{"title":"太阳星云中的氢同位素分馏及其对地球和太阳系内天体中水的影响","authors":"Abu Asaduzzaman","doi":"10.1021/acsearthspacechem.6c00183","DOIUrl":null,"url":null,"abstract":"<p>The origin of Earth’s water requires explanation\r\nof both\r\nits abundance and its elevated D/H ratio relative to the solar nebula.\r\nPrevious work (Asaduzzaman et al., 2015) demonstrated that dissociative\r\nchemisorption of water on olivine grains in the solar nebula could\r\nsupply several ocean equivalents of water to the growing Earth. However,\r\nthis mechanism has been challenged on isotopic grounds, as it does\r\nnot inherently explain the enrichment of D/H ratios relative to solar\r\nvalues. Here, I quantify hydrogen isotopic fractionation between nebular\r\ngas and a set of condensed phases using a combination of quantum chemical\r\ncalculations and statistical thermodynamics. Equilibrium fractionation\r\nfactors are determined as functions of temperature for (i) chemisorbed\r\nhydroxyls on olivine surfaces, (ii) structural hydroxyls in apatite\r\nand pyroxenes (including pigeonite), and (iii) representative organic\r\ncompounds. The results show that deuterium is preferentially partitioned\r\ninto condensed phases, with enrichment factors increasing systematically\r\nwith decreasing temperature. The calculated enrichment factors reach\r\nvalues comparable to those observed in terrestrial water, carbonaceous\r\nchondrites, Mars, and asteroid Vesta at temperatures of ∼175–300\r\nK. Kinetic constraints based on hydrogen diffusion in olivine indicate\r\nthat isotopic equilibration between gas and grain surfaces is plausible\r\nwithin the lifetime of the solar nebula. These findings demonstrate\r\nthat equilibrium gas–grain isotopic fractionation can naturally\r\ngenerate elevated D/H ratios in water adsorbed onto silicate grains.\r\nThis study offers an explanation to prior criticism of adsorption-based\r\nmodels by showing that nebular water can acquire terrestrial-like\r\nisotopic compositions through low-temperature equilibration with grain\r\nsurfaces. Chemisorption-mediated accretion therefore provides a plausible\r\ncomplementary mechanism for explaining both the abundance and isotopic\r\ncomposition of water in Earth and other inner solar system bodies,\r\nand may reduce part of the required contribution from carbonaceous\r\nchondrites.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 10","pages":"2326–2334"},"PeriodicalIF":2.6000,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogen Isotopic Fractionation in the Solar Nebula and Implications for Water in Earth and Inner Solar System Bodies\",\"authors\":\"Abu Asaduzzaman\",\"doi\":\"10.1021/acsearthspacechem.6c00183\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The origin of Earth’s water requires explanation\\r\\nof both\\r\\nits abundance and its elevated D/H ratio relative to the solar nebula.\\r\\nPrevious work (Asaduzzaman et al., 2015) demonstrated that dissociative\\r\\nchemisorption of water on olivine grains in the solar nebula could\\r\\nsupply several ocean equivalents of water to the growing Earth. However,\\r\\nthis mechanism has been challenged on isotopic grounds, as it does\\r\\nnot inherently explain the enrichment of D/H ratios relative to solar\\r\\nvalues. Here, I quantify hydrogen isotopic fractionation between nebular\\r\\ngas and a set of condensed phases using a combination of quantum chemical\\r\\ncalculations and statistical thermodynamics. Equilibrium fractionation\\r\\nfactors are determined as functions of temperature for (i) chemisorbed\\r\\nhydroxyls on olivine surfaces, (ii) structural hydroxyls in apatite\\r\\nand pyroxenes (including pigeonite), and (iii) representative organic\\r\\ncompounds. The results show that deuterium is preferentially partitioned\\r\\ninto condensed phases, with enrichment factors increasing systematically\\r\\nwith decreasing temperature. The calculated enrichment factors reach\\r\\nvalues comparable to those observed in terrestrial water, carbonaceous\\r\\nchondrites, Mars, and asteroid Vesta at temperatures of ∼175–300\\r\\nK. Kinetic constraints based on hydrogen diffusion in olivine indicate\\r\\nthat isotopic equilibration between gas and grain surfaces is plausible\\r\\nwithin the lifetime of the solar nebula. These findings demonstrate\\r\\nthat equilibrium gas–grain isotopic fractionation can naturally\\r\\ngenerate elevated D/H ratios in water adsorbed onto silicate grains.\\r\\nThis study offers an explanation to prior criticism of adsorption-based\\r\\nmodels by showing that nebular water can acquire terrestrial-like\\r\\nisotopic compositions through low-temperature equilibration with grain\\r\\nsurfaces. 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引用次数: 0
摘要
地球上的水的来源需要解释它的丰度和相对于太阳星云的高D/H比。先前的研究(Asaduzzaman et al, 2015)表明,太阳星云中橄榄石颗粒对水的解离半吸附可以为不断生长的地球提供相当于海洋的水。然而,这一机制在同位素的基础上受到了挑战,因为它不能从本质上解释相对于太阳值的D/H比值的富集。在这里,我使用量子化学计算和统计热力学相结合的方法,量化了星云气体和一组凝聚相之间的氢同位素分馏。平衡分馏因子被确定为(i)橄榄石表面的化学异构羟基,(ii)磷灰石和辉石(包括鸽石)中的结构羟基,以及(iii)代表性有机化合物的温度函数。结果表明,随着温度的降低,氘优先分配到凝聚相中,富集因子呈系统增加趋势。计算出的富集系数可与在温度为~ 175-300K的陆地水、碳球粒陨石、火星和灶神星小行星中观测到的富集系数相媲美。基于橄榄石中氢扩散的动力学约束表明,在太阳星云的生命周期内,气体和颗粒表面之间的同位素平衡是合理的。这些发现表明,平衡气粒同位素分馏可以自然地提高吸附在硅酸盐颗粒上的水的D/H比。这项研究通过表明星云水可以通过与颗粒表面的低温平衡获得类似地球的同位素组成,为先前对基于吸附模型的批评提供了解释。因此,化学吸附介导的吸积为解释地球和其他太阳系内天体中水的丰度和同位素组成提供了一种合理的补充机制,并可能减少碳质球粒的部分必要贡献。
Hydrogen Isotopic Fractionation in the Solar Nebula and Implications for Water in Earth and Inner Solar System Bodies
The origin of Earth’s water requires explanation
of both
its abundance and its elevated D/H ratio relative to the solar nebula.
Previous work (Asaduzzaman et al., 2015) demonstrated that dissociative
chemisorption of water on olivine grains in the solar nebula could
supply several ocean equivalents of water to the growing Earth. However,
this mechanism has been challenged on isotopic grounds, as it does
not inherently explain the enrichment of D/H ratios relative to solar
values. Here, I quantify hydrogen isotopic fractionation between nebular
gas and a set of condensed phases using a combination of quantum chemical
calculations and statistical thermodynamics. Equilibrium fractionation
factors are determined as functions of temperature for (i) chemisorbed
hydroxyls on olivine surfaces, (ii) structural hydroxyls in apatite
and pyroxenes (including pigeonite), and (iii) representative organic
compounds. The results show that deuterium is preferentially partitioned
into condensed phases, with enrichment factors increasing systematically
with decreasing temperature. The calculated enrichment factors reach
values comparable to those observed in terrestrial water, carbonaceous
chondrites, Mars, and asteroid Vesta at temperatures of ∼175–300
K. Kinetic constraints based on hydrogen diffusion in olivine indicate
that isotopic equilibration between gas and grain surfaces is plausible
within the lifetime of the solar nebula. These findings demonstrate
that equilibrium gas–grain isotopic fractionation can naturally
generate elevated D/H ratios in water adsorbed onto silicate grains.
This study offers an explanation to prior criticism of adsorption-based
models by showing that nebular water can acquire terrestrial-like
isotopic compositions through low-temperature equilibration with grain
surfaces. Chemisorption-mediated accretion therefore provides a plausible
complementary mechanism for explaining both the abundance and isotopic
composition of water in Earth and other inner solar system bodies,
and may reduce part of the required contribution from carbonaceous
chondrites.
期刊介绍:
The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.