江汉平原浅层含砷地下水稀土元素特征及其指示意义

郑天亮; 邓娅敏; 鲁宗杰; 甘义群

doi:10.3799/dqkx.2017.057

江汉平原浅层含砷地下水稀土元素特征及其指示意义

doi: 10.3799/dqkx.2017.057

1.
中国地质大学地质调查研究院，湖北武汉 430074
2.
中国地质大学环境学院，湖北武汉 430074

基金项目:

国家自然科学基金面上项目 No.41572226

中国地质调查局项目 No.12120114069301

中央高校基本科研业务费专项基金“摇篮计划”项目 No.CUGL140412

详细信息

作者简介:
郑天亮(1990-)，男，博士研究生，主要从事地下水污染与防治、地质微生物学等方面的研究.ORCID:0000-0001-7853-6719.E-mail: tinyshiny@126.com

通讯作者:
邓娅敏，ORCID:0000-0002-4815-7176.E-mail: yamin.deng@cug.edu.cn

中图分类号: P592
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出版历程
- 收稿日期: 2017-01-10
- 刊出日期: 2017-05-15

Geochemistry and Implications of Rare Earth Elements in Arsenic-Affected Shallow Aquifer from Jianghan Plain, Central China

1.
Geological Survey, China University of Geosciences, Wuhan 430074, China
2.
School of Environmental Studies, China University of Geosciences, Wuhan 430074, China

摘要

摘要: 江汉平原被确认为我国南方新的饮水型砷中毒病区，目前对于江汉平原高砷地下水的成因机理研究还有待完善.综合运用水文地球化学分析与PHREEQC地球化学模拟计算，分析了地下水和沉积物中REE分异特征及其沿地下水流向形态变化规律.江汉平原地下水REE含量为0.032~0.843 μg/L，富集LREE，具显著Eu正异常，且地下水中Eu异常与As含量呈正相关关系.地下水中REE形态主要以LnCO₃⁺及Ln(CO₃)₂^-为主，沿地下水流向LnCO₃⁺降低、Ln(CO₃)₂^2-升高.地下水REE浓度分布受到HCO₃^-的络合作用及Fe氧化物矿物的还原性解吸附过程控制，径流途径中继承沉积物矿物的REE配分模式及Fe氧化物矿物对LREE的优先解吸附可能是地下水富集LREE的原因，并且沿流向上REE形态分布受到pH控制.研究区中Eu含量及Eu正异常对地下水As富集程度具有一定的指示意义.
- 砷 /
- 地下水 /
- 稀土元素形态 /
- Eu异常 /
- 稀土配分模式 /
- 江汉平原 /
- 水文地质
Abstract: Jianghan plain has been determined as a new endemic arsenic-poisoning area in the southern China. In order to understand the role of rare earth elements (REE)on arsenic mobilization in groundwater from the Jianghan plain, REE concentrations were measured in 114 groundwater samples and 9 sediment samples from the shallow arsenic-affected aquifer system and the REE speciations along the groundwater flow path were caculated by the hydrogeochemical PHREEQC simulation. The results indicate that the REE concentrations range from 0.032 to 0.843 μg/L. The groundwater exhibite the enrichment of LREE and dramatically positive Eu anomalies, and the Eu anomalies are positively correlated with As concentration. The REE speciation mainly existes as LnCO₃⁺ and Ln(CO₃)₂^-, meanwhile the LnCO₃⁺ concentrations decrease and Ln(CO₃)₂^2- concentrations increased along the regional groundwater flow path. The distribution of REE concentrations was mainly affected by the complexation with HCO₃^- and the reductive dissolution of iron oxide minerals. The enrichment of LREE in the groundwater was affected by the REE distribution patterns of minerals in the aquifer and the preferential desorption with LREE of iron oxide minerals, and the REE speciation was controlled by the pH along the groundwater flow path. The Eu concentrations and positive Eu anomalies could indicate the enrichment of arsenic in the groundwater.
- arsenic /
- groundwater /
- REE speciation /
- Eu anomaly /
- REE distribution pattern /
- Jianghan plain /
- hydrogeology

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图 1 研究区位置以及地下水采样点As浓度分布

Fig. 1. Sampling sites and the distribution of As concentration in groundwater from Jianghan plain

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图 2 研究区地下水Piper三线图

Fig. 2. Piper diagram of groundwater in Jianghan plain

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图 3 地下水中REE与主要水化学参数之间的关系

Fig. 3. Relationship between REE and pH, As, Fe, HCO₃^-, SO₄^2-, Cl^- in groundwater from Jianghan plain

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图 4 沿地下水流向REE形态(以Nd，Gd和Er为例)及REE与HCO₃^-络合作用的变化规律

Fig. 4. Comparison of REE speciation(Nd, Gd and Er) and complexation with HCO₃^- along the flow path

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图 5 Eu异常的控制因素以及与As含量的变化规律

Fig. 5. Controlling factors of Eu anomalies and the relationship between Eu anomalies and As

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图 6 Ce异常的控制因素以及与As含量的变化规律

Fig. 6. Controlling factors of Ce anomalies and the relationship between Ce anomalies and As

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图 7 江汉平原高砷钻孔沉积物与地下水中稀土配分模式的对比

Fig. 7. Comparison of NASC-normalized REE patterns between the groundwater and the sediments in high-arsenic area from Jianghan plain

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图 8 中国典型高砷区含砷地下水中稀土元素特征的对比

Fig. 8. Comparison of different groundwater REE characteristics in Datong basin, Hetao basin and Jianghan plain

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表 1 江汉平原高砷地下水水化学及微量元素含量特征

Table 1. Water chemistry and concentrations of trace elements of high arsenic groundwater from Jianghan plain

采样点编号	经度	纬度	pH	Cl^- (mg/L)	SO₄^2- (mg/L)	As^Total (μg/L)	Fe (mg/L)	Mn (mg/L)	NO₃^- (mg/L)	U (μg/L)	HCO₃^- (mg/L)
JH001	113°40′39.37″	30°09′24.70″	7.15	6.15	0.00	1.00	0.80	1.55	2.51	4.034	592
JH002	113° 40′40.76″	30°09′24.39″	7.12	4.38	0.03	155	5.76	2.28	2.43	0.028	581
JH003	113° 40′41.41″	30°09′24.01″	7.09	4.28	0.09	108	5.68	2.45	2.29	0.006	567
JH004	113° 40′38.41″	30°09′24.13″	7.13	3.59	0.00	532	9.65	4.60	2.55	0.004	543
JH005	113° 40′40.22″	30°09′23.80″	7.22	4.13	0.00	18.6	0.02	2.35	2.56	1.177	597
JH006	113° 40′36.39″	30°09′24.24″	7.03	3.58	0.11	64.2	7.41	0.83	2.33	0.006	510
JH007	113° 40′37.66″	30°09′24.21″	7.05	3.69	0.02	75.1	9.16	1.25	2.43	0.003	509
JH012	113° 40′53.73″	30°08′40.38″	7.07	3.69	0.11	54.1	7.64	1.06	2.44	0.001	516
JH014	113° 41′07.89″	30°08′20.89″	7.11	0.46	0.14	6.40	3.96	0.31	2.30	0.008	472
JH016	113° 39′17.79″	30°08′17.84″	6.91	7.66	0.09	83.8	9.04	0.69	2.59	0.003	563
JH018	113°36′40.87″	30°10′51.08″	7.03	3.16	0.04	632	11.76	2.32	0.03	0.003	675
JH021	113°37′26.65″	30°10′25.08″	6.97	5.52	0.00	110	4.57	2.00	0.16	0.005	631
JH024	113°36′25.87″	30°23′19.85″	6.56	40.7	57.8	1.10	ND	2.56	7.71	4.654	415
JH031	113°24′45.79″	30°10′49.19″	6.77	9.73	2.45	44.8	9.01	0.24	0.03	0.005	435
JH038	113°29′38.80″	30°04′02.70″	7.48	4.80	0.06	2320	1.34	1.54	6.83	0.006	553
JH044	113°29′38.45″	30°04′00.60″	7.51	1.20	0.05	1510	4.82	0.91	4.05	0.002	439
JH045	113°29′41.40″	30°04′00.58″	7.06	1.16	0.02	323	0.75	1.47	0.08	0.005	517
JH047	113°29′50.84″	30°03′58.42″	7.24	1.60	0.08	24.9	3.31	1.19	0.22	0.004	462
JH051	113°30′28.89″	30°03′33.40″	7.25	0.97	0.06	8.43	1.81	0.12	0.20	0.002	486
JH056	113°22′28.04″	30°11′17.01″	6.87	7.70	0.07	51.3	12.95	0.12	0.26	0.006	469
JH057	113°45′35.10″	30°07′05.95″	7.15	4.94	0.09	387	1.08	0.35	0.13	0.004	532
JH058	113°45′33.65″	30°07′06.40″	7.27	6.25	0.08	188	2.39	0.07	0.08	0.007	530
JH061	113°45′29.86″	30°07′04.41″	7.25	0.48	0.05	111	3.40	0.08	0.02	0.012	530
JH067	113°45′33.67″	30°07′02.92″	7.33	4.45	0.06	95.8	3.96	0.08	0.10	0.005	531
JH068	113°45′33.00″	30°07′02.42″	7.33	4.90	0.07	122	4.17	0.10	0.18	0.009	519
JH072	113°27′05.38″	30°04′46.52″	6.95	71.7	0.02	9.80	8.46	0.30	0.24	0.002	521
JH076	113°50′08.88″	30°03′43.47″	7.24	1.45	0.03	180	2.45	0.09	0.22	0.002	613
JH080	113°47′14.32″	30°07′47.75″	7.34	10.9	0.11	47.5	1.85	0.08	0.39	0.002	552
JH088	112°51′47.54″	30°28′8.42″	6.70	39.3	101	8.55	0.64	0.80	0.06	4.920	769
JH089	112°57′10.89″	30°25′18.19″	6.64	70.8	34.2	0.57	0.34	0.47	0.01	0.851	799
JH091	112°45′14″	30°30′44.3″	6.75	6.29	2.45	22.1	12.3	0.18	0.07	0.096	783
JH111	113°36′38.39″	30°10′50.71″	6.99	4.51	0.04	21.6	3.09	2.68	0.03	0.012	638
JH113	113°37′26.65″	30°10′25.08″	6.97	5.52	0.00	1.28	6.87	8.45	0.09	5.795	631
JH114	113°39′10.18″	30°10′11.83″	7.11	3.95	0.07	71.6	12.4	11.39	0.01	0.149	511
注：“ND”表示not detected，即未测出结果.

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表 2 江汉平原高砷地下水稀土元素含量(μg/L)特征

Table 2. Concentrations of REEs (μg/L) in high arsenic groundwater from Jianghan plain

采样点编号	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	∑REE	[La/Yb]_N	[Er/Nd]_N	Eu/Eu^*	Ce/Ce^*
JH001	0.033 6	0.072 8	0.007 2	0.023 2	0.008 9	0.007 7	0.005 9	0.001 3	0.008 9	0.001 7	0.014 1	0.001 2	0.007 5	0.001 9	0.195 9	3.04	0.61	3.24	1.10
JH002	0.016 2	0.033 8	0.003 2	0.011 2	0.001 8	0.024 6	0.002 9	0.000 7	0.002 5	0.000 6	0.003 6	0.000 2	0.002 1	0.000 4	0.103 8	5.19	0.32	33.21	1.09
JH003	0.008 4	0.010 6	0.000 7	0.003 4	0.003 3	0.022 0	0.000 9	0.000 4	0.000 9	0.000 4	0.001 7	0.000 3	0.001 5	0.000 2	0.054 7	3.84	0.49	39.07	1.01
JH004	0.005 8	0.007 9	0.001 5	0.003 9	0.001 8	0.017 9	0.000 5	0.000 3	0.002 0	0.000 4	0.001 1	0.000 1	0.001 6	0.000 4	0.045 2	2.37	0.29	56.81	0.63
JH005	0.010 4	0.018 0	0.001 7	0.009 5	0.005 3	0.005 9	0.003 8	0.000 5	0.003 4	0.000 6	0.002 1	0.0004	0.0021	0.000 5	0.064 2	3.36	0.22	4.02	1.02
JH006	0.014 5	0.023 4	0.002 4	0.009 3	0.010 1	0.018 4	0.003 3	0.000 7	0.001 9	0.001 0	0.001 9	0.001 1	0.003 1	0.000 3	0.091 4	3.17	0.20	9.65	0.93
JH007	0.004 9	0.008 8	0.000 4	0.000 7	0.001 8	0.014 0	0.000 5	0.000 2	0.000 5	0.000 2	0.001 1	0.000 4	0.002 1	0.000 1	0.035 7	1.59	1.46	46.27	1.49
JH012	0.005 8	0.010 0	0.000 6	0.001 5	0.001 8	0.019 1	0.001 0	0.000 4	0.001 0	0.000 1	0.000 7	0.000 2	0.000 5	0.000 2	0.042 9	7.54	0.48	44.94	1.21
JH014	0.007 3	0.017 0	0.001 2	0.002 3	0.001 8	0.010 4	0.001 5	0.000 3	0.002 0	0.000 7	0.000 4	0.000 2	0.001 6	0.000 2	0.046 9	3.09	0.16	19.49	1.36
JH016	0.187 6	0.336 6	0.032 2	0.135 8	0.032 5	0.019 8	0.030 9	0.005 0	0.026 3	0.005 7	0.011 3	0.003 3	0.013 6	0.002 0	0.842 6	13.05	0.08	24.41	1.33
JH018	0.014 5	0.031 3	0.001 6	0.012 9	0.001 0	0.034 4	0.002 2	0.000 1	0.001 1	0.001 1	0.001 6	0.000 3	0.001 2	0.000 6	0.103 9	8.27	0.13	69.88	1.50
JH021	0.026 3	0.063 9	0.005 8	0.016 7	0.005 8	0.017 6	0.005 1	0.000 9	0.007 0	0.001 2	0.002 8	0.000 6	0.003 4	0.000 3	0.157 4	5.18	0.17	9.93	1.21
JH024	0.075 7	0.106 8	0.019 6	0.060 7	0.018 4	0.010 4	0.014 4	0.001 9	0.008 4	0.003 2	0.011 2	0.001 6	0.009 0	0.000 8	0.342 1	5.68	0.18	1.96	0.65
JH031	0.009 5	0.029 1	0.001 9	0.006 6	0.001 3	0.013 9	0.002 8	0.000 3	0.001 4	0.000 9	0.004 7	0.000 4	0.002 3	0.000 2	0.075 3	2.85	0.71	22.30	1.61
JH038	0.014 6	0.021 1	0.001 1	0.004 9	0.002 9	0.072 5	0.001 6	0.000 5	0.000 8	0.000 2	0.003 5	0.000 2	0.000 2	0.000 4	0.124 5	49.17	0.70	103.52	1.26
JH044	0.007 7	0.009 6	0.001 0	0.007 7	0.005 8	0.057 6	0.000 5	0.000 4	0.000 6	0.000 9	0.002 7	0.000 3	0.001 3	0.000 5	0.096 6	3.88	0.35	103.40	0.79
JH045	0.006 0	0.020 3	0.002 0	0.007 9	0.004 8	0.016 6	0.002 5	0.000 5	0.001 3	0.000 2	0.000 2	0.000 5	0.000 7	0.000 2	0.063 7	5.79	0.07	14.46	1.54
JH047	0.002 9	0.007 7	0.001 0	0.002 9	0.004 6	0.018 0	0.002 4	0.000 4	0.001 3	0.000 5	0.003 2	0.000 1	0.002 0	0.000 5	0.047 3	0.96	3.17	16.48	1.49
JH051	0.005 0	0.020 9	0.001 0	0.005 1	0.006 0	0.013 9	0.004 6	0.000 3	0.005 3	0.000 8	0.002 3	0.000 6	0.002 1	0.000 6	0.068 6	1.63	1.31	8.13	1.82
JH056	0.006 6	0.011 5	0.001 7	0.002 1	0.001 2	0.023 0	0.002 7	0.000 5	0.001 4	0.000 5	0.001 0	0.000 6	0.002 8	0.000 3	0.055 8	1.56	1.33	38.57	0.81
JH057	0.007 9	0.029 9	0.002 7	0.011 3	0.003 7	0.005 9	0.004 6	0.000 5	0.004 0	0.001 0	0.000 5	0.001 1	0.002 8	0.001 5	0.077 3	1.90	0.12	4.38	1.51
JH058	0.005 5	0.020 7	0.001 5	0.006 3	0.002 5	0.008 6	0.000 7	0.000 4	0.002 7	0.001 3	0.001 5	0.000 6	0.005 0	0.000 8	0.058 1	0.75	0.23	20.21	1.69
JH061	0.003 8	0.013 7	0.001 3	0.008 5	0.002 6	0.008 2	0.004 0	0.000 5	0.001 4	0.001 2	0.002 9	0.000 8	0.000 7	0.001 5	0.051 3	3.49	0.99	7.77	1.43
JH067	0.007 1	0.013 7	0.001 4	0.010 9	0.002 6	0.014 2	0.006 3	0.000 8	0.002 1	0.000 7	0.001 0	0.000 6	0.0008	0.000 7	0.062 9	6.36	0.09	10.74	1.04
JH068	0.004 2	0.015 4	0.001 4	0.008 9	0.005 3	0.009 6	0.003 6	0.000 8	0.004 3	0.000 3	0.000 5	0.000 5	0.0031	0.000 7	0.058 6	0.91	0.06	6.79	1.50
JH072	0.007 4	0.018 6	0.002 3	0.005 8	0.006 9	0.020 7	0.002 2	0.000 5	0.001 5	0.000 4	0.001 1	0.000 5	0.0040	0.001 3	0.073 2	1.24	0.18	16.10	1.06
JH076	0.003 8	0.010 9	0.000 7	0.012 3	0.005 9	0.024 6	0.002 3	0.000 9	0.001 6	0.000 4	0.003 9	0.000 6	0.0042	0.000 4	0.072 5	0.62	0.32	20.53	1.61
JH080	0.006 2	0.011 2	0.001 6	0.011 3	0.003 0	0.006 5	0.001 6	0.000 9	0.003 3	0.000 6	0.003 4	0.001 1	0.004 3	0.000 6	0.055 6	0.97	0.31	9.17	0.84
JH088	0.036 7	0.073 1	0.010 3	0.040 3	0.011 9	0.010 5	0.008 0	0.001 6	0.008 0	0.002 2	0.006 4	0.001 1	0.006 8	0.001 5	0.2183	3.67	0.45	3.29	0.88
JH089	0.029 8	0.060 9	0.005 6	0.029 9	0.008 7	0.006 1	0.007 2	0.001 5	0.007 5	0.002 1	0.003 3	0.001 0	0.004 7	0.001 0	0.169 2	4.30	0.32	2.35	1.11
JH091	0.183 5	0.315 3	0.033 0	0.128 1	0.030 5	0.018 3	0.024 0	0.003 8	0.022 7	0.004 4	0.014 1	0.002 6	0.013 5	0.002 2	0.796 0	9.15	0.31	2.07	0.95
JH111	0.026 5	0.054 1	0.005 9	0.026 1	0.008 3	0.010 7	0.005 4	0.001 5	0.005 1	0.001 2	0.005 3	0.001 1	0.004 1	0.001 2	0.1566	4.36	0.58	4.88	1.01
JH113	0.028 5	0.050 3	0.006 5	0.029 8	0.011 8	0.010 1	0.006 9	0.001 4	0.006 6	0.001 9	0.004 4	0.001 7	0.003 6	0.001 2	0.164 7	5.40	0.42	3.41	0.87
JH114	0.048 4	0.089 8	0.009 3	0.038 0	0.015 6	0.013 5	0.010 2	0.001 6	0.011 6	0.002 1	0.007 9	0.001 4	0.006 4	0.000 9	0.256 8	5.09	0.59	3.28	0.99
注：下标N表示北美页岩标准化值：(La/Yb)_N=(La_N/Yb_N)；Eu/Eu^=Eu_NASC/([Sm]_NASC^[Gd]_NASC)^0.5；(Ce/Ce^)_NASC=Ce_NASC/([La]_NASC^[Pr]_NASC)^0.5.

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表 3 江汉平原典型高砷钻孔沉积物岩性、砷及稀土元素含量特征

Table 3. Lithology, arsenic and REEs contents in high arsenic sediments from borehole SY03 in Jianghan plain

样品编号	深度(m)	岩性	As (mg/kg)	Fe₂O₃ (%)	稀土元素含量(mg/kg)
样品编号	深度(m)	岩性	As (mg/kg)	Fe₂O₃ (%)	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu
SY03-01	1.5	淤泥质粘土	12.2	7.03	46.48	87.93	11.08	40.64	8.14	1.67	7.53	1.31	7.58	1.50	4.22	0.70	4.40	0.59
SY03-02	2.5	粘土	19.2	8.75	44.16	84.81	10.36	37.38	7.29	1.59	6.41	1.04	5.90	1.19	3.17	0.52	3.19	0.46
SY03-03	7.1	粘质粉土	11.3	6.67	42.63	82.51	10.07	36.40	7.07	1.47	6.27	1.18	6.23	1.24	3.45	0.55	3.33	0.48
SY03-04	17.9	粘土	20.0	7.91	46.00	88.52	10.94	39.47	7.86	1.63	6.89	1.18	6.91	1.39	3.82	0.63	3.88	0.54
SY03-05	18.7	粉砂	88.2	6.16	41.33	79.26	9.82	35.59	7.03	1.47	6.31	1.06	6.08	1.21	3.37	0.53	3.19	0.44
SY03-06	20.1	细砂	107.5	5.08	35.68	67.92	8.49	30.87	5.89	1.28	5.27	0.87	4.94	1.00	2.74	0.43	2.50	0.35
SY03-07	23.3	中-粗砂	24.2	5.42	31.39	59.81	7.40	26.72	5.14	1.17	4.41	0.73	3.96	0.80	2.17	0.35	2.03	0.28
SY03-08	30.9	中-细砂	25.6	4.44	26.94	50.56	6.17	22.86	4.47	1.03	3.84	0.62	3.43	0.67	1.81	0.29	1.65	0.23
SY03-09	43.5	粘土	15.5	7.72	36.02	68.23	8.34	30.32	5.90	1.25	5.18	0.85	4.92	0.98	2.72	0.44	2.61	0.39

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江汉平原浅层含砷地下水稀土元素特征及其指示意义

doi: 10.3799/dqkx.2017.057

作者简介:
郑天亮(1990-)，男，博士研究生，主要从事地下水污染与防治、地质微生物学等方面的研究.ORCID:0000-0001-7853-6719.E-mail: tinyshiny@126.com

通讯作者:
邓娅敏，ORCID:0000-0002-4815-7176.E-mail: yamin.deng@cug.edu.cn

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Geochemistry and Implications of Rare Earth Elements in Arsenic-Affected Shallow Aquifer from Jianghan Plain, Central China

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留言板

江汉平原浅层含砷地下水稀土元素特征及其指示意义

doi: 10.3799/dqkx.2017.057

作者简介: 郑天亮(1990-)，男，博士研究生，主要从事地下水污染与防治、地质微生物学等方面的研究.ORCID:0000-0001-7853-6719.E-mail: tinyshiny@126.com

通讯作者: 邓娅敏，ORCID:0000-0002-4815-7176.E-mail: yamin.deng@cug.edu.cn

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Geochemistry and Implications of Rare Earth Elements in Arsenic-Affected Shallow Aquifer from Jianghan Plain, Central China

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作者简介:
郑天亮(1990-)，男，博士研究生，主要从事地下水污染与防治、地质微生物学等方面的研究.ORCID:0000-0001-7853-6719.E-mail: tinyshiny@126.com

通讯作者:
邓娅敏，ORCID:0000-0002-4815-7176.E-mail: yamin.deng@cug.edu.cn