高温烟气中煤焦气化行为

doi:10.16085/j.issn.1000-6613.2019-0601

摘要/Abstract

摘要：

针对高温烟气中煤焦的气化行为，本文采用FactSage 6.1计算了煤焦在高温烟气下的高温反应特性，并利用热重分析仪分析了煤焦气化行为。通过沉降炉实验进一步研究了不同温度、气体配比、粒径条件下气体产物的动态析出特性，同时计算了评价指标α、β、LHV值。结果表明：随着温度的升高，气体产物H₂和CO的含量增加，β、α、LHV值增大，CH₄和CO₂的含量下降。在温度为1200℃时，β、α值分别由CO₂/CO比为10∶70时的10.80%、5.21%增加到CO₂/CO比为50∶30时的24.71%、41.06%。同时，随着CO₂/CO比值的增大，高温烟气对煤焦气化反应抑制减弱。通过对比反应温度和粒径对煤焦气化反应的影响，得出反应温度远大于粒径对煤焦气化反应的影响。通过实验验证了向高温烟气中喷吹煤焦制备高品质可燃气体方法的可行性。

关键词: 煤焦, 高温烟气, 气体产物, 沉降炉

Abstract:

According to gasification behavior of coal chair in high temperature flue gas, high temperature reaction characteristics of coal char in high temperature flue gas, using FactSage 6.1 was calculated and gasification behavior was analyzed using thermogravimetric analyzer. Dynamic precipitation characteristics of gas products under different temperatures, gas ratios and particle sizes were further studied by conducting the settling furnace experiments. At the same time the evaluation indexes, including α, β and LHV values were calculated as well. The results showed that with the increase of temperature, the contents of gas products H₂ and CO increase, the values of β, α and LHVincrease, and the contents of CH₄ and CO₂ decrease. At a constant temperature of 1200℃, the values of β and α increased from 10.80% and 5.21% at a CO₂/CO ratio of 10∶70 to 24.71% and 41.06% at a CO₂/CO ratio of 50∶30, respectively. Moreover, with the increase of CO₂/CO ratio, the inhibition of the coal char gasification reaction was weakened by high temperature flue gas. By comparing the effects of reaction temperature and particle size of coal char on gasification, it can be concluded that the effect of reaction temperature on gasification reaction in coal char is much larger than the size of coal char. The feasibility of preparing high-quality flammable gas by spraying coke into high temperature flue gas was verified by experiments.

Key words: coal char, high temperature flue gas, gas product, settling furnace

中图分类号:

宋伟明,周建安,王宝,李数,杨健. 高温烟气中煤焦气化行为[J]. 化工进展, 2020, 39(1): 395-401.

Weiming SONG,Jian’an ZHOU,Bao WANG,Shu LI,Jian YANG. Gasification behavior of coal char in high temperature flue gas[J]. Chemical Industry and Engineering Progress, 2020, 39(1): 395-401.

图/表 10

参考文献 26

1	WANG Y , WANG Z , HUANG J , et al . Investigation into the characteristics of Na₂CO₃-catalyzed steam gasification for a high-aluminum coal char [J]. Journal of Thermal Analysis & Calorimetry, 2018, 131(2): 1213-1220.
2	YAN L , CAO Y , LI X , et al . Characterization of a dual fluidized bed gasifier with blended biomass/coal as feedstock [J]. Bioresource Technology, 2018, 254: 97-106.
3	MUKHERJEE A B , ZEVENHOVEN R , BHATTACHARYAB P , et al . Mercury flow via coal and coal utilization by-products: a global perspective [J]. Resources Conservation & Recycling, 2008, 52(4): 571-591.
4	KREYNIN E V . An analysis of new generation coal gasification projects [J]. International Journal of Mining Science & Technology, 2012, 22(4): 509-515.
5	BROEK M VAN DEN , FAAIJ A , TURKENBURG W . Planning for an electricity sector with carbon capture and storage: case of the Netherlands [J]. International Journal of Greenhouse Gas Control, 2008, 2(1): 105-129.
6	GERSSEN-GONDELACH S J , FAAIJ A P C . Performance of batteries for electric vehicles on short and longer term [J]. Journal of Power Sources, 2012, 212(9): 111-129.
7	UMEMOTO S , KAJITANI S , HARA S . Modeling of coal char gasification in coexistence of CO₂ and H₂O considering sharing of active sites [J]. Fuel, 2013, 103(1): 14-21.
8	KIM Y T , SEO D K, HWANG J . Study of the effect of coal type and particle size on char–CO₂ gasification via gas analysis [J]. Energy & Fuels, 2011, 25(11): 5044-5054.
9	FERMOSO J , GIL M V, GARCÍA S , et al . Kinetic parameters and reactivity for the steam gasification of coal chars obtained under different pyrolysis temperatures and pressures [J]. Energy & Fuels, 2011, 25(8): 3574-3580.
10	EVERSON R C , NEOMAGUS H W J P , KASAINI H , et al . Reaction kinetics of pulverized coal-chars derived from inertinite-rich coal discards: Gasification with carbon dioxide and steam [J]. Fuel, 2006, 85(7): 1076-1082.
11	YU J , ZENG X , ZHANG J W , et al . Isothermal differential characteristics of gas-solid reaction in micro-fluidized bed reactor [J]. Fuel, 2013, 103: 29-36.
12	FANG W , XI Z , WANG Y , et al . Non-isothermal coal char gasification with CO₂, in a micro fluidized bed reaction analyzer and a thermogravimetric analyzer [J]. Fuel, 2016, 164: 403-409.
13	GENG P , ZHANG Y , ZHENG Y . Experimental estimate of CO₂, concentration distribution in the stagnant gas layer inside the thermogravimetric analysis (TGA) crucible [J]. Fuel, 2018, 224: 250-254.
14	AHN D H, GIBBS B M , KO K H, et al . Gasification kinetics of an Indonesian sub-bituminous coal-char with CO₂, at elevated pressure [J]. Fuel, 2001, 80(11): 1651-1658.
15	KAJITANI S , SUZUKI N , ASHIZAWA M , et al . CO₂ gasification rate analysis of coal char in entrained flow coal gasifier [J]. Fuel, 2006, 85(2): 163-169.
16	ZHANG H , CEN K , YAN J , et al . The fragmentation of coal particles during the coal combustion in a fluidized bed [J]. Fuel, 2002, 81(14): 1835-1840.
17	WANG Q H , RONG N , FAN H T , et al . Enhanced hydrogen-rich gas production from steam gasification of coal in a pressurized fluidized bed with CaO as a CO₂ sorbent [J]. International Journal of Hydrogen Energy, 2014, 39(11): 5781-5792.
18	BAI Y , WANG Y , ZHU S , et al . Synergistic effect between CO₂ and H₂O on reactivity during coal chars gasification [J]. Fuel, 2014, 126(9): 1-7.
19	JAYARAMAN K , GOKALP I , JEYAKUMAR S . Estimation of synergetic effects of CO₂ in high ash coal-char steam gasification [J]. Applied Thermal Engineering, 2017, 110: 991-998.
20	MEI Z , ZHANG Z , QI Z , et al . Continuous high-temperature fluidized bed pyrolysis of coal in complex atmospheres: Product distribution and pyrolysis gas [J]. Journal of Analytical & Applied Pyrolysis, 2012, 97(6): 123-129.
21	KUHN L , PLOGMANN H . Reaction of catalysts with mineral matter during coal gasification [J]. Fuel, 1983, 62(2): 205-208.
22	TSAI C Y , SCARONI A W . Reactivity of bituminous coal chars during the initial stage of pulverized-coal combustion [J]. Fuel, 1987, 66(10): 1400-1406.
23	MUHLEN H J , HEEK K H V , JUNTGEN H . Kinetic studies of steam gasification of char in the presence of H₂, CO₂, and CO [J]. Fuel, 1985, 64(7): 944-949.
24	XU S , ZHOU Z , GAO X , et al . The gasification reactivity of unburned carbon present in gasification slag from entrained-flow gasifier [J]. Fuel Processing Technology, 2009, 90(9): 1062-1070.
25	RUI Z , WANG Q H , LUO Z Y , et al . Competition and inhibition effects during coal char gasification in the mixture of H₂O and CO₂ [J]. Energy & Fuels, 2013, 27(9): 5107-5115.
26	MANDAPATI R N , DAGGUPATI S , MAHAJANI S M , et al . Experiments and kinetic modeling for CO₂ gasification of Indian coal chars in the context of underground coal gasification [J]. Industrial & Engineering Chemistry Research, 2012, 51(46): 15041-15052.

工业分析/%					元素分析/%						灰熔点/℃
FC_ad	V_ad	A_ad	M_ad		C_ad	H_ad	N_ad	S_ad	O_ad		DT	ST	HT	FT
84.23	8.21	6.02	1.54		86.69	1.66	1.48	0.37	2.24		1235	1279	1298	1321

工业分析/%					元素分析/%						灰熔点/℃
FC_ad	V_ad	A_ad	M_ad		C_ad	H_ad	N_ad	S_ad	O_ad		DT	ST	HT	FT
84.23	8.21	6.02	1.54		86.69	1.66	1.48	0.37	2.24		1235	1279	1298	1321

编号	材料	粒度/目	CO∶CO₂∶N₂	温度/℃
1	煤焦	200(75μm)	5∶3∶2	900
2	煤焦	200(75μm)	5∶3∶2	1000
3	煤焦	200(75μm)	5∶3∶2	1100
4	煤焦	200(75μm)	5∶3∶2	1200
5	煤焦	200(75μm)	5∶3∶2	1300
6	煤焦	200(75μm)	7∶1∶2	1200
7	煤焦	200(75μm)	6∶2∶2	1200
8	煤焦	200(75μm)	5∶3∶2	1200
9	煤焦	200(75μm)	4∶4∶2	1200
10	煤焦	200(75μm)	3∶5∶2	1200
11	煤焦	100(150μm)	0∶10∶0	900~1300
12	煤焦	200(75μm)	0∶10∶0	900~1300
13	煤焦	300(48μm)	0∶10∶0	900~1300
14	煤焦	400(38μm)	0∶10∶0	900~1300

编号	材料	粒度/目	CO∶CO₂∶N₂	温度/℃
1	煤焦	200(75μm)	5∶3∶2	900
2	煤焦	200(75μm)	5∶3∶2	1000
3	煤焦	200(75μm)	5∶3∶2	1100
4	煤焦	200(75μm)	5∶3∶2	1200
5	煤焦	200(75μm)	5∶3∶2	1300
6	煤焦	200(75μm)	7∶1∶2	1200
7	煤焦	200(75μm)	6∶2∶2	1200
8	煤焦	200(75μm)	5∶3∶2	1200
9	煤焦	200(75μm)	4∶4∶2	1200
10	煤焦	200(75μm)	3∶5∶2	1200
11	煤焦	100(150μm)	0∶10∶0	900~1300
12	煤焦	200(75μm)	0∶10∶0	900~1300
13	煤焦	300(48μm)	0∶10∶0	900~1300
14	煤焦	400(38μm)	0∶10∶0	900~1300

[1]	杨莹, 侯豪杰, 黄瑞, 崔煜, 王兵, 刘健, 鲍卫仁, 常丽萍, 王建成, 韩丽娜. 利用煤焦油中酚类物质Stöber法制备碳纳米球用于CO₂吸附[J]. 化工进展, 2023, 42(9): 5011-5018.
[2]	罗成, 范晓勇, 朱永红, 田丰, 崔楼伟, 杜崇鹏, 王飞利, 李冬, 郑化安. 中低温煤焦油加氢反应器不同分配器中液体分布的CFD模拟[J]. 化工进展, 2023, 42(9): 4538-4549.
[3]	徐贤, 崔楼伟, 刘杰, 施俊合, 朱永红, 刘姣姣, 刘涛, 郑化安, 李冬. 原料组成对半焦中间相结构发展的影响[J]. 化工进展, 2023, 42(5): 2343-2352.
[4]	张乐乐, 钱运东, 朱华曈, 冯思龙, 杨秀娜, 于颖, 杨强, 卢浩. 加氢原料煤焦油脱水除盐预处理工艺优化限值[J]. 化工进展, 2023, 42(5): 2298-2305.
[5]	杨永斌, 董寅瑞, 钟强, 李骞, 王林, 姜涛. 高温煤焦油沥青黏结剂碳化固结作用在炭质型材中的应用与研究进展[J]. 化工进展, 2022, 41(12): 6419-6429.
[6]	郑金欣,田育成,郝博天,淡勇,李稳宏,黄晔,高峰,李冬. 中低温煤焦油基炭微球的制备[J]. 化工进展, 2020, 39(2): 649-657.
[7]	常秋连, 李文博, 赵鹏. 煤焦油渣炭化过程中孔结构及表面分形特征[J]. 化工进展, 2020, 39(10): 4305-4313.
[8]	邱泽刚,尹婵娟,李志勤,冯跃阔. 酚类加氢脱氧催化剂研究进展[J]. 化工进展, 2019, 38(08): 3658-3669.
[9]	陈康, 闫挺, 姜召, 方涛. 超临界流体改质煤焦油研究进展[J]. 化工进展, 2019, 38(04): 1702-1713.
[10]	杜博文, 陈康, 丁鑫, 姜召, 方涛. 超临界二氧化碳与二苯醚相平衡研究[J]. 化工进展, 2019, 38(04): 1662-1670.
[11]	马明明, 苏小平, 闵小建, 郑化安, 樊英杰, 万冲, 孙鸣, 马晓迅. 中低温煤焦油蒸馏过程中金属元素的迁移规律[J]. 化工进展, 2018, 37(09): 3355-3361.
[12]	张生娟, 高亚男, 陈刚, 姬鹏军, 石欣, 赵静, 赵丽信, 王艳红. 煤焦油中酚类化合物的分离及其组成结构鉴定研究进展[J]. 化工进展, 2018, 37(07): 2588-2596.
[13]	崔文岗, 李冬, 樊安, 潘柳依, 牛梦龙, 李稳宏. 低温煤焦油加氢制备清洁燃料油品中试试验研究[J]. 化工进展, 2018, 37(06): 2192-2202.
[14]	燕希敏, 苗鹏, 常国璋, 郭庆杰. Fe/赤泥催化水蒸气气化煤焦的反应性与微结构特性[J]. 化工进展, 2018, 37(05): 1753-1759.
[15]	胡林, 王光华, 何龙, 王晴东, 马志勇, 刘阳. 褐煤焦与NaNO₃对昭通褐煤微波提质特性研究[J]. 化工进展, 2017, 36(12): 4423-4429.