混合型生物炭对寒冷地区PAHs污染土壤微生物修复的强化作用

doi:10.16258/j.cnki.1674-5906.2023.11.005

生态环境学报 ›› 2023, Vol. 32 ›› Issue (11): 1942-1951.DOI: 10.16258/j.cnki.1674-5906.2023.11.005

混合型生物炭对寒冷地区PAHs污染土壤微生物修复的强化作用

苏丹¹^,^*(), 罗桥冰¹, 董昱杉¹, 杨彩霞¹, 王鑫²

1.辽宁大学环境学院，辽宁沈阳 110036
2.沈阳大学/区域污染环境生态修复教育部重点实验室，辽宁沈阳 110044

收稿日期:2022-08-17 出版日期:2023-11-18 发布日期:2024-01-17
通讯作者: *
作者简介:苏丹（1980年生），女，教授，博士，硕士研究生导师，研究领域为污染生态与环境工程。E-mail: iamsudan@126.com
基金资助:
国家自然科学基金项目(52170163);辽宁省教育厅面上项目(LJKZ0092);沈阳市中青年科技创新人才支持计划(RC220064);沈阳市科技计划项目(22-322-3-14)

Strengthening Effect of Mixed Biochar on Microbial Remediation of PAHs Contaminated Soil in Cold Areas

SU Dan¹^,^*(), LUO Qiaobing¹, DONG Yushan¹, YANG Caixia¹, WANG Xin²

1. School of Environmental Science, Liaoning University, Shenyang 110036, P. R. China
2. Key Laboratory of Regional Environment and Eco-Remediation, Ministry of Education/Shenyang University, Shenyang 110044, P. R. China

Received:2022-08-17 Online:2023-11-18 Published:2024-01-17

摘要/Abstract

摘要：

北方寒冷地区存在大面积中低浓度多环芳烃（PAHs）污染土壤，潜在威胁生态安全与人群健康。以混合型生物炭（C500+W500）为载体，以耐冷假单胞菌（Pseudomonas sp.，S4）与高山被孢霉（Mortierella alpine，J7）为PAHs降解混合菌，采用吸附固定化方法制备生物修复材料，研究了低温条件下混合型/单一型生物炭加载耐冷混合菌对土壤菲（Phe）、芘（Pyr）的降解效果，并探讨生物炭对土壤中PAHs微生物降解过程的强化机理。结果表明：混合型生物炭固定化微生物对土壤Phe、Pyr的修复效果高于游离菌，亦高于单一类型生物炭固定化菌剂，并且修复效果与生物炭的混合比例有关。15 ℃条件下修复30 d后，以w=1.34% C500与w=0.67% W500混合生物炭为载体的固定化混合菌（CWJ2:1）对Phe和Pyr的去除率分别为51.87%和45.28%，高于游离菌25.81%和23.65%，亦高于单一生物炭固定化组15.63%－18.96%和13.62%－16.07%。生物炭添加后，减少了土壤对Phe的吸附量，促进土壤中PAHs进入生物相，提高土壤PAHs微生物可利用性。在Phe的竞争吸附中CK-Biochar、CK-Soil、CWsoil与CW的平衡吸附量分别为0.01 μg∙mg⁻¹、25.45 μg∙g⁻¹、23.46 μg∙g⁻¹与26.46 μg∙mg⁻¹，生物炭对土壤Phe的竞争吸附过程接近于准二级动力学模型。该研究为寒冷地区有机污染土壤的微生物原位修复提供理论指导与借鉴。

关键词: 混合型生物炭, PAHs, 固定化微生物, 土壤修复, 有机污染物, 强化机理

Abstract:

There are large areas in the Northern cold region that consist of contaminated soils with low and medium concentrations of polycyclic aromatic hydrocarbons (PAHs). These contaminants pose potential threats to both ecological safety and human health. In this paper, a mixed biochar (C500+W500) was used as a carrier, and Pseudomonas sp. S4 and Mortierella alpine J7 were used as mixed bacteria capable of degrading PAHs. The bioremediation materials were prepared using an adsorption immobilization method. The study aimed to investigate the degradation capabilities of mixed biochar and single-type biochar loaded with cold-tolerant mixed bacteria on soil compounds such as phenanthrene (Phe) and pyrene (Pyr) under low-temperature conditions, and the mechanisms and advantages of biochar in the process of microbial degradation of PAHs in soil were discussed. The results showed that the remediation effects of mixed biochar immobilized microorganisms on Phe and Pyr in soil were higher than those of free bacteria as well as single biochar immobilized bacteria. The remediation effect was related to the mixing ratio of biochar. After 30 days of remediation at 15 ℃, the removal rates of Phe and Pyr were 51.87% and 45.28% respectively, when using immobilized mixed biochar with 1.34% C500 and 0.67% W500 mixed biochar as the carrier (CWJ 2:1). These rates were higher than the removal rates achieved by free bacteria (25.81% and 23.65%) and single biochar immobilized group (15.63%‒18.96% and 13.62%‒16.07%). Furthermore, mixed biochar affected the migration of PAHs in soil. The addition of biochar to soil reduced the adsorption of Phe, facilitating the entry of PAHs into the bio-facies in soil and improving the microbial availability of PAHs. In terms of Phe’s competitive adsorption, the equilibrium adsorption amounts of CK biochar, CK soil, CW_soil and CW were 0.01 μg∙mg⁻¹, 25.45 μg∙g⁻¹, 23.46 μg∙g⁻¹, and 26.46 μg∙mg⁻¹, respectively. The competitive adsorption process of soil Phe by biochar was found to align closely with the quasi second-order kinetic model. This study provides a theoretical reference for in-situ microbial remediation of PAH-contaminated soil in Northern cold areas.

Key words: mixed-biochar, PAHs, immobilized microorganism, soil remediation, organic pollutants, strengthening mechanism

中图分类号:

X592

苏丹, 罗桥冰, 董昱杉, 杨彩霞, 王鑫. 混合型生物炭对寒冷地区PAHs污染土壤微生物修复的强化作用[J]. 生态环境学报, 2023, 32(11): 1942-1951.

SU Dan, LUO Qiaobing, DONG Yushan, YANG Caixia, WANG Xin. Strengthening Effect of Mixed Biochar on Microbial Remediation of PAHs Contaminated Soil in Cold Areas[J]. Ecology and Environment, 2023, 32(11): 1942-1951.

图/表 8

表1 土壤修复效果实验的处理设置

Table 1 Treatment design for the soil remediation effect experiment

样品编号	处理
CK	不加生物炭不接种
J	污染土壤 (4 g)+游离混合菌
CW	污染土壤 (4 g)+混合生物炭 (w=2%)
C	污染土壤 (4 g)+固定化混合菌, 载体采用w=2% C500的单一生物炭
W	污染土壤 (4 g)+固定化混合菌, 载体采用w=2% W500的单一生物炭
CW1:1	污染土壤 (4 g)+固定化混合菌, 载体混合生物炭采用w=1.00% C500与w=1.00% W500
CW1:2	污染土壤 (4 g)+固定化混合菌,载体混合生物炭采用w=0.67% C500与w=1.34% W500
CW2:1	污染土壤 (4 g)+固定化混合菌, 载体混合生物炭采用w=1.34% C500与w=0.67% W500

表2 生物炭的pH、吸水能力、比表面积、总孔孔容、平均孔径

Table 2 pH, water absorption capacity, Specific surface area, total pore volume and average pore diameter of biochar

生物炭类型	pH	吸水量/ (g∙g⁻¹)	比表面积/ (m²∙g⁻¹)	总孔孔容/ (cm³∙g⁻¹)	平均孔径/ nm
C300	10.13±0.03	1.31±0.02	1.473	2.283	6.201
C500	9.44±0.03	1.37±0.01	3.591	4.454	4.961
W300	8.38±0.03	3.46±0.02	1.832	4.321	9.432
W500	8.18±0.02	3.85±0.01	2.929	1.674	2.286

表3 生物炭的元素组成

Table 3 Elemental analysis of biochar

生物炭类型	w_(N)/%	w_(C)/%	w_(H)/%	w_(O)/%	w_(C)/w_(H)	w_(C)/w_(N)
C300	1.09	74.17	4.12	19.92	17.99	67.73
C500	0.81	83.70	1.80	13.35	46.25	103.33
W300	0.20	72.86	4.42	22.42	16.45	364.32
W500	0.31	88.14	2.38	9.06	37.01	284.32

图1 供试生物炭SEM图

Figure 1 SEM of tested biochar

图2 修复材料固定化表面结构

Figure 2 Immobilized mixed consortium observed by SEM

图3 生物炭与土壤对Phe的吸附量 CK-Soil为仅含土壤处理组，CK-Biochar为仅含生物炭处理组，CW为土壤与生物炭混合处理组，CWBiochar为混合处理组中生物炭对Phe的吸附量，CWsoil为混合处理组中土壤对Phe的吸附量。Q为吸附量，图中的误差线为标准差（n=3），下同

Figure 3 Relationship between the amount of adsorption of Phe in biochar and soil with time

表4 生物炭吸附动力学拟合参数

Table 4 Parameters obtained from pseudo-first-order kinetics model, pseudo-second-order kinetics model for Phe adsorption on biochar and soil

处理	准一级动力学			准二级动力学
处理	平衡吸附量 (Q_e)	准一级吸附动力学常数 (k₁)	相关系数 (r²)	平衡吸附量 (Q_e)	准二级吸附动力学常数 (k₂)	相关系数 (r²)
CK-Biochar	4.473	0.561	0.88	5.249	0.129	0.99
CW_Biochar	1.015	0.037	0.91	1.273	0.030	0.99
CW	26.465	0.044	0.99	33.014	0.001	0.98
CK-Soil	25.459	0.044	0.99	30.807	0.002	0.98
CW_Soil	23.466	0.046	0.99	28.433	0.002	0.98

图4 不同处理修复后土壤中菲（a）与芘（b）的含量 CK为对照，不加生物炭不接种；J为接种PAHs降解菌处理组；CW为按w=2%添加混合型生物炭处理组；C为添加单一生物炭固定化混合菌，载体采用w=2% C500；W为添加单一生物炭固定化混合菌，载体采用2% W500; CWJ1:1为添加固定化混合菌，载体混合生物炭采用w=1.00% C500与w=1.00% W500；CWJ1:2为添加固定化混合菌，载体混合生物炭采用w=0.67% C500与w=1.34% W500；CWJ2:1为添加固定化混合菌，载体混合生物炭采用w=1.34% C500与w=0.67% W500。不同小写字母表示不同处理间差异性显著（P<0.05，n=3）

Figure 4 Phe (a) and Pyr (b) degradation rate of soil sample with different methods

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混合型生物炭对寒冷地区PAHs污染土壤微生物修复的强化作用

Strengthening Effect of Mixed Biochar on Microbial Remediation of PAHs Contaminated Soil in Cold Areas

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