纤维素与废轮胎微波共热解规律及产物特性

doi:10.7503/cjcu20170717

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (5): 964.doi: 10.7503/cjcu20170717

纤维素与废轮胎微波共热解规律及产物特性

王文亮^1,², 时宇杰¹, 王少华¹, 党泽攀¹, 李新平¹

1.陕西科技大学轻工科学与工程学院, 陕西省造纸技术及特种纸品开发重点实验室,轻化工程国家级实验教学示范中心, 西安 710021
2. 华南理工大学制浆造纸工程国家重点实验室, 广州 510640

收稿日期:2017-11-09 出版日期:2018-01-13 发布日期:2018-01-13
作者简介:
联系人简介: 王文亮, 男, 博士, 讲师, 主要从事生物质热化学转化研究. E-mail: wangwenliang@sust.edu.cn
基金资助:
制浆造纸工程国家重点实验室开放基金(批准号: 201820)、国家自然科学基金(批准号: 31370578)和陕西省科技厅自然科学基础研究面上项目(批准号: 2015JM3083)资助.

Pyrolysis Behavior and Product Characteristics of Microwave co-Pyrolysis of Cellulose and Waste Tire^†

WANG Wenliang^1,^2,^*, SHI Yujie¹, WANG Shaohua¹, DANG Zepan¹, LI Xinping^1,²

1. Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development,College of Bioresources Chemical and Materials Engineering,National Demonstration Center for Experimental Light Chemistry Engineering Education,Shaanxi University of Science & Technology, Xi’an 710021, China;
2. State Key Laboratory of Pulp and Paper Engineering, South China University of Technology,Guangzhou 510640, China

Received:2017-11-09 Online:2018-01-13 Published:2018-01-13
Contact: WANG Wenliang
Supported by:
Supported by the Open Fund of State Key Laboratory of Pulp and Paper Engineering of China(No.201820), the National Natural Science Foundation of China(No. 31370578) and the Natural Science Basic Research Project of Shaanxi Province, China(No. 2015JM3083).

摘要/Abstract

摘要：

采用热重分析仪(TG)、微波共热解实验装置、红外分析仪(FTIR)以及气质联用仪(GC-MS)考察了纤维素与废轮胎微波共热解过程变化规律及产物生成特性. 研究表明, 不同共混比例[有效氢碳比(H/C_eff)为0.2, 0.4, 0.6]下热失重残炭率均低于理论值, 微波共热解产物热解油产率相比理论值分别提高了4.7%, 6.4%和6.0%, 说明纤维素与废轮胎共热解过程存在协同效应, 有利于液体产物热解油的生成. 废轮胎微波热解油中检测到了79.5%的多环芳烃(PAHs), 由于纤维素的加入氧自由基的作用使得热解油中PAHs完全消失, 转化为高附加值的含氧有机物, 热解油品质得到提高.

关键词: 纤维素, 废轮胎, 微波共热解, 热解油, 协同效应

Abstract:

The pyrolysis behavior and product characteristics of microwave co-pyrolysis of cellulose and waste tire were investigated by thermogravimetric analyzer(TG), the equipment of microwave co-pyrolysis, Fourier transform infrared analyzer(FTIR) and gas chromatography/mass spectrometry(GC-MS). The results show that the contents of residual carbons from different H/C_eff ratios(0.2, 0.4, 0.6) are lower than the theoretical values. Compared with the theoretical values at H/C_eff ratios(0.2, 0.4, 0.6), the yields of pyrolysis oil increase by 4.7%, 6.4% and 6.0%, respectively, indicating the occurrence of synergistic effect during the co-pyrolysis of cellulose and waste tire. The relative content of 79.5% for polycyclic aromatic hydrocarbons(PAHs) was observed in pyrolysis oil of waste tire. However, the PAHs were totally disappeared and converted into valuable oxygen containing compounds after the adding of cellulose, resulting in the quality improvement of pyrolysis oil.

Key words: Cellulose, Waste tire, Microwave co-pyrolysis, Pyrolysis oil, Synergistic effect

中图分类号:

O643.3

TrendMD:

王文亮, 时宇杰, 王少华, 党泽攀, 李新平. 纤维素与废轮胎微波共热解规律及产物特性. 高等学校化学学报, 2018, 39(5): 964.

WANG Wenliang,SHI Yujie,WANG Shaohua,DANG Zepan,LI Xinping. Pyrolysis Behavior and Product Characteristics of Microwave co-Pyrolysis of Cellulose and Waste Tire^†. Chem. J. Chinese Universities, 2018, 39(5): 964.

图/表 9

参考文献 28

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Retention time/min	Compound	Relative content(%)
Retention time/min	Compound	H/C_eff=0	H/C_eff=0.2	H/C_eff=0.4	H/C_eff=0.6	H/C_eff=0.8
	Saccharides	50.53	39.01	31.79	17.46	0
21.33	Levoglucosenone	6.55	5.03	6.13	3.19
25.16	1,4∶3,6-Dianhydro-α-d-glucopyranose	7.68	4.78	4.72	6.53
35.93	D-Allose		29.21	20.93	7.74
36.80	Levoglucosan	31.86
38.73	Trehalose	4.44
	Furans	31.66	31.89	31.91	30.43	0
11.83	Furfural	8.82	9.72	9.48	8.47
14.26	2-Acetylfuran	2.62	2.06	1.91	1.46
15.12	2-(5H)-Furanone	1.28	1.16	0.99
16.00	5-Methylfurfural	3.60	2.92	2.81	3.31
16.89	3-Methylfuran-2(5H)-one	0.93
19.34	4-Methyl-2(5H)-furanone	1.49	2.10		1.08
20.16	2,5-Dimethyl-4-hydroxy-3(2H)-furanone		3.22	3.49
20.60	Methyl-2-furoate	3.05	2.20	1.95
22.54	5-Methyl-2-furanmethanol	0.82
26.06	5-Hydroxymethylfurfural	6.76	8.53	11.28	16.12
28.52	1-(2-Furyl)-2,3-dimethyl-3-butene-1,2-diol	2.30
	Hydrocarbons	0	1.79	0	6.34	100
15.56	(E)-2-Heptene				1.72
20.43	2-Nonyne				2.00
21.79	2,3,5-Trimethylhexane				2.63
22.13	1-(Cycloprop-2-en-1-yl)-2-methylbenzene					6.08
23.25	1-Methylidene-1H-indene					14.42
25.37	1,2-Dihydro-3-methylnaphthalene					14.35
26.36	2-Methylnaphthalene					7.77
26.77	1-Methylnaphthalene					8.96
28.31	1-Nonene		1.18
29.24	2,6-Dimethylnaphthalene					2.63
29.58	1-Hexadecene		0.61
29.67	2,7-Dimethylnaphthalene					5.72
30.01	2-Vinylnaphthalene					6.63
30.58	Biphenylene					5.88
32.31	4,6,8-Trimethylazulene					4.34
34.50	9-Fluorenemethanol					2.67
36.59	2-Methylfluorene					3.35
38.50	Phenanthrene					7.86
39.16	Diphenylethyne					1.81
40.82	Naphtho[1,2-b]norbornadiene					1.00
41.23	1-Methylphenanthrene					3.13
43.40	1,7-Dimethylphenanthrene					0.76
44.16	Fluoranthene					2.64
	Ketones	8.14	11.70	9.32	17.38	0
8.94	Hydroxyacetone	2.45	3.78	4.24	8.08
10.77	1-Hydroxy-2-butanone		1.89	1.22	3.10
13.02	4-Ethoxy-2-butanone		1.70
13.99	2-Methyl-2-cyclopentenone				0.65
15.63	4-Methylcyclohexanone		1.53
15.67	1,2-Cyclopentanedione	1.26
18.47	Methylcyclopentenolone			2.74	4.04
18.65	3-Methyl-1,2-cyclopentanedione	3.50	2.79	1.11	1.50
29.61	2-(1-Methyl-2-oxopropyl)-cyclohexanone	0.94
	Carboxylic acids	6.00	11.71	10.08	9.84	0
7.74	Formic acid	2.13	3.07	1.69

Retention time/min	Compound	Relative content(%)
Retention time/min	Compound	H/C_eff=0	H/C_eff=0.2	H/C_eff=0.4	H/C_eff=0.6	H/C_eff=0.8
	Saccharides	50.53	39.01	31.79	17.46	0
21.33	Levoglucosenone	6.55	5.03	6.13	3.19
25.16	1,4∶3,6-Dianhydro-α-d-glucopyranose	7.68	4.78	4.72	6.53
35.93	D-Allose		29.21	20.93	7.74
36.80	Levoglucosan	31.86
38.73	Trehalose	4.44
	Furans	31.66	31.89	31.91	30.43	0
11.83	Furfural	8.82	9.72	9.48	8.47
14.26	2-Acetylfuran	2.62	2.06	1.91	1.46
15.12	2-(5H)-Furanone	1.28	1.16	0.99
16.00	5-Methylfurfural	3.60	2.92	2.81	3.31
16.89	3-Methylfuran-2(5H)-one	0.93
19.34	4-Methyl-2(5H)-furanone	1.49	2.10		1.08
20.16	2,5-Dimethyl-4-hydroxy-3(2H)-furanone		3.22	3.49
20.60	Methyl-2-furoate	3.05	2.20	1.95
22.54	5-Methyl-2-furanmethanol	0.82
26.06	5-Hydroxymethylfurfural	6.76	8.53	11.28	16.12
28.52	1-(2-Furyl)-2,3-dimethyl-3-butene-1,2-diol	2.30
	Hydrocarbons	0	1.79	0	6.34	100
15.56	(E)-2-Heptene				1.72
20.43	2-Nonyne				2.00
21.79	2,3,5-Trimethylhexane				2.63
22.13	1-(Cycloprop-2-en-1-yl)-2-methylbenzene					6.08
23.25	1-Methylidene-1H-indene					14.42
25.37	1,2-Dihydro-3-methylnaphthalene					14.35
26.36	2-Methylnaphthalene					7.77
26.77	1-Methylnaphthalene					8.96
28.31	1-Nonene		1.18
29.24	2,6-Dimethylnaphthalene					2.63
29.58	1-Hexadecene		0.61
29.67	2,7-Dimethylnaphthalene					5.72
30.01	2-Vinylnaphthalene					6.63
30.58	Biphenylene					5.88
32.31	4,6,8-Trimethylazulene					4.34
34.50	9-Fluorenemethanol					2.67
36.59	2-Methylfluorene					3.35
38.50	Phenanthrene					7.86
39.16	Diphenylethyne					1.81
40.82	Naphtho[1,2-b]norbornadiene					1.00
41.23	1-Methylphenanthrene					3.13
43.40	1,7-Dimethylphenanthrene					0.76
44.16	Fluoranthene					2.64
	Ketones	8.14	11.70	9.32	17.38	0
8.94	Hydroxyacetone	2.45	3.78	4.24	8.08
10.77	1-Hydroxy-2-butanone		1.89	1.22	3.10
13.02	4-Ethoxy-2-butanone		1.70
13.99	2-Methyl-2-cyclopentenone				0.65
15.63	4-Methylcyclohexanone		1.53
15.67	1,2-Cyclopentanedione	1.26
18.47	Methylcyclopentenolone			2.74	4.04
18.65	3-Methyl-1,2-cyclopentanedione	3.50	2.79	1.11	1.50
29.61	2-(1-Methyl-2-oxopropyl)-cyclohexanone	0.94
	Carboxylic acids	6.00	11.71	10.08	9.84	0
7.74	Formic acid	2.13	3.07	1.69

Retention time/min	Compound	Relative content(%)
Retention time/min	Compound	H/C_eff=0	H/C_eff=0.2	H/C_eff=0.4	H/C_eff=0.6	H/C_eff=0.8
8.54	Acetic acid	3.87	4.21	5.96	6.85
9.70	Propanoic acid				2.98
37.76	Lauric acid			2.43
37.98	Tridecanoic acid		4.43
	Alcohols	0	0	11.02	13.26	0
13.33	2-Propoxyethanol			1.08
22.96	1-(2-butoxyethoxy)ethanol			0.76	1.34
24.06	4-Methylcyclohexanol			9.19	11.64
30.38	6,10,14-Trimethyl-pentadecan-2-ol				0.28
	Esters	2.69	2.17	3.92	5.04	0
7.79	Isobutyl formate				4.41
10.03	Diatol	2.69	2.17
10.26	Ethyl formate			2.88
15.72	α-Angelicalactone			1.04
32.10	Ethyl-7-oxooctanoate				0.63
	Aldehydes	0.98	1.73	1.96	0.25	0
7.42	Methylglyoxal	0.98	1.73	1.96
30.67	9-Acetoxynonanal				0.25

Retention time/min	Compound	Relative content(%)
Retention time/min	Compound	H/C_eff=0	H/C_eff=0.2	H/C_eff=0.4	H/C_eff=0.6	H/C_eff=0.8
8.54	Acetic acid	3.87	4.21	5.96	6.85
9.70	Propanoic acid				2.98
37.76	Lauric acid			2.43
37.98	Tridecanoic acid		4.43
	Alcohols	0	0	11.02	13.26	0
13.33	2-Propoxyethanol			1.08
22.96	1-(2-butoxyethoxy)ethanol			0.76	1.34
24.06	4-Methylcyclohexanol			9.19	11.64
30.38	6,10,14-Trimethyl-pentadecan-2-ol				0.28
	Esters	2.69	2.17	3.92	5.04	0
7.79	Isobutyl formate				4.41
10.03	Diatol	2.69	2.17
10.26	Ethyl formate			2.88
15.72	α-Angelicalactone			1.04
32.10	Ethyl-7-oxooctanoate				0.63
	Aldehydes	0.98	1.73	1.96	0.25	0
7.42	Methylglyoxal	0.98	1.73	1.96
30.67	9-Acetoxynonanal				0.25

纤维素与废轮胎微波共热解规律及产物特性

Pyrolysis Behavior and Product Characteristics of Microwave co-Pyrolysis of Cellulose and Waste Tire^†

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纤维素与废轮胎微波共热解规律及产物特性

Pyrolysis Behavior and Product Characteristics of Microwave co-Pyrolysis of Cellulose and Waste Tire†

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Pyrolysis Behavior and Product Characteristics of Microwave co-Pyrolysis of Cellulose and Waste Tire^†