淹水-落干条件下FeMnMg-LDH对污染底泥中砷迁移转化的调控研究

doi:10.16258/j.cnki.1674-5906.2023.07.008

生态环境学报 ›› 2023, Vol. 32 ›› Issue (7): 1249-1262.DOI: 10.16258/j.cnki.1674-5906.2023.07.008

淹水-落干条件下FeMnMg-LDH对污染底泥中砷迁移转化的调控研究

周宏光¹(), 甘艳平¹, 伍德权³, 杨延梅¹^,^*(), 张扬², 王璐瑶²

1.重庆交通大学/国家内河航道整治技术工程研究中心，重庆 400074
2.陕西省土地工程建设集团有限责任公司，陕西西安 710075
3.黔西南州广播电视大学，贵州兴义 562400

收稿日期:2023-03-12 出版日期:2023-07-18 发布日期:2023-09-27
通讯作者: * 杨延梅。Email: yymeicq@163.com
作者简介:周宏光（1987年生），男，副教授，博士，主要从事环境功能材料研制及水污染控制。Email: hgzhou@cqjtu.edu.cn
基金资助:
中国博士后科学基金项目(2018M643421);陕西省自然科学基础研究计划(2021JQ-959);重庆市自然科学基金面上项目(2022NSCQ-MSX2283)

Regulation of Arsenic Transport and Transformation in Contaminated Sediment by FeMnMg-LDH under Flooding-drying Conditions

ZHOU Hongguang¹(), GAN Yanping¹, WU Dequan³, YANG Yanmei¹^,^*(), ZHANG Yang², WANG Luyao²

1. National Engineering Research Center for Inland Waterway Regulation/Chongqing Jiaotong University, Chongqing 400074, P. R. China
2. Shaanxi Province Land Engineering Construction Group, Xi’an 710075, P. R. China
3. QianXiNan Radio And TeleVision University, Xingyi 562400, P. R. China

Received:2023-03-12 Online:2023-07-18 Published:2023-09-27

摘要/Abstract

摘要：

水库消落带因受到交替淹没与暴露的问题，其底泥As释放、迁移和转化受到影响，此外，腐殖酸（HA）作为底泥的主要有机成分，其对As的作用机制尚存在争议，因此通过钝化剂来稳定底泥中的As，对底泥资源化利用具有重要意义。采用改进的共沉淀法制备FeMnMg-LDH，在人工培养的As(Ⅴ)污染底泥上模拟淹水和落干试验，同时考虑HA的影响，以FeMnMg-LDH作为钝化剂对消落带地区的底泥进行稳定化处理，研究As的形态转化特征及浸出毒性变化，并分析两者的相关性。结果表明：淹水条件下HA促进As向上覆水体释放且HA水平越高释放量越多，60 mg·kg^-1和250 mg·kg^-1污染底泥向上覆水体释放的As质量浓度最高分别可达4.81×10³ μg·L^-1和1.22×10⁴ μg·L^-1，添加FeMnMg-LDH后有效抑制As由底泥向上覆水体释放；随FeMnMg-LDH添加水平的增加，淹水和落干条件下60 mg·kg^-1污染底泥中弱酸提取态砷（MASF-As）百分比降至0.06%和0.07%，250 mg·kg^-1污染底泥中MASF-As百分比均降至0.13%，MASF-As向更稳定的形态转变；随FeMnMg-LDH添加水平的增加，底泥中As的浸出质量浓度逐渐降低，稳定化效率逐渐升高，60 mg·kg^-1和250 mg·kg^-1污染底泥在淹水期稳定化效率高达到76.0%和74.1%，在落干期高达75.9%和73.3%；落干期底泥中As的浸出毒性风险高于淹水期；淹水及落干条件下HA的添加影响FeMnMg-LDH对污染底泥中As的稳定化作用，表现为正效应。相关性分析结果表明，由于淹水过程中底泥向上覆水体释放As，部分底泥As的浸出毒性与MASF-As和可还原态砷（RF-As）的相关性不显著；落干条件下底泥As的浸出毒性与MASF-As呈正相关，与RF-As呈负相关。综上所述，FeMnMg-LDH材料在消落带As污染底泥钝化修复工作中，具有一定的实践意义。

关键词: 砷, 底泥, FeMnMg-LDH, 淹水-落干, 稳定化

Abstract:

The reservoir subsidence zone is affected by alternate inundation and exposure, so the release, migration and transformation of As in the sediment are affected. In addition, the mechanism of the effect of action of humic acid (HA), as the main organic component of sediment, on As is still controversial. Therefore, it is of great significance to stabilize As in sediment by passivating agent for the utilization of sediment resources. In this paper, FeMnMg-LDH was prepared by a modified co-precipitation method to simulate flooding and drop-dry tests on artificially cultured As(V) contaminated sediment, while considering the effect of HA, and FeMnMg-LDH was used as a passivating agent to stabilize the sediment in the abatement zone area to study the morphological transformation characteristics and leaching toxicity changes of As, and to analyze the correlation between them. The results showed that HA promoted the release of As to the overlying water under flooding conditions, and the higher the HA level, the more the release amount. The maximum mass concentrations of As released from 60 mg·kg^-1 and 250 mg·kg^-1 contaminated sediment to the overlying water were 4.81×10³ μg·L^-1 and 1.22×10⁴ μg·L^-1, respectively, and the addition of FeMnMg-LDH effectively inhibited the release of As from the sediment to the overlying water. With the increase of FeMnMg-LDH addition level, the percentage of mild acido-soluble fraction arsenic (MASF-As) in 60 mg·kg^-1 contaminated sediment decreased to 0.06% and 0.07% under flooding and drying conditions; the percentage of MASF-As in 250 mg·kg^-1 contaminated sediment decreased to 0.13%; and MASF-As changed to a more stable form. With the increase of FeMnMg-LDH addition level, the leaching mass concentration of As in sediment decreased gradually, and the stabilization efficiency increased gradually. The stabilization efficiency of 60 mg·kg^-1 and 250 mg·kg^-1 contaminated sediment reached 76.0% and 74.1% in the flooding period, and 75.9% and 73.3% in the drying period. The leaching toxicity risk of As in the sediment during the drying period was higher than that during the flooding period. The addition of HA under flooding and drying conditions positively influenced the stabilization effect on As in contaminated sediment from FeMnMg-LDH. The results of correlation analysis showed that the leaching toxicity of As in some sediments was not significantly correlated with MASF-As and reducible fraction arsenic (RF-As) due to the release of As from sediments to overlying water during flooding. The leaching toxicity of As in sediment under dry conditions was positively correlated with MASF-As and negatively correlated with RF-As. In conclusion, FeMnMg-LDH materials are of practical significance in the passivation remediation of As-contaminated sediment in the abatement zone.

Key words: arsenic, sediment, FeMnMg-LDH, flooding-drying, stabilization

中图分类号:

周宏光, 甘艳平, 伍德权, 杨延梅, 张扬, 王璐瑶. 淹水-落干条件下FeMnMg-LDH对污染底泥中砷迁移转化的调控研究[J]. 生态环境学报, 2023, 32(7): 1249-1262.

ZHOU Hongguang, GAN Yanping, WU Dequan, YANG Yanmei, ZHANG Yang, WANG Luyao. Regulation of Arsenic Transport and Transformation in Contaminated Sediment by FeMnMg-LDH under Flooding-drying Conditions[J]. Ecology and Environment, 2023, 32(7): 1249-1262.

图/表 18

表1 供试底泥基本理化性质

Table 1 Basic physicochemical properties of sediment samples

样品	pH	w_{(total Pb)}/(mg·kg^-1)	w_{(total Cd)}/(mg·kg^-1)	w_{(total Fe)}/(mg·kg^-1)	w_{(total Mn)}/(mg·kg^-1)	w_{(total As)}/(mg·kg^-1)	CEC/(cmol·kg^-1)	w_有机质/(mg·kg^-1)
底泥	8.76	342	5.27	9.37	3.71×10²	6.10	22.4	1.45×10⁴

表2 试验设计

Table 2 Experimental design

As污染水平 (mg·kg^-1)	HA添加水平
As污染水平 (mg·kg^-1)	0%	2%	5%
60	As-60	As-60-2%	As-60-5%
250	As-250	As-250-2%	As-250-5%

表3 As元素形态顺序提取试剂及提取条件

Table 3 As element morphological order extraction reagents and extraction conditions

形态	提取试剂	提取条件
弱酸提取态 (MASF-As)	0.11 mol·L^-1 HAc	加入40 mL提取剂, 室温 (22±5) ℃振荡16 h, 3000 r·min^-1离心20 min, 倾析液体保存待测
可还原态 (RF-As)	0.50 mol·L^-1 NH₂OH·HCl	加入40 mL提取剂, 室温 (22±5) ℃振荡16 h, 3000 r·min^-1离心20 min, 倾析液体保存待测
可氧化态 (OF-As)	1.00 mol·L^-1 NH₄Ac (pH=2), H₂O₂(pH=2-3)	按标准操作多次加入H₂O₂对试样进行消化, 然后加入50 mL NH₄Ac, 室温 (22±5) ℃振荡16 h, 3000 r·min^-1离心20 min, 倾析液体保存待测
残渣态 (ResF-As)	王水水浴消解	加入10 mL王水 (1+1), 加塞于水浴锅中煮沸2 h, 期间摇动3-4次, 摇匀静置后取上清液待测

表4 风险评价准则

Table 4 Risk assessment criteria

风险等级	无风险	低风险	中等风险	高风险	非常高风险
MASF所占比例/%	<1	1-10	11-30	31-50	>50

图1 FeMnMg-LDH材料对底泥上覆水As质量浓度的影响图中数据为平均值±标准误，n=3。下同

Figure 1 Effect of FeMnMg-LDH on As mass concentration in overlying water of sediment

图2 HA添加下FeMnMg-LDH材料对底泥上覆水As质量浓度的影响

Figure 2 Effect of FeMnMg-LDH material on As mass concentration in overlying water of sediment under the influence of HA addition

图3 FeMnMg-LDH吸附As(V)前后XRD图谱

Figure 3 XRD patterns of FeMnMg-LDH and As-FeMnMg-LDH

图4 FeMnMg-LDH吸附As(V)前后SEM图

Figure 4 SEM photographs of samples: FeMnMg-LDH and As-FeMnMg-LDH

图5 FeMnMg-LDH吸附As(V)前后TEM图

Figure 5 TEM photographs of samples: FeMnMg-LDH and As-FeMgMn-LDH

图6 FeMnMg-LDH吸附As(V)前后FT-IR图

Figure 6 FT-IR photographs of samples: FeMnMg-LDH and As-FeMnMg-LDH

图7 FeMnMg-LDH吸附As(V)前后EDX图

Figure 7 EDX photographs of samples: FeMnMg-LDH and As-FeMnMg-LDH

图8 淹水条件下As各形态百分比的变化

Figure 8 Changes of percentage of different forms of As under flooding conditions

图9 落干条件下As各形态百分比的变化

Figure 9 Changes in the percentage of different forms of As under drying conditions

图10 FeMnMg-LDH材料稳定修复底泥中As的浸出毒性变化

Figure 10 The leaching toxicity change of As in sediment stabilized by FeMnMg-LDH material

图11 FeMnMg-LDH对底泥中As的稳定化效率

Figure 11 Stabilization efficiency of As in sediment by FeMnMg-LDH

图12 HA添加下FeMnMg-LDH材料稳定修复底泥中As的浸出毒性变化

Figure 12 Changes of leaching toxicity of As in sediment stabilized by FeMnMg-LDH with HA addition

表5 淹水条件下污染底泥中As的赋存形态与浸出毒性质量分数的Pearson相关性

Table 5 Pearson correlation between As fugacity pattern and leaching toxicity mass fraction in contaminated sediments under flooding conditions

赋存形态	浸出毒性
赋存形态	As-60	As-60-2%	As-60-5%	As-250	As-250-2%	As-250-5%
MASF-As	0.982* ¹⁾	0.891	0.849	0.994** ²⁾	0.999**	0.997**
RF-As	-0.979*	-0.892	-0.927	-0.840	-0.929	-0.996**
OF-As	-0.807	-0.963*	-0.885	-0.872	-0.999**	-0.943
ResF-As	0.879	0.919	0.929	0.667	0.956*	0.996**

表6 落干条件下污染底泥中As的赋存形态与浸出毒性质量分数的Pearson相关性

Table 6 Pearson correlation between As fugacity pattern and leaching toxicity mass fraction in contaminated sediments under drying conditions

赋存形态	浸出毒性
赋存形态	As-60	As-60-2%	As-60-5%	As-250	As-250-2%	As-250-5%
MASF-As	0.996**	0.999**	0.999**	0.999**	0.956*	0.975*
RF-As	-0.972*	-0.958*	-0.963*	-0.974*	-0.988*	-0.963*
OF-As	0.106	0.772	-0.685	-0.088	0.835	0.840
ResF-As	0.702	0.977*	0.844	0.994**	0.987*	0.995**

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淹水-落干条件下FeMnMg-LDH对污染底泥中砷迁移转化的调控研究

Regulation of Arsenic Transport and Transformation in Contaminated Sediment by FeMnMg-LDH under Flooding-drying Conditions

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