REE Concentration and Fractionation in Waters and Sediments from the Northern Branch of Ganjiang River, Poyang Lake Catchment

doi:10.19657/j.geoscience.1000-8527.2022.002

Abstract

Abstract:

The enhanced exploitation and widespread use of rare earth elements (REE) have led to increasing interest in REE distributions in environments and their geochemical behaviors. The Ganjiang River is one of the five major rivers in the Poyang Lake catchment, and is originated from the rare earth district in southern Ganzhou. However, the REE concentration and distribution in the downstream water bodies and surrounding groundwater are poorly understood. We investigated the REE geochemistry in waters and sediments of the northern branch of Ganjiang River. Results show that the total REE concentrations are of 230-1,146 ng/L (average 458.85 ng/L, surface water), 284-1,498 ng/L (average 634.94 ng/L, groundwater), and 177.9- 270.7 mg/kg (average 226.99 mg/kg, sediment). The PHREEQC simulation indicates that REEs are mainly in the form of carbonate complex (REEC0₃⁺) in the water samples. Both surface water and groundwater generally show enrichments of heavy REE (HREE) over light REE (LREE) and middle REE (MREE), while the sediments do not show significant enrichment features. The water samples are characterized by negative Ce and Eu anomalies, while the sediments show positive Ce but negative Eu anomalies, indicating that redox and water-rock reactions have influenced REE transformation in the water-sediment system. Along the flow path, REE concentrations tend to increase in groundwater, while both the degree of HREE enrichment and the REEC0₃⁺ proportion decreases. These behaviors reflect that REE concentrations are controlled by pH, colloidal sorption, complexation and surface water-groundwater interactions. The water HREE enrichment is likely attributed to carbonate complexation, and the negative Ce and Eu anomalies are related to the oxidative Ce precipitation and the parent rock REE inheritance. The positive Gd anomalies in the water samples from the middle and lower reaches of the river suggest anthropogenic REE input.

Key words: Ganjiang River, rare earth element, water-rock interaction, anthropogenic activity, anomalous enrichment, Poyang Lake

CLC Number:

P641.3

LIU Maohan, LIU Haiyan, ZHANG Weimin, WANG Zhen, WU Tonghang, WANG Yugang. REE Concentration and Fractionation in Waters and Sediments from the Northern Branch of Ganjiang River, Poyang Lake Catchment[J]. Geoscience, 2022, 36(02): 389-405.

Figures/Tables 19

Fig.1 Hydrogeological map of the study area and sampling sites distribution

Table 1 Reactions added to the WATEQ4F database (IS=0, T=25 ℃, REE denoting rare earth elements)

反应方程	平衡常数														参考文献
反应方程	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	参考文献
REE³⁺ + H₂O= REEOH²⁺ + H⁺	-8.81	-8.34	-8.32	-8.18	-7.84	-7.76	-7.83	-7.64	-7.59	-7.56	-7.52	-7.39	-7.24	-7.27	[27]
REE³⁺ + 2H₂O= REE(OH $) 2 +$ + 2H⁺	-18.14	-17.60	-17.27	-17.04	-16.51	-16.37	-16.37	-16.18	-16.10	-16.07	-15.96	-15.88	-15.74	-16.67	[28]
REE³⁺ + 3H₂O= REE(OH)₃ + 3H⁺	-27.90	-27.23	-26.63	-26.40	-25.91	-25.41	-2.28	-25.08	-24.83	-24.56	-24.35	-24.18	-23.85	-23.85	[28]
REE³⁺ + C $O 3 2 -$ = REEC $O 3 +$	7.12	7.40	7.57	7.69	7.81	8.00	7.97	8.08	8.14	8.18	8.24	8.32	8.40	8.43	[28]
REE³⁺ + 2C $O 3 2 -$ = REE(CO₃ $) 2 -$	11.30	11.76	12.08	12.17	12.53	12.63	12.48	12.78	12.91	13.00	13.12	13.27	13.30	13.37	[29]
REE³⁺ + S $O 4 2 -$ = REES $O 4 +$	3.62	3.59	3.62	3.64	3.66	3.66	3.66	3.64	3.61	3.59	3.59	3.59	3.59	3.59	[30]
REE³⁺ + F^-= REEF²⁺	3.12	3.28	3.48	3.56	3.58	3.63	3.75	3.85	3.89	3.95	3.98	3.99	4.02	4.05	[31]
REE³⁺ + Cl^-= REECl²⁺	0.74	0.68	0.71	0.71	0.67	0.69	0.71	0.67	0.70	0.71	0.70	0.71	0.69	0.67	[32]
REE³⁺ + 2Cl^-= REEC $l 2 +$	0.51	0.46	0.45	0.47	0.42	0.44	0.46	0.43	0.43	0.45	0.45	0.46	0.44	0.43	[32]
REE³⁺ + N $O 3 -$ = REE(NO₃)²⁺	0.58	0.69	0.69	0.79	0.78	0.83	0.47	0.51	0.15	0.25	0.15	0.20	0.25	0.56	[31]

Table 1 Reactions added to the WATEQ4F database (IS=0, T=25 ℃, REE denoting rare earth elements)

反应方程	平衡常数														参考文献
反应方程	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	参考文献
REE³⁺ + H₂O= REEOH²⁺ + H⁺	-8.81	-8.34	-8.32	-8.18	-7.84	-7.76	-7.83	-7.64	-7.59	-7.56	-7.52	-7.39	-7.24	-7.27	[27]
REE³⁺ + 2H₂O= REE(OH $) 2 +$ + 2H⁺	-18.14	-17.60	-17.27	-17.04	-16.51	-16.37	-16.37	-16.18	-16.10	-16.07	-15.96	-15.88	-15.74	-16.67	[28]
REE³⁺ + 3H₂O= REE(OH)₃ + 3H⁺	-27.90	-27.23	-26.63	-26.40	-25.91	-25.41	-2.28	-25.08	-24.83	-24.56	-24.35	-24.18	-23.85	-23.85	[28]
REE³⁺ + C $O 3 2 -$ = REEC $O 3 +$	7.12	7.40	7.57	7.69	7.81	8.00	7.97	8.08	8.14	8.18	8.24	8.32	8.40	8.43	[28]
REE³⁺ + 2C $O 3 2 -$ = REE(CO₃ $) 2 -$	11.30	11.76	12.08	12.17	12.53	12.63	12.48	12.78	12.91	13.00	13.12	13.27	13.30	13.37	[29]
REE³⁺ + S $O 4 2 -$ = REES $O 4 +$	3.62	3.59	3.62	3.64	3.66	3.66	3.66	3.64	3.61	3.59	3.59	3.59	3.59	3.59	[30]
REE³⁺ + F^-= REEF²⁺	3.12	3.28	3.48	3.56	3.58	3.63	3.75	3.85	3.89	3.95	3.98	3.99	4.02	4.05	[31]
REE³⁺ + Cl^-= REECl²⁺	0.74	0.68	0.71	0.71	0.67	0.69	0.71	0.67	0.70	0.71	0.70	0.71	0.69	0.67	[32]
REE³⁺ + 2Cl^-= REEC $l 2 +$	0.51	0.46	0.45	0.47	0.42	0.44	0.46	0.43	0.43	0.45	0.45	0.46	0.44	0.43	[32]
REE³⁺ + N $O 3 -$ = REE(NO₃)²⁺	0.58	0.69	0.69	0.79	0.78	0.83	0.47	0.51	0.15	0.25	0.15	0.20	0.25	0.56	[31]

Table 2 Chemical compositions of surface water samples from the study area

区域	统计量	pH	TDS	Cl^-	S $O 4 2 -$	N $O 3 -$	HC $O 3 -$	Ca²⁺	K⁺	Mg²⁺	Na⁺
上游	最大值	7.39	113.00	21.10	16.94	4.64	67.96	18.61	10.09	3.22	11.63
	最小值	6.94	87.95	15.75	7.31	1.14	54.37	17.51	3.51	3.08	9.50
	平均值	7.23	95.98	18.28	11.33	2.07	62.53	17.84	6.93	3.12	10.16
	标准差	0.18	9.77	2.23	4.24	1.50	7.44	0.45	2.76	0.06	0.86
	变异系数	0.02	0.10	0.12	0.37	0.73	0.12	0.03	0.40	0.02	0.08
中游	最大值	7.81	92.15	21.48	18.28	5.79	67.96	19.47	5.16	3.51	11.07
	最小值	7.34	88.45	11.19	6.94	1.17	40.78	17.65	3.26	3.12	10.09
	平均值	7.50	90.24	17.38	14.87	3.87	54.37	18.50	3.86	3.29	10.64
	标准差	0.21	1.73	4.63	5.35	1.96	11.10	0.78	0.89	0.19	0.50
	变异系数	0.03	0.02	0.27	0.36	0.51	0.20	0.04	0.23	0.06	0.05
下游	最大值	7.33	89.00	18.41	16.46	4.49	67.96	17.70	5.59	3.15	11.25
	最小值	7.19	86.95	12.93	7.15	1.17	54.37	16.95	3.25	3.09	10.13
	平均值	7.26	88.00	16.48	13.14	3.26	57.77	17.28	4.49	3.13	10.60
	标准差	0.06	0.84	2.47	4.38	1.52	6.80	0.31	1.22	0.02	0.48
	变异系数	0.01	0.01	0.15	0.33	0.47	0.12	0.02	0.27	0.01	0.05

Table 2 Chemical compositions of surface water samples from the study area

区域	统计量	pH	TDS	Cl^-	S $O 4 2 -$	N $O 3 -$	HC $O 3 -$	Ca²⁺	K⁺	Mg²⁺	Na⁺
上游	最大值	7.39	113.00	21.10	16.94	4.64	67.96	18.61	10.09	3.22	11.63
	最小值	6.94	87.95	15.75	7.31	1.14	54.37	17.51	3.51	3.08	9.50
	平均值	7.23	95.98	18.28	11.33	2.07	62.53	17.84	6.93	3.12	10.16
	标准差	0.18	9.77	2.23	4.24	1.50	7.44	0.45	2.76	0.06	0.86
	变异系数	0.02	0.10	0.12	0.37	0.73	0.12	0.03	0.40	0.02	0.08
中游	最大值	7.81	92.15	21.48	18.28	5.79	67.96	19.47	5.16	3.51	11.07
	最小值	7.34	88.45	11.19	6.94	1.17	40.78	17.65	3.26	3.12	10.09
	平均值	7.50	90.24	17.38	14.87	3.87	54.37	18.50	3.86	3.29	10.64
	标准差	0.21	1.73	4.63	5.35	1.96	11.10	0.78	0.89	0.19	0.50
	变异系数	0.03	0.02	0.27	0.36	0.51	0.20	0.04	0.23	0.06	0.05
下游	最大值	7.33	89.00	18.41	16.46	4.49	67.96	17.70	5.59	3.15	11.25
	最小值	7.19	86.95	12.93	7.15	1.17	54.37	16.95	3.25	3.09	10.13
	平均值	7.26	88.00	16.48	13.14	3.26	57.77	17.28	4.49	3.13	10.60
	标准差	0.06	0.84	2.47	4.38	1.52	6.80	0.31	1.22	0.02	0.48
	变异系数	0.01	0.01	0.15	0.33	0.47	0.12	0.02	0.27	0.01	0.05

Fig.2 Piper plot of water samples in the study area

Table 3 Chemical compositions of groundwater samples from the study area

区域	统计量	pH	TDS	Cl^-	S $O 4 2 -$	N $O 3 -$	HC $O 3 -$	Ca²⁺	K⁺	Mg²⁺	Na⁺
中游	最大值	6.94	264.00	31.16	87.25	70.90	135.93	44.49	46.72	12.54	33.06
	最小值	6.04	57.05	9.61	4.12	0.95	40.78	9.53	1.90	2.55	4.26
	平均值	6.58	156.69	21.02	24.30	17.34	85.44	26.23	12.57	8.04	15.89
	标准差	0.33	72.70	8.95	29.94	25.66	33.03	14.27	15.48	3.51	10.49
	变异系数	0.05	0.46	0.43	1.23	1.48	0.39	0.54	1.23	0.44	0.66
下游	最大值	7.57	263.50	74.63	50.09	88.31	108.74	57.01	17.39	25.82	45.64
	最小值	5.84	84.50	16.85	0.90	5.98	13.59	10.09	2.00	5.07	12.04
	平均值	6.37	179.79	43.91	22.99	52.42	55.88	30.44	5.93	12.18	23.26
	标准差	0.57	62.96	19.92	19.13	28.55	30.73	15.84	5.01	6.86	9.42
	变异系数	0.09	0.35	0.45	0.83	0.54	0.55	0.52	0.85	0.56	0.40

Table 3 Chemical compositions of groundwater samples from the study area

区域	统计量	pH	TDS	Cl^-	S $O 4 2 -$	N $O 3 -$	HC $O 3 -$	Ca²⁺	K⁺	Mg²⁺	Na⁺
中游	最大值	6.94	264.00	31.16	87.25	70.90	135.93	44.49	46.72	12.54	33.06
	最小值	6.04	57.05	9.61	4.12	0.95	40.78	9.53	1.90	2.55	4.26
	平均值	6.58	156.69	21.02	24.30	17.34	85.44	26.23	12.57	8.04	15.89
	标准差	0.33	72.70	8.95	29.94	25.66	33.03	14.27	15.48	3.51	10.49
	变异系数	0.05	0.46	0.43	1.23	1.48	0.39	0.54	1.23	0.44	0.66
下游	最大值	7.57	263.50	74.63	50.09	88.31	108.74	57.01	17.39	25.82	45.64
	最小值	5.84	84.50	16.85	0.90	5.98	13.59	10.09	2.00	5.07	12.04
	平均值	6.37	179.79	43.91	22.99	52.42	55.88	30.44	5.93	12.18	23.26
	标准差	0.57	62.96	19.92	19.13	28.55	30.73	15.84	5.01	6.86	9.42
	变异系数	0.09	0.35	0.45	0.83	0.54	0.55	0.52	0.85	0.56	0.40

Table 4 REE contents of surface water in the study area (ng/L)

区域	统计量	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	REE
上游	最大值	129	172	33	149	64	15	75	16	99	20	66	7	65	9	896
	最小值	63	83	13	53	17	4	14	3	21	4	16	1	18	2	338
	平均值	87.8	116.8	19.8	90.2	28.4	6.5	30.2	6.4	42	8.8	30	2.4	32.8	4	511.6
中游	最大值	58	84	13	53	22	4	25	2	19	5	17	1	23	3	336
	最小值	41	67	7	35	11	2	9	1	10	1	9	1	9	1	230
	平均值	49.75	75.75	9.5	44.75	14.75	2.4	14.5	1.25	15	3	13	1	15.25	2	271.75
下游	最大值	159	187	45	207	92	21	103	20	134	23	73	9	71	11	1 146
	最小值	67	109	15	52	16	2	18	1	23	5	19	1	16	2	360
	平均值	94.75	129	23	98.25	36.25	7.75	42.25	7	52.25	10.25	33	3.25	33.5	5	580

Table 5 REE contents of some major rivers in China and surface water in the study area (ng/L)

河流名称	La	Ce	Nd	Sm	Eu	Tb	Yb	Lu	REE	参考文献
长江河源区背景值	130	150	390	5	3	-	30	4	712	[33]
长江干流中下游	35	169	20	16	7	10	7	4	268	[34-36]
长江水系背景值	50	110	70	13	4	-	8	2	257	[33]
珠江广州河段	35	75	50	37	15	10	23	5	250	[37]
松花江水系	200	160	410	30	7	10	20	4	841	[37]
赣江上游均值	113	94	81	12	10	2	7	1	320	[23]
中国水体	60	120	60	10	5	3	8	2	268	[36]
赣江北支上游	88	117	90	28	12	6	33	4	378	本研究
赣江北支中游	50	76	45	15	12	1	15	2	216	本研究
赣江北支下游	95	129	98	36	12	7	34	5	416	本研究
赣江北支均值	78	108	79	27	12	5	28	4	340	本研究

Table 6 REE contents of groundwater in the study area (ng/L)

区域	统计量	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	REE
中游	最大值	174	281	53	252	50	8	46	4	33	7	28	3	27	4	985
	最小值	55	84	11	52	14	2	9	1	10	1	6	1	3	1	284
	平均值	91.29	150.57	21.43	99.43	23.57	3.55	22.14	1.57	19.57	3.71	14	1.29	14	1.71	520.71
下游	最大值	613	162	92	379	76	15	85	13	66	13	45	6	38	6	1 498
	最小值	58	52	9	34	11	2	9	1	11	1	7	1	7	1	281
	平均值	252.22	90	39	161.11	31.78	6.27	37	4.78	29.67	5.78	19.44	1.67	17	2.33	733.22

Fig.3 Distributions of total REE concentrations of surface and groundwater in the study area

Fig.4 REE speciation calculation results of water bodies in the study area

Table 7 Fractionation indices for surface water in the study area

分区	编号	距离 /km	(La/ Yb)_UCC	(La/ Sm)_UCC	(Gd/ Yb)_UCC	Ce/ Ce^*	Eu/ Eu^*
上游	gj-1	0	0.28	0.60	0.58	0.64	0.84
	gj-2	1.795	0.25	0.79	0.40	0.74	0.94
	gj-3	6.090	0.17	0.41	0.45	0.64	0.95
	gj-4	8.360	0.24	0.60	0.39	0.70	0.96
	gj-5	14.711	0.15	0.30	0.67	0.52	0.90
中游	gj-18	21.418	0.33	0.51	0.58	0.91	0.78
	gj-10	23.913	0.24	0.53	0.54	0.81	0.64
	gj-28	27.181	0.27	0.70	0.41	0.81	0.73
	gj-9	32.334	0.18	0.40	0.63	0.70	0.65
下游	gj-8	37.455	0.16	0.26	0.84	0.50	0.88
	gj-7	41.202	0.19	0.61	0.41	0.67	0.78
	gj-14	43.339	0.31	0.63	0.65	0.78	0.58
	gj-6	56.005	0.33	0.64	0.94	0.77	0.77

Table 8 Fractionation indices for groundwater in the study area

分区	编号	距离 /km	(La/ Yb)_UCC	(La/ Sm)_UCC	(Gd/ Yb)_UCC	Ce/ Ce^*	Eu/ Eu^*
中游	gj-19	19.65	0.23	0.49	0.58	0.63	1.00
	gj-30	22.323	0.64	0.66	1.07	0.85	1.36
	gj-29	26.109	0.38	0.56	0.90	1.04	0.71
	gj-13	26.525	0.47	0.52	0.99	0.67	1.18
	gj-27	29.630	1.34	0.59	2.32	0.79	1.56
	gj-17	34.054	0.77	0.63	0.87	0.73	0.94
	gj-26	34.219	0.67	0.78	1.01	0.91	1.56
下游	gj-25	36.800	0.39	0.62	0.90	0.80	0.83
	gj-15	38.165	1.47	1.91	0.74	0.33	0.94
	gj-16	38.194	0.39	0.62	0.63	0.51	1.56
	gj-24	38.445	0.42	0.63	0.79	0.46	0.65
	gj-23	39.723	1.00	1.18	1.13	0.12	0.79
	gj-22	43.071	0.66	0.76	1.35	0.35	0.99
	gj-21	44.096	1.01	0.96	1.30	0.46	0.80
	gj-12	53.064	1.33	1.03	1.70	0.12	0.88
	gj-11	55.795	2.81	2.55	2.13	0.09	1.08

Table 9 Sediment REE contents of the study area (mg/kg)

区域	统计量	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Ho	Er	Tm	Yb	Lu	REE	LREE/ HREE
中游	最大值	55.80	119.50	12.10	44.80	9.21	1.44	7.90	1.22	7.27	1.47	4.39	0.67	4.27	0.66	270.70	8.72
	最小值	36.50	78.30	8.12	29.40	6.08	0.88	5.18	0.82	4.93	1.00	2.98	0.44	2.82	0.45	177.90	8.55
	平均值	46.37	100.43	10.19	37.67	7.72	1.22	6.69	1.04	6.20	1.25	3.72	0.56	3.52	0.55	227.12	8.65
下游	最大值	48.20	105.50	12.30	44.60	8.68	1.33	6.80	1.10	6.43	1.34	3.87	0.57	3.86	0.60	244.98	8.97
	最小值	41.30	91.60	9.69	36.40	7.07	1.13	6.24	0.97	5.86	1.18	3.40	0.52	3.19	0.51	209.26	8.57
	平均值	45.37	98.57	10.71	39.80	7.82	1.23	6.61	1.05	6.18	1.26	3.66	0.54	3.50	0.55	226.85	8.71

Fig.5 UCC-normalized patterns for surface water (a), groundwater (b) and sediment (c) in the study area, and their fractionation characteristics (d)

Table 10 Fractionation indices for sediments in the study area

分区	编号	距离 /km	(La/ Yb)_UCC	(La/ Sm)_UCC	(Gd/ Yb)_UCC	Ce/ Ce^*	Eu/ Eu^*
	c-1	21.418	0.99	0.89	1.17	1.07	0.85
中游	c-2	23.913	0.95	0.90	1.06	1.04	0.74
	c-3	32.334	0.96	0.91	1.07	1.05	0.79
	c-4	37.455	0.92	0.83	1.02	0.99	0.69
下游	c-5	43.339	0.99	0.91	1.14	1.03	0.79
	c-6	56.005	0.95	0.88	1.13	1.04	0.94

Fig.6 Relationships between REE content and pH (a), Fe+Mn content (b), ORP (c) and Cl/ Ca (d) in the water samples of the study area

Fig.7 Gibbs diagrams of water samples from the study area

Fig.8 Plots of (La/Yb)UCC vs. pH (a), (La/Yb)UCC vs. (Fe+Mn) (b), Ce/Ce* vs. ORP (c), and Eu/Eu* vs. ORP (d) for the water samples from the study area

Fig.9 Gd anomalies statistical histogram (a) and distribution chart (b) in water samples from the study area

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