Equilibrium Zn isotope fractionation was inves- tigated using first-principles quantum chemistry methods at the B3LYP/6-311G level. The volume variable cluster model method was used to calculate isotope fractionation ...Equilibrium Zn isotope fractionation was inves- tigated using first-principles quantum chemistry methods at the B3LYP/6-311G level. The volume variable cluster model method was used to calculate isotope fractionation factors of sphalerite, smithsonite, calcite, anorthite, for- sterite, and enstatite. The water-droplet method was used to calculate Zn isotope fractionation factors of Zn^2＋-bearing aqueous species; their reduced partition function ratio factors decreased in the order [Zn（H2O）6]^2＋ 〉 [ZnCl（H2O）5]^ ＋ 〉 [ZnCl2（H2O）4] 〉 [ZnCl3（H20）2]^-〉 ZnCl4]^2-. Gas- eous ZnCl2 was also calculated for vaporization processes. Kinetic isotope fractionation of diffusional processes in a vacuum was directly calculated using formulas provided by Richter and co-workers. Our calculations show that in addition to the kinetic isotope effect of diffusional processes, equilibrium isotope fractionation also contributed nontriv- ially to observed Zn isotope fractionation of vaporization processes. The calculated net Zn isotope fractionation of vaporization processes was 7-7.5‰, with ZnCl2 as the gas- eous species. This matches experimental observations of the range of Zn isotope distribution of lunar samples. Therefore, vaporization processes may be the cause of the large distri- bution of Zn isotope signals found on the Moon. However, we cannot further distinguish the origin of such vaporization processes; it might be due either to igneous rock melting inmeteorite bombardments or to a giant impact event. Fur- thermore, isotope fractionation between Zn-bearing aqueous species and minerals that we have provided helps explain Zn isotope data in the fields of ore deposits and petrology.展开更多
1 Introduction Tibet has nurmerous salt lakes.Laguocuo is one of the salt lakes,which is located to the sorthern of Ali Plateau,31°59′02″N-32°04′08″N,84°02′03″E-84°12′03″E.Its lake water is...1 Introduction Tibet has nurmerous salt lakes.Laguocuo is one of the salt lakes,which is located to the sorthern of Ali Plateau,31°59′02″N-32°04′08″N,84°02′03″E-84°12′03″E.Its lake water is rich in potassium,magnesium,lithium,boron,rubidium,cesium and other resources.The study of展开更多
The Gas Hure Salt Lake(GHSL) in the northwestern Qaidam Basin, western China, is rich in boron(B) resources, but its B-resource origin is hardly known. Hydrochemical compositions and B isotope characteristics of diffe...The Gas Hure Salt Lake(GHSL) in the northwestern Qaidam Basin, western China, is rich in boron(B) resources, but its B-resource origin is hardly known. Hydrochemical compositions and B isotope characteristics of different waters were collected around the GHSL, including the river water, stream water, spring water, salt-lake brine, intercrystalline brine, well water, drilling brine, and solar pond brine. The hydrochemical signatures suggest that silicates, carbonates and evaporates are the main B-bearing rocks during the water dynamic. The reservoir estimation of B resources shows that the Kulamulekesay River(KLMR) and the Atekan River(ATKR) contribute annually 18.3 tons and 22.84 tons of B, respectively, with a total amount of 11.72 × 10^(4) tons of B during the past 5.7 ka. In comparison with the known B reservoir(32.96 × 10^(4) tons) in the GHSL, a significant amount of B in the GHSL was probably recharged from deep fluids and sediments around the GHSL. The B concentration and B-enrichment degree are shaped by the evaporation process, which are highly elevated at the carnallite and bischofite stages.展开更多
基金support from973 Program Fund(No.2014CB440904)Chinese National Science Fund Projects(Nos.41530210,41490635,41403051)
文摘Equilibrium Zn isotope fractionation was inves- tigated using first-principles quantum chemistry methods at the B3LYP/6-311G level. The volume variable cluster model method was used to calculate isotope fractionation factors of sphalerite, smithsonite, calcite, anorthite, for- sterite, and enstatite. The water-droplet method was used to calculate Zn isotope fractionation factors of Zn^2＋-bearing aqueous species; their reduced partition function ratio factors decreased in the order [Zn（H2O）6]^2＋ 〉 [ZnCl（H2O）5]^ ＋ 〉 [ZnCl2（H2O）4] 〉 [ZnCl3（H20）2]^-〉 ZnCl4]^2-. Gas- eous ZnCl2 was also calculated for vaporization processes. Kinetic isotope fractionation of diffusional processes in a vacuum was directly calculated using formulas provided by Richter and co-workers. Our calculations show that in addition to the kinetic isotope effect of diffusional processes, equilibrium isotope fractionation also contributed nontriv- ially to observed Zn isotope fractionation of vaporization processes. The calculated net Zn isotope fractionation of vaporization processes was 7-7.5‰, with ZnCl2 as the gas- eous species. This matches experimental observations of the range of Zn isotope distribution of lunar samples. Therefore, vaporization processes may be the cause of the large distri- bution of Zn isotope signals found on the Moon. However, we cannot further distinguish the origin of such vaporization processes; it might be due either to igneous rock melting inmeteorite bombardments or to a giant impact event. Fur- thermore, isotope fractionation between Zn-bearing aqueous species and minerals that we have provided helps explain Zn isotope data in the fields of ore deposits and petrology.
文摘1 Introduction Tibet has nurmerous salt lakes.Laguocuo is one of the salt lakes,which is located to the sorthern of Ali Plateau,31°59′02″N-32°04′08″N,84°02′03″E-84°12′03″E.Its lake water is rich in potassium,magnesium,lithium,boron,rubidium,cesium and other resources.The study of
基金Financial support for this research was provided by the “Western Light” Fund of the Chinese Academy of Science Foundation (Y910061016)The National Natural Science Foundation of China (No. 42007169)+3 种基金The Key deployment projects of the Chinese academy of sciences (ZDRW-ZS-2020-3)Funds for the Natural Science Foundation of Qinghai Province (No. 2020-ZJ-932Q2020-ZJ-7322019-ZJ-7028)。
文摘The Gas Hure Salt Lake(GHSL) in the northwestern Qaidam Basin, western China, is rich in boron(B) resources, but its B-resource origin is hardly known. Hydrochemical compositions and B isotope characteristics of different waters were collected around the GHSL, including the river water, stream water, spring water, salt-lake brine, intercrystalline brine, well water, drilling brine, and solar pond brine. The hydrochemical signatures suggest that silicates, carbonates and evaporates are the main B-bearing rocks during the water dynamic. The reservoir estimation of B resources shows that the Kulamulekesay River(KLMR) and the Atekan River(ATKR) contribute annually 18.3 tons and 22.84 tons of B, respectively, with a total amount of 11.72 × 10^(4) tons of B during the past 5.7 ka. In comparison with the known B reservoir(32.96 × 10^(4) tons) in the GHSL, a significant amount of B in the GHSL was probably recharged from deep fluids and sediments around the GHSL. The B concentration and B-enrichment degree are shaped by the evaporation process, which are highly elevated at the carnallite and bischofite stages.
