FIB-TEM解析微生物铀矿化:以松辽盆地海力锦砂岩型铀矿为例

doi:10.19657/j.geoscience.1000-8527.2024.133

摘要/Abstract

摘要：

针对砂岩型铀矿中微生物与矿物互作机制证据链薄弱的关键科学问题,本研究以松辽盆地海力锦矿床姚家组下段含铀独居石为研究对象,通过微区矿物学分析揭示其溶蚀过程与铀活化机理。基于钻孔岩心系统取样,采用FIB-TEM联用技术首次在独居石溶蚀界面识别出氢铀云母与沥青铀矿纳米矿物组合,结合电子探针原位分析发现溶蚀相独居石平均损失75%初始铀。研究揭示:(1)石英包裹效应导致独居石选择性溶蚀特征,开放体系下溶蚀强度提升3~4个数量级;(2)溶蚀界面纳米矿物相的定向分布指示微生物代谢产生的有机酸主导磷铀耦合释放过程;(3)建立的生物膜催化动力学模型显示,微生物介导的界面反应使铀活化至沉淀。该研究不仅为微生物与纳米矿物间协同成矿机制提供了关键的显微尺度证据,而且对于促进铀矿地质学研究向更精细的微观领域深入拓展具有重要的意义。

关键词: 海力锦铀矿床, 独居石溶解动力学, 微生物铀矿化, FIB-TEM联用技术, 纳米矿物

Abstract:

Resolving the evidentiary gap in microbe-mineral interactions within sandstone-hosted uranium systems, this study presents nanoscale evidence elucidating the biogeochemical controls on uranium mobilization.Focusing on uranium-bearing monazite in the Lower Yaojia Formation of the Hailijin deposit, we integrate FIB-TEM nanotomography with EPMA geochemical mapping to decode dissolution-uranium release coupling mechanisms.Three pivotal findings emerge: (1) Quartz-encapsulated monazite preserves pristine surfaces, whereas exposed grains exhibit 75% uranium depletion with intense dissolution features; (2) FIB-TEM nanotomography reveals epitaxial overgrowths of chernikovite and uraninite nanoparticles along dissolution fronts, forming characteristic U-P biogeochemical halos; (3) The established biofilm catalytic kinetics model shows that the microbe-mediated interfacial reaction activates uranium to precipitation.This study not only provides critical microscopic-scale evidence elucidating synergistic mineralization mechanisms between microorganisms and nano-minerals, but also holds significant implications for advancing uranium deposit geology research into refined microscopic domains.

Key words: Hailijin uranium deposit, monazite dissolution kinetics, microbial uranium mineralization, FIB-TEM nanotomography, nanoscale mineral

中图分类号:

P619.14

金伟国, 尹烁, 王庆飞, 潘家永. FIB-TEM解析微生物铀矿化:以松辽盆地海力锦砂岩型铀矿为例[J]. 现代地质, 2025, 39(02): 248-262.

JIN Weiguo, YIN Shuo, WANG Qingfei, PAN Jiayong. Deciphering Microbial-Mediated Uranium Mineralization via FIB-TEM Nanotomography: A Case Study from the Hailijin Deposit, Songliao Basin[J]. Geoscience, 2025, 39(02): 248-262.

图/表 14

图1 松辽盆地南部构造单元及矿床地质简图(据文献[7]修改) (a)松辽盆地一级构造单元区划图;(b)松辽盆地南部构造单元区划图;(c)海力锦矿床及其邻近地区地质简图;Ⅰ.开鲁坳陷区; Ⅱ.西南隆起区; Ⅲ.西部斜坡区; Ⅳ.中央坳陷区; Ⅴ.西缘斜坡带; Ⅰ1.陆家堡凹陷; Ⅰ2.哲中凹陷; Ⅰ3.乌兰花凸起; Ⅰ4.钱家店凹陷; Ⅱ1.白音花凹陷; Ⅱ2.三棵树鼻状凸起; Ⅱ3.瞻榆凹陷; Ⅱ4.架玛吐凸起; Ⅱ5.巴彦塔拉凸起; Ⅱ6.大林凹陷; Ⅱ7.金宝屯凹陷; Ⅱ8.宝格吐凹陷; Ⅱ9.张强凹陷; Ⅱ10.安乐凹陷

Fig.1 Simplified geological map for the Hailijin deposit and tectonic units of the southern Songliao Basin (modified from reference [7])

图2 海力锦铀矿床姚家组A-A'质剖面简图(据文献[11,13]修改)

Fig.2 A-A' simplified geological profile of Yaojia Formation in Hailijin uranium deposit (modified from references [11,13])

图3 海力锦铀矿床地层相关厚度及ZKL4-5钻孔柱状图(据文献[12-13]修改) (a)海力锦矿床地层及相关厚度;(b)岩心ZKL4-5钻探获得的含铀地层岩性、深度、铀矿分布及手标本照片

Fig.3 Regional strata, related thickness and ZKL4-5 sedimentary column of drill core in the Hailijin uranium deposit (modified from references [12-13])

图4 铀矿物赋存相态特征 (a)磷灰石和相邻高岭石边缘吸附纳米铀矿物;(b)纳米铀矿物集合体出现在多孔的高岭石表面;(c)碎屑状铀矿物集合体分布在石英、钾长石和钛铁矿颗粒孔隙间;(d)含钛铀矿物填充蚀变铁钛氧化物孔隙;Ap.磷灰石;Ilm.钛铁矿;Kfs.钾长石;Kln.高岭石;Qtz.石英

Fig.4 Paragenetic types and occurrence modes of uranium minerals

图5 独居石与磷灰石背散射电子显微对比 (a)—(c)石英包裹的碎屑独居石颗粒;(d)—(f)被严重溶蚀的独居石,表面见大量暗色点状、针状孔隙;(g)—(i)磷灰石在高对比度下结构较为完整;Ap.磷灰石;Ilm.钛铁矿;Kfs.钾长石;Kln.高岭石;Mnz.独居石;Qtz.石英

Fig.5 Comparative backscattered electron (BSE) microscopy of monazite-apatite assemblages

图6 独居石结构中La2O3-Ce2O3-Nd2O3三种主要轻稀土的三元相图

Fig.6 Ternary diagram between the dominant three LREEs La2O3-Ce2O3-Nd2O3 in the structure of monazite

图7 溶蚀独居石的BSE显微结构与FIB制样定位 (a)(b)溶蚀独居石背散射图片,其中(b)黄色区域为FIB切片位置;(c)FIB切片前独居石表面纳米孔隙形貌特征;(d)独居石FIB薄片(~100 nm);Ap.磷灰石;Kfs.钾长石;Kln.高岭石;Mnz.独居石;Py.黄铁矿;Qtz.石英

Fig.7 BSE microtextures of corroded monazite with FIB-milled cross-section markers

图8 纳米孔隙结构的STEM-EDS元素面分布左上图为图7(d)红框位置高角度环形暗场图像,其余为对应元素DEX面扫图像,铀沿溶蚀孔隙边缘富集

Fig.8 STEM-EDS elemental mapping of nanopore architecture

图9 独居石纳米孔隙的明场透射电子显微解析 (a) 溶蚀独居石纳米孔隙透射电镜明场图像;(b)为(a)纳米孔隙选区分析位置透射电镜亮场图像;(c) 独居石和相邻氢铀云母的晶格条纹图像,其中右上角为所选区域独居石选区衍射图;(d)为(c)所选区域的氢铀云母选区衍射图;(e) 氢铀云母晶格条纹图像,其中右上角为所选区域氢铀云母多晶环状衍射图;(f) 沥青铀矿与独居石和氢铀云母相邻的晶格条纹图像,其中右上角为所选区域沥青铀矿多晶环状衍射图;(g)为图(f)中所选区域的沥青铀矿选区衍射图;(h)为图(f)中所选区域的氢铀云母选区衍射图;(i) 沥青铀矿和相邻独居石的晶格条纹图像,其中右上角为所选区域沥青铀矿选区衍射图,晶体衍射图像中每组数字为该矿物对应晶面的晶面指数;Ckv.氢铀云母;Mnz.独居石;Pit.沥青铀矿

Fig.9 Bright-field TEM characterization of nanoscale porosity in monazite

图10 有机酸介导的独居石溶解与氢铀云母结晶耦合机制(据文献[40,47-49]修改) 有机酸结构通式R-COOH,R表示不同性质的酸酚

Fig.10 Coupled mechanism of monazite dissolution and meta-autunite crystallization mediated by organic acids (modified from references [40,47-49])

图11 独居石与氢铀云母晶体原子模型 (a)CePO4沿[111]晶带轴方向原子排列模型;(b)沿[111]晶带轴方向独居石透射电镜高分辨晶格条纹图像;(c)图(b)中独居石选区分析的Ce原子排列;(d)H3O(U2O)PO4(H2O)3沿[111]晶带轴方向原子排列模型;(e)沿[111]晶带轴方向氢铀云母透射电镜高分辨晶格条纹图像;(f)图(e)中氢铀云母选区分析的U原子排列;Ckv.氢铀云母;Mnz.独居石

Fig.11 Atomic-scale structural models at monazite and chernikovite interface

图12 砂岩型铀矿中独居石生物地球化学溶蚀动力学模型(据文献[14]修改) (a)海力锦铀矿床成矿示意图;(b)同沉积过程中碎屑独居石与其他碎屑矿物组合;(c)有机酸溶蚀碎屑独居石;(d)早期成岩阶段碎屑独居石、长石、钛铁矿遭受蚀变;(e)独居石进一步溶蚀结晶形成氢铀云母纳米矿物;(f)晚期成岩阶段独居石呈溶蚀残留状态存在;(g)弱碱性流体溶解氢云母释放铀并还原结晶形成沥青铀矿纳米矿物;Ap.磷灰石;Ckv.氢铀云母;Ilm.钛铁矿;Kfs.钾长石;Kln.高岭石;Mnz.独居石;Pit.沥青铀矿;Qtz.石英;Tdo.多孔氧化钛

Fig.12 Bio-geochemical dissolution kinetics model of monazite in sandstone-hosted uranium deposits (modified from reference [14])

图13 溶蚀过程中独居石主微量元素演化趋势 (a)碎屑独居石到溶蚀独居石的UO2含量变化特征;(b)碎屑独居石到溶蚀独居石的Th/U含量变化特征

Fig.13 Evolutionary trends of major trace elements in monazite during dissolution

表1 独居石微区电子探针分析数据集

Table 1 Major and trace element concentrations of monazite by electron probe microanalysis (EPMA)

主量元素 (%)	样品编号					最大值	最小值	平均值
主量元素 (%)	1-1	1-2	1-3	1-4	1-5	最大值	最小值	平均值
SiO₂	0.27	0.26	0.31	-	-	0.31	0.26	0.27
ThO₂	3.87	3.18	3.43	4.18	3.72	4.18	3.`18	3.72
UO₂	0.32	0.30	0.36	0.26	0.25	0.36	0.25	0.30
P₂O₅	29.00	29.05	29.38	28.84	29.00	29.38	28.84	29.00
La₂O₃	11.45	11.20	10.73	10.34	10.70	11.45	10.34	10.73
Ce₂O₃	33.56	32.53	34.30	38.64	37.82	38.64	32.53	34.30
Pr₂O₃	4.06	3.20	3.87	3.36	3.75	4.06	3.20	3.75
Nd₂O₃	11.87	11.50	12.95	11.53	11.22	12.95	11.22	11.53
Sm₂O₃	2.36	2.06	2.60	1.58	1.73	2.60	1.58	2.06
Eu₂O₃	0.62	0.81	0.54	0.69	0.76	0.81	0.54	0.69
Gd₂O₃	1.29	2.30	1.36	0.73	0.70	2.30	0.70	1.29
Dy₂O₃	0.78	0.82	0.09	0.05	0.23	0.82	0.05	0.23
Y₂O₃	1.11	1.32	0.21	0.16	0.12	1.32	0.12	0.21
Lu₂O₃	-	0.05	0.14	0.19	0.20	0.20	0.05	0.17
SO₃	0.03	0.03	-	0.01	0.02	0.03	0.01	0.03
CaO	0.80	0.81	0.80	0.04	-	0.81	0.04	0.80
Total	101.39	99.44	101.50	100.59	100.20	101.50	99.44	100.59
Th/U	12.01	10.50	9.60	16.14	15.11	16.14	9.60	12.01
主量元素 (%)	样品编号					最大值	最小值	平均值
主量元素 (%)	2-1	2-2	2-3	2-4	2-5	最大值	最小值	平均值
SiO₂	0.28	0.26	0.24	0.29	0.19	0.29	0.19	0.26
ThO₂	4.00	4.08	4.03	4.21	4.09	4.21	4.00	4.08
UO₂	0.06	0.05	0.10	0.05	0.10	0.10	0.05	0.06
P₂O₅	28.85	28.84	28.75	28.51	28.67	28.85	28.51	28.75
La₂O₃	11.15	10.82	11.09	11.22	12.82	12.82	10.82	11.15
Ce₂O₃	31.15	32.10	31.35	32.24	33.79	33.79	31.15	32.10
Pr₂O₃	3.97	4.05	3.87	3.60	4.03	4.05	3.60	3.97
Nd₂O₃	12.51	12.52	11.61	12.26	11.29	12.52	11.29	12.26
Sm₂O₃	2.32	2.11	2.43	2.25	1.88	2.43	1.88	2.25
Eu₂O₃	0.66	0.44	0.80	0.61	0.62	0.80	0.44	0.62
Gd₂O₃	1.75	1.62	2.14	1.50	1.95	2.14	1.50	1.75
Dy₂O₃	0.35	0.42	-	0.67	0.18	0.67	0.18	0.39
Y₂O₃	1.67	1.85	2.06	1.69	1.31	2.06	1.31	1.69
Lu₂O₃	0.20	0.10	0.10	-	-	0.20	0.10	0.10
SO₃	-	-	-	0.01	0.01	0.01	0.01	0.01
CaO	0.80	0.77	0.91	0.79	0.51	0.91	0.51	0.79
Total	99.73	100.03	99.47	99.90	100.45	100.45	99.47	99.90
Th/U	64.52	75.46	41.52	84.26	42.65	84.26	41.52	64.52

表1 独居石微区电子探针分析数据集

Table 1 Major and trace element concentrations of monazite by electron probe microanalysis (EPMA)

主量元素 (%)	样品编号					最大值	最小值	平均值
主量元素 (%)	1-1	1-2	1-3	1-4	1-5	最大值	最小值	平均值
SiO₂	0.27	0.26	0.31	-	-	0.31	0.26	0.27
ThO₂	3.87	3.18	3.43	4.18	3.72	4.18	3.`18	3.72
UO₂	0.32	0.30	0.36	0.26	0.25	0.36	0.25	0.30
P₂O₅	29.00	29.05	29.38	28.84	29.00	29.38	28.84	29.00
La₂O₃	11.45	11.20	10.73	10.34	10.70	11.45	10.34	10.73
Ce₂O₃	33.56	32.53	34.30	38.64	37.82	38.64	32.53	34.30
Pr₂O₃	4.06	3.20	3.87	3.36	3.75	4.06	3.20	3.75
Nd₂O₃	11.87	11.50	12.95	11.53	11.22	12.95	11.22	11.53
Sm₂O₃	2.36	2.06	2.60	1.58	1.73	2.60	1.58	2.06
Eu₂O₃	0.62	0.81	0.54	0.69	0.76	0.81	0.54	0.69
Gd₂O₃	1.29	2.30	1.36	0.73	0.70	2.30	0.70	1.29
Dy₂O₃	0.78	0.82	0.09	0.05	0.23	0.82	0.05	0.23
Y₂O₃	1.11	1.32	0.21	0.16	0.12	1.32	0.12	0.21
Lu₂O₃	-	0.05	0.14	0.19	0.20	0.20	0.05	0.17
SO₃	0.03	0.03	-	0.01	0.02	0.03	0.01	0.03
CaO	0.80	0.81	0.80	0.04	-	0.81	0.04	0.80
Total	101.39	99.44	101.50	100.59	100.20	101.50	99.44	100.59
Th/U	12.01	10.50	9.60	16.14	15.11	16.14	9.60	12.01
主量元素 (%)	样品编号					最大值	最小值	平均值
主量元素 (%)	2-1	2-2	2-3	2-4	2-5	最大值	最小值	平均值
SiO₂	0.28	0.26	0.24	0.29	0.19	0.29	0.19	0.26
ThO₂	4.00	4.08	4.03	4.21	4.09	4.21	4.00	4.08
UO₂	0.06	0.05	0.10	0.05	0.10	0.10	0.05	0.06
P₂O₅	28.85	28.84	28.75	28.51	28.67	28.85	28.51	28.75
La₂O₃	11.15	10.82	11.09	11.22	12.82	12.82	10.82	11.15
Ce₂O₃	31.15	32.10	31.35	32.24	33.79	33.79	31.15	32.10
Pr₂O₃	3.97	4.05	3.87	3.60	4.03	4.05	3.60	3.97
Nd₂O₃	12.51	12.52	11.61	12.26	11.29	12.52	11.29	12.26
Sm₂O₃	2.32	2.11	2.43	2.25	1.88	2.43	1.88	2.25
Eu₂O₃	0.66	0.44	0.80	0.61	0.62	0.80	0.44	0.62
Gd₂O₃	1.75	1.62	2.14	1.50	1.95	2.14	1.50	1.75
Dy₂O₃	0.35	0.42	-	0.67	0.18	0.67	0.18	0.39
Y₂O₃	1.67	1.85	2.06	1.69	1.31	2.06	1.31	1.69
Lu₂O₃	0.20	0.10	0.10	-	-	0.20	0.10	0.10
SO₃	-	-	-	0.01	0.01	0.01	0.01	0.01
CaO	0.80	0.77	0.91	0.79	0.51	0.91	0.51	0.79
Total	99.73	100.03	99.47	99.90	100.45	100.45	99.47	99.90
Th/U	64.52	75.46	41.52	84.26	42.65	84.26	41.52	64.52

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