中印度洋海盆富稀土沉积地球化学特征及富集机制研究

孙懿; 石学法; 鄢全树; 刘希军; 于淼; 黄牧; 毕东杰; 李佳; 朱爱美; 高晶晶; 汪虹敏; 张兆祺

doi:10.12284/hyxb2022135

中印度洋海盆富稀土沉积地球化学特征及富集机制研究

doi: 10.12284/hyxb2022135

孙懿^{1, 2, 3,},
石学法^{1, 2, ,},
鄢全树^{1, 2},
刘希军^3, ,,
于淼^{1, 2},
黄牧^{1, 2},
毕东杰^{1, 2},
李佳^{1, 2},
朱爱美^{1, 2},
高晶晶^{1, 2},
汪虹敏^{1, 2},
张兆祺^{1, 2, 3}

1.
自然资源部第一海洋研究所自然资源部海洋地质与成矿作用重点实验室，山东青岛 266061
2.
青岛海洋科学与技术试点国家实验室海洋地质过程与环境功能实验室，山东青岛 266237
3.
桂林理工大学广西隐伏金矿产勘查重点实验室，广西桂林 541004

基金项目: 青岛海洋科学与技术试点国家实验室山东省专项（2021QNLM020003-1）；国家自然科学基金（91858209，41706061）；中国大洋矿产资源研究项目（DY135-R2-1-01）；泰山学者攀登计划项目（tspd20181216）；青岛海洋科学与技术国家实验室海洋地质过程与环境功能实验室开放基金资助项目（MGQNLM201901）。

详细信息

作者简介:
孙懿（1996-），男，河北省沧州市人，研究方向为地质资源与地质工程。E-mail：sunyii_777@163.com

通讯作者:
石学法（1965-），男，山东省昌邑市人，研究员，研究方向为海洋沉积和成矿作用。E-mail：xfshi@fio.org.cn

刘希军（1980-），男，甘肃省张掖市人，教授，研究方向为元素/同位素地球化学，地幔动力学和火成岩岩石学。E-mail：xijunliu@glut.edu.cn

中图分类号: P736.21⁺2
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出版历程
- 收稿日期: 2022-03-14
- 修回日期: 2022-05-25
- 网络出版日期: 2022-08-01
- 刊出日期: 2022-11-03

The study on geochemical characteristics and enrichment mechanism of deep sea REY-rich sediments in the Central Indian Ocean Basin

Sun Yi^{1, 2, 3
,},
Shi Xuefa^{1, 2
, ,},
Yan Quanshu^{1, 2},
Liu Xijun^{3
, ,},
Yu Miao^{1, 2},
Huang Mu^{1, 2},
Bi Dongjie^{1, 2},
Li Jia^{1, 2},
Zhu Aimei^{1, 2},
Gao Jingjing^{1, 2},
Wang Hongmin^{1, 2},
Zhang Zhaoqi^{1, 2, 3}

1.
Key Laboratory of Marine Geology and Metallogeny, First Institute of Oceanography, Ministry of Natural Resources, Qingdao 266061, China
2.
Laboratory for Marine Geology, Pilot National Laboratory for Marine Science and Technology (Qingdao), Qingdao 266237, China
3.
Guangxi Key Laboratory of Hidden Metallic Ore Deposils Exploration, Guilin University of Technology, Guilin 541004, China

摘要

摘要: 本文对中印度洋海盆深海富稀土沉积区两根柱样GC02和GC06开展了沉积物涂片观察，X-射线衍射分析，主量、微量和稀土元素分析，以及单矿物原位微区地球化学分析等，探讨了其地球化学特征、物质来源及稀土元素（REY）的富集机制。结果表明，GC02柱状沉积物类型为钙质黏土和沸石黏土，GC06柱状沉积物类型为钙质黏土、含沸石黏土和沸石黏土。稀土元素主要在含沸石黏土和沸石黏土中富集。北美页岩标准化（NASC）配分模式指示沉积物的REY主要来源于海水，矿物学和地球化学等特征表明该地区沉积物陆源组分可能主要源于澳大利亚的风尘物质。元素相关性和CaO/P₂O₅比值等指示了深海富稀土沉积中REY的主要赋存矿物为生物磷灰石（鱼牙/骨等），其次为铁锰微结核。本文总结和探讨了深海富稀土沉积的形成机制，完善了深海富稀土沉积形成过程的概念模型。
- 中印度洋海盆 /
- 富稀土深海沉积物 /
- 地球化学 /
- 稀土来源 /
- 赋存矿物 /
- 富集机制
Abstract: In this paper, sediment smear observations, X-ray diffraction analyses, major, trace and rare earth elements analyses, and in situ micro zone geochemical analyses of single minerals were carried out on samples of core GC02 and GC06 from the rare earth-rich deep-sea sediments in the Central Indian Ocean Basin to explore their geochemical characteristics, material sources and enrichment mechanisms of rare earth elements (REY). The results show that the sediment types of core GC02 are calcareous clay and zeolitic clay, and the sediment types of core GC06 are calcareous clay, zeolite-bearing clay and zeolitic clay. Rare earth elements are enriched in zeolite-bearing clays and zeolitic clays. The North American Shale Composite (NASC) Standardized patterns of REY in the sediments indicate a possible seawater origin. Mineralogical and geochemical signatures indicate that the terrestrial fraction of these sediments in the study area should be the eolian dust material originated primarily from Australian. Elemental correlations and CaO/P₂O₅ ratios indicate that the main host mineral of REY in REY-rich deep-sea sediments is bioapatite (fish teeth/bone), followed by Fe-Mn micronodule. This study summarizes and discusses the formation mechanism of REY-rich sediments and improves a conceptual model for the formation process of REY-rich sediments.
- Central Indian Ocean Basin /
- rare earth-rich deep-sea sediments /
- geochemistry /
- rare earth sources /
- REY-host minerals /
- enrichment mechanism

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图 1 采样位置及研究区地质背景

a. 全球主要风尘物质运输路径图（参考文献[33]）；b. 样品采样点位置图。底图数据来自GEBCO（http://www.gebco.net）

Fig. 1 Sampling location and geological background of the study area

a. Major global transport routes of eolian dust (refer to reference[33]); b. schematic diagram of the sampling positions. Base map data from GEBCO (http://www.gebco.net)

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图 2 GC02和GC06柱状沉积物类型和典型涂片照片

Fig. 2 Core sediments types and typical smear photos of column cores GC02 and GC06

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图 3 GC06柱样沉积物X-射线衍射特征图

Mnt：蒙脱石；Qtz：石英；Php：钙十字沸石；Ill：伊利石；Fsp：钾长石；Pl：斜长石；Gt：针铁矿；Hal：岩盐；Ap：磷灰石；Px：辉石；Am：角闪石；Cal：方解石；Kln：高岭石；Gp：石膏

Fig. 3 X-Ray diffraction characteristics of sediment samples from GC06

Mnt: Montmorillonite; Qtz: Quartz; Php: Phillipsite; Ill: Illite; Fsp: Feldspar; Pl: Plagioclase; Gt: Goethite; Hal: Halite; Ap: Apatite; Px : Pyroxene; Am: Amphibole; Cal: Calcite; Kln: Kaolinite; Gp: Gypsum

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图 4 GC02和GC06柱状沉积物主量元素和稀土元素总量随深度分布

Fig. 4 Major element and ∑REY (REE and Y) contents distribution with depth for sediment samples from GC02 and GC06

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图 5 GC02和GC06柱状沉积物微量元素和δCe、δEu随深度分布

Fig. 5 Distributions of trace element contents and δCe, δEu with depth in sediments from GC02 and GC06

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图 6 不同类型深海沉积物的北美页岩标准化配分模式（太平洋CC区钙质软泥和西太平洋硅质软泥数据参考文献[2]；北美页岩数据参考文献[37]，下文相同）

Fig. 6 North American shale standardized (NASC)-normalized REY patterns for different types of deep-sea sediments (the data of calcareous ooze from the CC Zone of the Pacific Ocean and siliceous ooze from the western Pacific Ocean refer to reference [2]; NASC date refer to reference [37], the same as below)

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图 7 印度洋不同区域柱状沉积物中稀土元素总量（∑REY）和P₂O₅、CaO、MnO、Al₂O₃、δCe、TFe₂O₃相关关系（DSDP 和ODP站位数据参考文献[24-25]）

Fig. 7 Cross-plots of ∑REY versus P₂O₅, CaO, MnO, Al₂O₃, δCe and TFe₂O₃ for sediments from different regions in the Indian Ocean (the DSDP and ODP site data refer to references [24-25])

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图 8 GC02和GC06柱状沉积物及其中鱼牙CaO/P₂O₅−∑REY相关关系

a. 印度洋不同站位沉积物的CaO/P₂O₅−∑REY；b. 样品中鱼牙CaO/P₂O₅−∑REY。鱼牙中CaO/P₂O₅的范围（1.30~1.90）参考文献[53]，DSDP 和ODP站位数据参考文献[24–25]

Fig. 8 Cross-plots of CaO/P₂O₅ versus ∑REY for sediments and fish teeth from GC02 and GC06

a. Cross-plot of CaO/P₂O₅ versus ∑REY for sediments from different stations in the Indian Ocean; b. cross-plot of CaO/P₂O₅ versus ∑REY for fish teeth in GC02 and GC06. The range of CaO/P₂O₅ in fish teeth (1.30−1.90) refer to reference [53], and the DSDP and ODP site data refer to references [24–25]

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图 9 不同物质稀土元素含量的北美页岩标准化配分模式图对比

洋中脊玄武岩数据参考文献[54]；澳大利亚风尘沉积物数据参考文献[55]；孔隙水数据参考文献[56]；海水数据参考文献[57]；热液数据参考文献[58]；北美页岩标准化数据参考文献[37]

Fig. 9 North American shale standardized-normalized rare earth elements patterns for different materials

Mid-ocean ridge basalt data refer to reference [54]; Australian wind-dust sediment data refer to reference [55]; pore water data refer to reference [56]; seawater data refer to reference [57]; hydrothermal data refer to reference [58]; NASC data refer to reference [37]

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图 10 研究样品中矿物含量和稀土元素总量（∑REY）相关关系

Fig. 10 Cross-plot of ∑REY versus mineral contents in the studied samples

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图 11 印度洋不同地区的柱样沉积物Y/Ho−∑REY散点图的比较

Fig. 11 Plot of Y/Ho−∑REY for sediments from different parts of the Indian Ocean

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图 12 GC06柱状沉积物中鱼牙不同部分的北美页岩标准化配分模式对比

Fig. 12 Comparison of North American shale standardized-normalized rare earth elements patterns for different parts of fish teeth form the sediments from GC06

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图 13 GC06柱状沉积物中微结核类型判别图

a. 底图参考文献[72]，图中虚线表示混合两种成因过程的趋势，即水成作用和热液作用、水成作用和成岩作用之间存在连续体。实线箭头表示两种作用相互不影响，即只与一种作用相关；b. 底图参考文献[73]

Fig. 13 Discrimination schemes for the genetic classification of the micronodules from the sediments in GC06

Picture on a refer to reference [72], the dotted present the mixing trends between two genetic processes highlighting the continuum existing between hydrogenetic-hydrothermal crusts and hydrogenetic-diagenetic nodules, solid arrows show evolution trends of a sample set related to only one genetic process without influence of another one; picture on b refer to reference [73]

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图 14 GC06柱样沉积物中水成微结核和成岩微结核的北美页岩标准化配分模式

Fig. 14 North American shale standardized-normalized rare earth elements patterns of hydrogenetic and diagenetic micronodules in sediments from GC06

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图 15 深海富稀土沉积形成过程示意

Fig. 15 Schematic diagram for the formation process of deep-sea rare earth elements-rich sediments

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表 1 北美页岩的稀土元素平均含量^[37]

Tab. 1 Average value of the rare earth elements content in the North American shale^[37]

元素	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb	Dy	Y	Ho	Er	Tm	Yb	Lu
含量/（mg·kg^-1）	32	73	7.9	33	5.7	1.24	5.2	0.85	5.2	27	1.04	3.4	0.5	3.1	0.48

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表 2 样品主量元素特征值（单位：wt%）

Tab. 2 Characteristic values of major element contents (unit: wt%)

		SiO₂	Al₂O₃	CaO	TFe₂O₃	K₂O	MgO	MnO	Na₂O	P₂O₅	TiO₂
钙质黏土	最小值	26.84	7.59	3.32	6.32	1.61	1.90	1.98	4.40	0.51	0.33
	最大值	42.54	12.66	21.82	11.26	2.85	2.99	3.71	5.96	1.93	0.57
	平均值	37.96	11.30	8.37	9.52	2.40	2.72	2.79	5.36	0.99	0.51
含沸石黏土	最小值	43.12	12.35	1.79	9.76	2.64	2.88	2.68	4.86	0.72	0.57
	最大值	45.62	13.74	2.55	10.77	2.99	3.15	3.39	5.81	1.39	0.68
	平均值	44.20	13.27	2.16	10.27	2.84	3.00	3.11	5.12	1.12	0.63
沸石黏土	最小值	40.06	11.75	2.06	10.61	2.62	2.75	3.10	4.86	0.98	0.53
	最大值	43.74	13.54	3.39	12.89	3.02	3.17	3.67	6.08	2.01	0.65
	平均值	41.80	13.08	2.38	11.82	2.82	3.00	3.35	5.39	1.30	0.60

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表 3 样品主量元素和稀土元素总量的相关性系数

Tab. 3 Correlation coefficients between major element and ∑REY (REE and Y) contents in the sediments

		SiO₂	Al₂O₃	CaO	TFe₂O₃	K₂O	MgO	MnO	Na₂O	P₂O₅	TiO₂	∑REY
钙质黏土	SiO₂	1
	Al₂O₃	0.994	1
	CaO	–0.988	–0.997	1
	TFe₂O₃	0.847	0.886	–0.917	1
	K₂O	0.964	0.966	–0.983	0.936	1
	MgO	0.981	0.994	–0.999	0.930	0.981	1
	MnO	0.710	0.726	–0.781	0.915	0.872	0.787	1
	Na₂O	0.869	0.899	–0.869	0.727	0.764	0.875	0.418	1
	P₂O₅	0.533	0.532	–0.597	0.757	0.731	0.599	0.956	0.147	1
	TiO₂	0.991	0.999	–0.999	0.902	0.973	0.998	0.750	0.890	0.559	1
	∑REY	0.631	0.642	–0.702	0.858	0.813	0.708	0.992	0.300	0.985	0.668	1
含沸石黏土	SiO₂	1
	Al₂O₃	0.567	1
	CaO	–0.847	–0.467	1
	TFe₂O₃	–0.706	–0.295	0.694	1
	K₂O	–0.897	–0.500	0.901	0.546	1
	MgO	0.879	0.620	–0.883	–0.465	–0.926	1
	MnO	–0.887	–0.382	0.965	0.773	0.888	–0.839	1
	Na₂O	0.069	–0.398	–0.266	–0.102	–0.160	0.061	–0.361	1
	P₂O₅	–0.888	–0.427	0.981	0.652	0.943	–0.911	0.977	–0.328	1
	TiO₂	0.848	0.767	–0.690	–0.482	–0.801	0.865	–0.645	–0.384	–0.699	1
	∑REY	–0.882	–0.412	0.952	0.668	0.926	–0.900	0.964	–0.304	0.978	–0.710	1
沸石黏土	SiO₂	1
	Al₂O₃	0.375	1
	CaO	–0.451	–0.755	1
	TFe₂O₃	–0.431	0.347	–0.502	1
	K₂O	–0.333	0.356	–0.492	0.666	1
	MgO	0.793	0.426	–0.351	–0.271	–0.513	1
	MnO	–0.052	0.053	–0.367	0.276	0.527	–0.197	1
	Na₂O	–0.116	–0.010	0.192	0.170	–0.226	0.112	–0.719	1
	P₂O₅	–0.363	–0.396	0.013	0.265	0.486	–0.541	0.779	–0.562	1
	TiO₂	0.766	0.620	–0.501	–0.250	–0.339	0.892	0.008	–0.211	–0.467	1
	∑REY	–0.406	–0.088	–0.236	0.459	0.797	−0.658	0.793	–0.542	0.876	–0.466	1

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表 4 鱼牙/骨的原位主量元素特征值（单位：wt%）

Tab. 4 Characteristic values of major element contents for fish teeth/bones (unit: wt%)

	Na₂O	MgO	Al₂O₃	F	SiO₂	P₂O₅	Cl	K₂O
Min	0.56	0.08	0	0	0	32.63	0	0
Max	1.29	0.46	0.29	4.27	0.73	41.02	0.09	0.04
Ave	0.90	0.26	0.04	2.64	0.03	37.88	0.03	0.01

	CaO	SO₃	CoO	TiO2	CuO	MnO	FeO	NiO
Min	42.42	0.08	0	0	0	0	0	0
Max	52.66	1.31	0.19	0.10	0.19	0.08	2.26	0.06
Ave	46.91	0.52	0.03	0.01	0.03	0.01	0.09	0.01

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表 5 鱼牙/骨的原位稀土元素特征值（单位：mg/kg）

Tab. 5 Characteristic values of rare earth element contents for fish teeth/bones (unit: mg/kg)

	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb
Min	65.88	3.39	18.65	81.97	17.05	4.75	25.86	3.86
Max	3 313.65	904.16	1 038.16	4 765.49	1 275.60	300.89	1 627.31	250.79
Ave	1 016.35	207.46	270.77	1 172.90	289.57	73.65	381.27	60.89

	Dy	Y	Ho	Er	Tm	Yb	Lu	REY
Min	25.34	184.90	5.90	16.00	2.25	14.07	2.88	480.55
Max	1 586.88	10 069.98	331.56	959.10	140.98	829.39	170.17	27 225.97
Ave	401.24	2817.15	87.23	261.20	39.88	243.94	45.29	7 368.81

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表 6 微结核的原位主量元素特征值（单位：wt%）

Tab. 6 Characteristic values of major element contents for micronodules (unit: wt%)

	Na₂O	MgO	Al₂O₃	F	SiO₂	P₂O₅	Cl	K₂O
Min	0	0.67	0.43	0	1.06	0	0.01	0
Max	0.39	6.26	13.00	0.45	22.10	1.64	0.13	1.68
Ave	0.13	1.70	1.97	0.10	4.53	0.30	0.06	0.12

	CaO	SO₃	CoO	TiO2	CuO	MnO	FeO	NiO
Min	1.72	0	0	0.05	0.10	25.82	0.61	0.15
Max	4.29	0.51	2.10	2.37	2.34	55.85	23.01	2.46
Ave	3.19	0.30	1.02	1.01	0.54	40.24	13.16	0.65

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表 7 微结核的原位稀土元素特征值（单位：mg/kg）

Tab. 7 Characteristic values of rare earth element contents for micronodules (unit: mg/kg)

	La	Ce	Pr	Nd	Sm	Eu	Gd	Tb
Min	17.36	100.21	4.63	17.28	3.57	0.79	3.84	0.49
Max	151.85	1 833.82	36.26	156.72	36.03	8.44	42.79	4.67
Ave	71.11	1 118.55	13.09	48.74	10.63	2.64	12.10	1.78

	Dy	Y	Ho	Er	Tm	Yb	Lu	REY
Min	3.46	9.17	0.76	2.07	0.25	1.59	0.27	177.31
Max	34.42	151.07	5.97	19.00	2.23	13.10	2.10	2 109.70
Ave	10.85	42.16	2.16	6.31	0.98	6.53	0.97	1 348.61

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表 8 GC02和GC06柱状沉积物判别函数（DF）计算（Al/Ti）

Tab. 8 Discriminant function (DF) calculation for sediments in GC02 and GC06 (Al/Ti)

目标地区样品号	卡拉哈里沙漠	墨累−达令盆地	孟加拉扇
GC02	0.31	0.15	0.13
GC06	0.31	0.14	0.12
注：卡拉哈里沙漠数据参考文献[46]，墨累−达令盆地数据参考文献[47]，孟加拉扇数据参考文献[24−25]。

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表 9 GC02和GC06柱状沉积物判别函数（DF）计算（Zr/Hf）

Tab. 9 Discriminant function (DF) calculation for sediments in GC02 and GC06 (Zr/Hf)

目标地区样品号	卡拉哈里沙漠	墨累−达令盆地	孟加拉扇
GC02	0.41	0.01	0.13
GC06	0.33	0.04	0.06
注：卡拉哈里沙漠数据参考文献[46]，墨累−达令盆地数据参考文献[47]，孟加拉扇数据参考文献[24−25]。

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