地下水曝气-砂滤处理产生的废弃石英砂中铁砷含量与形态分布

doi:10.13745/j.esf.sf.2021.2.17

地学前缘 ›› 2021, Vol. 28 ›› Issue (5): 208-214.DOI: 10.13745/j.esf.sf.2021.2.17

地下水曝气-砂滤处理产生的废弃石英砂中铁砷含量与形态分布

张耀强¹(), 胡冰冰¹, 谢世伟², 袁松虎¹^,^*()

1.中国地质大学(武汉) 生物地质与环境地质国家重点实验室, 湖北武汉 430074
2.武汉科技大学城市建设学院, 湖北武汉 430065

收稿日期:2020-05-12 修回日期:2020-09-18 出版日期:2021-09-25 发布日期:2021-10-29
通信作者: 袁松虎
作者简介:张耀强(1996—),男,硕士研究生,主要从事地下水污染修复技术研究。E-mail: 383103273@qq.com
基金资助:
国家自然科学基金创新群体项目(41521001);湖北省自然科学基金创新群体项目(2018CFA028)

Content and speciation distributions of Fe and As in disposed quartz sand from groundwater treatment by sequential aeration and sand filtration

ZHANG Yaoqiang¹(), HU Bingbing¹, XIE Shiwei², YUAN Songhu¹^,^*()

1. State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences (Wuhan), Wuhan 430074, China
2. School of Urban Construction, Wuhan University of Science and Technology, Wuhan 430065, China

Received:2020-05-12 Revised:2020-09-18 Online:2021-09-25 Published:2021-10-29
Contact: YUAN Songhu

摘要/Abstract

摘要：

高铁高砷地下水严重威胁饮水质量,曝气-砂滤法因处理效果好且成本低在农村地区得到广泛应用。砂滤过程石英砂表面富集铁和砷后需定期更换,然而废弃石英砂堆置具有砷释放风险。本文以江汉平原某水厂砂滤池废弃石英砂为研究对象,采用激光剥蚀-等离子体质谱(LA-ICP-MS)、拉曼光谱(Raman)、X射线衍射(XRD)和分步化学提取等手段,研究了砂样中的Fe和As含量及形态分布。结果表明,砂粒表面形成了一层厚度为20100 μm的高铁砷薄层,薄层内部Fe和As含量显著高于两侧,Fe和As分布高度相关(R²=0.985)。砂样表面铁矿物以无定型/弱结晶型为主,同时检出赤铁矿和臭葱石等矿物。砂样中Fe和As总含量分别为20.1 mg/g和53.4 μg/g。砂样表面铁主要以易溶解态、碳酸盐结合态和易还原态为主,As主要吸附在铁矿物上。研究区降雨充沛,当废弃石英砂遭遇雨水冲刷或淹没时,可能导致铁砷薄层中As解吸或随Fe矿物还原溶解而释放。

关键词: 废弃石英砂, 高砷地下水, 砷释放, 砂滤, 饮用水处理

Abstract:

Drinking water security is threatened by elevated iron (Fe) and arsenic (As) concentrations in groundwater. Sequential aeration and sand filtration has been widely used for the high-performance, low-cost groundwater treatment in rural areas. During filtration, Fe, As-enriched quartz sand needs periodic replacement. The disposed sand frequently piles up on land, risking As release. In this research, the content and speciation distributions of Fe and As in disposed quartz sand collected from a drinking water treatment plant in the Jianghan plain, were investigated by LA-ICP-MS, Raman spectroscopy, X-ray diffraction and sequential chemical extraction. The results show that the sand surface was coated with a 20-100 μm thick Fe, As-rich layer, with Fe and As significantly concentrated in the central layer than on the outer layers; the As and Fe spatial distributions in the coating were highly correlated (R²> 0.985). The Fe phases were mainly amorphous and weakly crystalline, and the presence of hematite and scorodite was detected. The total contents of Fe and As in the quartz were 20.1 mg/g and 53.4 μg/g, respectively. The highly dissolvable Fe (oxy)hydroxides and carbonate-bound, reducible Fe species predominated in the coatings, whereas As was mainly adsorbed on the surface of Fe phases. Due to the abundant rainfall in the study area, As release from the disposed quartz sand could occur as a consequence of rain washing or anaerobic Fe bio-reduction.

Key words: disposed quartz sand, high-arsenic groundwater, arsenic release, sand filtration, drinking water treatment

中图分类号:

X523
P641.8

张耀强, 胡冰冰, 谢世伟, 袁松虎. 地下水曝气-砂滤处理产生的废弃石英砂中铁砷含量与形态分布[J]. 地学前缘, 2021, 28(5): 208-214.

ZHANG Yaoqiang, HU Bingbing, XIE Shiwei, YUAN Songhu. Content and speciation distributions of Fe and As in disposed quartz sand from groundwater treatment by sequential aeration and sand filtration[J]. Earth Science Frontiers, 2021, 28(5): 208-214.

图/表 5

表1 废弃石英砂分步化学提取过程

Table 1 Step-by-step chemical extraction procedure for the disposed quartz sand

步骤	提取条件	目标形态	测试结果		参考文献
步骤	提取条件	目标形态	Fe含量/(mg·g^-1)	As含量/(μg·g^-1)	参考文献
(1)氯化钙	1 mol·L^-1 CaCl₂, pH=7,24 h	离子交换态Fe和As	<0.0	0.5±0.0	Heron等^[18]
(2)醋酸钠	1 mol·L^-1 醋酸钠, pH=4.5,24 h	碳酸盐结合态Fe及易溶解态的铁(氢)氧化物,表面吸附态As及该形态对应的As	11.7±0.2	22.6±0.3	Poulton等^[19], Javed等^[20], Neumann等^[21]
(3)盐酸羟胺	1 mol·L^-1 HONH₂HCl, 48 h	易还原态Fe,包括水铁矿、纤铁矿等,与该铁形态共存的As	8.4±2.0	32.2±0.4	Poulton等^[19]

图1 砂样LA-ICP-MS线扫Fe和As含量分布(a)及Fe和As含量相关性(b)

Fig.1 Iron and As content distributions measured by LA-ICP-MS linear scan along the transect of sand grain (a) and correlation between Fe and As contents (b)

图2 砂样LA-ICP-MS分层面扫Fe和As信号值分布

Fig.2 Iron and As LA-ICP-MS signal intensity distributions in different transverse sections of sand grain

图3 砂样的拉曼光谱表征结果

Fig.3 Characteristic Raman spectra of sand grain sample

图4 Fe和As分步提取归一化结果

Fig.4 Normalized results of stepwise Fe and As extraction

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地下水曝气-砂滤处理产生的废弃石英砂中铁砷含量与形态分布

Content and speciation distributions of Fe and As in disposed quartz sand from groundwater treatment by sequential aeration and sand filtration

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