气候变化领域集成服务门户(CCPortal): Recognizing the pathways of microbial methanogenesis through methane isotopologues in the subsurface biosphere

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DOI	10.1016/j.epsl.2021.116960
	Recognizing the pathways of microbial methanogenesis through methane isotopologues in the subsurface biosphere
	Shuai Y.; Xie H.; Zhang S.; Zhang Y.; Eiler J.M.
发表日期	2021
ISSN	0012821X
卷号	566
英文摘要	Microbial methanogenesis is a significant component in the global carbon cycle, a driver of greenhouse warming from atmospheric methane, and contributes to natural gas resources. There are several metabolic pathways of methanogenesis, and it is challenging to discriminate between them and quantify their relative contributions in natural settings. Here we measure and compile four rare isotopologues of methane (13CH4, 12CH3D, 13CH3D and 12CH2D2) from the Qaidam Basin (China) and a large set of previous data across the world to identify distinctive fingerprints of two principal sources of subsurface microbial methane — hydrogenotrophic and methylotrophic methanogenesis — and use those fingerprints to deconvolve the budgets of microbial methane in the Qaidam Basin. Our data show that biogenic methanes in the Qaidam Basin have equilibrium Δ18/Δ13CH3D values respect to reservoir temperature without anaerobic methane oxidation. Our results suggest that methylotrophic methanogenesis produces methane with large deficits in 13CH3D and 12CH2D2 relative to that controlled by homogeneous equilibrium among methane isotopologues at ambient environmental temperatures, whereas hydrogenotrophic methanogenesis produces methane with 13CH3D abundance near equilibrium and relatively subtle 12CH2D2 deficits. We find a good linear correlation between the Δ13CH3D value of natural biogenic methane and independent estimates of the fraction of hydrogenotrophic (methylotrophic) methanogenesis, based on established interpretations of hydrogen isotope data. These findings are consistent with studies of laboratory cultures, which also show methylotrophic methane is more depleted in clumped isotopologues (13CH3D and 12CH2D2) than hydrogenotrophic methane, though both forms of cultured (hydrogenotrophic vs. methylotrophic) methane exhibit strong deficits in both isotopic species. The sensitivity of clumped isotopologues to methanogenesis pathways in natural settings provides a powerful tool for monitoring the activity of methanogenic microbial communities in the subsurface. Anomalies of both studied clumped isotopologues (Δ13CH3D and Δ12CH2D2) decrease over time in wells that have been re-sampled repeatedly, suggesting that such measurements are capable of detecting and quantifying shifts in proportions of these two metabolic pathways over the timescales of gas production history. © 2021 Elsevier B.V.
关键词	biogenic methane clumped isotopologue hydrogenotrophic methanogenesis metabolism pathway Δ13CH3D proxy
英文关键词	Atmospheric chemistry; Budget control; Energy resources; Isotopes; Metabolism; Natural gas; Natural gas deposits; Biogenic methane; Biogenics; Clumped isotopologue; Hydrogenotrophic methanogenesis; Isotopologues; Metabolic pathways; Metabolism pathway; Methanogenesis; Qaidam basin; Δ13CH3D proxy; Methane; biogenic deposit; biosphere; gas production; isotopic analysis; metabolism; methane; methanogenesis; methanogenic bacterium; China; Qaidam Basin; Qinghai
语种	英语
来源期刊	Earth and Planetary Science Letters
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/203293
作者单位	Research Institute of Petroleum Exploration and Development (PetroChina), Beijing, China; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, United States; Research Institute of Qinghai Oil Field Branch Company (PetroChina), Dunhuang, 736202, China
推荐引用方式 GB/T 7714	Shuai Y.,Xie H.,Zhang S.,et al. Recognizing the pathways of microbial methanogenesis through methane isotopologues in the subsurface biosphere[J],2021,566.
APA	Shuai Y.,Xie H.,Zhang S.,Zhang Y.,&Eiler J.M..(2021).Recognizing the pathways of microbial methanogenesis through methane isotopologues in the subsurface biosphere.Earth and Planetary Science Letters,566.
MLA	Shuai Y.,et al."Recognizing the pathways of microbial methanogenesis through methane isotopologues in the subsurface biosphere".Earth and Planetary Science Letters 566(2021).