典型碱金属碱土金属对焦炭-CO_2反应性影响的研究
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摘要
焦炭热态反应性能够较好地反映其在高炉中抵抗化学侵蚀的能力,是评价焦炭质量的重要指标。
本文以研究典型碱金属、碱土金属对不同变质程度煤焦-CO_2反应性,以及同种煤不同密度级富集物焦-CO_2反应性的催化作用关系为目的,通过添加K_2CO_3、Na_2CO_3、CaCO_3和MgO到煤(或各密度级富集物)中炼焦,研究了碱金属、碱土金属对焦炭催化溶损反应动力学,初步探讨了焦炭的溶损反应原因,得出了碱对不同煤岩组成的催化作用关系。
研究结果表明:添加碱金属、碱土金属对气煤焦炭反应性的影响小于对焦煤焦炭的影响。同种碱金属、碱土金属随添加量的增加,焦炭转化率越大。随溶损反应时间的增加,焦炭转化率逐步增加。其他条件相同时,添加K_2CO_3对焦炭转化率的影响最大,其他依次为Na_2CO_3,CaCO_3和MgO。对于焦煤而言,加碱后镜质组对应的焦炭显微结构的反应活性变大。自身碱含量低的焦炭,加碱后溶损反应中CO_2转化率增加幅度大于自身碱含量高的焦炭。
动力学研究表明,对于气煤焦炭,加碱的催化作用在于降低了反应的活化能。而焦煤焦炭添加0.5%的Na_2CO_3、CaCO_3和MgO时,活化能增加,表明反应速率对温度的敏感程度加强,且指前因子相应增大,表明提供了更多的反应活性点,随添加量的增加,活化能降低成为影响反应速率的主要因素。碱金属、碱土金属对焦炭溶损反应的催化作用是由降低反应活化能和增加活性中心共同作用的结果。
The coke reactivity index (CRI) is a significant index for evaluating coke qualities, which is more suitable for the abilities of the coke for resisting chemical destruction in blast furnace.
With the purposes of studying the catalysis relationship of typical alkali and alkaline metals to the coke reactivity, by adding K_2CO_3、Na_2CO_3、CaCO_3 and MgO to different rank coals and adding K_2CO_3 and CaCO_3 to different density levels of one kind of coal for caking, the catalysis dissolution reaction kinetics of typical alkali and alkaline metals to cokes is studied, the reason of coke dissolution reaction is discussed and the catalysis relationship of typical alkali and alkaline metals to different maceral compositions are elicited. The summery of the results as follows:
The influence of typical alkali and alkaline metals to the reactivity of coke from gas coal is lower than it from coking coal. Along with the increasing of quantities of typical alkali and alkaline metals or reaction time, the percent conversion of coke increased. Under the same conditions, the influence sequence of coke percent conversion is K_2CO_3, Na_2CO_3、CaCO_3 and MgO. With catalysis of typical alkali and alkaline metals, the coke with lower alkali itself have higher percent conversion. And the microstructure composition corresponding the vitrinite of coking coal has higher reactivity.
The kinetics studying shows that adding alkali can reduce the activity energy of coke dissolution reaction which from gas coal. Adding 0.5% Na_2CO_3、CaCO_3 and MgO to coking coal for caking, the activity energy of the coke dissolution reaction increasing, it means that the sensitivity degree of reaction rate to temperature is stronger. At the same time, the increasing pre-exponential factor means more active spots, Along with the increase of adding quantity, activity energy decreased which becoming the main factor of influencing reaction rate. The catalysis of typical alkali and alkaline metals to the coke reactivity is the result of activity energy decrease and active spots increase.
本文以研究典型碱金属、碱土金属对不同变质程度煤焦-CO_2反应性,以及同种煤不同密度级富集物焦-CO_2反应性的催化作用关系为目的,通过添加K_2CO_3、Na_2CO_3、CaCO_3和MgO到煤(或各密度级富集物)中炼焦,研究了碱金属、碱土金属对焦炭催化溶损反应动力学,初步探讨了焦炭的溶损反应原因,得出了碱对不同煤岩组成的催化作用关系。
研究结果表明:添加碱金属、碱土金属对气煤焦炭反应性的影响小于对焦煤焦炭的影响。同种碱金属、碱土金属随添加量的增加,焦炭转化率越大。随溶损反应时间的增加,焦炭转化率逐步增加。其他条件相同时,添加K_2CO_3对焦炭转化率的影响最大,其他依次为Na_2CO_3,CaCO_3和MgO。对于焦煤而言,加碱后镜质组对应的焦炭显微结构的反应活性变大。自身碱含量低的焦炭,加碱后溶损反应中CO_2转化率增加幅度大于自身碱含量高的焦炭。
动力学研究表明,对于气煤焦炭,加碱的催化作用在于降低了反应的活化能。而焦煤焦炭添加0.5%的Na_2CO_3、CaCO_3和MgO时,活化能增加,表明反应速率对温度的敏感程度加强,且指前因子相应增大,表明提供了更多的反应活性点,随添加量的增加,活化能降低成为影响反应速率的主要因素。碱金属、碱土金属对焦炭溶损反应的催化作用是由降低反应活化能和增加活性中心共同作用的结果。
The coke reactivity index (CRI) is a significant index for evaluating coke qualities, which is more suitable for the abilities of the coke for resisting chemical destruction in blast furnace.
With the purposes of studying the catalysis relationship of typical alkali and alkaline metals to the coke reactivity, by adding K_2CO_3、Na_2CO_3、CaCO_3 and MgO to different rank coals and adding K_2CO_3 and CaCO_3 to different density levels of one kind of coal for caking, the catalysis dissolution reaction kinetics of typical alkali and alkaline metals to cokes is studied, the reason of coke dissolution reaction is discussed and the catalysis relationship of typical alkali and alkaline metals to different maceral compositions are elicited. The summery of the results as follows:
The influence of typical alkali and alkaline metals to the reactivity of coke from gas coal is lower than it from coking coal. Along with the increasing of quantities of typical alkali and alkaline metals or reaction time, the percent conversion of coke increased. Under the same conditions, the influence sequence of coke percent conversion is K_2CO_3, Na_2CO_3、CaCO_3 and MgO. With catalysis of typical alkali and alkaline metals, the coke with lower alkali itself have higher percent conversion. And the microstructure composition corresponding the vitrinite of coking coal has higher reactivity.
The kinetics studying shows that adding alkali can reduce the activity energy of coke dissolution reaction which from gas coal. Adding 0.5% Na_2CO_3、CaCO_3 and MgO to coking coal for caking, the activity energy of the coke dissolution reaction increasing, it means that the sensitivity degree of reaction rate to temperature is stronger. At the same time, the increasing pre-exponential factor means more active spots, Along with the increase of adding quantity, activity energy decreased which becoming the main factor of influencing reaction rate. The catalysis of typical alkali and alkaline metals to the coke reactivity is the result of activity energy decrease and active spots increase.
引文
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2.H.Marsh.Introduction to Carbon Science,Butterworths,1989
3.周师庸.高炉焦炭质量指标探析.炭素技术,2004(3):19-22
4.Coil T,Perales J.F,Arnaldos J,Casal J..Coal Pyrolysis:Thermogravimetric Study and Kinetic Modelling,Thermochimica Acta,1992,196(1):53
5.Norton GA.A Review of the Derivative Thermogravimetric Technique for Fuel Combustion Studies,Thermochimica Acta,1993,214(2):171
6.杨俊和,李依丽,冯安祖.煤中矿物质对焦炭光学显微组份的作用.煤炭转化,1999(22):3-48
7.崔秀文.中国金属学会炼焦论文集.鞍山热能研究院.1992:74
8.王建华.焦炭抗碱能力的提高及其成本的降低.煤化工,1998(3):4
9.汪海涛,胡红玲,付利俊,金蝶翔.焦炭反应性及反应后强度和焦炭抗碱性试验研究.内蒙古科技与经济,2004(24):44-46
10.姚昭章.炼焦学.冶金工业出版社.1995
11.傅永宁.高炉焦炭.冶金工业出版社.1995
12.杜鹤桂,杨俊和.矿物质对高炉焦炭溶损反应的催化作用.炼铁,2002,21(4):22-24
13.胡军,孔凡朔,赵晓明等.高炉喷吹高反应性煤对焦炭高温性能的影响.煤炭学报,2003,28(4):419-422
14.Leth-Millera R,Jensenb A.D,Jensenb J..Comparative Study of Reactivity to CO_2 of C okes Used in Stone Wool Production.Fuel Processing Technology,2005,86:551-563
15.杨俊和,冯安祖,杜鹤桂.高炉焦炭中矿物质的化学形态和物种.钢铁研究学报,2001,13(2):1-5
16.M.Hatano,T.Miyazaki,Y.lwanaga.Influence of Alkali on the Coke Properties,Trans.I SIJ.,1980(20):592
17.W-K.Lu,G.Samaan,M.Uribe(来华讲学材料)
18.付永宁,金慧军,黄永福.焦炭的深部溶损和在高炉中的行为.钢铁,1990,25(1):1
19.D.J.Harris,D.J.Yong.Ptassium effect in solution loss reaction of metallurgical coke,Ir onmaking and Steelmaking,1989,16(6):399
20.徐国忠,陈德浩,周师庸.模拟焦炭在高炉软融带碳溶反应的研究.鞍山科技大学学报,2003(26):48-52
21.T.K.Baker,R.F.Lund.Catalytic Gasification of Graphite by Barium in Steam,Carbon Dioxide,Oxygen,and Hydrogen.Journal of Catalysis,1984,87:255
22.邹德余,何生平,许原,周培土,梁明昭.添加剂对焦炭反应性的影响.钢铁.37卷
23.Lang R.T.et al.Behaviour of Calcium as a Steam Gasification Catalyst,Fuel,1982,61:620
24.A.Linares-Solano,M.Almela-Alarcon,C.Salinas,CO_2 Chemisorption Calcium Catalysts in Carbon Gasification Reaction Journal of Catalysis,1990,125:401
25.Jacob A.Moulijin.Mechanism of the potassium catalysed gasification of carbon in CO_2.Fuel,1984(63):1043-1047
26.藤田英夫.焦炭通报(日木).1980(29):218
27.K.Mikio et al.AIME Iron Making Proc.1981(40):454
28.D.W.McKee.Chemistry and physics of carbon.Marcel Dekker Inc.1981,16
29.徐秀峰,顾永达,陈诵英.煤焦气化反应的影响因素和反应机理的研究进展.煤炭转化, 1996.2:51
30.Amarigilio,H.And Duval,X.,Plasma Activation of Carbon Cloth,Carbon,1986,24:325
31.Muralidhara HS.Sears J.T.,Coal Process Technology,1978,4:22
32.Mckee D.W.and Chaterji D.,Kinetic and Microscopy Aspects of Catalytic Carbon Growth,Carbon,1975,13:381
33.C.Y.Wen,Cata.Rev.Sci.Eng.1980(22)
34.肖慧敏.焦炭破损机理研究.武钢技术,1985,(1):1
35.Yokoyama et al.Nippon Kagaku Kaishi.1980(6):974
36.Kenji Hashimoto et al.Relation between the gasification rate of carbons supporting alkali metal salts and the amount of oxygen trapped by the metal.Fuel,1986(65):489-494
37.The late Thomas D.Hengei et al.Catalysis of lignite char gasification by exchangeable calcium and magnesium.Fuel,1984(63):1214-1219
38.Robert T.Hamilton et al.Variation of rate during potassium-catalysed CO_2 gasification of coal char.Fuel,1984(63):1008-1012
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