Construction and verification of BGL coal gasification kinetic model

doi:10.11949/0438-1157.20220815

Abstract

Abstract:

At the moment of energy saving and emission reduction, more and more attention is paid to the equipment development and performance optimization of the BGL coal gasification technology. The analysis and prediction of BGL coal gasification performance still mainly use the equilibrium model and the overall reaction model, but the prediction accuracy is still insufficient. Aiming at the BGL coal gasification process, the research improves the reduced core model, subdivides the carbon core into the interface reaction zone and the inner reaction zone, and improves the adaptability of the model. The final yield and composition of coal pyrolysis gas are predicted by combining device calibration data and pyrolysis data, which simplifies the iterative optimization process. The general pyrolysis kinetic model is used to predict the height of coal seam, and the calculated value is 1.22 m, which is more in line with the actual situation. The calculation results of BGL one-dimensional coal gasification model constructed in this work show that the calculated value of crude gas composition is very close to the calibration check value. The gas phase temperature near the burner is 2012℃, and the particle phase temperature is 1978℃, which is consistent with the empirical estimation value. The crude gas outlet temperature is 549℃, and the measured crude gas outlet temperature is about 538℃.

Key words: coal gasification, pyrolysis, improved shrinking model, reaction kinetics, numerical simulation

摘要：

在目前节能减排需求下，针对BGL煤气化技术的装备研发与性能优化正越来越受重视。BGL煤气化性能分析和预测仍主要采用平衡模型和整体反应模型，但在预测准确度上仍显不足。本文针对BGL煤气化过程，改进缩核模型，将碳核细分为界面反应区和内部反应区，改善了模型适应性。煤热解气最终产率和组成预测采用装置标定数据和热解数据相结合预测，简化了迭代寻优过程。煤热解层高度预测采用通用热解动力学模型，计算值为1.22 m，较符合实际情况。本文构建的BGL煤气化一维模型计算结果表明：粗煤气组成计算值与标定校核值很接近；烧嘴邻近区气相温度2012℃，颗粒相温度1978℃，与经验估测值一致；粗煤气出口温度549℃，实测粗煤气出口温度约538℃。

关键词: 煤气化, 热解, 改进缩核模型, 反应动力学, 数值模拟

CLC Number:

TQ 018

Lihe ZHANG, Fan ZHANG, Changlun LI, Deping XU, Zhengang XU, Yonggang WANG. Construction and verification of BGL coal gasification kinetic model[J]. CIESC Journal, 2022, 73(10): 4668-4678.

张利合, 张凡, 李昌伦, 许德平, 徐振刚, 王永刚. BGL煤气化动力学模型构建与验证[J]. 化工学报, 2022, 73(10): 4668-4678.

Figures/Tables 16

Fig.1 Shrinking model structure

Table 1 Reaction kinetic parameters and equilibrium constant model of BGL coal gasification

反应		指前因子	活化能	文献
异相反应	R1	1.766×10⁷ mol/(mol C·MPa·s)	1.1304×10⁵ J/mol	[1,14,16]
	R2	2298.49 mol/(mol C·MPa·s)	1.3634×10⁵ J/mol	[1,14,16]
	R3	1376.34 mol/(mol C·MPa·s)	1.3634×10⁵ J/mol	[1,14,16]
	R4	1.2918 mol/(mol C·MPa·s)	1.0803×10⁵ J/mol	[1,14,16]
均相反应	R5	1.35×10⁶ mol/(m³·s)	60.09×10⁶ J/mol	[1,32]
	R6	3.0×10¹⁰ mol/(m³·s)	2.40×10⁵ J/mol	[9,25]
	R7	3.09×10¹¹ mol/(m³·s)	99.760×10³ J/mol	[1,32]
平衡常数
R2		lnK_eq = -21000/T +21.4		[1,16]
R3		lgK_eq = 2.554 - 6740.5/T + 1.556lgT - 1.092×10^-4T - 3.71×10^-7T²		[1,16]
R4		lgK_eq = 11.79+ 3348/T - 5.957lgT +1.86×10^-3T - 1.095×10^-7T²		[1,16]
R5		lgK_eq = 2.4943 - 2232/T -8.463×10^-3lgT -2.203×10^-4T		[1,16]

Table 2 Proximate analysis and ultimate analysis of raw coal

样品	工业分析/%					元素分析/%					Q_gr,ad/(MJ/kg)	Q_net,ar/(MJ/kg)
样品	M_t	M_ad	A_ad	V_ad	FC_ad	C_daf	H_daf	O_daf	N_daf	S_t,daf	Q_gr,ad/(MJ/kg)	Q_net,ar/(MJ/kg)
标定期原料煤	10.85	1.65	6.52	32.88	58.95	82.35	4.80	10.93	1.14	0.77	—	24.42
热解试验煤样	7	1.66	12.72	34.12	51.5	80.54	4.91	11.38	1.21	1.96	28.51	27.59

Fig.2 Relationship between internal efficiency factor η and temperature

Fig.3 Comparison of apparent reaction rates between two models

Fig.4 Relationship between rate coefficient and temperature in shrinking models of different reaction

Table 3 Composition of pyrolysis gas of raw coal

热解气	体积分数/%
合计	100
CO	17.93
CO₂	1.84
CH₄	38.80
H₂	21.72
C₂H₄	1.94
H₂O	14.23
N₂	2.31
H₂S	1.23

Fig.5 Temperature change of gas-solid phase in pyrolysis section

Fig.6 Volatilization curve of pyrolysis section

Table 4 Physical property parameter model of pyrolysis section simulation

名称	模型	文献
煤高位发热量/(MJ/kg)	$Q g r, d a f = 334.5 C d a f + 1275.4 H d a f - 108.7 O d a f + 92 S t, d a f - m a x 0, 25.1 (A d - 10)$	[19]
挥发分热解焓/(J/mol)
煤低位发热量/(MJ/kg)	$Q n e t, a d = Q g r, a d - 212.1 H a d - 0.775 O a d - 24.24 M a d$
固定碳显焓/(J/mol)	$h f c = R 380 g 0 380 T + 3600 g 1 1800 T$ $g 0 = 1 e z - 1$ , $g 1 = e z z e z - 1 2$	[16,20]
挥发分比热容/(J/(kg·K))	$C p, v o l = 0.9 C p, v o l 1 + 0.1 C p, v o l 2$ 基本挥发分 $C p, v o l 1 = 728 + 3.391 T$ 次级挥发分 $C p, v o l 2 = 2273 + 2.554 T$	[25]
灰分比热容/(J/(kg·K))	$C p, v o l 1 = 594 + 0.586 T$	[19]
焦油比热容/(J/(mol·K))	$C p, t a r = 88.627 + 0.12074 T - 0.12735 × 10 - 4 T 2 - 0.36688 × 10 - 7 T - 2$	[33]

Table 4 Physical property parameter model of pyrolysis section simulation

名称	模型	文献
煤高位发热量/(MJ/kg)	$Q g r, d a f = 334.5 C d a f + 1275.4 H d a f - 108.7 O d a f + 92 S t, d a f - m a x 0, 25.1 (A d - 10)$	[19]
挥发分热解焓/(J/mol)
煤低位发热量/(MJ/kg)	$Q n e t, a d = Q g r, a d - 212.1 H a d - 0.775 O a d - 24.24 M a d$
固定碳显焓/(J/mol)	$h f c = R 380 g 0 380 T + 3600 g 1 1800 T$ $g 0 = 1 e z - 1$ , $g 1 = e z z e z - 1 2$	[16,20]
挥发分比热容/(J/(kg·K))	$C p, v o l = 0.9 C p, v o l 1 + 0.1 C p, v o l 2$ 基本挥发分 $C p, v o l 1 = 728 + 3.391 T$ 次级挥发分 $C p, v o l 2 = 2273 + 2.554 T$	[25]
灰分比热容/(J/(kg·K))	$C p, v o l 1 = 594 + 0.586 T$	[19]
焦油比热容/(J/(mol·K))	$C p, t a r = 88.627 + 0.12074 T - 0.12735 × 10 - 4 T 2 - 0.36688 × 10 - 7 T - 2$	[33]

Fig.7 One-dimensional model program framework of BGL coal gasification

Table 5 Overall simulation input conditions of BGL coal gasification

名称	单位	数值	名称	单位	数值
操作压力	MPa	4.09	蒸汽	kg/s	3.23
原料煤	kg/s	9.46	氧气	kg/s	4.25
煤粒度	mm	6.00	气化剂温度	℃	266
煤真密度	kg/m³	1400	熔渣碳残留率	%	0.10

Fig.8 Axial distribution curve of gas-solid two-phase flow

Fig.9 Axial change of composition molar flow rate of gas

Table 6 Comparison between calculated value and calibration value of crude gas composition

组成	计算值 (湿基）/%	计算值 (干基）/%	标定实测 (干基）/%	标定校核值（湿基）/%
合计	100.00	100.00	100.00	100.00
CO	54.03	60.30	58.05	52.46
CO₂	3.57	3.98	4.23	3.72
H₂	23.00	25.67	28.30	25.18
CH₄	7.70	8.59	7.16	7.66
H₂O	10.40	0	—	9.97
O₂	0.28	0.31	0.10	0
C₂H₄	0.36	0.40	—	0.36
N₂	0.43	0.48	1.96	0.41
H₂S	0.23	0.26	0.20	0.24

Main data of coal pyrolysis test results

序号	试验方法		单次煤样/g		粒度/mm	加热终温/℃		操作压力/MPa	产率/%（质量）
序号	试验方法		单次煤样/g		粒度/mm	加热终温/℃		操作压力/MPa	半焦	焦油	热解气	水
a	铝甑热解试验		20		<0.2	650		0.1	73.00	10.70	8.55	7.75
b	加压低温干馏试验		60		0.5~2.0	650		0.1	68.67	8.85	12.82	9.66
c	加压低温干馏试验		60		0.5~2.0	650		3.0	74.32	3.75	14.93	7.00
d	固定床热解试验		3000		10~50	650		0.1	76.73	5.90	8.98	8.39
序号	热解气组成/%
序号	H₂	CO	CO₂	O₂	N₂	CH₄	C₂H₄	C₂H₆	C₃H₆	C₃H₈	C _n H _m	合计
b	49.01	14.34	2.93	0.31	2.02	25.29	0.26	4.05	0.65	1.12	0.02	100.00
c	15.99	7.66	12.40	0.45	1.79	58.44	0.09	1.99	0.84	0.33	0.02	100.00
d	33.88	11.97	7.63	0.25	1.45	37.86	—	—	—	—	6.96	100.00

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