垃圾焚烧烟气中芳香烃化合物在线监测和选择性催化还原脱除研究

doi:10.11949/0438-1157.20241320

化工学报 ›› 2025, Vol. 76 ›› Issue (6): 3018-3028.DOI: 10.11949/0438-1157.20241320

垃圾焚烧烟气中芳香烃化合物在线监测和选择性催化还原脱除研究

龚丽芳¹^,²(), 任美慧³^,⁴, 蒋吉春³^,⁴, 郭光召², 胡红云¹, 黄永达¹, 姚洪¹()

^1.华中科技大学煤燃烧与低碳利用全国重点实验室，湖北武汉 430074
^2.瀚蓝绿电固废处理（佛山）有限公司，广东佛山 528200
^3.中国科学院大连化学物理研究所，辽宁大连 116023
^4.辽宁省质谱技术与仪器重点实验室，辽宁大连 116023

收稿日期:2024-11-18 修回日期:2025-01-13 出版日期:2025-06-25 发布日期:2025-07-09
通讯作者: 姚洪
作者简介:龚丽芳（1988—），女，硕士研究生，高级工程师，gonglifang@grandblue.cn
基金资助:
国家自然科学基金国际（地区）合作与交流项目(52220105006);国家自然科学基金青年科学基金项目(2230060516)

Study on on-line monitoring and selective catalytic reduction removal of aromatic hydrocarbon from the flue gas of waste incineration

Lifang GONG¹^,²(), Meihui REN³^,⁴, Jichun JIANG³^,⁴, Guangzhao GUO², Hongyun HU¹, Yongda HUANG¹, Hong YAO¹()

^1.State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^2.Grandblue (Foshan) Green Electricity Solid Waste Management Co. , Ltd. , Foshan 528200, Guangdong, China
^3.Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, Liaoning, China
^4.Liaoning Key Laboratory for Mass Spectrometry Technology and Instrumentation, Dalian 116023, Liaoning, China

Received:2024-11-18 Revised:2025-01-13 Online:2025-06-25 Published:2025-07-09
Contact: Hong YAO

摘要/Abstract

摘要：

垃圾焚烧具有减量化和资源化等优点，近年来已逐渐替代垃圾填埋而成为世界各国大力发展的固废处置重要方式。垃圾组分复杂且有害物质多样，经焚烧处理后不可避免地会产生有毒有害的芳香烃化合物，对大气环境和人体健康产生危害。研制了基于光电离飞行时间质谱的垃圾焚烧烟气中芳香烃化合物在线监测系统，并利用在线监测系统对某大型垃圾焚烧厂的选择性催化还原（selective catalytic reduction，SCR）装置出入口烟气中的苯系物、酚类化合物、多环芳烃化合物和氯代芳烃化合物的代表性物质进行在线监测和动态排放特征研究，明确了SCR装置对垃圾焚烧烟气中典型芳香烃化合物的脱除效果。结果表明，研制的在线监测系统对芳香烃化合物的检出限可达ppb级别，且连续监测5000 min信号强度的相对偏差（RSD）仅为4.2%；SCR装置入口和出口烟气中芳烃化合物的分布模式显著不同，二甲苯和甲苯对差异的贡献最大；SCR装置对烟气中的芳香烃化合物均具有较好的脱除效果，烟气流经SCR装置后，苯系物、酚类、多环芳烃类、氯苯类、氯酚类、氯甲苯类和氯甲酚类化合物的信号强度分别下降11.3%~91.5%、47.7%~93.0%、66.3%~94.9%、26.4%~84.5%、48.5%~88.7%、53.9%~89.5%和67.3%~91.0%。

关键词: 垃圾焚烧, 芳香烃化合物, 在线监测, 选择性催化还原装置, 脱除特性

Abstract:

Waste incineration has the advantages of volume reduction and resource utilization. In recent years, it has gradually replaced landfill and become an important way of solid waste disposal vigorously developed by countries around the world. Waste components are complex and harmful substances are diverse. After incineration, toxic and harmful aromatic hydrocarbon compounds will inevitably be produced, which will harm the atmospheric environment and human health. This paper developed an online monitoring system for aromatic hydrocarbon compounds in waste incineration flue gas based on photoionization time-of-flight mass spectrometry. The online monitoring system was then used to study the online monitoring and dynamic emission characteristics of representative substances such as benzene series, phenolic compounds, polycyclic aromatic hydrocarbons, and chlorinated aromatic hydrocarbons at the inlet and outlet of the selective catalytic reduction (SCR) device in a large-scale waste incineration plant. The study clarified the removal effect of the SCR device on typical aromatic hydrocarbon compounds in waste incineration flue gas. The results showed that the detection limit of the on-line monitoring system can reach ppb level, and the relative deviation (RSD) of the signal intensity of continuous monitoring for 5000 min was only 4.2%. The profile of aromatic hydrocarbon in the flue gases at inlet of SCR equipment was obviously different from that at the outlet, among which xylene and toluene were found to be the major contributors to this distinction. The SCR equipment has a good effect on the removal of aromatic hydrocarbon in flue gas. After flowing through the SCR equipment, the signal intensity of BTEX, phenols, PAHs, chlorobenzene, chlorophenol, chlorotoluene and chlorocresol decreased by 11.3%—91.5%, 47.7%—93.0%, 66.3%—94.9%, 26.4%— 84.5%, 48.5%—88.7%, 53.9%—89.5% and 67.3%—91.0%, respectively.

Key words: waste incineration, PAHs, on-line monitoring, SCR, removal characteristic

中图分类号:

X 859

龚丽芳, 任美慧, 蒋吉春, 郭光召, 胡红云, 黄永达, 姚洪. 垃圾焚烧烟气中芳香烃化合物在线监测和选择性催化还原脱除研究[J]. 化工学报, 2025, 76(6): 3018-3028.

Lifang GONG, Meihui REN, Jichun JIANG, Guangzhao GUO, Hongyun HU, Yongda HUANG, Hong YAO. Study on on-line monitoring and selective catalytic reduction removal of aromatic hydrocarbon from the flue gas of waste incineration[J]. CIESC Journal, 2025, 76(6): 3018-3028.

图/表 9

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参数	数值
垃圾日处理量/(t/d)	500
锅炉额定蒸发量/(t/h)	50.5
烟气流量（SCR）/(m³/h，标准工况)	96439
炉温/℃	>850
一次风温/℃	230
省煤器出口烟温/℃	220
反应塔出口温度/℃	139
SCR反应器温度/℃	180
SO₂日均值/(mg/m³，标准工况)	50
NO _x 日均值/(mg/m³，标准工况)	150
CO日均值/(mg/m³，标准工况)	50
HCl日均值/(mg/m³，标准工况)	10
颗粒物日均值/(mg/m³,标准工况)	10

参数	数值
垃圾日处理量/(t/d)	500
锅炉额定蒸发量/(t/h)	50.5
烟气流量（SCR）/(m³/h，标准工况)	96439
炉温/℃	>850
一次风温/℃	230
省煤器出口烟温/℃	220
反应塔出口温度/℃	139
SCR反应器温度/℃	180
SO₂日均值/(mg/m³，标准工况)	50
NO _x 日均值/(mg/m³，标准工况)	150
CO日均值/(mg/m³，标准工况)	50
HCl日均值/(mg/m³，标准工况)	10
颗粒物日均值/(mg/m³,标准工况)	10

序号	编号	名称	分子式	精确质量数	提取质量数	质量数偏差
1	A1	苯	C₆H₆	78.04695	78.05300	0.00605
2	A2	甲苯	C₇H₈	92.06260	92.07000	0.00740
3	A3	二甲苯/乙苯	C₈H₁₀	106.07825	106.07900	0.00075
4	A4	三甲苯	C₉H₁₂	120.09390	120.10300	0.00910
5	A5	四甲苯	C₁₀H₁₄	134.10955	134.12600	0.01645
6	B1	苯酚	C₆H₆O	94.04187	94.04200	0.00013
7	B2	甲基苯酚	C₇H₈O	108.05752	108.05800	0.00048
8	B3	二甲基苯酚	C₈H₁₀O	122.07317	122.07900	0.00583
9	B4	硝基苯酚	C₆H₅NO₃	139.02696	139.02000	-0.00696
10	C1	萘	C₁₀H₈	128.06260	128.06900	0.00640
11	C2	苊烯	C₁₂H₈	152.06260	152.06300	0.00040
12	C3	苊	C₁₂H₁₀	154.07825	154.07900	0.00075
13	C4	芴	C₁₃H₁₀	166.07825	166.05300	-0.02525
14	C5	菲蒽	C₁₄H₁₀	178.07825	178.08200	0.00375
15	C6	荧蒽芘	C₁₆H₁₀	202.07825	202.08700	0.00875
16	C7	苯并[a]蒽䓛	C₁₈H₁₂	228.09390	228.09500	0.00110
17	C8	苯并[b]荧蒽苯并[k]荧蒽苯并[a]芘	C₂₀H₁₂	252.09390	252.10500	0.01110
18	C9	茚并[1,2,3-c,d]芘苯并[g,h,i]芘	C₂₂H₁₂	276.09390	276.09400	0.00010
19	C10	二苯并[a, h]蒽	C₂₂H₁₄	278.10955	278.11000	0.00045
20	C11	二苯并对二英	C₁₂H₈O₂	184.05244	184.05300	0.00056
21	C12	二苯并呋喃	C₁₂H₈O	168.05752	168.05800	0.00048
22	D1	一氯苯	C₆H₅Cl	112.00798	111.98100	-0.02698
23	D2	二氯苯	C₆H₄Cl₂	145.96901	145.98200	0.01299
24	D3	三氯苯	C₆H₃Cl₃	179.93004	179.94500	0.01496
25	D4	四氯苯	C₆H₂Cl₄	215.88811	215.88900	0.00089
26	D5	五氯苯	C₆HCl₅	249.84915	249.85000	0.00085
27	D6	六氯苯	C₆Cl₆	283.81017	283.81100	0.00083
28	E1	一氯苯酚	C₆H₅OCl	128.00290	127.98000	-0.02290
29	E2	二氯苯酚	C₆H₄OCl₂	161.96393	162.00000	0.03607
30	E3	三氯苯酚	C₆H₃OCl₃	195.92496	195.97200	0.04704
31	E4	四氯苯酚	C₆H₂OCl₄	231.88303	231.88400	0.00097
32	E5	五氯苯酚	C₆HOCl₅	265.84407	265.84500	0.00093
33	F1	一氯甲苯	C₇H₇Cl	126.02362	126.03500	0.01138
34	F2	二氯甲苯	C₇H₆Cl₂	159.98466	160.00300	0.01834
35	F3	三氯甲苯	C₇H₅Cl₃	193.94569	193.97000	0.02431
36	F4	四氯甲苯	C₇H₄Cl₄	229.90376	229.90400	0.00024
37	F5	五氯甲苯	C₇H₃Cl₆	298.83365	298.83400	0.00035
38	G1	一氯甲酚	C₇H₇ClO	142.01854	142.01900	0.00046
39	G2	二氯甲酚	C₇H₆Cl₂O	175.97958	175.98000	0.00042
40	G3	三氯甲酚	C₇H₅Cl₃O	209.94061	209.94100	0.00039
41	G4	四氯甲酚	C₇H₄Cl₄O	245.89868	245.89900	0.00032

序号	编号	名称	分子式	精确质量数	提取质量数	质量数偏差
1	A1	苯	C₆H₆	78.04695	78.05300	0.00605
2	A2	甲苯	C₇H₈	92.06260	92.07000	0.00740
3	A3	二甲苯/乙苯	C₈H₁₀	106.07825	106.07900	0.00075
4	A4	三甲苯	C₉H₁₂	120.09390	120.10300	0.00910
5	A5	四甲苯	C₁₀H₁₄	134.10955	134.12600	0.01645
6	B1	苯酚	C₆H₆O	94.04187	94.04200	0.00013
7	B2	甲基苯酚	C₇H₈O	108.05752	108.05800	0.00048
8	B3	二甲基苯酚	C₈H₁₀O	122.07317	122.07900	0.00583
9	B4	硝基苯酚	C₆H₅NO₃	139.02696	139.02000	-0.00696
10	C1	萘	C₁₀H₈	128.06260	128.06900	0.00640
11	C2	苊烯	C₁₂H₈	152.06260	152.06300	0.00040
12	C3	苊	C₁₂H₁₀	154.07825	154.07900	0.00075
13	C4	芴	C₁₃H₁₀	166.07825	166.05300	-0.02525
14	C5	菲蒽	C₁₄H₁₀	178.07825	178.08200	0.00375
15	C6	荧蒽芘	C₁₆H₁₀	202.07825	202.08700	0.00875
16	C7	苯并[a]蒽䓛	C₁₈H₁₂	228.09390	228.09500	0.00110
17	C8	苯并[b]荧蒽苯并[k]荧蒽苯并[a]芘	C₂₀H₁₂	252.09390	252.10500	0.01110
18	C9	茚并[1,2,3-c,d]芘苯并[g,h,i]芘	C₂₂H₁₂	276.09390	276.09400	0.00010
19	C10	二苯并[a, h]蒽	C₂₂H₁₄	278.10955	278.11000	0.00045
20	C11	二苯并对二英	C₁₂H₈O₂	184.05244	184.05300	0.00056
21	C12	二苯并呋喃	C₁₂H₈O	168.05752	168.05800	0.00048
22	D1	一氯苯	C₆H₅Cl	112.00798	111.98100	-0.02698
23	D2	二氯苯	C₆H₄Cl₂	145.96901	145.98200	0.01299
24	D3	三氯苯	C₆H₃Cl₃	179.93004	179.94500	0.01496
25	D4	四氯苯	C₆H₂Cl₄	215.88811	215.88900	0.00089
26	D5	五氯苯	C₆HCl₅	249.84915	249.85000	0.00085
27	D6	六氯苯	C₆Cl₆	283.81017	283.81100	0.00083
28	E1	一氯苯酚	C₆H₅OCl	128.00290	127.98000	-0.02290
29	E2	二氯苯酚	C₆H₄OCl₂	161.96393	162.00000	0.03607
30	E3	三氯苯酚	C₆H₃OCl₃	195.92496	195.97200	0.04704
31	E4	四氯苯酚	C₆H₂OCl₄	231.88303	231.88400	0.00097
32	E5	五氯苯酚	C₆HOCl₅	265.84407	265.84500	0.00093
33	F1	一氯甲苯	C₇H₇Cl	126.02362	126.03500	0.01138
34	F2	二氯甲苯	C₇H₆Cl₂	159.98466	160.00300	0.01834
35	F3	三氯甲苯	C₇H₅Cl₃	193.94569	193.97000	0.02431
36	F4	四氯甲苯	C₇H₄Cl₄	229.90376	229.90400	0.00024
37	F5	五氯甲苯	C₇H₃Cl₆	298.83365	298.83400	0.00035
38	G1	一氯甲酚	C₇H₇ClO	142.01854	142.01900	0.00046
39	G2	二氯甲酚	C₇H₆Cl₂O	175.97958	175.98000	0.00042
40	G3	三氯甲酚	C₇H₅Cl₃O	209.94061	209.94100	0.00039
41	G4	四氯甲酚	C₇H₄Cl₄O	245.89868	245.89900	0.00032

垃圾焚烧烟气中芳香烃化合物在线监测和选择性催化还原脱除研究

Study on on-line monitoring and selective catalytic reduction removal of aromatic hydrocarbon from the flue gas of waste incineration

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