循环流化床锅炉内石灰石脱硫研究进展
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摘要
循环流化床(CFB)锅炉是燃用劣质煤的最佳设备,炉内石灰石脱硫具有操作简单、成本低等优势,但也存在脱硫效率不够高、石灰石利用率低等问题,在当前燃煤超净排放的背景下,有必要探索CFB内石灰石高效脱硫的理论和技术。本文综述了近年来石灰石脱硫研究的新进展,包括水蒸气对CaO硫化反应的影响及机理、石灰石同时煅烧硫化反应及模型等;介绍了近年来提出的改善炉内脱硫效果的方法,包括采用小粒径石灰石和吸收剂的活化等。着重介绍了石灰石同时煅烧/硫化反应新概念,阐述了CFB内石灰石可能无法完全热解的现象及原因,以及该反应的研究进展和需要继续开展的工作。介绍了CaO硫化反应模型的研究进展,并提出了石灰石同时煅烧硫化反应的随机孔模型,将石灰石煅烧、烧结和CaO硫化反应同时考虑在内,更精确地描述炉内石灰石反应的过程。指出研究者应重视炉内脱硫的真实反应过程,避免对CFB脱硫过程做过度简化,否则研究结论很难反映炉内脱硫的真实规律。
Circulating fluidized bed(CFB) boilers are the best device to utilize inferior coal. In-situ SO_2 removal with limestone is easy and low-cost, but the desulfurization efficiency and calcium utilization are not high enough. Under the circumstance of the ultra-low emission of coal-fired boilers, it is still necessary to investigate the way to improve the sulfur removal performance in CFB boilers. In this paper,SO_2 removal with limestone was reviewed. The effect of H_2 O on CaO sulfation was introduced, as well as the simultaneous calcination/sulfation reaction and the model. The use of smaller limestone particles and sorbents reactivation was also introduced. The emphasis was put on the simultaneous calcination/sulfation reaction of limestone, in which the phenomenon that CaCO_3 in limestone cannot decompose completely under CFB conditions was analyzed. The research progress of this reaction as well as the work still need to be done was described. A new model was put forward, which is based on the random pore concept and considered the calcination, sintering and sulfation reaction simultaneously. The new model can describe the reaction process of limestone in CFB more accurately. The research of desulfurization in CFB should be based on the real reaction process of limestone, and the simplification of this reaction should be limited to the reasonable bounds, otherwise the research conclusion cannot reflect its real characteristics.
Circulating fluidized bed(CFB) boilers are the best device to utilize inferior coal. In-situ SO_2 removal with limestone is easy and low-cost, but the desulfurization efficiency and calcium utilization are not high enough. Under the circumstance of the ultra-low emission of coal-fired boilers, it is still necessary to investigate the way to improve the sulfur removal performance in CFB boilers. In this paper,SO_2 removal with limestone was reviewed. The effect of H_2 O on CaO sulfation was introduced, as well as the simultaneous calcination/sulfation reaction and the model. The use of smaller limestone particles and sorbents reactivation was also introduced. The emphasis was put on the simultaneous calcination/sulfation reaction of limestone, in which the phenomenon that CaCO_3 in limestone cannot decompose completely under CFB conditions was analyzed. The research progress of this reaction as well as the work still need to be done was described. A new model was put forward, which is based on the random pore concept and considered the calcination, sintering and sulfation reaction simultaneously. The new model can describe the reaction process of limestone in CFB more accurately. The research of desulfurization in CFB should be based on the real reaction process of limestone, and the simplification of this reaction should be limited to the reasonable bounds, otherwise the research conclusion cannot reflect its real characteristics.
引文
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[4]吉云,陈鸿伟,王春波,等.钙基脱硫剂颗粒同时煅烧和烧结的数学描述[J].锅炉技术,2005,36(2):76-80.JI Y,CHEN H W,WANG C B,et al.A mathematical model for the simultaneous calcination and sintering of calcium-based sorbents[J].Boiler Technology,2005,36(2):76-80.
[5]ESCARDINO A,GARCIA-TEN J,FELIU C.Kinetic study of calcite particle(powder)thermal decomposition:PartⅠ[J].Journal of the European Ceramic Society,2008,28(16):3011-3020.
[6]WANG C,ZHANG Y,JIA L,et al.Effect of water vapor on the pore structure and sulfation of CaO[J].Fuel,2014,130:60-65.
[7]杨振森,刘彬,陈宁武,等.提高CFB锅炉炉内脱硫效率的试验研究[J].洁净煤技术,2012,18(6):72-75.YANG Z S,LIU B,CHEN N W,et al.Experimental research on desulfuration efficiency improvement of CFB boiler[J].Clean Coal Technology,2012,18(6):72-75.
[8]LAS O M,DIEGO L F,GARCíA-LABIANO F,et al.Modeling of limestone sulfation for typical oxy-fuel fluidized bed combustion conditions[J].Energy&Fuels,2013,27(4):2266-2274.
[9]MAHULI S K,AGNIHOTRI R,CHAUK S,et al.Pore-structure optimization of calcium carbonate for enhanced sulfation[J].AIChEJournal,1997,43(9):2323-2335.
[10]HSIA C,S T.PIERRE G R,RAGHUNATHAN K,et al.Diffusion through CaSO4formed during the reaction of CaO with SO2and O2[J].AIChE Journal,1993,39(4):698-700.
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[12]DUO W,LAURSEN K,LIM J,et al.Crystallization and fracture:product layer diffusion in sulfation of calcined limestone[J].Industrial&Engineering Chemistry Research,2004,43(18):5653-5662.
[13]钱超然.石灰石颗粒磨损特性与机制研究[D].重庆:重庆大学,2013.QIAN C R.Experimental study on attrition characteristics and mechanisms of limestone particles[D].Chongqing:Chongqing University,2013.
[14]CHEN Z,GRACE J R,JIM LIM C.Limestone particle attrition and size distribution in a small circulating fluidized bed[J].Fuel,2008,87(7):1360-1371.
[15]SAASTAMOINEN J,TOURUNEN A,LEINO T,et al.Modeling of particle size distribution of limestone in sulfur capture in air and oxyfuel circulating fluidized bed combustion[J].Energy and Emission Control Technologies,2016,4(8):41-52.
[16]钱超然,张力,杨仲卿.石灰石颗粒碰撞磨损特性实验研究[J].材料导报,2013,27(16):131-135.QIAN C R,ZHANG L,YANG Z Q.Experimental research of impact attrition characteristics for limestone particles[J].Materials Review,2013,27(16):131-135.
[17]YAO X,ZHANG H,YANG H,et al.An experimental study on the primary fragmentation and attrition of limestones in a fluidized bed[J].Fuel Processing Technology,2010,91(9):1119-1124.
[18]SCALA F,SALATINO P.Limestone fragmentation and attrition during fluidized bed oxyfiring[J].Fuel,2010,89(4):827-832.
[19]WANG C,JIA L,TAN Y,et al.The effect of water on the sulphation of limestone[J].Fuel,2010,89(9):2628-2632.
[20]DUAN L,JIANG Z,CHEN X,et al.Investigation on water vapor effect on direct sulfation during wet-recycle oxy-coal combustion[J].Applied Energy,2013,108(8):121-127.
[21]JIANG Z,DUAN L,CHEN X,et al.Effect of water vapor on indirect sulfation during oxy-fuel combustion[J].Energy&Fuels,2013,27(3):1506-1512.
[22]姜中孝,段伦博,陈晓平,等.空气燃烧与O2/CO2燃烧气氛下水蒸气对石灰石煅烧/硫化特性的影响[J].中国电机工程学报,2013,33(26):14-20.JIANG Z X,DUAN L B,CHEN X P,et al.Effect of water vapor on indirect sulfation during air and O2/CO2combustion[J].Proceedings of the CSEE,2013,33(26):14-20.
[23]STEWART M C,MANOVIC V,ANTHONY E J,et al.Enhancement of indirect sulphation of limestone by steam addition[J].Environmental Science&Technology,2010,44(22):8781-8786.
[24]WANG C,CHEN L,JIA L,et al.Simultaneous calcination and sulfation of limestone in CFBB[J].Applied Energy,2015,155:478-484.
[25]王子铭,陈亮,岳爽,等.同时煅烧硫化反应中石灰石微观孔结构演变特性[J].化工学报,2018,69(5):2149-2157.WANG Z M,CHEN L,YUE S,et al.Microstructure evolution of procedural products during limestone simultaneous calcination/sulfation[J].CIESC Journal,2018,69(5):2149-2157.
[26]SAASTAMOINEN J,PIKKARAINEN T,TOURUNEN A,et al.Model of fragmentation of limestone particles during thermal shock and calcination in fluidised beds[J].Powder Technology,2008,187(3):244-251.
[27]DIEGO L F,LAS O M,GARCíA-LABIANO F,et al.Characterization of a limestone in a batch fluidized bed reactor for sulfur retention under oxy-fuel operating conditions[J].International Journal of Greenhouse Gas Control,2011,5(5):1190-1198.
[28]OLAS M,KOBY?ECKI R,BIS Z.Simultaneous calcination and sulfation of limestone-based sorbents in CFBC-effect of mechanical activation[C]//Proceedings of the 9th International Conference on Circulating Fluidized Beds,in Conjunction with the 4th International VGB Workshop"Operating Experience with Fluidized Bed Firing Systems",Hamburg,Germany,2008.
[29]CHEN L,WANG C,WANG Z,et al.The kinetics and pore structure of sorbents during the simultaneous calcination/sulfation of limestone in CFB[J].Fuel,2017,208:203-213.
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