深度脱水污泥好氧堆肥中多环芳烃的含量与风险削减研究

王宁; 郝智能; 刘吉宝; 鲍振; 李雪怡; 王侨; 解立平; 刘景富; 魏源送

doi:10.13198/j.issn.1001-6929.2022.11.24

深度脱水污泥好氧堆肥中多环芳烃的含量与风险削减研究

doi: 10.13198/j.issn.1001-6929.2022.11.24

王宁^{1, 2,},
郝智能^2, ,,
刘吉宝^{3, 4},
鲍振^{1, 3, 4},
李雪怡⁵,
王侨⁵,
解立平^1, ,,
刘景富²,
魏源送^{3, 4}

1.
天津工业大学环境科学与工程学院，天津　300387
2.
中国科学院生态环境研究中心，环境化学与生态毒理学国家重点实验室，北京　100085
3.
中国科学院生态环境研究中心，环境模拟与污染控制国家重点联合实验室，北京　100085
4.
中国科学院生态环境研究中心水污染控制实验室，北京　100085
5.
北京首创污泥处置技术有限公司，北京　100044

基金项目: 国家重点研发计划项目(No.2019YFC1906502)；山东省重点研发计划项目(No.2020CXGC011202)

详细信息

作者简介:
王宁（1997-），女，山东临沂人，1640812021@qq.com

通讯作者:
①郝智能(1984-)，男，湖北宜昌人，副研究员，博士，主要从事风险有机物的分析与转化研究，znhao@rcees.ac.cn

②解立平(1963-)，男，内蒙古呼和浩特人，教授，博士，主要从事固体废弃物洁净能源化、资源化综合利用研究，xielp991@tiangong.edu.cn

中图分类号: X705
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出版历程
- 收稿日期: 2022-07-11
- 修回日期: 2022-11-16

Content and Risk Reduction of Polycyclic Aromatic Hydrocarbons in Deep Dewatered Sludge Aerobic Composting

WANG Ning^{1, 2
,},
HAO Zhineng^{2
, ,},
LIU Jibao^{3, 4},
BAO Zhen^{1, 3, 4},
LI Xueyi⁵,
WANG Qiao⁵,
XIE Liping^{1
, ,},
LIU Jingfu²,
WEI Yuansong^{3, 4}

1.
School of Environmental Science and Engineering, Tiangong University, Tianjin 300387, China
2.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
3.
State Key Joint Laboratory of Environmental Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
4.
Department of Water Pollution Control Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
5.
Beijing Capital Sludge Disposal Technology Co., Ltd., Beijing 100044, China

Funds: National Key Research and Development Program of China (No.2019YFC1906502); Key Research and Development Program of Shandong Province, China (No.2020CXGC011202)

摘要

摘要: 多环芳烃(polycyclic aromatic hydrocarbons, PAHs)是影响污泥安全资源化的重要因素. 以无机药剂调理的深度脱水污泥有利于污泥的好氧堆肥处置，但对于该处置过程中深度脱水污泥PAHs的降解和风险削减尚缺乏认识. 主要以复合铝镁盐调理的深度脱水污泥为对象，分析不同好氧堆肥条件下污泥中PAHs的含量、来源和风险，以明确好氧堆肥工艺过程对风险有机物的削减效果及潜在影响因素. 通过气相色谱-质谱仪、特征比值法和风险熵法分析污泥中美国EPA优先控制的16种PAHs的含量、来源和风险，重点考察了深度脱水污泥在好氧堆肥前后PAHs含量和风险变化. 结果表明：①16种PAHs在6组污泥中均有检出，其总量范围为777.78~1 878.38 ng/g，组成以中高环芳烃为主，主要来源为石油污染和燃烧的混合源. ②堆肥28 d后6组污泥中PAHs的去除率分别为37.66%、54.29%、12.38%、15.40%、56.78%和34.25%，表明添加颗粒大的返混料或辅料更有利于PAHs的降解. ③污泥中的PAHs整体处于中低风险，好氧堆肥后除组1的苯并[a]芘和组2的芴由低风险上升为中风险外，其余组中PAHs的风险均保持不变或者下降. 研究显示，深度脱水污泥好氧堆肥应注重堆体的通气性，添加颗粒大的返混料或辅料能有效改善好氧堆肥过程的通气性，从而促进PAHs的降解和风险削减. 此外，堆肥过程及堆肥产品中PAHs应作为一项重要指标进行监测，以避免因长期暴露引发累积性生态风险.
- 污泥 /
- 好氧堆肥 /
- PAHs /
- 减毒 /
- 生态风险
Abstract: Polycyclic aromatic hydrocarbons (PAHs) are important factors affecting the safety of sludge application. Deep dewatered sludge conditioned with inorganic chemicals is beneficial to the disposal of aerobic composting of sludge, but the degradation and risk reduction of PAHs in deep dewatered sludge during its aerobic composting remains unclear. Focusing on the deep dewatered sludge conditioned by aluminum magnesium salt, this study investigated the content, source and risk of PAHs in the sludge during the aerobic composting process under different conditions, to elucidate the risk reduction of organic pollutants and potentially influencing factors. By using gas chromatography-mass spectrometry, characteristic ratio and risk quotient method, the contents, potential sources and risk of 16 PAHs prioritized by the US EPA were analyzed. Especially, the changes of risk of PAHs in deep dewatered sludge before and after aerobic composting were investigated. The results showed that: (1) 16 PAHs were detected in all sludge, their total content ranged from 777.78 to 1878.38 ng/g. The detected PAHs were mainly medium and high cyclic PAHs and were mainly from mixed sources of petroleum pollution and combustion. (2) After 28 days of aerobic composting, the degradation rates of PAHs in 6 groups were 37.66%, 54.29%, 12.38%, 15.40%, 56.78% and 34.25%, respectively. It showed that the addition of back mixing and auxiliary materials with large particle sizes were conducive to the degradation of PAHs. (3) The overall risk of PAHs before composting was medium to low. Except that the risk of BaP in group 1 and Flu in group 2 increased from low level to medium level, the risk of PAHs in all other groups did not change or decreased after aerobic composting. This study proposed that the air permeability was an key impact factor for aerobic composting, and the addition of back mixing and auxiliary materials with large particles could effectively improve the air permeability to promote the degradation efficiency and risk reduction of PAHs during aerobic composting of deep dewatered sludge. Moreover, PAHs in sludge composting and the compost products should be monitored as important indicators to avoid cumulative ecological risks caused by long-term exposure.
- sludge /
- aerobic composting /
- PAHs /
- attenuation /
- ecological risk

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图 1 深度脱水污泥试验设计示意

Figure 1. Flow chart of aerobic composting of deep dewatered sludge

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图 2 深度脱水污泥PAHs的来源解析

Figure 2. Source apportionment of PAHs in deep dewatered sludge

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图 3 深度脱水污泥好氧堆肥前后PAHs含量情况

Figure 3. Content of individual PAHs in deep dewatered sludge before and after aerobic composting

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图 4 深度脱水污泥好氧堆肥前后PAHs组成情况

Figure 4. Compositions of PAHs in deep dewatered sludge before and after aerobic composting

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表 1 深度脱水污泥的好氧堆肥组别设计(以污泥湿质量计)

Table 1. Group design of the aerobic composting for deep dewatered sludge (in terms of wet weight of sludge)

组别	脱水药剂	稻壳/%	返混料/%	筛分料/%	含水率/%	最高温度/℃	高温期/d	有机质含量
组1	复合铝镁盐	0	30	0	62	73.8±0.5	8	63.3%±6.8%
组2	复合铝镁盐	0	100	0	62	73.2±1.7	6	60.8%±2.2%
组3	复合铝镁盐	0	0	15	62	62.7±1.3	10	32.1%±1.1%
组4	复合铝镁盐	7	0	28	47	60.7±3.6	6	45.6%±4.9%
组5	无药剂	14	0	50	53	63.5±0.6	11	44.0%±0.4%
组6	无药剂	14	84	0	63	55.5±0.5	8	59.3%±2.2%
注：筛分料为堆肥结束后的筛分成品；返混料为堆肥结束后的直接出槽成品；有机质含量以污泥干质量计.

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表 2 深度脱水污泥好氧堆肥前后∑PAHs含量的变化情况

Table 2. Total content of 16 PAHs in deep dewatered sludge before and after aerobic composting

组别	好氧堆肥前				好氧堆肥后
组别	∑PAHs含量/(ng/g)	HMW含量/(ng/g)	LMW含量/(ng/g)	HMW/LMW	∑PAHs含量/(ng/g)	HMW含量/(ng/g)	LMW含量/(ng/g)	HMW/LMW
组1	1050.64±19.63	856.95±28.84	193.69±8.87	4.45	654.99±19.52	484.50±17.16	170.50±2.36	2.93
组2	1878.38±77.56	1586.53±71.42	291.85±6.14	5.45	858.63±37.78	613.51±36.29	245.11±1.49	2.50
组3	1 662.00±40.62	1 435.89±41.78	226.11±12.21	6.47	1456.19±137.71	1324.38±98.62	199.90±7.53	6.58
组4	777.78±18.66	513.60±16.21	250.47±11.59	1.99	658.05±23.83	493.00±26.09	165.04±2.41	3.00
组5	1506.75±112.23	1338.14±107.69	173.88±9.67	8.14	651.26±9.76	524.81±8.83	126.45±3.49	4.15
组6	823.07±3.67	705.28±4.90	118.31±1.26	5.90	541.19±21.92	392.46±16.40	148.73±11.08	2.64
注：HMW表示高分子量(4环及以上)PAHs；LMW表示低分子量(2~3环)PAHs.

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表 3 深度脱水污泥好氧堆肥前后PAHs的风险值

Table 3. RQ of PAHs in deep dewatered sludge before and after aerobic composting

PAHs	好氧堆肥前RQ_NCs						好氧堆肥前RQ_MPCs
PAHs	组1	组2	组3	组4	组5	组6	组1	组2	组3	组4	组5	组6
Nap	52.75	120.74	88.52	45.53	45.69	31.61	0.528	1.207	0.885	0.455	0.457	0.316
Any	13.27	16.22	13.50	15.23	7.69	6.95	0.133	0.162	0.135	0.152	0.077	0.069
Acp	12.29	17.41	13.99	17.64	11.20	7.47	0.123	0.174	0.140	0.176	0.112	0.075
Flu	0.59	0.53	0.55	1.28	0.69	0.49	0.006	0.005	0.005	0.013	0.007	0.005
Phe	7.09	7.82	6.71	20.14	7.40	5.01	0.071	0.078	0.067	0.201	0.074	0.050
Ant	30.95	22.48	13.70	15.84	19.40	15.29	0.310	0.225	0.137	0.158	0.194	0.153
Flt	42.41	44.71	55.41	38.50	56.94	31.71	0.424	0.447	0.554	0.385	0.569	0.317
Pyr	68.59	83.56	79.36	57.61	73.88	43.64	0.686	0.836	0.794	0.576	0.739	0.436
BaA	2.54	21.65	19.74	2.28	22.73	1.36	0.025	0.216	0.197	0.023	0.227	0.014
Chr	0.33	0.63	0.54	0.25	0.66	0.25	0.003	0.006	0.005	0.003	0.007	0.002
BbF	33.32	45.15	42.55	33.87	51.85	25.10	0.333	0.451	0.425	0.339	0.518	0.251
BkF	3.44	4.77	4.50	3.45	5.40	2.62	0.034	0.048	0.045	0.035	0.054	0.026
BaP	0.98	1.35	1.50	1.46	2.26	0.78	0.010	0.013	0.015	0.015	0.023	0.008
DahA	1.12	1.12	1.16	1.09	1.24	1.031	0.011	0.011	0.012	0.011	0.012	0.010
IcdP	0.50	0.54	0.60	0.67	1.12	0.352	0.005	0.005	0.006	0.007	0.011	0.004
BghiP	5.24	12.08	10.36	0.66	7.48	4.710	0.052	0.121	0.104	0.007	0.075	0.047

PAHs	好氧堆肥后RQ_NCs						好氧堆肥后RQ_MPCs
PAHs	组1	组2	组3	组4	组5	组6	组1	组2	组3	组4	组5	组6
Nap	60.98	91.29	76.22	60.03	38.87	51.92	0.610	0.913	0.762	0.600	0.389	0.519
Any	7.92	10.88	9.37	8.55	6.15	6.51	0.079	0.109	0.094	0.085	0.061	0.065
Acp	13.22	11.10	13.35	14.52	5.82	11.29	0.132	0.111	0.134	0.145	0.058	0.113
Flu	0.38	1.45	0.50	0.36	0.45	0.43	0.004	0.014	0.005	0.004	0.004	0.004
Phe	5.54	5.94	5.86	5.18	5.12	4.75	0.055	0.059	0.059	0.052	0.051	0.048
Ant	18.26	18.66	19.23	17.07	16.60	16.11	0.183	0.187	0.192	0.171	0.166	0.161
Flt	47.16	43.53	48.16	40.07	41.77	38.05	0.472	0.435	0.482	0.401	0.418	0.380
Pyr	58.49	68.97	62.88	54.49	50.02	43.76	0.585	0.690	0.629	0.545	0.500	0.438
BaA	10.60	3.02	17.58	10.85	11.20	7.95	0.106	0.030	0.176	0.108	0.112	0.079
Chr	0.25	0.43	0.48	0.26	0.27	0.16	0.002	0.004	0.005	0.003	0.003	0.002
BbF	28.87	45.66	37.61	32.27	33.41	23.52	0.289	0.457	0.376	0.323	0.334	0.235
BkF	2.95	4.65	3.89	3.29	3.39	2.34	0.029	0.047	0.039	0.033	0.034	0.023
BaP	1.01	1.50	1.38	1.11	1.12	0.75	0.010	0.015	0.014	0.011	0.011	0.008
DahA	0.95	1.03	1.05	0.92	0.99	0.88	0.010	0.010	0.011	0.009	0.010	0.009
IcdP	0.50	0.45	0.63	0.49	0.54	0.38	0.005	0.004	0.006	0.005	0.005	0.004
BghiP	0.690	0.65	9.81	0.60	0.74	0.55	0.007	0.007	0.098	0.006	0.007	0.006

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