| 硅酸盐熔体-流体共存体系中Cu分配系数的实验研究 |
| 其他题名 | Experimental research on the partitioning coefficients of copper between silicate melts and liquid coexisting
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| 唐群力
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| 2003
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| 学位授予单位 | 中国科学院地球化学研究所
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| 学位授予地点 | 中国科学院地球化学研究所
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| 学位名称 | 博士
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| 学位专业 | 地球化学
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| 关键词 | 实验地球化学
分配系数
硅酸盐固相
液相
盐酸
高温高压
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| 摘要 | 硅酸盐固相与液相共存体系中Cu分配系数研究近年来取得重大进展，但大部分工作主要集中在研究流体组分的变化对Cu分配系数的影响。而固相组成的变化对Cu分配系数的影响则少有涉及。本文作者在相同实验条件、实验流程下成功合成了数个硅酸盐组分初始凝胶。初始凝胶基于精确改变AIUAI，Na/K的相对摩尔比值及SiO_2，Na+K的摩尔含量分为四组，而且同一组内其它组分的相对摩尔含量控制不变。分配实验条件设定为温度800℃，压力Ikbar，时间5天，在此实验条件下讨论了不同成分的初始硅酸盐固相与共存流体相（0.1mol／l的HCI）中Cu的分配系数。通过上述研究，主要得出如下初步认识。在初始固相组成中，Alk＋Al所占的总相对摩尔含量不变，改变初始固相Alk/Al的摩尔比。实验结果表明：在本文实验条件下，铜的分配系数明显地受Alk/Al比值改变的制约。随着Alk/Al的比值从0.666增大到1.500，铜的分配系数由54.16线性下降到16.55。即Al／Alk比值增大有利于硅酸盐固相与液相共存体系中铜在流体相中富集。控制Na＋K在初始固相中的摩尔百分含量不变，改变Na/K的比值。实验结果表明：尽管Na/K的比值在一个较大的范围内变化，但Cu的分配系数值在10上下很小一个范围内摆动，基本上可以认为是不变的。即在本文实验条件下，初始固相组成中Na/K比值的变化不影响硅酸盐固相与液相共存体系中Cu的分配系数。故可初步认为：初始固相中Na、K对Cu分配作用的贡献可能是一致的。单独改变初始固相中Na＋K的总摩尔含量，实验表明：随着Na＋K．的总相对摩尔含量增大，铜的分配系数线性下降。我们还可以结合Al/Al的改变对铜分配系数的影响可得到相似的结果。又上一小段结论认为：在Na＋K含量不变的情况下，Na/K比值改变不影响铜的分配系数。综合上述几方面进一步认为：在可能制约Cu分配系数的因子中，Na＋K的总含量变化是影响铜分配系数的一个重要因素；而Na＋K的总含量不变的情况下，Na/K的相对改变并不会影响铜的分配系数。改变SiO_2的初始摩尔相对含量，实验结果的规律性不是很明显，但从整体上分析分配系数，仍可发现一些可能的趋势：SiO_2的相对摩尔含量越高，铜的分配系数有下降的趋势。该组实验结果的不确定性，可能与SiO_2初始含量的基数大有关。铜的分配系数受流体的pH值的的制约。实验结果认为，酸性流体有利于铜在分配过程中进入流体相。虽则所有实验初始流体浓度及量是一样的，但实验后流体组成中铜的浓度与氯的浓度却呈正相关线性关系。本文实验与前人通过改变初始流体氯的浓度来讨论铜的分配系数实验相比，虽然实验体系各异，但在流体相中却得到相同的铜与氯的浓度关系。从而更有力地说明了流体相中铜与氯之间的互相依存关系，很可能流体相中铜与氯结合成络合物的形式存在。 |
| 其他摘要 | Significant advances have been obtained in the field of partitioning coefficient of copper between silicate melt and liquid in the late years, but most experiments focuses on the effect of the difference of liquid composition. Seldom experiment concerns about the influence of the difference of melt composition. In this paper, we synthesized successfully several silicate gels under the same experimental condition. According to the composition variation of Alk/Al,Na/K,SiO_2,Na+K, with other compositions remaining constant , we classified all the gels as four groups. The experimental studies on partitioning coefficients of copper between varied silicate melts and liquid were conducted at 800℃ and lkbar,with 0.1mol/1 HC1 as liquid and gel as starting material. The conclusions are summarized as follows: To the starting gels composition, we firstly change the mole ratio of Alk/Al but keep Alk+Al content constant. The experiments of this group were done at 800℃ and lkbar,with 0.1mol/1 HC1 as liquid, the results indicate that the partitioning coefficients of copper are restricted obviously by the variety of Alk/Al. The partitioning coefficients decrease from 54.16 to 16.55 with the increasing of ratios of Alk/Al from 0.666 to 1.500. The increasing of the ratio of Al/Alk is favourable for copper to be concentrated in the aqueous phase. We secondly change the ratios of Na/K but fix the mole percent content of Na+K in the original gels. Experimental results show that partitioning coefficients of copper are swinging around 10. It indicates that the change of Na/K don't affect the partitioning coefficients of copper in the coexisting system of silicate melts and liquid. So we come to the conclusion that it is equivalent that the effect of Na or K on the partitioning behavior of copper. As we only change the bulk mole percent proportion of Na+K in the original gels, the experimental results show that the partitioning coefficients of copper decrease linearly with the increasing of the bulk mole percent proportion of Na+K. This can be proved by the relation between partitioning coefficient and variety of Alk/Al. Also as the above sect: it is equivalent for Na or K to affect the partitioning behavior of copper. So, further we conclude: among the factors of affecting partitioning coefficient of copper, the bulk percent proportion of Na+K is an important factor while the variety of Na/K doesn't act on partitioning coefficient of copper. To the variation of the SiC_2 relative mole content in the original gels, experimental results have no very clear orderliness. But if we analyse the partitioning coefficients as a whole, we could find some possible inclination. Partitioning coefficients of copper have a little reducing inclination with the increasing of the SiO_2 relative mole content. The uncertainty of the experimental results may relate with the high content of SiO_2 originally. The PH of the fluid affects partitioning coefficient of copper. The experimental results indicate: acid liquid benefits copper entering fluid phase in the partitioning process. Although the content and concentration of all the original fluids are constant, we find that it has good linearly positive correlation between the aqueous copper concentration and the aqueous chlorine concentration. This agrees with the experimental conclusions of the literitures concerning the different concentration of chlorine in the original fluid. So the combination of copper and chlorine as coexisting complex can illustrate the mutual-depending relationship of copper and chlorine in the aqueous phase theoretically. |
| 页数 | 52
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| 语种 | 中文
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| 文献类型 | 学位论文
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| 条目标识符 | http://ir.gyig.ac.cn/handle/352002/3662
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| 专题 | 研究生_研究生_学位论文
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推荐引用方式
GB/T 7714 |
唐群力. 硅酸盐熔体-流体共存体系中Cu分配系数的实验研究[D]. 中国科学院地球化学研究所. 中国科学院地球化学研究所,2003.
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