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Fractionation of hydrogen isotopes caused by the difference of the crystal structure of hydrous minerals.

含水矿物晶体结构差异引起的氢同位素分馏。

基本信息

批准号：
13640491
负责人：
KAKIUCHI Masahisa
金额：
$ 2.24万
依托单位：
Gakushuin University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2001
资助国家：
日本
起止时间：
2001 至 2003
项目状态：
已结题

项目摘要

The purpose of this study was to present results for D/H fractionation in the crystal water-saturated solution-water vapor system of hydrous minerals. The D/H fractionation factors between the crystal water in crystalline hydrates and the saturated solution of transition metal dichloride, α_<CW-st.sol>, were experimentally determined under equilibrium condition. The empirical relationship between lnα_<C.W.-st.sol> and 1/T^2 on the crystal water of cobalt dichloride hexahydrate in the temperature range from 10 to 43℃ was obtained as : 10^3ln α_<CW-st.sol> = -2.46(10^6/T^2) + 17.6. The temperature dependence of In α_<C.W.-st.sol> is very small in comparison with that of the D/H fractionation factor between pure water and its vapor. The crystal water of cobalt dichloride dehydrate exhibits larger depletion of deuterium than that of cobalt dichloride hexahydrate. The value of α_<CW-st.sol> in cobalt dichloride dehydrate shoves similar to that of copper dichloride dehydrate at 25℃. The D/H fractionation factor between the crystal water in crystalline hydrate and saturated solution strongly depends on the structure of crystalline hydrate rather than the chemical species of cation and/or the crystallized temperature.In order to ensure that the vapor pressure of H_2O and D_2O is accurately and precisely obtained using the capacitance manometer, the apparatus of the vapor pressure measurement was made by Pyrex glass tube and was produced a vacuum. The dissociation pressure far CoCl_26H_2O and CoCl_26D_2O and the vapor pressure in equilibrium with the saturated solution of CoCl_2 in H_2O and D_2O were measured. It was found that the dissociation pressure of crystalline hydrate in H_2O is higher than that in D_2O and is slightly different from the vapor pressure in equilibrium with its saturated solution.

本文研究了含水矿物结晶水-饱和溶液-水蒸气体系中的D/H分馏。在平衡条件下，实验测定了水合物中结晶水与过渡金属氯化物饱和溶液之间的D/H分馏因子α_<CW-st.sol>。在<C.W.-st.sol>10 ~ 43℃温度范围内，六水合二氯化钴结晶水的lnα_与1/T^2的经验关系式为：10^3ln α_<CW-st.sol>= -2.46（10^6/T^2）+17.6。与<C.W.-st.sol>纯水及其蒸汽之间的D/H分馏因子相比，In α_的温度依赖性很小。二氯化钴结晶水的氘消耗量大于六水合二氯化钴结晶水。在<CW-st.sol>25℃时，二氯化钴的α_值与二氯化铜的α_值相近。结晶水合物中结晶水与饱和水之间的D/H分馏因子与结晶水合物的结构密切相关，而与阳离子的化学种类和结晶温度无关。蒸汽压测量装置由派热克斯玻璃管制成，并产生真空。测定了CoCl_26H_2O和CoCl_26D_2O的离解压以及CoCl_2在H_2O和D_2O中饱和溶液的平衡蒸气压。结果表明，结晶水合物在水溶液中的离解压高于在重水溶液中的离解压，且与饱和水溶液平衡时的蒸汽压略有不同。