离子吸附型稀土矿床形成的矿物表/界面反应机制

doi:10.13745/j.esf.sf.2021.8.8

地学前缘 ›› 2022, Vol. 29 ›› Issue (1): 29-41.DOI: 10.13745/j.esf.sf.2021.8.8

• 稀土金属矿床成矿机制与成矿模式 • 上一篇下一篇

离子吸附型稀土矿床形成的矿物表/界面反应机制

梁晓亮(), 谭伟, 马灵涯, 朱建喜, 何宏平^*()

1.中国科学院广州地球化学研究所矿物学与成矿学重点实验室, 广东广州 510640
2.中国科学院广州地球化学研究所广东省矿物物理与材料研究开发重点实验室, 广东广州 510640

收稿日期:2021-05-20 修回日期:2021-06-22 出版日期:2022-01-25 发布日期:2022-02-22
通讯作者: 何宏平
作者简介:梁晓亮(1984—),男,博士,研究员,博士生导师,主要从事矿物结构与表/界面反应性研究。E-mail: liangxl@gig.ac.cn
基金资助:
广东省基础与应用基础研究重大项目(2019B030302013);中国科学院地质与地球物理研究所重点部署项目(IGGCAS-201901);广州市科技计划重点项目(201804020037);国家自然科学基金项目(41921003);国家自然科学基金项目(41773113);国家自然科学基金项目(41702041);国家自然科学基金项目(42022012)

Mineral surface reaction constraints on the formation of ion-adsorption rare earth element deposits

LIANG Xiaoliang(), TAN Wei, MA Lingya, ZHU Jianxi, HE Hongping^*()

1. Key Laboratory of Mineralogy and Metallogeny, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
2. Key Laboratory of Mineral Physics and Materials of Guangdong Province, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China

Received:2021-05-20 Revised:2021-06-22 Online:2022-01-25 Published:2022-02-22
Contact: HE Hongping

摘要/Abstract

摘要：

华南离子吸附型稀土矿床提供了全球超过90%的重稀土,是我国优势的战略性关键金属矿产资源。掌握这类矿床的成矿机制和禀赋特征,可为增加稀土资源储量和高效利用稀土资源提供理论支撑。离子吸附型稀土矿床主要发育在富稀土花岗岩、浅变质岩及火山岩的风化壳中。基岩中的(含)稀土矿物是风化壳中离子态稀土的主要来源,其矿物组合很大程度上决定了稀土矿床的禀赋和分异特征。在物理-化学风化和微生物作用下,造岩矿物、含稀土矿物和稀土独立矿物逐渐溶解,使稀土元素活化和再富集。一方面,母岩风化形成的黏土矿物和铁锰氧化物具有较大的比表面积和一定的表面电荷密度,是稀土离子的主要载体;另一方面,稀土离子通过离子交换、表面吸附与络合、共沉淀,以及形成次生稀土矿物等途径富集在次生矿物表面,其富集-分异特征和赋存状态受矿物类型、pH、微生物活动等因素所控制。利用高分辨透射电镜结合选区电子衍射和电子能量损失谱,以及同步辐射X射线吸收精细结构谱,有望在原子级尺度查明稀土的微观赋存状态。未来研究需更多关注基岩中(含)稀土矿物组合及其演化路径的制约因素、微生物风化对离子吸附型稀土矿床成矿作用的约束,以及稀土元素的微观赋存状态等问题。

关键词: 离子吸附型稀土矿床, 矿物溶解, 矿物演化, 稀土元素富集-分异, 微生物风化, 矿物表/界面反应

Abstract:

The ion-adsorption rare earth element (IAR) deposits in South China produce more than 90% of the world’s heavy rare earth elements (HREEs). They are a key strategic metal resource of China. Thus, a better understanding of the metallogenic mechanism and resource characteristics of IAR deposits can provide a theoretical basis for increasing REE reserves and better utilization of REE resources. The IAR deposits are mainly developed in the weathering crusts of REE-rich granite, epimetamorphic and volcanic rocks. The REE-bearing minerals in protolith are the main sources of REE cations in weathering crust, where mineral association greatly determines the concentration and fractionation characteristics of REEs. Under physical/chemical weathering and microbial action, the dissolution of rock-forming minerals, REE-bearing minerals and REE minerals results in the activation and re-enrichment of REEs. On one hand, weathering of protolith produces clay minerals and Fe-Mn (hydr)oxides with a large specific surface area and high surface charge density. On the other hand, these secondary minerals can adsorb REE cations via ion exchange, surface adsorption/complexation or formation of secondary REE minerals. The adsorption mechanism, enrichment-fractionation characteristics and occurrence state of REEs are affected by mineral types, pH and microbial activity. By using high-resolution transmission electron microscopy (HRTEM) coupled with selected area electron diffraction (SAED) and electron energy loss spectroscopy (EELS) and synchrotron radiation X-ray absorption fine structure spectroscopy (XAFS), the atomic occurrence state of REEs can be determined. In the future, more attention should be paid to research areas including the association of REE-bearing minerals in protoliths and its evolutionary pathway and mechanism, the constraints of microbial weathering on the formation of IAR deposits, and the microscopic occurrence state of REEs.

Key words: ion-adsorption type rare earth element deposit, mineral dissolution, mineral evolution, enrichment and fractionation of rare earth elements, microbial weathering, mineral surface reaction

中图分类号:

P618.7
P595

梁晓亮, 谭伟, 马灵涯, 朱建喜, 何宏平. 离子吸附型稀土矿床形成的矿物表/界面反应机制[J]. 地学前缘, 2022, 29(1): 29-41.

LIANG Xiaoliang, TAN Wei, MA Lingya, ZHU Jianxi, HE Hongping. Mineral surface reaction constraints on the formation of ion-adsorption rare earth element deposits[J]. Earth Science Frontiers, 2022, 29(1): 29-41.

图/表 8

图1 离子吸附型稀土矿床形成机理及剖面示意图

Fig.1 Formation mechanism and cross-section of IAR deposits

表1 离子吸附型稀土矿基岩中(含)稀土矿物分类

Table 1 Classification of REE-bearing minerals in IAR deposits

基岩类型	岩性	(含)稀土矿物	典型矿床
花岗岩类	黑/白云母花岗岩	独居石、氟碳钙钇矿、硅钍钇矿、锆石、磷灰石、磷钇矿、钛铁矿、烧绿石等	江西省足洞矿区^[5]
	花岗闪长岩	独居石、锆石、磷灰石等	赣南清溪岩体稀土矿区^[14]
	石英正长/二长岩	独居石、榍石、锆石、磁铁矿、钛铁矿等	福建龙岩万安稀土矿区^[15]
	花岗斑岩	独居石、褐帘石、磁铁矿、磷灰石、锆石等	广东省仁居矿区^[16]
变质岩类	板岩	独居石、磷钇矿、锆石、含稀土钛铁矿、含稀土金红石	江西宁都葛藤嘴地区^[17,18]
	千枚岩	独居石、磷钇矿、锆石、含稀土钛铁矿
	片岩	独居石、磷钇矿、锆石、含稀土钛铁矿、磷铝酸盐类、褐帘石
	变砂岩	独居石、磷钇矿、锆石、磷铝酸盐、水磷酸盐、褐帘石
	变质凝灰岩	独居石、磷钇矿、锆石、含稀土金红石、含稀土绿泥石、含稀土钍石、方铈石
	变粒岩	独居石、磷钇矿、锆石、含稀土绿泥石
火山岩类	流纹岩/英安岩	独居石、磷钇矿、锆石、磷灰石等	江西省寻乌河岭矿区^[19]
碱性岩类	碱性正长岩	独居石、磷钇矿、烧绿石、水磷镧石、水磷铈石、水菱钇矿、氟碳镧矿等	云南省建水普雄铌稀土矿^[20]

图2 广东仁居矿床风化壳中含稀土矿物的扫描电镜背散射图 a—基岩中它形的榍石和锆石;b—绿帘石包裹褐帘石分布于黑云母边缘;c—在半风化层中,磷灰石颗粒表面风化严重,出现大量的溶蚀坑和裂隙;d—在表土层,次生稀土矿物方铈矿(CeO2)以球状集合体的形式分布于高岭石表面。

Fig.2 SEM backscattered electron images of REE-bearing minerals from the weathering crust at the Renjü deposit in Guangdong Province

表2 可溶解(含)稀土矿物的部分微生物菌种

Table 2 Specific microorganisms that can dissolve rare earth minerals

(含)稀土矿物	微生物菌种	参考文献
三水铝石	嗜酸氧化亚铁硫杆菌(Acidithiobacillus ferrooxidans)	[36]
氟碳铈矿	链霉菌属(Streptomyces sp.)	[37]
	微球菌属(Micrococcus sp.)
	小单孢菌属(Micromonospora sp.)
独居石	曲霉菌属(Aspergillus sp.)	[38]
	假单胞菌属(Pseudomonas sp.)	[34]
	芽孢杆菌属(Bacillus sp.)	[39]
	产气肠杆菌(Enterobacter aerogenes)	[40]
	拟青霉属(Paecilomyces sp.)	[41]
	醋杆菌属(Acetobacter sp.)	[39]
	嗜酸氧化亚铁硫杆菌(Acidithiobacillus ferrooxidans)	[42]
锆石	嗜酸硫杆菌属(Acidithiobacillus sp.)	[43]
锆石	甲醇醋杆菌(Acetobacter methanolicus)	[44]

图3 黏土矿物的演化路径(据文献[52]修改)

Fig.3 Clay mineral transformation pathways. Modified after [52].

图4 广东省仁居矿床风化壳中铁氧化物形成与转变的扫描电镜背散射图 a—细脉状或块状的针铁矿集合体在半风化层-全风化层下部分布于高岭石附近;b—纤维状的针铁矿生长于在全风化层下部的孔洞中;c—在全风化层上部,“米粒状”的赤铁矿于“层状”的高岭石集合体的层间出现;d—在表土层,颗粒状的赤铁矿集合体附着于板状高岭石表面。

Fig.4 SEM backscattered electron images of iron oxides from the weathering crust at the Renju deposit in Guangdong Province

图5 高岭石和埃洛石对稀土元素的吸附特征及机制(据文献[72]修改)

Fig.5 Characteristics and mechanism of REE adsorption on kaolinite and halloysite. Modified after [72].

图6 微生物对重稀土元素的富集特征和机制(b据文献[93]修改) a—枯草芽孢杆菌细胞壁模式图;b—枯草芽孢杆菌与水溶液中REE的分配系数Kd。 K d ( L / g ) = [ REE ] init - [ REE ] fil c ( g / L ),其中[REE]init为稀土初始浓度,[REE]fil为滤液中稀土浓度,c(g/L)为细菌干重与水的比值。

Fig.6 Microbial enrichment of HREEs. (a) Basillus subtilis cell wall model showing REE entrapment. (b) Plot of REE partition coefficients between microorganism and aqueous solution (modified after [93]).

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离子吸附型稀土矿床形成的矿物表/界面反应机制

Mineral surface reaction constraints on the formation of ion-adsorption rare earth element deposits

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