污泥超高温堆肥衍生胡敏酸对Pb2+的结合机制

doi:10.16085/j.issn.1000-6613.2022-1869

化工进展 ›› 2023, Vol. 42 ›› Issue (9): 4957-4966.DOI: 10.16085/j.issn.1000-6613.2022-1869

污泥超高温堆肥衍生胡敏酸对Pb²⁺的结合机制

李昕¹(), 杨早¹, 钟欣茹¹, 韩昊轩¹, 庄绪宁², 白建峰², 董滨¹^,³(), 徐祖信¹

^1.同济大学环境科学与工程学院，上海 200092
^2.上海第二工业大学资源与环境工程学院, 上海 201209
^3.中国长江三峡集团有限公司长江生态环境工程研究中心，北京 100038

收稿日期:2022-10-09 修回日期:2022-12-20 出版日期:2023-09-15 发布日期:2023-09-28
通讯作者: 董滨
作者简介:李昕（1996—），女，博士研究生，研究方向为污泥处理处置与资源化。E-mail：2110531@tongji.edu.cn。
基金资助:
国家自然科学基金(52270136);国家重点研发计划(2020YFC1908702)

Binding mechanism of Pb²⁺ onto humic acids from sludge hyper-thermophilic composting

LI Xin¹(), YANG Zao¹, ZHONG Xinru¹, HAN Haoxuan¹, ZHUANG Xuning², BAI Jianfeng², DONG Bin¹^,³(), XU Zuxin¹

^1.College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
^2.School of Resources and Environmental Engineering, Shanghai Polytechnic University, Shanghai 201209, China
^3.YANGTZE Eco-Environment Engineering Research Center, China Three Gorges Corporation, Beijing 100038, China

Received:2022-10-09 Revised:2022-12-20 Online:2023-09-15 Published:2023-09-28
Contact: DONG Bin

摘要/Abstract

摘要：

污泥稳定化产物中含有丰富的功能有机物，能够直接参与重金属的络合过程。超高温堆肥作为一种更有优势的污泥稳定化手段，明晰其产物中的典型功能有机质与重金属结合特性，对于评估其土地利用的价值至关重要。本文采用吸附实验对比分析了超高温堆肥（HTC）、高温堆肥（TC）和生污泥（RS）样品中典型功能有机物胡敏酸（HAs）与Pb²⁺的吸附效果。结果表明，HTC和TC中HAs对Pb²⁺的理论最大吸附量（ $q_{m}$ ）会随着堆肥进行而逐渐增大。在堆肥过程中HTC的HAs含量相对TC也有明显增加，第21天即达到最高值。HTC堆肥（21天）衍生HAs对Pb²⁺的吸附量（29.6mg/g）比TC（17.3mg/g）高70.7%，这表明HTC产物在土壤重金属污染修复方面更具优势。¹³C NMR结果表明，在堆肥过程中HTC衍生HAs的酚基碳与芳香碳增加更多，堆肥前期（0~21天）HTC衍生HAs的芳香碳增加比TC更快速。进一步采用红外光谱，结合二维相关光谱和移动窗口技术解析，表明HTC堆肥衍生HAs的多糖类物质会最先与Pb²⁺进行结合。其中，HTC堆肥衍生HAs与Pb²⁺结合最重要的官能团是酚羟基和芳香族基团。基于上述认识，可知HTC的高腐殖化特性使酚羟基和芳香族基团等基团增加是HTC具有更强结合Pb²⁺能力的关键，HTC有利于污泥的高效土地利用。

关键词: 超高温堆肥, 胡敏酸, 铅, 结合机制, 土地利用

Abstract:

Sludge and its stabilized products are rich in functional organic matter, which can directly participate in the complexation process of heavy metals. By defining the binding properties of its products and heavy metals, hyper-thermophilic composting (HTC), a more advantageous sludge stabilization technique, might better assess the value of its land use. Adsorption experiments were used to investigate the binding capacities of Pb²⁺ to humic acids (HAs) derived from raw sludge (RS), thermophilic composting (TC) and HTC. The findings demonstrated that with composting time, the maximum adsorption values (q_m) of HAs derived from HTC and TC to Pb²⁺ steadily increased. During composting, the HTC-derived HAs content also increased significantly in comparison to TC-derived HAs, peaking on the 21st day. The adsorption capacity (on a dry basis) of HTC-derived HAs to Pb²⁺ (21d, 29.6mg/g) was 70.7% higher than HTC-derived HAs (21d, 17.3mg/g), indicating that HTC products had more benefits in the remediation of soil heavy metal contamination. The ¹³C NMR data showed that the phenolic and aromatic carbons of HTC-derived HAs increased more during composting, and the aromatic carbons of HTC-derived HAs grew more rapidly than TC in the early stage of composting (0—21d). Infrared spectroscopy, two-dimensional correlation spectroscopy and moving window analysis all indicated that the polysaccharides in HTC-derived HAs would initially combine with Pb²⁺. For the binding of Pb²⁺ to HTC-derived HAs, phenolic hydroxyl and aromatic groups were more important among them. Based on the previous insights, it was evident that HTC’s higher degree of humification and the rise in phenolic hydroxyl and aromatic groups were the main contributors to its stronger ability to bind, and HTC was helpful for the land use of sludge.

Key words: hyper-thermophilic compost, humic acids, lead, binding mechanism, land use

中图分类号:

X705

李昕, 杨早, 钟欣茹, 韩昊轩, 庄绪宁, 白建峰, 董滨, 徐祖信. 污泥超高温堆肥衍生胡敏酸对Pb²⁺的结合机制[J]. 化工进展, 2023, 42(9): 4957-4966.

LI Xin, YANG Zao, ZHONG Xinru, HAN Haoxuan, ZHUANG Xuning, BAI Jianfeng, DONG Bin, XU Zuxin. Binding mechanism of Pb²⁺ onto humic acids from sludge hyper-thermophilic composting[J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4957-4966.

图/表 8

参考文献 40

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原料	含水率/%	有机质质量分数/%	pH
生污泥	68.3±3.9	75.5±1.2	8.0±0.1
小麦秸秆	11.1±0.1	88.4±0.1	6.6±0.1
超高温堆肥腐熟料	21.9±0.4	35.2±1.1	7.8±0.2
传统高温堆肥腐熟料	31.2±1.4	44.3±0.8	8.1±0.3

原料	含水率/%	有机质质量分数/%	pH
生污泥	68.3±3.9	75.5±1.2	8.0±0.1
小麦秸秆	11.1±0.1	88.4±0.1	6.6±0.1
超高温堆肥腐熟料	21.9±0.4	35.2±1.1	7.8±0.2
传统高温堆肥腐熟料	31.2±1.4	44.3±0.8	8.1±0.3

项目	q_m/mg·g^-1	K_L/L·mg^-1	R²
RS	209.51	0.030	0.8221
TC
7d	274.88	0.062	0.9786
21d	297.69	0.301	0.9964
35d	307.99	0.034	0.7972
49d	303.28	0.011	0.8498
HTC
7d	317.07	0.020	0.9712
21d	309.73	0.00034	0.9398
35d	316.35	0.0055	0.9295
49d	338.97	0.045	0.9758

项目	q_m/mg·g^-1	K_L/L·mg^-1	R²
RS	209.51	0.030	0.8221
TC
7d	274.88	0.062	0.9786
21d	297.69	0.301	0.9964
35d	307.99	0.034	0.7972
49d	303.28	0.011	0.8498
HTC
7d	317.07	0.020	0.9712
21d	309.73	0.00034	0.9398
35d	316.35	0.0055	0.9295
49d	338.97	0.045	0.9758

项目	δ为0~65	δ为65~110	δ为110~140	δ为140~160	δ为160~190	δ为190~220
项目	脂肪族碳	醚、羟基碳	芳香碳	酚醛碳	羧酸碳	羰基碳
RS	45.06	12.01	12.38	7.76	16.94	5.86
TC
7d	43.07	14.31	12.41	7.66	16.44	6.12
21d	38.89	15.28	14.32	8.86	15.65	7.02
35d	36.75	16.36	15.28	9.9	15.64	6.07
49d	39.65	14.46	13.86	8.81	16.43	6.8
HTC
7d	43.91	12.65	13.39	7.68	15.88	6.49
21d	40.88	12.2	15.01	8.8	16.77	6.34
35d	38.6	13	15.83	9.45	16.5	6.62
49d	38.46	13.39	15.49	9.28	16.72	6.67

污泥超高温堆肥衍生胡敏酸对Pb²⁺的结合机制

Binding mechanism of Pb²⁺ onto humic acids from sludge hyper-thermophilic composting

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参考文献 40

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波长/cm^-1	1736	1672	1514	1381	1225	982	868
RS
1736	+	+(-)	+(-)	-(-)	+(-)	+(+)	+(+)
1672		+	+(-)	-(-)	+(+)	+(+)	+(+)
1514			+	-(-)	+(+)	+(+)	+(+)
1381				+	-(+)	-(-)	-(+)
1225					+	+(+)	+(+)
982						+	+(-)
868							+
波长/cm^-1	1738	1523	1383	1184	995	889	798
TC-21d
1738	+	-(-)	-(-)	+(+)	+(-)	+(+)	-(-)
1523		+	-(+)	-(-)	+(-)	+(-)	+(-)
1383			+	-(+)	-(+)	-(+)	-(+)
1184				+	+(-)	+(-)	+(-)
995					+	+(-)	+(-)
889						+	+(-)
798							+
波长/cm^-1	1736	1585	1504	1385	1319	1176	1093	764
HTC-21d
1736	+	-(+)	-(+)	-(+)	-(+)	+(+)	+(+)	+(+)
1585		+	+(+)	+(-)	+(-)	+(-)	+(-)	+(-)
1504			+	+(-)	+(-)	-(-)	+(-)	-(-)
1385				+	+	+(-)	+(-)	-(-)
1319					+	+(-)	+(-)	+(-)
1176						+	+(+)	+(-)
1093							+	+(-)
764								+

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