尕斯库勒盐湖卤水与沉积物中铀的分布及富集机理
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摘要
盐湖蕴藏着丰富的矿产资源而被广泛关注。铀在盐湖中的分布及其来源的研究一直是很多研究者感兴趣的问题。尕斯库勒盐湖位于青海省柴达木盆地西北部，已有研究发现该盐湖卤水中铀含量不但远远超过海水中铀的浓度，而且也高于柴达木盆地盐湖的平均值。因此，对该盐湖卤水和沉积物中铀的分布、来源、富集因素进行研究具有特殊意义。
本论文在充分收集资料和现场调查之后，采集了该盐湖周缘和内部的水样、沉积物以及干盐滩盐滩卤水和沉积物样品，主要分析了铀含量、水化学组分、铀同位素等，并开展了室内实验。在详细研究该盐湖区域地质、水文地质、沉积特征、水文地球化学环境特征、孢粉组合特征、280ka以来古气候变化的基础上，结合盐湖铀源、沉积物和卤水中铀的分布，从构造背景、铀源条件、地下水动力条件、沉积旋回、古气候条件、水体演化6个方面分析了铀在盐湖中分布的影响因素，最后总结了该盐湖铀富集模式。取得了如下研究成果：
1.淡水中，浅部水体（河水、沼泽水、潜水）铀含量平均值约为深部水体（承压水、井水、油田水）的10倍。盐滩卤水平均铀含量为78.08μg/L，与柴达木盆地盐湖湖表卤水平均铀含量相当，且分布不均匀。横向上，盐滩卤水中铀的分布受淡水补给影响严重，即离补给源越近铀含量越低，反之亦然；纵向上，铀含量相对高的卤水主要分布在蒸发岩沉积期，而碎屑沉积期相对较低，且同一个晶间卤水层内铀含量垂直分异明显，随深度增加而递减。卤水铀含量变化范围为13.90～933.00μg/L，平均值为274.17μg/L，为海水平均铀含量的83.08倍，为柴达木盆地盐湖湖表卤水平均铀含量的2.83倍。湖表卤水-晶间卤水-盐田卤水，铀含量逐渐升高，而到了老卤水铀含量有一定程度降低。
2.钻孔沉积物铀含量分布范围为0.19～15.80μg/g，平均含量为3.37μg/g。各钻孔沉积物之间的铀含量差别较大。横向上，与卤水中铀含量分布规律类似，钻孔沉积物铀含量受淡水补给影响大，即距离补给源越远，则铀含量越高，反之亦然；纵向上，铀含量相对高值主要分布在碎屑沉积期，而蒸发岩沉积期的铀含量相对较低，且同一个晶间卤水层或者碎屑物沉积层内铀含量垂直分异明显，存在着随深度增加而递增的规律。纯盐类（石盐、泻利盐、石膏）中平均铀含量为1.02μg/g，约为沉积物中铀含量的1/3。该盐湖沉积物中2/3的铀被粘土质点吸附，1/3的铀夹杂在盐类矿物中。盐湖所有固体的平均铀含量为3.33μg/g。干盐滩中毛细蒸发和淋滤作用等的化学沉积分异作用对卤水和沉积物中铀的富集具有十分重要的意义。
3. ZK06孔沉积物共统计陆生植物花粉7863粒，平均每个样品315粒，孢粉较丰富，共发现并鉴定了32个科属的植物。参照植物生态习性所反映的气候特性，结合岩性特征将其自下而上划分为6个孢粉组合带。根据孢粉组合特征，该盐湖自280ka以来植被演化趋势为：疏林草原→灌丛草原→荒漠草原，气候：凉略湿→凉略干→冷干。铀含量与孢粉总浓度、灌木、蒿属呈明显的正相关，与草本植物浓度呈正相关。凉湿气候带内平均铀含量为冷干气候带的3倍，因此气候越干旱和寒冷，沉积物中的铀含量越低，而气候凉湿对沉积物富集铀有利。
4.通过淋滤实验表明盐湖周缘第四纪沉积物中的U最容易被淋出，上新世含盐岩系中的U次之，蚀源区岩石难淋出。由悬浮平衡实验可知，在盐湖内U从悬浮颗粒物进入悬浮液的迁移能力一般。而且U在卤水和沉积物间的迁移系数KU变化趋势与悬浮液中U含量变化趋势一致。通过淋滤实验和悬浮平衡实验确定了该盐湖铀的来源主要为上新世含盐岩系的风化淋滤作用、周边岩石风化剥蚀作用和深部水补给。利用铀系法计算得知，三种补给来源分别占该盐湖铀补给总量的80.4%、18.7%、0.9%。
5.该盐湖铀富集的机理可概括为多因素复合成因模式，具体富集过程为：外围山系基岩、含盐岩系、第四纪沉积物经过降水和地表水淋滤之后进入盐湖，与深部水混合之后在盐湖表面蒸发、浓缩而进一步富集，在富集过程中，受到地下水动力、沉积旋回、古气候、水体演化等因素的控制。其中，铀源条件和水体演化是主要控制因素，区域构造背景、古气候条件和地下水动力条件次之，而沉积旋回对铀富集影响较小。
Salt lakes have been extensively studied owing for its abundant mineralresources. Thus，many researchers pay high attention to the questions about thedistribution of U in the salt lake and its source. It has been found that the uranium inGasikule Salt Lake which located at the northwest of Qaidam Basin is not only higherthan the concentration of the average seawater but also exceed that of the averagebrines in the Qaidam Basin. Therefore，it is particularly significant to study thedistribution，sources，and enrichment factors of uranium in the Gasikule Salt Lake.
When I started my this study，I collected all kinds of information about thewaters，brines and sediments of periphery area and eastern playa’s boreholes in theGasikule Salt Lake. Then，I measured the uranium concentration，hdyrochemicalcomposition，trace elements，chronology，uranium isotope. Based on the regionalgeology，hydrogeology，sedimentary characteristics，hydrogeochemistry，sedimentarygeochemistry， pollen assemblage characteristics， palaeoclimate since280ka， Ianalysed the factors which influenced the uranium distribution in the salt lake fromtectonic setting，sources，hydrodynamic conditions，sedimentary cycle，palaeoclimateto water evolution. I showed the uranium enrichment mode in the end. From all ofabove，the main results can be summaried as follows.
1. In fresh water，uranium concentration in shallow water (stream water，swampwater，phreatic water) is higher than in deep water (artesian water，well water，oilfield water) for10times. The average uranium concentration of drillcores brines is78.08μg/L，which is the same as the superficial brines in Qaidam Basin. Horizontally，the distribution of uranium in drillcores brines was seriously affected by the freshwater supply，ie the uranium concentrations generally increase with farmer from thefresh water. Vertically，uranium concentrations in evaporite deposition’s brine higherthan debris deposition. Moreover，uranium contentations vertical differentiationsignificantly in a crystal brine layer and decreasing with increasing depth. Theconcentrations of uranium in brines range between13.90～933.00μg/L， averaging of274.17μg/L，which is not only the83.08times of the seawater，but also the2.83timesof the superficial brines in Qaidam Basin. Uranium concentrations increase from superficial brines，intercrystalline brines to salt-bond brines，while decrease in thebittern brines.
2. The concentrations of uranium sedimentation range between0.19～15.80μg/g，averaging of3.37μg/g. There was large different uranium concentration indrillcores sedimentations. Horizontally，the distribution of uranium in drillcoressedimentations was seriously affected by the fresh water supply，ie the uraniumconcentrations generally increase with farmer from the fresh water. Vertically，uranium concentrations in debris deposition were higher than evaporite period.Moreover，uranium contentations vertical differentiation significantly in a crystalbrine layer or debris layer and increasing with deeper sedimentation. The averageuranium concentration in pure salts (halite，epsomite，gypsum) was1.02μg/g，whichwas approximately one third of sedimentations. Therefore，two thirds of uranium insedimentation was absorbed by clay while one third uranium was mingled with salineminerals. Chemical sedimentary differentiation in play such as capillary evaporationand leaching was very significant to uranium enrichment in brines andsedimentations.
3. Through laboratory analysis，about7863terrestrial plant pollens were found inZK06drillcore sedimentations and an average of315per sample. According to plantecological habits，we divided into six pollen assemblage zones combined with itslithology from102.69m. Referring to pollen assemblage characteristics，Gasikule SaltLake’s paleo-vegetation changed from veld to desert steppe，and the paleo-climatechanged from cool and mid wet to cold and dry from280ka. Uranium concentration insediments was significantly correlated with total Sporo-pollen concentration，Shrubsand Artemisia，and also with herb concentration. The uranium concentration incool-mid climatical zones is very high，averagely three times as high as that in cold-dry zones. This climate evolution was benefit for uranium transform fromprovenance to salt lake and pre-enrichment.
4. Based on the data of equilibration experiments and leaching experiments，uranium in the Salt Lake peripheral Quaternary sediments most easily to be leachedout，salt bearing rock in Pliocene was secondly，and provenance rocks were mostdifficult. Ability of uranium migrated from suspended particles to suspended liquid is normal. Moreover，the trend of migration coefficient (KU) between brines andsedimentations was consistent with uranium concentrations in suspended liquid.Through the leaching experiment and equilibration experiments，we could concludethat uranium in this salt lake come from Pliocene salt bearing rocks，provenance rocksand depth water. According to U-series nuclides calculation，uranium recharge ratiofrom Pliocene salt bearing rocks，provenance rocks and depth water account for about18.7%，80.4%and0.9%respectively.
5. Uranium enrichment mechanism in Gasikule Salt Lake could be summarizedas a compound origin model which would be specific showed as follow. Uraniumfrom peripherial base rock，salt bearing rock and Quaternary sediments was leachatedby rain and superficial water and then enter salt lake. Uranium was foremore enrichedin salt lake after mingled with deep water. During the enrichment process，uraniumconcentrations were affected by the hydrodynamic conditions，deposition cycle，palaeoclimate and water evolution. In all influential factors，sources and waterevolution were dominance principles， tectonic setting， palaeoclimate andhydrodynamic conditions were secondary affecting factors，but deposition cycle wasminimum factor.
本论文在充分收集资料和现场调查之后，采集了该盐湖周缘和内部的水样、沉积物以及干盐滩盐滩卤水和沉积物样品，主要分析了铀含量、水化学组分、铀同位素等，并开展了室内实验。在详细研究该盐湖区域地质、水文地质、沉积特征、水文地球化学环境特征、孢粉组合特征、280ka以来古气候变化的基础上，结合盐湖铀源、沉积物和卤水中铀的分布，从构造背景、铀源条件、地下水动力条件、沉积旋回、古气候条件、水体演化6个方面分析了铀在盐湖中分布的影响因素，最后总结了该盐湖铀富集模式。取得了如下研究成果：
1.淡水中，浅部水体（河水、沼泽水、潜水）铀含量平均值约为深部水体（承压水、井水、油田水）的10倍。盐滩卤水平均铀含量为78.08μg/L，与柴达木盆地盐湖湖表卤水平均铀含量相当，且分布不均匀。横向上，盐滩卤水中铀的分布受淡水补给影响严重，即离补给源越近铀含量越低，反之亦然；纵向上，铀含量相对高的卤水主要分布在蒸发岩沉积期，而碎屑沉积期相对较低，且同一个晶间卤水层内铀含量垂直分异明显，随深度增加而递减。卤水铀含量变化范围为13.90～933.00μg/L，平均值为274.17μg/L，为海水平均铀含量的83.08倍，为柴达木盆地盐湖湖表卤水平均铀含量的2.83倍。湖表卤水-晶间卤水-盐田卤水，铀含量逐渐升高，而到了老卤水铀含量有一定程度降低。
2.钻孔沉积物铀含量分布范围为0.19～15.80μg/g，平均含量为3.37μg/g。各钻孔沉积物之间的铀含量差别较大。横向上，与卤水中铀含量分布规律类似，钻孔沉积物铀含量受淡水补给影响大，即距离补给源越远，则铀含量越高，反之亦然；纵向上，铀含量相对高值主要分布在碎屑沉积期，而蒸发岩沉积期的铀含量相对较低，且同一个晶间卤水层或者碎屑物沉积层内铀含量垂直分异明显，存在着随深度增加而递增的规律。纯盐类（石盐、泻利盐、石膏）中平均铀含量为1.02μg/g，约为沉积物中铀含量的1/3。该盐湖沉积物中2/3的铀被粘土质点吸附，1/3的铀夹杂在盐类矿物中。盐湖所有固体的平均铀含量为3.33μg/g。干盐滩中毛细蒸发和淋滤作用等的化学沉积分异作用对卤水和沉积物中铀的富集具有十分重要的意义。
3. ZK06孔沉积物共统计陆生植物花粉7863粒，平均每个样品315粒，孢粉较丰富，共发现并鉴定了32个科属的植物。参照植物生态习性所反映的气候特性，结合岩性特征将其自下而上划分为6个孢粉组合带。根据孢粉组合特征，该盐湖自280ka以来植被演化趋势为：疏林草原→灌丛草原→荒漠草原，气候：凉略湿→凉略干→冷干。铀含量与孢粉总浓度、灌木、蒿属呈明显的正相关，与草本植物浓度呈正相关。凉湿气候带内平均铀含量为冷干气候带的3倍，因此气候越干旱和寒冷，沉积物中的铀含量越低，而气候凉湿对沉积物富集铀有利。
4.通过淋滤实验表明盐湖周缘第四纪沉积物中的U最容易被淋出，上新世含盐岩系中的U次之，蚀源区岩石难淋出。由悬浮平衡实验可知，在盐湖内U从悬浮颗粒物进入悬浮液的迁移能力一般。而且U在卤水和沉积物间的迁移系数KU变化趋势与悬浮液中U含量变化趋势一致。通过淋滤实验和悬浮平衡实验确定了该盐湖铀的来源主要为上新世含盐岩系的风化淋滤作用、周边岩石风化剥蚀作用和深部水补给。利用铀系法计算得知，三种补给来源分别占该盐湖铀补给总量的80.4%、18.7%、0.9%。
5.该盐湖铀富集的机理可概括为多因素复合成因模式，具体富集过程为：外围山系基岩、含盐岩系、第四纪沉积物经过降水和地表水淋滤之后进入盐湖，与深部水混合之后在盐湖表面蒸发、浓缩而进一步富集，在富集过程中，受到地下水动力、沉积旋回、古气候、水体演化等因素的控制。其中，铀源条件和水体演化是主要控制因素，区域构造背景、古气候条件和地下水动力条件次之，而沉积旋回对铀富集影响较小。
Salt lakes have been extensively studied owing for its abundant mineralresources. Thus，many researchers pay high attention to the questions about thedistribution of U in the salt lake and its source. It has been found that the uranium inGasikule Salt Lake which located at the northwest of Qaidam Basin is not only higherthan the concentration of the average seawater but also exceed that of the averagebrines in the Qaidam Basin. Therefore，it is particularly significant to study thedistribution，sources，and enrichment factors of uranium in the Gasikule Salt Lake.
When I started my this study，I collected all kinds of information about thewaters，brines and sediments of periphery area and eastern playa’s boreholes in theGasikule Salt Lake. Then，I measured the uranium concentration，hdyrochemicalcomposition，trace elements，chronology，uranium isotope. Based on the regionalgeology，hydrogeology，sedimentary characteristics，hydrogeochemistry，sedimentarygeochemistry， pollen assemblage characteristics， palaeoclimate since280ka， Ianalysed the factors which influenced the uranium distribution in the salt lake fromtectonic setting，sources，hydrodynamic conditions，sedimentary cycle，palaeoclimateto water evolution. I showed the uranium enrichment mode in the end. From all ofabove，the main results can be summaried as follows.
1. In fresh water，uranium concentration in shallow water (stream water，swampwater，phreatic water) is higher than in deep water (artesian water，well water，oilfield water) for10times. The average uranium concentration of drillcores brines is78.08μg/L，which is the same as the superficial brines in Qaidam Basin. Horizontally，the distribution of uranium in drillcores brines was seriously affected by the freshwater supply，ie the uranium concentrations generally increase with farmer from thefresh water. Vertically，uranium concentrations in evaporite deposition’s brine higherthan debris deposition. Moreover，uranium contentations vertical differentiationsignificantly in a crystal brine layer and decreasing with increasing depth. Theconcentrations of uranium in brines range between13.90～933.00μg/L， averaging of274.17μg/L，which is not only the83.08times of the seawater，but also the2.83timesof the superficial brines in Qaidam Basin. Uranium concentrations increase from superficial brines，intercrystalline brines to salt-bond brines，while decrease in thebittern brines.
2. The concentrations of uranium sedimentation range between0.19～15.80μg/g，averaging of3.37μg/g. There was large different uranium concentration indrillcores sedimentations. Horizontally，the distribution of uranium in drillcoressedimentations was seriously affected by the fresh water supply，ie the uraniumconcentrations generally increase with farmer from the fresh water. Vertically，uranium concentrations in debris deposition were higher than evaporite period.Moreover，uranium contentations vertical differentiation significantly in a crystalbrine layer or debris layer and increasing with deeper sedimentation. The averageuranium concentration in pure salts (halite，epsomite，gypsum) was1.02μg/g，whichwas approximately one third of sedimentations. Therefore，two thirds of uranium insedimentation was absorbed by clay while one third uranium was mingled with salineminerals. Chemical sedimentary differentiation in play such as capillary evaporationand leaching was very significant to uranium enrichment in brines andsedimentations.
3. Through laboratory analysis，about7863terrestrial plant pollens were found inZK06drillcore sedimentations and an average of315per sample. According to plantecological habits，we divided into six pollen assemblage zones combined with itslithology from102.69m. Referring to pollen assemblage characteristics，Gasikule SaltLake’s paleo-vegetation changed from veld to desert steppe，and the paleo-climatechanged from cool and mid wet to cold and dry from280ka. Uranium concentration insediments was significantly correlated with total Sporo-pollen concentration，Shrubsand Artemisia，and also with herb concentration. The uranium concentration incool-mid climatical zones is very high，averagely three times as high as that in cold-dry zones. This climate evolution was benefit for uranium transform fromprovenance to salt lake and pre-enrichment.
4. Based on the data of equilibration experiments and leaching experiments，uranium in the Salt Lake peripheral Quaternary sediments most easily to be leachedout，salt bearing rock in Pliocene was secondly，and provenance rocks were mostdifficult. Ability of uranium migrated from suspended particles to suspended liquid is normal. Moreover，the trend of migration coefficient (KU) between brines andsedimentations was consistent with uranium concentrations in suspended liquid.Through the leaching experiment and equilibration experiments，we could concludethat uranium in this salt lake come from Pliocene salt bearing rocks，provenance rocksand depth water. According to U-series nuclides calculation，uranium recharge ratiofrom Pliocene salt bearing rocks，provenance rocks and depth water account for about18.7%，80.4%and0.9%respectively.
5. Uranium enrichment mechanism in Gasikule Salt Lake could be summarizedas a compound origin model which would be specific showed as follow. Uraniumfrom peripherial base rock，salt bearing rock and Quaternary sediments was leachatedby rain and superficial water and then enter salt lake. Uranium was foremore enrichedin salt lake after mingled with deep water. During the enrichment process，uraniumconcentrations were affected by the hydrodynamic conditions，deposition cycle，palaeoclimate and water evolution. In all influential factors，sources and waterevolution were dominance principles， tectonic setting， palaeoclimate andhydrodynamic conditions were secondary affecting factors，but deposition cycle wasminimum factor.
引文
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