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A Review of H2, CH4, and Hydrocarbon Formation in Experimental Serpentinization Using Network Analysis
Frontiers in Earth Science ( IF 2.9 ) Pub Date : 2020-05-19 , DOI: 10.3389/feart.2020.00209
Samuel Barbier , Fang Huang , Muriel Andreani , Renbiao Tao , Jihua Hao , Ahmed Eleish , Anirudh Prabhu , Osama Minhas , Kathleen Fontaine , Peter Fox , Isabelle Daniel

The origin of methane and light hydrocarbons (HCs) in natural fluids from serpentinization has commonly been attributed to the abiotic reduction of oxidized carbon by H2 through Fischer-Tropsch-type (FTT) reactions. Multiple experimental serpentinization studies attempted to identify the parameters that control the abiotic production of H2, CH4, and light HC. H2 is systematically and significantly formed in experiments, indicating that its production during serpentinization is well established. However, the large variance in concentration (eight orders of magnitude) is difficult to address because of the large number of parameters that vary from one experiment to another. CH4 and light HC production is much lower and also highly variable, leading to a vivid debate on potential role of metal catalysts and organic contamination. We have built a dataset that includes experimental setups, conditions, reactants, and products from 30 peer-reviewed articles reporting on experimental serpentinization and performed dimensionality reduction and network analysis to achieve an unbiased reading of the literature and fuel the debate. Our analysis distinguishes four experimental communities that highlights usual experimental protocols and the conditions tested so far. As expected, H2 production is mainly controlled by T and P though a strong variability remains within a given P-T range. Accessory metal-bearing phases seem to favor H2 production, while their role as catalyst or reactant is hampered by the lack of mineralogical characterization. CH4 and light HC concentrations are highly variable, uncorrelated to each other, and much lower than concentrations of potential reactants (H2, initial carbon). Accessory phases proposed as FTT catalysts do not enhance CH4 production, confirming the inefficiency of this reaction. CH4 only displays a positive correlation with temperature suggesting a kinetic/thermal control on its forming reaction. The carbon budget of some experiments indicates contamination in agreement with available labeled 13C studies. Salts in initial solutions are possible sources of organic contaminants. Natural systems certainly exploit longer reaction time or other reactional paths to form the observed CH4 and HC. The reducing potential of serpentinization can also produce intermediate metastable carbon phases in liquid or solid as observed in natural samples that should be targeted in future experiments.



中文翻译:

网络分析法评价蛇纹石化过程中H2,CH4和碳氢化合物的形成

蛇纹石化天然流体中甲烷和轻烃(HCs)的起源通常归因于费托型(FTT)反应通过H 2非生物还原氧化碳。多项实验性蛇纹石化研究试图确定控制H 2,CH 4和轻型HC非生物产生的参数。H 2在实验中系统地和显着地形成,表明在蛇纹石化过程中其产生已得到充分证实。但是,由于大量参数在一个实验之间发生变化,因此很难解决浓度的大差异(八个数量级)。通道4轻质HC的生产量要低得多,而且变化很大,这引发了关于金属催化剂和有机污染物的潜在作用的激烈争论。我们已经建立了一个数据集,其中包括来自30篇经过同行评审的文章的实验设置,条件,反应物和产物,这些文章报告了实验蛇纹石化,并进行了降维和网络分析,以实现文献的公正阅读并推动辩论。我们的分析将四个实验社区区分开来,这些社区突出了通常的实验方案和迄今为止测试的条件。正如预期的那样,尽管在给定的PT范围内仍存在很大的变异性,但H 2的产生主要受T和P控制。辅助含金属相似乎偏爱H 2缺乏矿物学特征阻碍了它们作为催化剂或反应物的生产。CH 4和轻质HC的浓度变化很大,彼此不相关,并且比潜在反应物(H 2,初始碳)的浓度低得多。提议作为FTT催化剂的辅助相不能提高CH 4的产生,证实了该反应的效率低下。CH 4仅与温度显示正相关,表明对其形成反应进行动力学/温度控制。一些实验的碳预算表明污染与可用的标记13一致C研究。初始溶液中的盐可能是有机污染物的来源。天然系统肯定会利用更长的反应时间或其他反应路径来形成观察到的CH 4和HC。如天然样品中观察到的那样,减少蛇纹石化作用的潜力还可以在液体或固体中产生中间亚稳碳相,应在未来的实验中确定目标。

更新日期:2020-05-19
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