次烟煤与半焦富氧混燃特性热重分析

LI Zhao-yang; NIU Sheng-li; HAN Kui-hua; LI Ying-jie; WANG Yong-zheng; LU Chun-mei

doi:10.1016/S1872-5813(22)60002-1

次烟煤与半焦富氧混燃特性热重分析

doi: 10.1016/S1872-5813(22)60002-1

山东大学能源与动力工程学院, 山东济南 250061

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中图分类号: TK121
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出版历程
- 收稿日期: 2022-01-02
- 修回日期: 2022-02-18
- 录用日期: 2022-02-18
- 网络出版日期: 2022-03-18
- 刊出日期: 2022-08-26

Thermogravimetric analysis on the characteristics of oxy-fuel co-combustion of sub-bituminous coal and semi-coke

School of Energy and Power Engineering, Shandong University (Shandong 250061,China)

Funds: The project was supported by the Primary Research & Development Plan of Shandong Province, China (2018GGX104027).

More Information

Corresponding author: Tel: +86 531 88392414. E-mail: nsl@sdu.edu.cn

摘要

摘要: 低阶煤与煤制半焦混燃对解决中国半焦过剩的问题具有重要意义。通过热重分析研究了准东次烟煤与烟煤半焦的富氧混燃特性。与空气气氛相比，富氧燃烧将着火温度和燃尽温度分别提高了10和40 ℃。氧气浓度提高到30%可以大幅补偿富氧条件下燃烧参数的轻微降低并获得更好的共燃性能。利用Flynn-Wall-Ozawa (FWO)、Kissinger-Akahira-Sunose (KAS)和Starink法计算活化能，活化能随质量转化率的变化可分为两个不同阶段，次烟煤、混合燃料和半焦的平均活化能分别为49.31、50.82和59.00 kg/mol。计算了焓变、吉布斯自由能变和熵变等热力学参数，相互作用指数表明在共燃过程中两种燃料发生了明显的相互作用，动力学和热力学计算结果表明30%的半焦参比促进了共燃。同时，X射线荧光光谱（XRF）和灰熔融分析表明与半焦掺烧能降低次烟煤灰的结渣倾向。
- 富氧混燃 /
- 煤半焦 /
- 热重分析 /
- 动力学 /
- 热力学 /
- 灰熔融
Abstract: The co-combustion of the low-rank coal with coal derived semi-coke is of great significance to solve the urgent problem of excessively produced semi-coke in China. In this research, the oxy-fuel co-combustion characteristics of Zhundong sub-bituminous coal with bituminous coal derived semi-coke are systematically investigated using thermogravimetric analysis. Compared with air combustion, oxy-fuel atmosphere increased the ignition and burnout temperature by 10 and 40 °C, respectively. Increasing the oxygen concentration to 30% strongly compensated for the slight reduction of the combustion parameters under oxy-fuel condition and much better co-combustion performance was obtained. Three iso-conversional methods, namely, Flynn-Wall-Ozawa (FWO), Kissinger-Akahira-Sunose (KAS) and Starink, were applied to estimate the activation energy, which can be divided into two stages during the co-combustion process. The average activation energy of sub-bituminous coal, the blend and semi-coke were 49.31, 50.82 and 59.00 kg/mol, respectively. Further, the pre-exponential factor and thermodynamic parameters of the enthalpy change, Gibbs free energy change and entropy change were calculated. Interaction indices were innovatively used for both kinetic-thermodynamic parameters and DTG values. An obvious interaction can be observed during the co-combustion process. The kinetic and thermodynamic results demonstrated that the 30% semi-coke ratio was beneficial to co-combustion. Meanwhile, X-ray fluorescence (XRF) and ash fusion analyses proved that the slagging tendency of sub-bituminous coal ash reduced by blending of semi-coke.
- oxy-fuel co-combustion /
- coal semi-coke /
- thermogravimetric analysis /
- kinetics /
- thermodynamics /
- ash sintering

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FIG. 1764. FIG. 1764.

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Figure 1 Sub-bituminous coal and semi-coke combustion TG and DTG curves in different atmosphere

(Note: SC and SB indicate the abbreviation of semi-coke and sub-bituminous coal, respectively)

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Figure 2 TG and DTG curves of the blends under oxy-fuel atmosphere

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Figure 3 TG and DTG curves of the 30% semi-coke blend under different O₂ concentration

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Figure 4 Regression lines of different iso-conversional methods for pure semi-coke activation energy calculation: (a) FWO, (b) KAS, (c) Starink

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Figure 5 Interaction indices for: (a) DTG of the blends, (b) kinetic-thermodynamic parameters of the 30% semi-coke blend

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Figure 6 Ash analysis of semi-coke and sub-bituminous coal: (a) XRF, (b) ash fusion temperature

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Table 1 Proximate and ultimate analyses of sub-bituminous coal and the bituminous coal derived semi-coke

Fuel	Proximate analysis w_ad/%				Ultimate analysis w_ad/%
Fuel	M	V	FC	A	C	H	O	N	S
SB	1.11	30.20	65.19	3.50	70.30	3.55	20.78	0.51	0.25
SC	0.50	8.78	58.45	32.27	60.10	1.92	2.31	1.06	1.84
Note: the subscript ad indicates the abbreviation of air-dried basis, M, V, FC and A indicate moisture, volatile, fixed carbon and ash, respectively

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Table 2 Combustion characteristic parameters of the blends

Sample	T_i/°C	T_m/°C	T_f/°C	DTG_max/(%·min⁻¹)	DTG_ave/(%·min⁻¹)	CCI/10⁻⁷	R_w/10³
SB	363.6	439.8	640.6	8.08	5.62	5.36	4.34
SC10%SB90%	377.6	470.1	670.6	6.70	5.03	3.52	3.24
SC30%SB70%	391.3	501.9	693.2	6.01	4.65	2.63	2.63
SC50%SB50%	410.1	569.6	711.0	5.88	4.52	2.22	2.16
SC70%SB30%	451.1	599.9	713.6	5.76	4.64	1.84	1.82
SC	510.0	620.6	750.2	5.99	4.81	1.48	1.63

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Table 3 Combustion parameters of 30% semi-coke blend in different O₂ concentration

O₂ content w/%	T_i/°C	T_m/°C	T_f/°C	DTG_max/(%·min⁻¹)	DTG_ave/(%·min⁻¹)	CCI/10⁻⁷	R_w/10³
10	454.1	515.0	869.3	4.24	3.13	0.74	1.56
15	417.2	504.3	747.5	4.93	4.11	1.56	2.01
20	391.3	501.9	677.6	6.01	4.85	2.81	2.63
25	355.2	482.0	631.2	7.47	5.34	5.01	3.75
30	330.9	465.0	609.6	8.68	5.54	7.21	4.84

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Table 4 Activation energies (E_a) for the samples using different iso-conversional approaches

Sample	α/%	FWO		KAS		Starink		k₀
Sample	α/%	E_a/(kJ·mol⁻¹)	R	E_a/(kJ·mol⁻¹)	R	E_a/(kJ·mol⁻¹)	R	k₀
SB	10	43.17	0.9635	35.21	0.9856	35.59	0.9857	2.12
	15	89.92	0.9572	83.83	0.9843	84.19	0.9843	3.50×10⁴
	20	119.84	0.9623	115.05	0.9654	115.40	0.9655	1.40×10⁷
	25	90.61	0.9856	84.14	0.9872	84.51	0.9872	3.72×10⁴
	30	75.85	0.9874	68.46	0.9676	68.86	0.9677	1.75×10³
	35	67.43	0.9877	59.44	0.9689	59.85	0.9692	2.96×10²
	40	62.06	0.9877	53.63	0.9788	54.05	0.9788	93.06
	45	58.30	0.9869	49.51	0.9826	49.94	0.9826	40.66
	50	54.95	0.9868	45.81	0.9704	46.25	0.9704	19.25
	55	51.58	0.9826	42.10	0.9859	42.55	0.9860	9.03
	60	48.42	0.9894	38.60	0.9901	39.06	0.9881	4.39
	65	45.93	0.9902	35.80	0.9887	36.27	0.9887	2.45
	70	43.96	0.9853	33.54	0.9886	34.02	0.9886	1.53
	75	42.11	0.9827	31.39	0.9888	31.88	0.9887	0.97
	80	39.93	0.9643	28.90	0.9864	29.40	0.9865	0.57
	85	37.93	0.9604	26.59	0.9684	27.10	0.9684	0.35
	90	36.16	0.9615	24.50	0.9653	25.02	0.9654	0.22
	95	35.06	0.9623	23.08	0.9614	23.61	0.9615	0.16
Average		57.96		48.87		49.31
SB70SC30	10	65.23	0.9974	57.92	0.9865	58.30	0.9867	1.18×10²
	15	87.68	0.9846	81.00	0.9814	81.38	0.9823	8.97×10³
	20	100.17	0.9954	93.83	0.9855	94.21	0.9834	9.59×10⁴
	25	89.26	0.9681	82.17	0.9937	82.57	0.9965	1.12×10⁴
	30	74.39	0.9634	66.35	0.9614	66.77	0.9693	5.86×10²
	35	65.83	0.9917	57.17	0.9618	57.60	0.9643	1.03×10²
	40	60.51	0.9925	51.39	0.9756	51.84	0.9784	34.27
	45	56.49	0.9745	46.99	0.9672	47.45	0.9639	14.65
	50	53.45	0.9986	43.62	0.9896	44.09	0.9793	7.60
	55	50.93	0.9740	40.80	0.9763	41.28	0.9814	4.37
	60	48.95	0.9674	38.53	0.9804	39.02	0.9876	2.80
	65	47.21	0.9689	36.52	0.9795	37.02	0.9746	1.88
	70	45.75	0.9855	34.8	0.9788	35.31	0.9789	1.33
	75	44.66	0.9987	33.46	0.9874	33.97	0.9901	1.02
	80	43.94	0.9954	32.50	0.9884	33.02	0.9885	0.84
	85	44.17	0.9825	32.53	0..9798	33.06	0.9841	0.84
	90	46.57	0.9734	34.79	0.9756	35.33	0.9785	1.34
	95	53.78	0.9655	42.04	0.9602	42.58	0.9603	5.66
average		59.94		50.36		50.82
SC	10	72.22	0.9961	63.12	0.9946	63.59	0.9946	25.88
	15	82.71	0.9997	73.86	0.9996	74.32	0.9996	1.36×10²
	20	84.94	0.9997	75.99	0.9996	76.46	0.9996	1.89×10²
	25	83.43	0.9997	74.22	0.9996	74.70	0.9996	1.45×10²
	30	80.88	0.9991	71.37	0.9988	71.86	0.9988	93.36
	35	78.06	0.9983	68.25	0.9976	68.75	0.9976	57.69
	40	75.20	0.9969	65.08	0.9956	65.59	0.9957	35.36
	45	72.56	0.9953	62.16	0.9931	62.67	0.9932	22.44
	50	70.00	0.9934	59.31	0.9901	59.84	0.9903	14.39
	55	67.80	0.9909	56.85	0.9860	57.38	0.9863	9.78
	60	65.36	0.9887	54.13	0.9823	54.67	0.9826	6.37
	65	63.37	0.9856	51.89	0.9770	52.44	0.9775	4.47
	70	61.55	0.9825	49.83	0.9714	50.38	0.9720	3.22
	75	59.89	0.9796	47.92	0.9659	48.48	0.9667	2.37
	80	58.50	0.9752	46.30	0.9577	46.87	0.9587	1.83
	85	57.25	0.9692	44.81	0.9465	45.39	0.9478	1.44
	90	56.48	0.9623	43.82	0.9434	44.41	0.9450	1.23
	95	56.41	0.9400	43.54	0.9426	44.14	0.9446	1.17
average		69.26		58.47		59.00

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Table 5 Thermodynamic parameters of the samples

Sample	α /%	ΔH/(kJ·mol⁻¹)	ΔG/(kJ·mol⁻¹)	ΔS/(kJ·mol⁻¹)
SB	10	30.60	197.65	−252.80
	15	78.89	192.92	−172.56
	20	109.95	191.19	−122.95
	25	78.99	192.90	−172.38
	30	63.26	194.03	−197.89
	35	54.19	194.80	−212.79
	40	48.32	195.36	−222.52
	45	44.13	195.79	−229.51
	50	40.37	196.21	−235.85
	55	36.59	196.67	−242.25
	60	33.02	197.14	−248.36
	65	30.16	197.55	−253.32
	70	27.82	197.90	−257.38
	75	25.60	198.26	−261.29
	80	23.04	198.70	−265.84
	85	20.64	199.15	−270.15
	90	18.47	199.59	−274.10
	95	16.93	199.91	−276.90

SB70SC30	10	53.04	205.69	−219.86
	15	75.84	203.77	−184.24
	20	88.52	202.92	−164.77
	25	76.80	203.68	−182.75
	30	60.92	204.91	−207.37
	35	51.68	205.76	−221.92
	40	45.84	206.37	−231.20
	45	41.37	206.88	−238.38
	50	37.93	207.31	−243.94
	55	35.04	207.69	−248.65
	60	32.70	208.01	−252.49
	65	30.62	208.32	−255.92
	70	28.83	208.59	−258.89
	75	27.41	208.81	−261.27
	80	26.36	208.97	−263.01
	85	26.30	208.97	−263.09
	90	28.43	208.58	−259.46
	95	35.51	207.51	−247.72

SC	10	57.28	257.96	−234.00
	15	67.86	256.84	−220.37
	20	69.89	256.64	−217.77
	25	68.05	256.81	−220.11
	30	65.13	257.08	−223.83
	35	61.94	257.40	−227.92
	40	58.71	257.74	−232.07
	45	55.72	258.06	−235.93
	50	52.82	258.39	−239.71
	55	50.29	258.69	−243.00
	60	47.52	259.03	−246.64
	65	45.22	259.33	−249.67
	70	43.09	259.62	−252.48
	75	41.12	259.89	−255.10
	80	39.43	260.13	−257.35
	85	37.87	260.36	−259.43
	90	36.81	260.52	−260.86
	95	36.43	260.56	−261.35

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