河水入渗过程中近岸带地下水中砷的形成与影响因素研究

doi:10.13745/j.esf.sf.2021.10.3

地学前缘 ›› 2022, Vol. 29 ›› Issue (4): 455-467.DOI: 10.13745/j.esf.sf.2021.10.3

河水入渗过程中近岸带地下水中砷的形成与影响因素研究

鹿帅¹^,²^,³(), 苏小四⁴, 冯晓语⁵, 孙超⁶

1.河北地质大学水资源与环境学院, 河北石家庄 050031
2.河北省水资源可持续利用与开发重点实验室, 河北石家庄 050031
3.河北省水资源可持续利用与产业结构优化协同创新中心, 河北石家庄 050031
4.吉林大学水资源与环境研究所, 吉林长春 130021
5.河北地质大学宝石与材料学院, 河北石家庄 050031
6.河北省地质环境监测院河北省地质资源环境监测与保护重点实验室, 河北石家庄 050021

收稿日期:2020-07-23 修回日期:2021-11-05 出版日期:2022-07-25 发布日期:2022-07-28
作者简介:鹿帅(1990—),男,博士,讲师,硕士生导师,主要从事水文地球化学、水文地质学等方面的教学与科研工作。E-mail: lushuaij@163.com
基金资助:
国家自然科学基金项目(41372238);国家自然科学基金项目(42107100);河北省专业学位研究生教学案例建设项目(KCJSZ2021098);河北省地质资源环境监测与保护重点实验室开放课题项目(JCYKT202003);河北地质大学博士科研启动基金项目(BQ2019046)

Sources and influencing factors of arsenic in nearshore zone during river water infiltration

LU Shuai¹^,²^,³(), SU Xiaosi⁴, FENG Xiaoyu⁵, SUN Chao⁶

1. School of Water Resources and Environment, Hebei GEO University, Shijiazhuang 050031, China
2. Hebei Province Key Laboratory of Sustained Utilization and Development of Water Resources, Shijiazhuang 050031, China
3. Hebei Province Collaborative Innovation Center for Sustainable Utilization of Water Resources and Optimization of Industrial Structure, Shijiazhuang 050031, China
4. Institute of Water Resources and Environment, Jilin University, Changchun 130021, China
5. School of Gemology and Material, Hebei GEO University, Shijiazhuang 050031, China
6. Hebei Key Laboratory of Geological Resources and Environment Monitoring and Protection, Hebei Institute of Environmental Geology Exploration, Shijiazhuang 050021, China

Received:2020-07-23 Revised:2021-11-05 Online:2022-07-25 Published:2022-07-28

摘要/Abstract

摘要：

沈阳黄家水源地是我国北方地区典型的傍河地下水水源地,近岸带地下水中铁(Fe)、锰(Mn)、砷(As)含量严重超标。为查明地下水中As的来源与影响因素,对研究区河水、地下水以及土壤样品进行采集与测试,分析了水样常规指标与碳硫稳定同位素、土样中典型矿物、砷的含量及赋存形态。结果表明,研究区河水中As含量很低,而地下水中As含量普遍超标。河水入渗初期,氧化性河水使部分含As矿物发生氧化而释放As;随着河水入渗,地下水向还原环境转变,含As的Fe/Mn矿物发生还原性溶解,地下水中As含量逐渐升高。研究区典型矿物有黄铁矿、菱铁矿、软锰矿、赤铁矿、针铁矿、菱锰矿等,通过可交换态砷解吸、有机质结合态砷氧化、铁锰氧化物结合态砷还原性溶解等,介质中的As释放至地下水中。地下水中As含量与酸碱度(pH)、氧化还原电位(Eh)呈一定负相关,与溶解有机碳(DOC)、 $HCO 3 -$ 、Fe、Mn含量呈正相关。

关键词: 河水入渗, 近岸带, 地下水, 砷, 沈阳黄家水源地

Abstract:

The Shenyang Huangjia water source area is a typical riverside groundwater source area in northern China. In its nearshore zone the iron (Fe), manganese (Mn) and arsenic (As) contents were well above the safety standard. In order to find out the sources and influencing factors of groundwater As in the affected area, samples of river water, groundwater and soils of the study area were collected and tested. Water quality indexes and carbon and sulfur stable isotopes of water samples, and the contents and occurrences of typical minerals and As in soil samples were analyzed. The results showed that As contents were very low in river water samples but generally exceeded the standard in groundwater samples. In the early stage of river water infiltration, some As-bearing minerals were oxidized by oxidizing river water and As was released. Later on, the groundwater environment became reductive with the infiltration of river water, and reductive dissolution of As-bearing Fe/Mn minerals resulted in the gradual increase of groundwater As. Typical minerals in the study area were pyrite, siderite, pyrolusite, hematite, goethite, rhodochrosite, etc. Through desorption of exchangeable arsenic, oxidation of organic matter-bound arsenic, and reductive dissolution of iron-manganese oxide-bound arsenic, As was release into the groundwater. To a certain extent, As content in the groundwater was negatively correlated with groundwater pH and redox potential (Eh) and positively correlated with the dissolved organic carbon (DOC), $HCO 3 -$ , Fe and Mn contents.

Key words: river water infiltration, nearshore zone, groundwater, arsenic, Shenyang Huangjia water source area

中图分类号:

P641
X523

鹿帅, 苏小四, 冯晓语, 孙超. 河水入渗过程中近岸带地下水中砷的形成与影响因素研究[J]. 地学前缘, 2022, 29(4): 455-467.

LU Shuai, SU Xiaosi, FENG Xiaoyu, SUN Chao. Sources and influencing factors of arsenic in nearshore zone during river water infiltration[J]. Earth Science Frontiers, 2022, 29(4): 455-467.

图/表 15

图1 研究区位置

Fig.1 Geography of the study area

表1 监测井相关参数

Table 1 Monitoring well related parameters

井号	井深/m	过滤器深度/m	止水深度/m
井号	井深/m	过滤器深度/m	顶部	底部
HB1-2\HB2-2\HB3-2\HB4-2	6.0	4.0~<5.0	3.0~<4.0	5.0~<6.0
HB1-3\HB2-3\HB3-3\HB4-3	7.0	5.0~<6.0	4.0~<5.0	6.0~<7.0
HB1-4\HB2-4\HB3-4\HB4-4	8.0	6.0~<7.0	5.0~<6.0	7.0~<8.0
HB1-5\HB2-5\HB3-5\HB4-5	9.0	7.0~<8.0	6.0~<7.0	8.0~<9.0
HB1-6\HB2-6\HB3-6\HB4-6	10.0	8.0~<9.0	7.0~<8.0	9.0~<10.0
HB3-7\HB4-7	11.0	9.0~10.0	8.0~9.0	10.0~11.0

图2 河水入渗过程中pH值、Eh值、DO浓度变化图其中地下水取样深度为5.0~6.0 m。

Fig.2 Diagram of pH, Eh, and DO concentration during river water infiltration (The sampling depth of groundwater is 5.0-6.0 m)

图3 河水入渗过程中DOC、 HCO 3 -、Mn2+、Fe2+、 SO 4 2 -、As浓度变化图其中地下水取样深度为5.0~6.0 m。

Fig.3 Diagram of DOC, HCO 3 -, Mn2+, Fe2+, SO 4 2 -, As concentration during river water infiltration (The sampling depth of groundwater is 5.0-6.0 m)

图4 近岸带水化学指标垂向变化图地下水取样位置为距离河岸6.5 m处。

Fig.4 Vertical variation diagram of hydrochemical index in nearshore zone (The sampling location of groundwater is 6.5 m away from the riverbank)

图5 研究区典型矿物扫描电镜照片

Fig.5 Scanning electron microscope images of typical minerals in the study area

图6 介质中总砷含量

Fig.6 Total arsenic content in the medium

图7 序列提取试验各步提取态砷含量百分比

Fig.7 The percentage of arsenic content in sequence extraction test

图8 介质中有效态砷含量和F1-As/EFC-As、F3-As/EFC-As、F4-As/EFC-As、As/TAs比值

Fig.8 Effective arsenic content and F1-As/EFC-As, F3-As/EFC-As, F4-As/EFC-As, As/TAs percentages in the medium

图9 介质中F1-Fe/EFC-Fe、F3-Fe/EFC-Fe、As/TAs、Fe2+/TFe比值

Fig.9 F1-Fe/EFC-Fe, F3-Fe/EFC-Fe, As/Tas, Fe2+/TFe percentages in the medium

图10 地下水中As浓度与pH值、Eh值关系图

Fig.10 Relationship between arsenic concentration and pH, Eh in groundwater

图11 地下水中As浓度与DOC、δ13CDIC-δ13CDOC关系图

Fig.11 Relationship of As-DOC, δ13CDIC-δ13CDOC in groundwater

图12 地下水中As浓度与 HCO 3 -浓度关系图

Fig.12 Relationship between arsenic content and HCO 3 - concentration in groundwater

图13 地下水中As浓度与Fe、Mn浓度关系图

Fig.13 Relationship between arsenic concentration and Fe, Mn concentration in groundwater

图14 地下水中 As-SO 4 2 -、δ34 S-SO 4 2 -关系图

Fig.14 Relationship of As-SO 4 2 -, δ34 S- SO 4 2 - in groundwater

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河水入渗过程中近岸带地下水中砷的形成与影响因素研究

Sources and influencing factors of arsenic in nearshore zone during river water infiltration

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