S<sup>2-</sup>对河砂吸附砷的影响及其作用机理

杜海玲; 单慧媚; 陈辉; 彭三曦; 黄健

doi:10.19509/j.cnki.dzkq.2022.0123

S^2-对河砂吸附砷的影响及其作用机理

doi: 10.19509/j.cnki.dzkq.2022.0123

杜海玲^{a, b,},
单慧媚^{a, b, ,},
陈辉^{a, b},
彭三曦^c,
黄健^{a, b}

a.
桂林理工大学广西环境污染控制理论与技术重点实验室, 广西桂林 541004
b.
桂林理工大学岩溶地区水污染控制与用水安全保障协同创新中心, 广西桂林 541004
c.
桂林理工大学地球科学学院, 广西桂林 541004

基金项目:

国家自然科学基金项目 41877194

国家自然科学基金项目 41502232

广西自然科学基金项目 2017GXNSFAA198096

广西自然科学基金项目 2018AD19142

详细信息

作者简介:
杜海玲(1997-), 女, 现正攻读水利工程专业硕士学位, 主要从事地下水污染与防治研究。E-mail: 1102231518@qq.com

通讯作者:
单慧媚(1985-), 女, 副教授, 主要从事地下水污染与防治、水文地球化学方面的研究。E-mail: shanhuimei@glut.edu.cn

中图分类号: X141
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- 文章访问数: 397
- PDF下载量: 22
- 被引次数: 0
出版历程
- 收稿日期: 2021-04-27
- 网络出版日期: 2022-09-07

Effects of S^2- on arsenic adsorption to river sand and its mechanisms

Du Hailing^{a, b
,},
Shan Huimei^{a, b
, ,},
Chen Hui^{a, b},
Peng Sanxi^c,
Huang Jian^{a, b}

a.
Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin Guangxi 541004, China
b.
Collaborative Innovation Center for Water Pollution Control and Water Safety in Karst Area, Guilin University of Technology, Guilin Guangxi 541004, China
c.
College of Earth Science, Guilin University of Technology, Guilin Guangxi 541004, China

摘要

摘要:
水体中S^2-与砷(As)的迁移富集密切相关, 但不同含水介质中其作用机理尚不明确。为了查明潜流带中常见含水介质河砂在S^2-作用下对As的吸附特征, 设计并开展了As在河砂上的吸附动力学实验, 以及S^2-作用下河砂对As的吸附实验, 结合PHREEQC模拟计算, XRD、SEM-EDS、XPS和FTIR等表征测试技术, 进一步识别其作用机理。结果表明: 固液比为25 g/L情况下, 河砂对As的吸附在200 h左右达到吸附平衡, 且对As(Ⅴ)的吸附量明显高于As(Ⅲ); 随着S^2-浓度的增加, 河砂对As吸附能力逐渐减弱; 模拟及表征测试结果显示, 少量As被吸附在河砂表面, 主要与其表面的Fe、Al结合, 其中As(Ⅲ)的吸附可能还与Si-O键断裂后与S^2-结合形成的SiS₂有关。S^2-对河砂吸附As的主要影响机理为: ①S^2-的加入使得溶液pH值升高、Eh值降低, 从而抑制了As的吸附; ②添加S^2-条件下河砂表面的Fe、Al等能与S和As形成AlAs、AlAsO₄、FeS₂及Fe₄As₂O₁₁等化合物, 减少了河砂表面吸附As的活性位点。研究结果有助于丰富As-S作用机理, 以及As在地下水环境中迁移过程的认识。
- 硫 /
- 河砂 /
- 表征 /
- 影响机理
Abstract:
Sulfur (S^2-) is closely related to the migration and enrichment of arsenic (As) in the water environment, but its mechanism of action in different aqueous medium is still unclear. To determine the adsorption characteristics of As by river sand, a common aqueous medium in the hyporheic zone, under the action of S^2-, the adsorption kinetics experiment of As on river sand and the adsorption experiment of As by river sand under the action of S^2- are designed and carried out. Combined with simulation calculation by PHREEQC and characterization tests based on XRD, SEM-EDS, XPS and FTIR, the mechanism of action is further identified. The results show that the adsorption of As by river sand reaches adsorption equilibrium at approximately 200 h and the adsorption capacity of As(Ⅴ) is significantly higher than that of As(Ⅲ) at the solid-to-liquid ratio of 25 g/L; with increasing S^2- concentration, the adsorption capacity of river sand to As decreases gradually. The simulation and characterization test results show that a small amount of As is adsorbed on the surface of river sandandis mainly combined with Fe and Al on its surface. The adsorption of As (Ⅲ) may also be related to SiS₂ that is formed after the fracture of the Si-O bondwith S^2-. The main influence mechanism of S^2- on the adsorption of As by river sand is as follows: ① the addition of S^2- increases the pH of the solution and decreases Eh, thus inhibiting the adsorption of As; ②under the condition of adding S^2-, Fe and Al on the surface of river sand can form compounds such as AlAs, AlAsO₄, FeS₂ and Fe₄As₂O₁₁ with S and As, which reduces the active sites of As adsorption on the surface of river sand.
- sulfur /
- river sand /
- characterization /
- influence mechanism

HTML全文

图 1 河砂对As吸附量随时间的变化曲线

Figure 1. Changes in As adsorption capacity of the river sand with time

下载: 全尺寸图片幻灯片

图 2 不同S^2-浓度下反应平衡后溶液中As的浓度

Figure 2. Concentration of As in the solution after the reaction equilibrium at different S^2- concentrations

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图 3 反应前后溶液中ρ(S^2-)变化(其中Ⅰ、Ⅱ、Ⅲ和Ⅳ代表了ρ(S^2-)初始分别为0.1, 1.0, 5.0, 20.0 mg/L的实验组)

Figure 3. Changes in the S^2- concentration before and after the reaction (among them, Ⅰ, Ⅱ, Ⅲ and Ⅳ represent the experimental groups with S^2-initial concentrations of 0.1, 1.0, 5.0, 20.0 mg/L, respectively)

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图 4 河砂反应前后的SEM-EDS图

Figure 4. SEM-EDS diagram of river sand before and after the reaction

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图 5 反应前后各体系河砂XRD图谱

Figure 5. XRD patterns of river sand before and after the reaction

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图 6 河砂反应后As3d窄谱谱图

Figure 6. As3d narrow spectrum of river sand after the reaction

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图 7 河砂反应前后的FTIR图谱

Figure 7. FTIR spectra of river sand before and after the reaction

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表 1 河砂主要成分

Table 1. Main composition of river sand

成分	SiO₂	Al₂O₃	K₂O	Fe₂O₃	CaO	TiO₂	MgO	Na₂O	MnO
w_B/%	90.69	5.91	1.62	1.51	0.32	0.17	0.15	0.14	0.06

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表 2 不同ρ(S^2-)条件下反应前后溶液的pH和Eh对比

Table 2. Comparison of pH and Eh before and after the reaction at different S^2- concentrations

初始ρ(S^2-)/(mg·L^-1)		0.1	1.0	5.0	20.0
As(Ⅲ)	反应前pH	7.58	9.91	10.09	11.01
	反应后pH	6.77	7.23	6.96	9.64
	反应前Eh/mV	-256.40	-316.90	-338.90	-398.50
	反应后Eh/mV	223.90	174.00	115.60	-191.30
As(Ⅴ)	反应前pH	7.22	9.24	10.28	11.01
	反应后pH	6.57	7.15	7.38	9.76
	反应前Eh/mV	-283.40	-343.50	-375.10	-401.70
	反应后Eh/mV	243.93	46.93	47.6	-195.93

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表 3 PHREEQC模拟中选取部分矿物饱和指数结果

Table 3. Selected mineral saturation index results in the PHREEQC simulation

反应体系	ρ(S^2-)/(mg·L^-1)	As₂O₃	As₂O₅	As₂S₃	AsS	S
反应体系	ρ(S^2-)/(mg·L^-1)	饱和指数SI
S^2--As(Ⅲ)	0.1	-8.52	-44.05	-5.56	-1.62	-5.22
	1.0	-9.62	-45.73	-12.03	-3.81	-7.92
	5.0	-9.89	-46.7	-9.85	-3.56	-6.97
	20.0	-11.59	-48.26	-16.68	-25.12	-8.46
S^2--As(Ⅴ)	0.1	-8.74	-35.38	-59.22	-21.76	-18.58
	1.0	-9.03	-44.51	-8.87	-2.82	-6.13
	5.0	-10.24	-46.14	-12.81	-4.23	-7.25
	20.0	-11.60	-47.82	-16.71	-19.57	-8.25

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