贵州云峰铝土矿中铀矿物的发现
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摘要
有关铝土矿中铀富集的报道很多,但至今未见独立铀矿物存在的相关文献。本次研究采用岩相学观察、X衍射(XRD)、ICP-MS、电子探针(EPMA)、拉曼光谱分析等手段,对黔中典型的铝土矿——云峰铝土矿中的晶质铀矿进行了研究。研究发现该铝土矿床中,铀富集明显(w(U)(18×10~(-6)～62×10~(-6)),平均值35×10~(-6)),铀矿物大小呈微米至亚微米级,围绕锐钛矿边缘生长、或充填于高岭石微裂隙中、或散布于与黄铁矿密切相关的高岭石或硬水铝石中。铀矿物的主要组分为UO_2(w(UO_2)为52.2%～80.88%)和TiO_2(w(TiO_2)为1.85%～14.98%);电子探针面扫描显示铀矿物中钛分布不均匀;铀矿物的拉曼特征波长为442 cm~(-1)和454 cm~(-1),因此,初步推测铀矿物为晶质铀矿和含钛晶质铀矿。其形成过程大致如下,来源于下寒武统牛蹄塘组黑色岩系中的铀(U~(4+))在风化过程中氧化为U~(6+)、析出、被Al~-, Fe~-氧化物/氢氧化物吸附;在沉积和成岩过程中,随着三水铝石转变为勃姆石和硬水铝石、铁氧化/氢氧化物转变为黄铁矿,吸附的铀解吸、还原(U~(6+)至U~(4+))、最后形成铀矿物。
Elevated concentrations of uranium have been found in many bauxite deposits, however, occurrence of separate U-minerals in the bauxite deposits has not yet been reported. In this paper, the authors carried out petrographic, XRD,ICP-MS, electron probe micro-analyzer(EPMA) and Raman spectroscopic studies of bauxite ores from the Yunfeng deposit, one of typical bauxite deposits in central Guizhou. The results show that the bauxite ores are characterized by high content of uranium(18×10~(-6) to 62×10~(-6), averagely 35×10~(-6)). Micron-to submicron-sized grains uraninite occurs as rims of Ti-oxides, fillings of micro-fractures in kaolinite, and disseminated grains in association with sulfides in the matrix of diaspore and kaolinite. EPMA analysis indicates that the U-minerals are mainly composed of UO_2(w(UO_2)52.2% to 80.88%) and TiO_2(w(TiO_2) 1.85% to 14.98%) which are unevenly distributed in the U-minerals. Raman spectroscopic analyses show that the Raman peaks appear at around 442 cm~(-1) and 454 cm~(-1) for the U-minerals.The U-mine rals are suggested to be uraninite and Ti-bearing uraninite. The formation of uraninite is inferred as fol-lowing stages, during weathering stage, uranium was liberated from the source rock(the Lower Cambrian black shales of the Niutitang Formation) due to oxidation uranium from U~(4+)to U~(6+), subsequently, most of the U~(6+)was absorbed by Al~-, Fe-Oxide/hydroxide. During deposition and diagenesis stages, the majority of U~(6+)was liberated from the Al~-, Fe-Oxide/hydroxide, reduced to U~(4+)again and finally converted to uraninite, together with the convention of gibbsite to boehmite and diaspore as well as the Fe-Oxide/hydroxide to pyrite.
Elevated concentrations of uranium have been found in many bauxite deposits, however, occurrence of separate U-minerals in the bauxite deposits has not yet been reported. In this paper, the authors carried out petrographic, XRD,ICP-MS, electron probe micro-analyzer(EPMA) and Raman spectroscopic studies of bauxite ores from the Yunfeng deposit, one of typical bauxite deposits in central Guizhou. The results show that the bauxite ores are characterized by high content of uranium(18×10~(-6) to 62×10~(-6), averagely 35×10~(-6)). Micron-to submicron-sized grains uraninite occurs as rims of Ti-oxides, fillings of micro-fractures in kaolinite, and disseminated grains in association with sulfides in the matrix of diaspore and kaolinite. EPMA analysis indicates that the U-minerals are mainly composed of UO_2(w(UO_2)52.2% to 80.88%) and TiO_2(w(TiO_2) 1.85% to 14.98%) which are unevenly distributed in the U-minerals. Raman spectroscopic analyses show that the Raman peaks appear at around 442 cm~(-1) and 454 cm~(-1) for the U-minerals.The U-mine rals are suggested to be uraninite and Ti-bearing uraninite. The formation of uraninite is inferred as fol-lowing stages, during weathering stage, uranium was liberated from the source rock(the Lower Cambrian black shales of the Niutitang Formation) due to oxidation uranium from U~(4+)to U~(6+), subsequently, most of the U~(6+)was absorbed by Al~-, Fe-Oxide/hydroxide. During deposition and diagenesis stages, the majority of U~(6+)was liberated from the Al~-, Fe-Oxide/hydroxide, reduced to U~(4+)again and finally converted to uraninite, together with the convention of gibbsite to boehmite and diaspore as well as the Fe-Oxide/hydroxide to pyrite.
引文
Cai Y Q,Zhang J D,Li Z Y,Guo Q Y,Song J Y,Fan H H,Liu W S,Qi F C and Zhuang M L.2015.Qutilne of uranium resources characteristics and metallogenetic regularity in China[J].Acta Geologica Sinica,89(6):1051-1069(in Chinese with English abstract).
Cumberland S A,Douglas G,Grice K and Moreau J W.2016.Uranium mobility in organic matter-rich sediments:A review of geological and geochemical processes[J].Earth-Science Reviews,159:160-185.
Deng X,Yang K G,Liu Y L and She Z B.2010.Characteristics and tectonic evolution of Qianzhong Uplift[J].Earth Science Frontiers,17(3):79-89(in Chinese with English abstract).
Hanil?i N.2013.Geological and geochemical evolution of the Bolkarda?i bauxite deposits,Karaman,Turkey:Transformation from shale to bauxite[J].Journal of Geochemical Exploration,133:118-137.
Hou B H,Keeling J and Li Z.2017.Paleovalley-related uranium deposits in Australia and China:A review of geological and exploration models and methods[J].Ore Geology Reviews,88:201-234.
Huang Z L,Jin Z G,Xiang X L,Gu J,Wu G H,Chen X L,Su Z L,Zhao Y Y,Ye L and Zuo L.2014.Mectallogenic theory and prediction of bauxite deposits in the Wuchunan-Zheng’an-Daozhen area,northern Guizhou Province,China[M].Beijing:Science Press.89-99(in Chinese).
Jaireth S,Roach I C,Bastrakov E and Liu S F.2015.Basin-related uranium mineral systems in Australia:A review of critical features[J].Ore Geology Reviews,76:360-394.
Ju Y Z,Lin G M,Jing W P,Wen Z,Peng C A and Zhang Z.2018.Carbon and oxygen isotope characteristics and mineralization of black shale-hosted manganese carbonate of Datangpo Formation in Tongren,Guizhou Province[J].Mineral Deposits,37(1):50-66(in Chinese with English abstract).
Li J,Yu B S and Guo F.2013.Depositional setting and tectonic background analysis on Lower Cambrian black shales in the North of Guizhou Province[J].Acta Sedimentologica Sinica,31(1):20-31(in Chinese with English abstract).
Liao S F.1989.Ancient geography and metallogenic conditions of ancient weathering bauxite deposits of early carboniferous in Guizhou-Sichuan-Hunan-Hubei[J].Acta Geologica Sinica,63(2):148-157(in Chinese).
Ling K Y,Zhu X Q,Tang H S,Wang Z G,Yan H W,Han T and Chen W Y.2015.Mineralogical characteristics of the karstic bauxite deposits in the Xiuwen ore belt,Central Guizhou Province,southwest China[J].Ore Geology Reviews,65:86-96.
Long Y Z,Chi G X,Liu J P,Jin Z G and Dai T G.2017.Trace and rare earth elements constraints on the sources of the Yunfeng paleokarstic bauxite deposit in the Xiuwen-Qingzhen area,Guizhou,China[J].Ore Geology Reviews,91:404-418.
Mao J W.2001.Study trends of ore deposits about the black shale series[J].Mineral Deposidts,20(4):402-403(in Chinese).
Min M Z,Peng X J,Wang G and Yin J H.2006.Existing state of uranium in ore from interlayer oxidation zone sandstone-hosted uranium deposits,NW China[J].Uranium Geology,22(4):193-201(in Chinese with English abstract).
No.245 Team of Hunan Provincial Nonferrous Geological Exploration Bureau.1960.Radioactivity survey report in Lijiatian bauxite deposit,Luxi,Hunan[R].(in Chinese).
Palacios M L and Taylor S H.2000.Characterization of uranium oxides using in-situ microRaman spectroscopy[J].Applied Spectroscopy,54:1372-1378.
Pi D H,Liu C Q,Shields-Zhou G A and Jiang S Y.2013.Trace and rare earth element geochemistry of black shale and kerogen in the Early Cambrian Niutitang Formation in Guizhou Province,South China:Constraints for redox environments and origin of metal enrichments[J].Precambrian Research,225:218-229.
Pisarzowaka A,Berner Z A and Racki G.2014.Geochemistry of Early Frasnian(Late Devonian)pyrite-ammonoid level in the Kostom?oty Basin,Poland,and a new proxy parameter for assessing the relative amount of syngenetic and diagenetic pyrite[J].Sedimentary Geology,308:18-31.
Tang C,Shao L Y and Xing W L.2017.Analysis of the safety problem of China’s uranium resources[J].China Mining Magazine,26(5):1-6(in Chinese with English abstract).
Tao S,Tang D Z,Zou C Y,Li F,Li J J and Chen X.2009.Element geochemical characteristics of the lower assemblage hydrocarbon source rocks in southeast Sichuan-Central Guizhou(Chuandongnan-Qianzhong)region and its periphery areas and their implications to sedimentary environments[J].Geology in China,36(2):397-403(in Chinese with English abstract).
Taylor S R and McLennan S M.1985.The continental crust:Its composition and evolution[M].Oxford:Blackwell.1-312.
Villar LP,Bruno J,Campos R,Gomez P,Cozar J S,Garralon A,Buil B,Arcos D,Carretero G,Sanchez-porro J R and Hernan P.2002.The uranium ore from Mina Fe(Salamanca,Spain)as a natural analogue of processes in a spent fuel repository[J].Chemical Geology,190:395-415.
Wang Q,Liu X,Yan C,Cai S,Li Z,Wang Y,Zhao J and Li G.2012.Mineralogical and geochemical studies of boron-rich bauxite ore deposits in the Songqi region,SW Henan,China[J].Ore Geology Reviews,48:258-270.
Wang W G.2015.The Discover of Brannerite and Uraninite in Lower Cambrian U-bearing phosphorite in West Hunan[J].Uranium Geology.31(1):19-28(in Chinese with English abstract).
Wilkin R T,Arthur M A and Dean W E.1997.History of water-column anoxia in the Black Sea indicated by pyrite framboid size distributions[J].Earth and Planetary Science Letters,148:517-525.
Wilkin R T,Barnes H L and Brantley S L.1996.The size distribution of framboidal pyrite in modern sediments:An indicator of redox conditions[J].Geochimica et Cosmochimica Acta,60(20):3897-3912.
Xiao J Q,Wang Y,Zhong J R and Zhu X H.2012.Raman spectroscopy and its application in analysis of uranium material[J].Chinese Journal of Spectroscopy Laboratory,6:3830-3835(in Chinese with English abstract).
Yang X Y,Ling M X,Sun W D,Luo X D,Lai X D,Liu C Y,Miao J Yand Sun W.2009.The genesis of sandstone-type uranium deposits in the Ordos Basin,NW China:Constraints provided by fluid inclusions and stable isotopes[J].International Geology Review,51(5):422-455.
Yi C,Wang G,Li X D,Zhang K and Wang Y J.2018.A tentative discussion on uranium enrichment characteristics and metallogenic model in Zhiluo Formation,northeastern Ordos Basin[J].Mineral Deposits,37(4):835-852(in Chinese with English abstract).
Zhang Q,Wang Q L,Li Q,Hu E M,Zhang H C and Yang J.2014.Preparation of aluminum hydroxide colloid and its adsorption mechanism for uranium(Ⅵ)[J].CIESC Journal,65(4):1279-1286(in Chinese with English abstract).
Zhang Z W,Zhou L J,Li Y J,Wu C Q and Zheng C F.2013.The“coalbauxite-iron”structure in the ore-bearing rock series as a prospec ting indicator for southeastern Guizhou bauxite mines[J].Ore Geology Reviews,53:145-158.
Zhao K D,Jiang S Y,Chen W F,Chen P R and Ling H F.2014.Mineralogy,geochemistry and ore genesis of the Dawan uranium deposit in southern Hunan Province,South China[J].Journal of Geochemical Exploration,138:59-71.
蔡煜琦,张金带,李子颖,郭庆银,宋继叶,范洪海,刘武生,漆富成,张明林.2015.中国铀矿资源特征及成矿规律概要[J].地质学报,89(6):1051-1069.
邓新,杨坤光,刘彦良,佘振兵.2010.黔中隆起性质及其构造演化[J].地学前缘,17(3):79-89.
湖南有色地勘局245队,1960.湖南湘西李家田铝土矿放射性调查报告[R].
黄智龙,金中国,向贤礼,谷静,武国辉,陈兴龙,苏之良,赵远由,叶霖,邹林.2014.黔北务正道铝土矿成矿理论及预测[M].北京:科学出版社.3-167.
李娟,于炳松,郭峰.2013.黔北地区下寒武统底部黑色页岩沉积环境条件与源区构造背景分析[J].沉积学报,31(1):20-31.
廖士范.1989.黔川湘鄂早石炭世古风化壳铝土矿床的古地理与成矿条件的研究[J].地质学报,63(2):148-157.
毛景文.2001.与黑色页岩系有关的矿床研究的动向[J].矿床地质,20(4):402-403.
闵茂中,彭新建,王果,殷建华.2006.我国西北地区层间氧化带砂岩型铀矿床中铀的赋存形式[J].铀矿地质,22(4):193-201.
瞿永泽,徐林刚,毛景文,潘文,占朋才,安正泽.2018.贵州铜仁地区南华系大塘坡组黑色页岩型菱锰矿碳、氧同位素特征及锰矿成矿作用[J].矿床地质,37(1):50-66
唐超,邵龙义,邢万里.2017.中国铀矿资源安全分析[J].中国矿业,26(5):1-6.
陶树,汤达祯,周传祎,李凤,李婧婧,陈晓智.2009.川东南-黔中及其周边地区下组合烃源岩元素地球化学特征及沉积环境意义[J].中国地质,36(2):397-403.
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张琪,王清良,李乾,胡鄂明,张洪灿,杨敬.2014.Al(OH)3胶体的制备及其对铀的吸附机理[J].化工学报,65(4):1279-1286.
Cumberland S A,Douglas G,Grice K and Moreau J W.2016.Uranium mobility in organic matter-rich sediments:A review of geological and geochemical processes[J].Earth-Science Reviews,159:160-185.
Deng X,Yang K G,Liu Y L and She Z B.2010.Characteristics and tectonic evolution of Qianzhong Uplift[J].Earth Science Frontiers,17(3):79-89(in Chinese with English abstract).
Hanil?i N.2013.Geological and geochemical evolution of the Bolkarda?i bauxite deposits,Karaman,Turkey:Transformation from shale to bauxite[J].Journal of Geochemical Exploration,133:118-137.
Hou B H,Keeling J and Li Z.2017.Paleovalley-related uranium deposits in Australia and China:A review of geological and exploration models and methods[J].Ore Geology Reviews,88:201-234.
Huang Z L,Jin Z G,Xiang X L,Gu J,Wu G H,Chen X L,Su Z L,Zhao Y Y,Ye L and Zuo L.2014.Mectallogenic theory and prediction of bauxite deposits in the Wuchunan-Zheng’an-Daozhen area,northern Guizhou Province,China[M].Beijing:Science Press.89-99(in Chinese).
Jaireth S,Roach I C,Bastrakov E and Liu S F.2015.Basin-related uranium mineral systems in Australia:A review of critical features[J].Ore Geology Reviews,76:360-394.
Ju Y Z,Lin G M,Jing W P,Wen Z,Peng C A and Zhang Z.2018.Carbon and oxygen isotope characteristics and mineralization of black shale-hosted manganese carbonate of Datangpo Formation in Tongren,Guizhou Province[J].Mineral Deposits,37(1):50-66(in Chinese with English abstract).
Li J,Yu B S and Guo F.2013.Depositional setting and tectonic background analysis on Lower Cambrian black shales in the North of Guizhou Province[J].Acta Sedimentologica Sinica,31(1):20-31(in Chinese with English abstract).
Liao S F.1989.Ancient geography and metallogenic conditions of ancient weathering bauxite deposits of early carboniferous in Guizhou-Sichuan-Hunan-Hubei[J].Acta Geologica Sinica,63(2):148-157(in Chinese).
Ling K Y,Zhu X Q,Tang H S,Wang Z G,Yan H W,Han T and Chen W Y.2015.Mineralogical characteristics of the karstic bauxite deposits in the Xiuwen ore belt,Central Guizhou Province,southwest China[J].Ore Geology Reviews,65:86-96.
Long Y Z,Chi G X,Liu J P,Jin Z G and Dai T G.2017.Trace and rare earth elements constraints on the sources of the Yunfeng paleokarstic bauxite deposit in the Xiuwen-Qingzhen area,Guizhou,China[J].Ore Geology Reviews,91:404-418.
Mao J W.2001.Study trends of ore deposits about the black shale series[J].Mineral Deposidts,20(4):402-403(in Chinese).
Min M Z,Peng X J,Wang G and Yin J H.2006.Existing state of uranium in ore from interlayer oxidation zone sandstone-hosted uranium deposits,NW China[J].Uranium Geology,22(4):193-201(in Chinese with English abstract).
No.245 Team of Hunan Provincial Nonferrous Geological Exploration Bureau.1960.Radioactivity survey report in Lijiatian bauxite deposit,Luxi,Hunan[R].(in Chinese).
Palacios M L and Taylor S H.2000.Characterization of uranium oxides using in-situ microRaman spectroscopy[J].Applied Spectroscopy,54:1372-1378.
Pi D H,Liu C Q,Shields-Zhou G A and Jiang S Y.2013.Trace and rare earth element geochemistry of black shale and kerogen in the Early Cambrian Niutitang Formation in Guizhou Province,South China:Constraints for redox environments and origin of metal enrichments[J].Precambrian Research,225:218-229.
Pisarzowaka A,Berner Z A and Racki G.2014.Geochemistry of Early Frasnian(Late Devonian)pyrite-ammonoid level in the Kostom?oty Basin,Poland,and a new proxy parameter for assessing the relative amount of syngenetic and diagenetic pyrite[J].Sedimentary Geology,308:18-31.
Tang C,Shao L Y and Xing W L.2017.Analysis of the safety problem of China’s uranium resources[J].China Mining Magazine,26(5):1-6(in Chinese with English abstract).
Tao S,Tang D Z,Zou C Y,Li F,Li J J and Chen X.2009.Element geochemical characteristics of the lower assemblage hydrocarbon source rocks in southeast Sichuan-Central Guizhou(Chuandongnan-Qianzhong)region and its periphery areas and their implications to sedimentary environments[J].Geology in China,36(2):397-403(in Chinese with English abstract).
Taylor S R and McLennan S M.1985.The continental crust:Its composition and evolution[M].Oxford:Blackwell.1-312.
Villar LP,Bruno J,Campos R,Gomez P,Cozar J S,Garralon A,Buil B,Arcos D,Carretero G,Sanchez-porro J R and Hernan P.2002.The uranium ore from Mina Fe(Salamanca,Spain)as a natural analogue of processes in a spent fuel repository[J].Chemical Geology,190:395-415.
Wang Q,Liu X,Yan C,Cai S,Li Z,Wang Y,Zhao J and Li G.2012.Mineralogical and geochemical studies of boron-rich bauxite ore deposits in the Songqi region,SW Henan,China[J].Ore Geology Reviews,48:258-270.
Wang W G.2015.The Discover of Brannerite and Uraninite in Lower Cambrian U-bearing phosphorite in West Hunan[J].Uranium Geology.31(1):19-28(in Chinese with English abstract).
Wilkin R T,Arthur M A and Dean W E.1997.History of water-column anoxia in the Black Sea indicated by pyrite framboid size distributions[J].Earth and Planetary Science Letters,148:517-525.
Wilkin R T,Barnes H L and Brantley S L.1996.The size distribution of framboidal pyrite in modern sediments:An indicator of redox conditions[J].Geochimica et Cosmochimica Acta,60(20):3897-3912.
Xiao J Q,Wang Y,Zhong J R and Zhu X H.2012.Raman spectroscopy and its application in analysis of uranium material[J].Chinese Journal of Spectroscopy Laboratory,6:3830-3835(in Chinese with English abstract).
Yang X Y,Ling M X,Sun W D,Luo X D,Lai X D,Liu C Y,Miao J Yand Sun W.2009.The genesis of sandstone-type uranium deposits in the Ordos Basin,NW China:Constraints provided by fluid inclusions and stable isotopes[J].International Geology Review,51(5):422-455.
Yi C,Wang G,Li X D,Zhang K and Wang Y J.2018.A tentative discussion on uranium enrichment characteristics and metallogenic model in Zhiluo Formation,northeastern Ordos Basin[J].Mineral Deposits,37(4):835-852(in Chinese with English abstract).
Zhang Q,Wang Q L,Li Q,Hu E M,Zhang H C and Yang J.2014.Preparation of aluminum hydroxide colloid and its adsorption mechanism for uranium(Ⅵ)[J].CIESC Journal,65(4):1279-1286(in Chinese with English abstract).
Zhang Z W,Zhou L J,Li Y J,Wu C Q and Zheng C F.2013.The“coalbauxite-iron”structure in the ore-bearing rock series as a prospec ting indicator for southeastern Guizhou bauxite mines[J].Ore Geology Reviews,53:145-158.
Zhao K D,Jiang S Y,Chen W F,Chen P R and Ling H F.2014.Mineralogy,geochemistry and ore genesis of the Dawan uranium deposit in southern Hunan Province,South China[J].Journal of Geochemical Exploration,138:59-71.
蔡煜琦,张金带,李子颖,郭庆银,宋继叶,范洪海,刘武生,漆富成,张明林.2015.中国铀矿资源特征及成矿规律概要[J].地质学报,89(6):1051-1069.
邓新,杨坤光,刘彦良,佘振兵.2010.黔中隆起性质及其构造演化[J].地学前缘,17(3):79-89.
湖南有色地勘局245队,1960.湖南湘西李家田铝土矿放射性调查报告[R].
黄智龙,金中国,向贤礼,谷静,武国辉,陈兴龙,苏之良,赵远由,叶霖,邹林.2014.黔北务正道铝土矿成矿理论及预测[M].北京:科学出版社.3-167.
李娟,于炳松,郭峰.2013.黔北地区下寒武统底部黑色页岩沉积环境条件与源区构造背景分析[J].沉积学报,31(1):20-31.
廖士范.1989.黔川湘鄂早石炭世古风化壳铝土矿床的古地理与成矿条件的研究[J].地质学报,63(2):148-157.
毛景文.2001.与黑色页岩系有关的矿床研究的动向[J].矿床地质,20(4):402-403.
闵茂中,彭新建,王果,殷建华.2006.我国西北地区层间氧化带砂岩型铀矿床中铀的赋存形式[J].铀矿地质,22(4):193-201.
瞿永泽,徐林刚,毛景文,潘文,占朋才,安正泽.2018.贵州铜仁地区南华系大塘坡组黑色页岩型菱锰矿碳、氧同位素特征及锰矿成矿作用[J].矿床地质,37(1):50-66
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