Remobilization and transferring of rare earth elements in the formation of regolith-hosted REE deposits
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摘要: 稀土元素（REE）广泛应用于新能源、国防军工等高科技产业中，是一类战略性关键矿产资源。风化壳型稀土矿床是中国最具竞争优势的稀土资源，其供应了全球90%以上的重稀土。阐明这类稀土矿床的成矿机制，可为寻找和高效开采利用该类稀土资源提供理论支持。文章以稀土元素的活化和迁移这两个关键过程为切入点，总结近年来取得的最新研究成果，并对未来的研究方向提出展望。该类矿床主要发育于富稀土花岗岩类的风化壳中，其中稀土配分模式主要受基岩控制。花岗岩类风化壳的形成以化学风化和生物风化作用为主。长石、云母和角闪石等主要造岩矿物风化形成的黏土矿物和铁锰氧化物是该类矿床中离子态稀土的主要赋存载体。而离子态稀土则来源于基岩中易风化和中等抗风化（含）稀土副矿物的风化和分解。此外，微生物分泌的有机酸等代谢产物可以促进难风化的独居石和磷钇矿等副矿物的风化和分解，加速稀土元素活化−迁移。与此同时，微生物作用还会导致轻稀土和重稀土的显著分异，其中革兰氏阳性细菌对重稀土的选择性显著高于轻稀土。在风化淋积过程中，稀土元素的络合离子可能是风化壳中稀土迁移的主要形式，主要受pH值、次生矿物形成和络合环境影响。值得注意的是，除了F−和${\mathrm{CO}}_3^{2-} $等无机配体，有机质也可以直接与稀土离子络合或螯合，充当有机配体促进稀土的运移。因此，风化壳型稀土矿床中稀土元素的活化和迁移机制主要受化学风化和生物风化过程控制，是无机和有机共同作用的结果，但其对该类矿床形成的贡献尚待定量评估。Abstract:
Objective Rare earth elements (REEs) are indispensable for high-tech industries, such as clean energy, national defense, and military industries, rendering them strategically critical minerals. In China, regolith-hosted REE deposits constitute one of the most important REE resources, supplying over 90% global heavy rare earth elements (HREE). Understanding the formation of such REE deposits can provide a theoretical basis for their efficient utilization. Methods This paper summarizes the recent research results on the two key processes of REE remobilization and transferring and puts forward prospects for future research to deepen the knowledge and understanding of the formation of regolith-hosted REE deposit. Results These deposits developed primarily in the weathering crusts of REE-rich granitic rocks, with the REE distribution patterns largely reflecting those of the underlying bedrock. The granitoid weathering crusts are primarily developed by chemical and biological weathering. Clay minerals and Fe–Mn (hydr) oxides, resulting from the weathering of major rock-forming minerals, such as feldspar, mica, and amphibole, serve as the primary hosts for REE ions in weathered crusts. These REE ions originate from the weathering and decomposition of REE-bearing accessory minerals in the bedrock, which exhibit varying degrees of susceptibility to weathering. Furthermore, metabolites such as microbial organic acids can breakdown refractory minerals like monazite and xenotime, facilitating REE remobilization. Simultaneously, microbial action can cause significant REE fractionation, and gram-positive bacteria are significantly more selective for HREE than for LREE. During weathering and leaching processes, REE primarily form REE complex ions within weathering crusts and are then transferred by meteoric water or groundwater. This process is primarily controlled by factors such as pH, secondary mineral formation, and the weathering environment. Notably, in addition to inorganic ligands, such as F− and ${\mathrm{CO}}_3^{2-} $, organic matter can directly interact with REE, acting as organic ligands that aid in REE transfer. Conclusion Consequently, the REE remobilization and transferring mechanisms in regolith-hosted REE deposits are predominantly controlled by chemical and biological weathering processes, which result from interactions between inorganic and organic agents. However, the quantitative impact of these processes on the formation of these deposits requires further evaluation. -
图 1 华南地区风化壳型稀土矿床分布图（据Li et al., 2019修改）
Figure 1. The distribution of regolith-hosted rare earth element (REE) deposits in South China (modified from Li et al., 2019)
图 2 华南风化壳剖面及其REE分布特征（据王登红等，2013修改）
A—表土层；B—全风化层；C—半风化层；P—基岩
Figure 2. Profile and rare earth element (REE) distribution of the weathering crusts in South China (modified from Wang et al., 2013)
(a) Aopsoil; (b) Completely weathered horizon; (c) Semi-weathered horizon; (d) Bedrock
图 3 江西大埠弱风化花岗岩中造岩矿物风化的背散射电子（BSE）图像
a—钠长石局部风化形成高岭石；b—风化残余的钠长石；c—黑云母风化形成高岭石；d—白云母局部风化形成高岭石
Figure 3. Backscattered electron (BSE) images of the weathering of rock-forming minerals in the Dabu weakly weathered granites, Jiangxi Province
(a) Albite is partly weathered to kaolinite; (b) Residual albite after weathering; (c) Biotite is weathered to kaolinite; (d) Muscovite is partly weathered to kaolinite
图 4 广东仁居风化壳型轻稀土矿床中不同层位的褐帘石、榍石和磷灰石风化的BSE图像
a—弱风化基岩中褐帘石溶蚀洞及其填充的氟碳铈矿；b—半风化层下部的褐帘石风化碎片；c—半风化层下部的榍石风化裂隙和溶蚀坑；d—半风化层上部的榍石风化崩解；e—半风化层上部的磷灰石溶蚀坑；f—全风化层下部磷灰石密集的溶蚀坑
Figure 4. Backscattered electronic (BSE) images of the weathering of allanite, titanite and apatite in the profiles of the Renju regolith-hosted light rare earth element (LREE) deposit, Guangdong Province
(a) The etch holes filled by bastnaesite in allanite in weakly weathered bedrock; (b) Fragments of allanite weathering in the lower part of the semi-weathered horizon; (c) Weathering fractures and etch pits of titanite in the lower part of the semi-weathered horizon; (d) The disintegration of titanite in the upper part of the semi-weathered horizon; (e) The etch pits of apatite in the upper part of the semi-weathered horizon; (f) Massive etch pits of apatite in the lower part of the completely weathered horizon
图 5 江西大埠风化壳型重稀土矿床中石榴子石风化的BSE图像
a—弱风化基岩中石榴子石沿着边界和裂隙风化形成高岭石；b—弱风化基岩中石榴子石沿着裂隙风化形成高岭石；c—全风化层下部石榴子石风化形成溶蚀洞；d—全风化层上部石榴子石风化形成大量小溶蚀洞
Figure 5. Backscattered electronic (BSE) images of the weathering of garnet in the Dabu regolith-hosted heavy rare earth element (HREE) deposit, Jiangxi Province
(a) Garnet weathering along the grain boundaries and fractures to form kaolinite in weakly weathered bedrock; (b) Garnet weathering at the fractures to form kaolinite in weakly weathered bedrock; (c) Weathering etch holes in garnet from the lower part of the completely weathered horizon; (d) Massive etch holes in garnet from the upper part of the completely weathered horizon
图 6 不同细菌在30天内对稀土元素的浸出量（据He et al., 2023修改）
Figure 6. The contents of rare earth element (REE) leached by different bacteria in 30 days (modified from He et al., 2023)
图 7 微生物附着在矿物表面并留下溶蚀痕迹
a—矿物裂隙中的真菌菌丝；b—真菌菌丝在矿物表面造成溶蚀痕迹；c—黏附在矿物表面的细菌；d—细菌在矿物表面分泌的胞外分泌物；a—d均为二次电子图像
Figure 7. Microbial adhesion to mineral surfaces forms dissolution traces
(a) Fungal hypha in mineral fractures; (b) Dissolution traces caused by fungal hyphae on mineral surfaces; (c) Bacteria adhering to mineral surfaces; (d) Extracellular secretions secreted by bacteria on mineral surfaces. (a–d) are secondary electron images.
图 8 风化过程中微生物活化−富集稀土元素机理图
Figure 8. Mechanism diagram of microbial rare earth element (REE) activation and enrichment during weathering
图 9 广东仁居风化壳型轻稀土矿床中次生矿物的BSE图像
a—表土层中方铈矿与高岭石紧密接触；b—表土层中方铈矿集合体；c—全风化层中水磷铈矿；d—全风化层中铁锰氧化物
Figure 9. BSE images of the secondary minerals in the Renju regolith-hosted light rare earth element (LREE) deposit, Guangdong Province
(a) Cerianite associated with kaolinite in topsoil; (b) Cerianite aggregates in topsoil; (c) Churchite in the completely weathered horizon; (d) Fe−Mn (hydr) oxides in the completely weathered horizon
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