火山气体中的氢和硫化氢:丰度、过程和大气通量

IF 2 4区 地球科学 Q3 GEOSCIENCES, MULTIDISCIPLINARY Comptes Rendus Geoscience Pub Date : 2023-09-26 DOI:10.5802/crgeos.235
Alessandro Aiuppa, Yves Moussallam
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引用次数: 0

摘要

氢(h2)和硫化氢(h2s)在火山气体排放中通常仅以微量到痕量的水平存在,但鉴于它们对火山气体还原能力(例如,它们去除大气o2的能力)的控制,它们在火山脱气研究中起着关键作用。与其他主要化合物结合,h2和h2s也是从观测到的岩浆气体组成中提取源岩浆条件(温度和氧化还原)信息的关键。在这里,我们从地质文献中提取了岩浆-混合(岩浆-热液)气体的代表性分析,并编制了一个目录,以回顾控制火山气体中h2和h2 S丰度的过程。研究表明,火山气体中的h2浓度和h2 / h2o比值均表现出强烈的正温度依赖性,而h2s浓度和h2s / so2比值总体上对温度不敏感。高H 2浓度(和低H 2 S / 2组成,平均0.1∼)在高温(> 1000°C)岩浆气体整体一致与热力学预测假设外部氧化还原缓冲由硅酸盐熔体共存,在氧气无常从ΔFMQ 1 - 0 (non-arc火山)ΔFMQ 0到+ 2(弧火山)(ΔFMQ氧逸度表示为一个对数单位差异相对于Fayalite-Magnetite-Quartz氧逸度缓冲区)。温度较低(<1000°C)的火山气体表现出更多的氧化还原条件(通常高于镍-镍氧化物缓冲液),这是由(i)气体缓冲系统中封闭系统(仅气相)绝热冷却期间的气体再平衡和(ii)非均相(气-矿物)反应的组合引起的。我们特别指出,h2 - h2 - h2 - h2 - h2o - so2系统的气相平衡在冷却至~ 600℃时总体上保持,而在较高的冷却程度(例如,在T<600℃时)更频繁地观察到较高温度平衡的淬火(在该温度下,表观平衡温度,AETs,大大超过测量的放电温度)。在这种温度较低的火山环境中,气-矿物反应也变得越来越重要,它清除岩浆中的so2并将其转化为h2s和热液矿物(硫酸盐和硫化物)。当这些非均相反应发生时,还可以控制火山气体h2 / h2o比的温度依赖性。最后,通过将我们的火山气体数据集与最近公布的全球火山so2和CO 2预算相结合,我们提供了总h2s的精确估计(中位数为1.4 Tg/yr;范围,0.9-8.8 Tg/yr)和h2(中位数,0.23 Tg/yr;范围,0.06-1 Tg/yr)来自全球陆上火山活动的通量。
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Hydrogen and hydrogen sulphide in volcanic gases: abundance, processes, and atmospheric fluxes
Hydrogen (H 2 ) and hydrogen sulphide (H 2 S) are typically present at only minor to trace levels in volcanic gas emissions, and yet they occupy a key role in volcanic degassing research in view of the control they exert on volcanic gas reducing capacity (e.g., their ability to remove atmospheric O 2 ). In combination with other major compounds, H 2 and H 2 S are also key to extracting information on source magma conditions (temperature and redox) from observed magmatic gas compositions. Here, we use a catalogue, compiled by extracting from the geological literature a selection of representative analyses of magmatic to mixed (magmatic–hydrothermal) gases, to review the processes that control H 2 and H 2 S abundance in volcanic gases. We show that H 2 concentrations and H 2 /H 2 O ratios in volcanic gases both exhibit strong positive temperature dependences, while H 2 S concentrations and H 2 S/SO 2 ratios are temperature insensitive overall. The high H 2 concentrations (and low H 2 S/SO 2 compositions, of ∼0.1 on average) in high-temperature (>1000 °C) magmatic gases are overall consistent with those predicted thermodynamically assuming external redox buffering operated by the coexisting silicate melt, at oxygen fugacities ranging from ΔFMQ -1 to 0 (non-arc volcanoes) to ΔFMQ 0 to +2 (arc volcanoes) (where ΔFMQ is oxygen fugacity expresses as a log unit difference relative to the Fayalite–Magnetite–Quartz oxygen fugacity buffer). Lower temperature (<1000 °C) volcanic gases exhibit more oxidizing redox conditions (typically above the Nickel–Nickel Oxide buffer) that are caused by a combination of (i) gas re-equilibration during closed-system (gas-phase only) adiabatic cooling in a gas-buffered system, and (ii) heterogenous (gas–mineral) reactions. We show, in particular, that gas-phase equilibrium in the H 2 –H 2 S–H 2 O–SO 2 system is overall maintained upon cooling down to ∼600 °C, while quenching of higher temperature equilibria (at which Apparent Equilibrium Temperatures, AETs, largely exceed measured discharge temperatures) is more frequently observed for higher extents of cooling (e.g., at T<600 °C). In such lower temperature volcanic environments, gas–mineral reactions also become increasingly important, scavenging magmatic SO 2 and converting it into H 2 S and hydrothermal minerals (sulphates and sulphides). These heterogeneous reactions, when occurring, can also control the temperature dependence of the volcanic gas H 2 /H 2 O ratios. Finally, by using our volcanic gas dataset in tandem with recently published global volcanic SO 2 and CO 2 budgets, we provide refined estimates for total H 2 S (median, 1.4 Tg/yr; range, 0.9–8.8 Tg/yr) and H 2 (median, 0.23 Tg/yr; range, 0.06–1 Tg/yr) fluxes from global subaerial volcanism.
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来源期刊
Comptes Rendus Geoscience
Comptes Rendus Geoscience 地学-地球科学综合
CiteScore
2.80
自引率
14.30%
发文量
68
审稿时长
5.9 weeks
期刊介绍: Created in 1835 by physicist François Arago, then Permanent Secretary, the journal Comptes Rendus de l''Académie des sciences allows researchers to quickly make their work known to the international scientific community. It is divided into seven titles covering the range of scientific research fields: Mathematics, Mechanics, Chemistry, Biology, Geoscience, Physics and Palevol. Each series is led by an editor-in-chief assisted by an editorial committee. Submitted articles are reviewed by two scientists with recognized competence in the field concerned. They can be notes, announcing significant new results, as well as review articles, allowing for a fine-tuning, or even proceedings of symposia and other thematic issues, under the direction of invited editors, French or foreign.
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