首页|Rebuilding the theory of isotope fractionation for evaporation of silicate melts under vacuum condition

Rebuilding the theory of isotope fractionation for evaporation of silicate melts under vacuum condition

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Rebuilding the theory of isotope fractionation for evaporation of silicate melts under vacuum condition
Isotope effects are pivotal in understanding sili-cate melt evaporation and planetary accretion processes.Based on the Hertz-Knudsen equation,the current theory often fails to predict observed isotope fractionations of labo-ratory experiments due to its oversimplified assumptions.Here,we point out that the Hertz-Knudsen-equation-based theory is incomplete for silicate melt evaporation cases and can only be used for situations where the vaporized spe-cies is identical to the one in the melt.We propose a new model designed for silicate melt evaporation under vacuum.Our model considers multiple steps including mass trans-fer,chemical reaction,and nucleation.Our derivations reveal a kinetic isotopic fractionation factor(KIFF or α)αour model=[m(1species)/m(2species)]0.5,where m(species)is the mass of the reactant of reaction/nucleation-limiting step or species of diffusion-limiting step and superscript 1 and 2 represent light and heavy isotopes,respectively.This model can effectively reproduce most reported KIFFs of laboratory experiments for various elements,i.e.,Mg,Si,K,Rb,Fe,Ca,and Ti.And,the KIFF-mixing model referring that an over-all rate of evaporation can be determined by two steps jointly can account for the effects of low PH2 pressure,composition,and temperature.In addition,we find that chemical reac-tions,diffusion,and nucleation can control the overall rate of evaporation of silicate melts by using the fitting slope in ln(-lnf)versus ln(t).Notably,our model allows for the theo-retical calculations of parameters like activation energy(Ea),providing a novel approach to studying compositional and environmental effects on evaporation processes,and shed-ding light on the formation and evolution of the proto-solar and Earth-Moon systems.

EvaporationKinetic isotopic fractionationChemical kineticsHertz-Knudsen equationCAIS

Jie Wang、Yun Liu

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Research Center for Planetary Science,College of Earth and Planetary Sciences,Chengdu University of Technology,Chengdu 610059,China

State Key Laboratory of Ore Deposit Geochemistry,Institute of Geochemistry,Chinese Academy of Sciences,Guiyang 550081,China

CAS Center for Excellence in Comparative Planetology,Hefei 230026,China

Evaporation Kinetic isotopic fractionation Chemical kinetics Hertz-Knudsen equation CAIS

2024

地球化学学报(英文版)
中国科学院地球化学研究所

地球化学学报(英文版)

EI
影响因子:0.33
ISSN:2096-0956
年,卷(期):2024.43(4)