 in a shallow pond slurry reactor [J]. Dyes Pigm., 2006, 68 (1): 53-60
[58]	Dijkstra M F J, Buwalda H, de Jong A W F, Michorius A, Winkelman J G M, Beenackers A. Experimental comparison of three reactor designs for photocatalytic water purification [J]. Chem. Eng. Sci., 2001, 56 (2): 547-555
[59]	Zhang C L, Hughes J B, Nishino S F, Spain J C. Slurry-phase biological treatment of 2,4-dinitrotoluene and 2,6-dinitrotoluene: role of bioaugmentation and effects of high dinitrotoluene concentrations [J]. Environ. Sci. Technol., 2000, 34 (13): 2810-2816
[60]	Shen Wenjie (申文杰), Zhou Jinglai (周敬来), Zhang Bijiang (张碧江). Reactors for the Fischer-Tropsch synthesis [J]. Chem. Eng. (China) (化学工程), 1995, 23 (6): 7-12
[61]	Jager B, Espinoza R. Advances in low-temperature Fischer-Tropsch synthesis [J]. Catal. Today, 1995, 23 (1): 17-28
[62]	Miao Peng (苗鹏), Xiao Cuiwei (肖翠微), Wang Naiji (王乃继), Xu Zhengang (徐振刚). Advances in technology of Fischer-Tropsch synthesis of slurry-bed reactor [J]. Coal Quality Technol. (煤质技术), 2008, (3): 46-49
[63]	Tijm P J A, Waller F J, Brown D M. Methanol technology developments for the new millennium [J]. App. Catal., A, 2001, 221 (1/2): 275-282
[64]	Mills P L, Chaudhari R V. Multiphase catalytic reactor engineering and design for pharmaceuticals and fine chemicals [J]. Catal. Today, 1997, 37 (4): 367-404
[65]	Stitt E H. Alternative multiphase reactors for fine chemicals-a world beyond stirred tanks? [J].Chem. Eng. J., 2002, 90 (1/2): 47-60
[66]	Qian Zhibin (骞志彬). General review on the production and applications of H2O2 [J]. Modern Chem. Ind. (现代化工), 1992, 12 (5): 24-27
[67]	Liu Guozhu (刘国柱), Wang Li (王莅), Mi Zhentao(米镇涛), Chen Sihai (陈四海), Ling Taiping (凌太平). Hydrogenation reactors in hydrogen peroxide production by anthraquinone process [J]. Modern Chem. Ind. (现代化工), 2003, 23 (2): 19-22
[68]	Gaikwad A G, Sansare S D, Choudhary V R. Direct oxidation of hydrogen to hydrogen peroxide over Pd-containing fluorinated or sulfated Al2O3, ZrO2, CeO2, ThO2, Y2O3 and Ga2O3 catalysts in stirred slurry reactor at ambient conditions [J]. J. Mol. Catal. A: Chem., 2002, 181 (1/2): 143-149
[69]	Tang Yujuan (汤育娟), Xu Zehui (徐泽辉). Production and application of m-xylene diamine [J]. Techno-Econ. Petrochem. (石油化工技术与经济), 2012 (3): 6-9
[70]	Nagao S, Kumano T, Nakaya K, Shigematsu R, Kato K. The preparation method of benzene dimethylamine [P]: CN, 200980137104. 2011-08-17
[71]	Dahmen K, Huber S, Hugo R, Preiss T. The preparation method of benzene dimethylamine [P]: CN, 200680035201. 2008-09-24
[72]	Wang Tiefeng (王铁峰), Yu Wei (于伟), Liu Malin (刘马林), Wang Zhanwen (汪展文), Jin Yong (金涌), Wang Jinfu (王金福), Wei Fei (魏飞). A multi-stage reacto [P]: CN,1923351 A. 2007-03-07
[73]	Chang Yanhong (常雁红), Han Yizhuo (韩怡卓), Wang Xinkui (王心葵). Production, application and development of down stream products of dimethyl ether [J]. Nat. Gas Chem. Ind. (天然气化工), 2000, 25 (3): 45-49
[74]	Lu Zhigang (陆志刚). A new energy-saving and environmental protection process of dimethyl sulphate [J]. Sulphuric Acid Ind. (硫酸工业), 2010 (2): 10-13
[75]	Zhang Kaishi (张开仕). Production technology and research progress of trichlorosilane [J]. Inorg. Chem. Ind. (无机化工), 2011, 43 (8): 11-13
[76]	Zhou Guocheng (周国成), Gou Yongtao (苟永桃), Jiang Ying (蒋英), Zhang Rao (张饶). Research on synthesis of trichlorosilane in slurry reactor [J]. Chem. Intermed. (化工中间体), 2009 (12): 58-62
[77]	Izumisawa Y, Kawahara T, Toyosawa A. Process for producing highly purified terephthalic acid [P]: US, 08/550, 400.1996-10-22
[78]	Li Xi (李希), Xie Gang (谢刚). Bubbling tower device used in the terephthalic acid oxidation reaction [P]: CN, 2654608. 2004-11-10
[79]	Li Xi (李希), Luo Wende (罗文德), Song Jingzhen (宋景祯), Xiegang (谢刚). External circulating bubble column oxidation device for producing terephthalic acid [P]: CN, 2652929. 2004-11-03
[80]	Strasser W, Wonders A. Hydrokinetic optimization of commercial scale slurry bubble column reactor [J]. AIChE J., 2012, 58 (3): 946-956
[81]	Bhattacharyya A. Process for producing terephthalic acid [P]: US, PCT/US2012/060715.2013-04-07
[82]	Kumar J, Peglow M, Warnecke G, Heinrich S. An efficient numerical technique for solving population balance equation involving aggregation, breakage, growth and nucleation [J]. Powder Technol., 2008, 182 (1): 81-104
[83]	Wu Chuanbo (武传波), Ma Bo (马波), Wang Shaojun (王少军), Ling Fengxiang (凌凤香). Study on the changes of asphaltene properties in processing residue feed by fixed-bed hydrotreating [J]. Petroleumprocessing and Petrochemicals, 2010, 41 (6): 7-11
[84]	Santacesaria E, Tesser R, Di Serio M, Guida M, Gaetano D, Agreda A G, Cammarota F. Comparison of different reactor configurations for the reduction of free acidity in raw materials for biodiesel production [J]. Ind. Eng. Chem. Res., 2007, 46 (25): 8355-8362
[85]	Liu Yuandong (刘元东), Gao Liang (郜亮), Wen Langyou (温朗友), Zong Baoning (宗保宁). Development of slurry bed technologies for upgrading heavy oils [J]. Chem. Ind. Eng. Progress (化工进展), 2010, 29 (9): 1589-1596
[86]	Marangozis J, Keramidas O B, Paparisvas G. Rate and mechanism of hydrogenation of cottonseed oil in slurry reactors [J]. Ind. Eng. Chem. Process Des. Dev., 1977, 16 (3): 361-369
[87]	Dossin T F, Reyniers M F, Berger R J, Marin G B. Simulation of heterogeneously MgO-catalyzed transesterification for fine-chemical and biodiesel industrial production [J]. Appl. Catal. B: Environ., 2006, 67 (1/2): 136-148
[88]	Zhang Dongxiang (张东翔), Lu Yingmei (陆英梅), Li Hansheng (黎汉生). Study on photocatalytic oxidation of wastewater in biologic pharmacy [J]. Environ. Prot. (环境保护), 2004 (12): 25-28
[89]	Meng Y, Huang X, Yang Q, Qian Y, Kubota N, Fukunaga S, Treatment of polluted river water with a photocatalytic slurry reactor using low-pressure mercury lamps coupled with a membrane [J]. Desalination, 2005, 181 (1): 121-133
[90]	Chong M N, Jin B, Chow C W, Saint C. Recent developments in photocatalytic water treatment technology: a review [J]. Water Res., 2010, 44 (10): 2997-3027