中国民用生物质和煤炭燃烧细颗粒物中二噁英的排放特征及排放清单

吴剑; 彭勇; 孔少飞; 胡尧; 覃旭菁; 吴铮; 祁士华

doi:10.3799/dqkx.2025.090

中国民用生物质和煤炭燃烧细颗粒物中二噁英的排放特征及排放清单

doi: 10.3799/dqkx.2025.090

吴剑^{1, 2,},
彭勇¹,
孔少飞^{1, 2},
胡尧¹,
覃旭菁¹,
吴铮¹,
祁士华^{2, 3}

1.
中国地质大学(武汉)环境学院, 湖北武汉 430078
2.
湖北省大气复合污染研究中心, 湖北武汉 430078
3.
中国地质大学(武汉)地质微生物与环境全国重点实验室, 湖北武汉 430078

基金项目:

国家自然科学基金青年资助项目 42205116

科技部国家重点研发计划课题 2023YFC3709900

博士后科学基金面上项目 2022M712947

详细信息

作者简介:
吴剑（1991-），男，副教授，主要从事高时空分辨率排放清单的构建与应用.E-mail：kerim@cug.edu.cn

中图分类号: P404
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出版历程
- 收稿日期: 2025-04-04
- 刊出日期: 2025-09-25

Emission Characteristics and Inventory of PCDD/Fs in Fine Particulate Matter from Domestic Biomass and Coal Combustion in China

Wu Jian^{1, 2
,},
Peng Yong¹,
Kong Shaofei^{1, 2},
Hu Yao¹,
Qin Xujing¹,
Wu Zheng¹,
Qi Shihua^{2, 3}

1.
School of Environmental Studies, China University of Geosciences (Wuhan), Wuhan 430078, China
2.
Research Center for Complex Air Pollution of Hubei Province, Wuhan 430078, China
3.
State Key Laboratory of Geomicrobiology and Environmental Changes, China University of Geosciences (Wuhan), Wuhan 430078, China

摘要

摘要:
基于稀释通道采样系统开展室内模拟燃烧实验，采用同位素稀释高分辨气相色谱‒高分辨质谱法，分析了民用生物质和煤炭燃烧细颗粒物（PM_2.5）中二噁英（PCDD/Fs）的排放特征并计算得到其排放因子.结合中国燃料消耗和人口密度数据，基于“自下而上”的方法构建了中国民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的排放清单.研究结果表明：（1）民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的质量浓度在0.181~4.700 pg/m³之间，国际毒性当量（I-TEQ）浓度范围为0.081~2.300 pg I-TEQ/m³，其中，2，3，7，8-四氯二苯并对二噁英（2，3，7，8-T₄CDD）（P < 0.01，R²=0.90）这一单体同系物的质量浓度与总I-TEQ浓度存在强相关性，可作为民用生物质和煤炭燃烧PM_2.5中PCDD/Fs毒性的良好指标.（2）民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的质量浓度排放因子分别为（1.82±0.97）ng/kg和（4.09±2.76）ng/kg；I-TEQ浓度排放因子分别为（0.40±0.21）ng I-TEQ/kg和（0.53±0.24）ng I-TEQ/kg.（3）2021年，民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的排放量为90.0 g I-TEQ，从空间上看，PCDD/Fs的高排放区主要集中在东北和华东地区，排放高值大于8 μg I-TEQ/km².与前人研究相比，垃圾焚烧（22.56 g I-TEQ）和工业燃烧（208 g I-TEQ）PM_2.5中PCDD/Fs的排放量分别是民用生物质和煤炭燃烧排放量的0.2倍和1.5倍.这表明，民用生物质和煤炭燃烧是PM_2.5中PCDD/Fs排放不容忽视的重要来源.（4）民用生物质和煤炭燃烧PM_2.5中PCDD/Fs排放导致的个人吸入的平均健康风险分别为（9.5±7.2）×10^-5和（3.1±1.7）×10^-5，分别是从事各类工业生产活动的职业工人（（2.88±2.45）×10^-5）的3.3倍和1.1倍.
- 微粒排放 /
- 二噁英 /
- 民用生物质 /
- 民用煤炭 /
- 排放特征 /
- 排放清单 /
- 大气污染
Abstract:
Indoor simulation combustion experiments were performed using a dilution tunnel sampling system. The emission characteristics of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion were analyzed using isotope dilution high-resolution gas chromatography/mass spectrometry (HRGC/HRMS), with subsequent calculation of emission factors. By integrating China's fuel consumption and population density data, we developed a "bottom-up" emission inventory for PM_2.5-bound PCDD/Fs from domestic biomass and coal combustion in China. The key findings are as follows: (1) The mass concentrations of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion ranged from 0.181 to 4.700 pg/m³, with international toxic equivalent (I-TEQ) concentrations of 0.081 to 2.300 pg I-TEQ/m³. Congener analysis revealed that 2, 3, 7, 8-T₄CDD (P < 0.01, R²=0.90) showed strong correlations with I-TEQ concentration, suggesting its potential as reliable toxicity indicators for PM_2.5-bound PCDD/Fs from domestic biomass and coal combustion. (2) The mass-based emission factors of PCDD/Fs in PM_2.5 were (1.82±0.97) ng/kg for biomass combustion and (4.09±2.76) ng/kg for coal combustion. The corresponding I-TEQ emission factors were (0.40±0.21) ng I-TEQ/kg (domestic biomass) and (0.53±0.24) ng I-TEQ/kg (domestic coal). (3) In 2021, the total emissions of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion reached 90.0 g I-TEQ. With spatial analysis showing emission hotspots (> 8 μg I-TEQ/km²) concentrated in Northeast and East China. Compared to previous studies, the emissions of PCDD/Fs in PM_2.5 from waste incineration (22.56 g I-TEQ) and industrial combustion (208 g I-TEQ) were 0.2 times and 1.5 times those from domestic biomass and coal combustion, respectively. These results highlight that domestic biomass and coal combustion represent non-negligible and substantial sources of PCDD/Fs in PM_2.5. (4) The estimated inhalation cancer risks were (9.5±7.2)×10^-5 for domestic biomass combustion and (3.1±1.7)×10^-5 for domestic coal combustion, representing 3.3-fold and 1.1-fold increases respectively over occupational exposure risks for industrial workers ((2.88±2.45)×10^-5).
- particulate emissions /
- PCDD/Fs /
- domestic biomass /
- domestic coal /
- emission characteristics /
- emission inventory /
- air pollution

HTML全文

图 1 民用生物质和煤炭PM_2.5中基于质量浓度和I-TEQ浓度的PCDD/Fs占比

图a为基于质量浓度的PCDD/Fs占比；图b为基于I-TEQ浓度的PCDD/Fs占比

Fig. 1. The proportion of PCDD/Fs in PM_2.5 from domestic biomass and coal based on mass concentration and I-TEQ concentration

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图 2 单体同系物与I-TEQ浓度相关性

图a为2，3，7，8-T₄CDF；图b为2，3，7，8-T₄CDD

Fig. 2. Correlation between congener homologues and I-TEQ concentration

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图 3 民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的排放因子

图a为基于质量浓度的PCDD/Fs排放因子；图b为基于I-TEQ浓度的PCDD/Fs排放因子

Fig. 3. Emission factors of PCDD/Fs in PM_2.5 from domestic biomass and coal fuel combustion

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图 4 不同省份民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的排放量

Fig. 4. Emission of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion in different provinces

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图 5 不同年份民用生物质和煤炭燃烧PM_2.5中PCDD/Fs的排放量

Fig. 5. Emission of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion in different years

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图 6 2021年中国民用生物质和煤炭燃烧PM_2.5中PCDD/Fs排放空间分布（1 km×1 km）

Fig. 6. The spatial distribution of PCDD/Fs emissions from domestic biomass and coal combustion in PM_2.5 in China (1 km× 1 km) for 2021

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图 7 个人吸入PCDD/Fs的健康风险

Fig. 7. Health risks of personal inhalation exposure to PCDD/Fs

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表 1 民用生物质和煤炭的燃料特性

Table 1. Characteristics of domestic biomass and coal fuels

	C(%)	H(%)	N(%)	S(%)
木柴	41.21	6.00	0.56	0.03
杉木	47.95	6.24	0.45	1.36
竹子	41.07	6.04	0.43	0.05
荔枝木	69.20	1.00	2.30	2.30
煤炭1	90.90	4.30	1.20	0.90
煤炭2	48.60	2.00	0.70	0.90
煤炭3	89.30	4.90	1.60	0.90

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表 2 民用生物质和煤炭燃烧PM_2.5中的PCDD/Fs浓度

Table 2. The concentration of PCDD/Fs in PM_2.5 from domestic biomass and coal combustion

PCDD/Fs		ΣPCDD	ΣPCDF	Total PCDD/Fs (pg/m³)	Total PCDD/Fs (pg I-TEQ/m³)	PCDFs/PCDDs
木柴	MC	0.170	1.400	1.570		8.240
木柴	IC	0.100	0.140		0.240	1.400
杉木	MC	1.300	3.400	4.700		2.620
杉木	IC	0.560	0.390		0.950	0.700
竹子	MC	0.074	0.470	0.544		6.350
竹子	IC	0.110	0.071		0.181	0.650
荔枝木	MC	0	1.100	1.100		/
荔枝木	IC	0.130	0.150		0.280	1.150
平均值	MC	0.386	1.593	1.979
平均值	IC	0.225	0.188		0.413
标准误差	MC	0.531	1.096	1.613
标准误差	IC	0.194	0.121		0.312
煤炭1	MC	1.100	1.200	2.300		1.090
煤炭1	IC	0.120	0.120		0.240	1.000
煤炭2	MC	0.076	0.410	0.490		5.390
煤炭2	IC	0.034	0.048		0.082	1.410
煤炭3	MC	0.074	0.330	0.410		4.460
煤炭3	IC	0.041	0.039		0.081	0.950
平均值	MC	0.417	0.647	1.070
平均值	IC	0.065	0.069		0.134
标准误差	MC	0.483	0.393	0.873
标准误差	IC	0.039	0.036		0.075
注：MC和IC分别代表质量浓度和I-TEQ浓度；“/”表示分母为0，不予考虑.

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表 3 生物质和工业燃烧源PM_2.5中基于I-TEQ浓度的PCDD/Fs排放因子（ng I-TEQ/kg）

Table 3. Emission factors (ng I-TEQ/kg) of PCDD/Fs in PM_2.5 from biomass and industrial combustion sources based on I-TEQ concentration

燃料类型		平均EF	EF范围	参考文献
民用生物质燃烧	玉米秸秆	0.24, 0.26	0.07~0.57	陈德翼等，2011；Zhang et al., 2022
	水稻秸秆	1.04	12.6~14.5	陈德翼等，2011；Chang et al., 2014
	薪柴	0.63	0.10~1.49	陈德翼等，2011
	甘蔗	0.49, 1.60		Black et al., 2012; Zhang et al., 2022
露天生物质燃烧	甘蔗、谷类作物	52.6	0.01~150	Black et al., 2012; Zhang et al., 2022
露天生物质燃烧	森林、草地	0.7	0.4~1.0	Black et al., 2012
工业燃烧	工业煤炭	0.223	0.025~0.550	Lin et al., 2007; Cheng et al., 2015
	工业煤炭（经APCDs处理）	0.039		Li et al., 2015a
	燃煤电厂	0.620, 0.087		Chen, 2004; Lin et al., 2007
垃圾焚烧	城市生活垃圾	8.8, 12.8	0.32~166.56	Zhang et al., 2019; Lei et al., 2021
	气化炉	50.04		Lei et al., 2017
	水泥窑共处理废物		0.028~0.084	Yang et al., 2019
	医疗垃圾		0.78~473.97	Gao et al., 2009
	城市生活垃圾	30		USEPA, 2025
	城市生活垃圾（经APCDs处理）	0.5		USEPA, 2025

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