scholarly journals Intramolecular isotopic evidence for bacterial oxidation of propane in subsurface natural gas reservoirs

2019 ◽  
Vol 116 (14) ◽  
pp. 6653-6658 ◽  
Author(s):  
Alexis Gilbert ◽  
Barbara Sherwood Lollar ◽  
Florin Musat ◽  
Thomas Giunta ◽  
Songcan Chen ◽  
...  

Microbial anaerobic oxidation of hydrocarbons is a key process potentially involved in a myriad of geological and biochemical environments yet has remained notoriously difficult to identify and quantify in natural environments. We performed position-specific carbon isotope analysis of propane from cracking and incubation experiments. Anaerobic bacterial oxidation of propane leads to a pronounced and previously unidentified13C enrichment in the central position of propane, which contrasts with the isotope signature associated with the thermogenic process. This distinctive signature allows the detection and quantification of anaerobic oxidation of hydrocarbons in diverse natural gas reservoirs and suggests that this process may be more widespread than previously thought. Position-specific isotope analysis can elucidate the fate of natural gas hydrocarbons and provide insight into a major but previously cryptic process controlling the biogeochemical cycling of globally significant greenhouse gases.

2020 ◽  
Author(s):  
Alexis Gilbert ◽  
Maxime Julien ◽  
Naohiro Yoshida ◽  
Yuichiro Ueno

<p>Hydrocarbons are the main constituents of natural gas. Their chemical and isotope abundance is a window to biogeochemical processes occurring in the subsurface. Stable isotopes of natural gas hydrocarbons are traditionally measured through compound-specific isotope analysis (CSIA) where each hydrocarbon is separated before its isotope ratio is determined.</p><p>Recently a variety of methods have been developed to determine position-specific isotope composition of propane, the first hydrocarbon with two distinct isotopomers: central and terminal [1][2][3][4]. The relative abundance of propane isotopomers (e.g. Δ<sup>13</sup>C<sub>central</sub> = δ<sup>13</sup>C<sub>central</sub> - δ<sup>13</sup>C<sub>terminal</sub>) is a promising tool for tracing sources and sinks of hydrocarbons in natural gas reservoirs. In particular, anaerobic oxidation of propane starts with a fumarate addition at the central position, which is expected to lead to a specific enrichment of the central <sup>13</sup>C-isotopomer of the remaining propane.</p><p>We measured Δ<sup>13</sup>C<sub>central</sub> values of propane throughout the course of its oxidation by bacteria BuS5 [5] and showed that the isotope fractionation is located mainly on the central position, which differs from the signature expected for thermogenic evolution [6]. The approach has been used to detect anaerobic oxidation of propane in several natural gas reservoirs: Southwest Ontario (Canada), Carnarvon Basin (Australia), Michigan (USA) [6], and more recently Tokamachi mud volcano in Japan [7]. In addition, isotopomers of n-butane and i-butane analysed using the same technique allows gaining insights into the mechanism of their microbial oxidation.</p><p>The isotopomer approach presented here can thus shed light on the fate of natural gas hydrocarbons. In combination with clumped isotope measurements of methane and ethane, the approach can provide unprecedented information regarding carbon cycling in the subsurface.</p><p> </p><p>[1] Gilbert et al., <strong>2016</strong> GCA v177, p205</p><p>[2] Piasecki et al., <strong>2016 </strong>GCA v188 p58</p><p>[3] Gao et al., <strong>2016</strong> Chem Geol. v435, p1</p><p>[4] Liu et al., <strong>2018</strong> Chem Geol. v491, p14</p><p>[5] Kniemeyer et al., <strong>2007</strong> Nature v449, p898</p><p>[6] Gilbert et al., <strong>2019</strong> PNAS v116, p6653</p><p>[7] Etiope et al., <strong>2011</strong> Appl. Geochem. v26, p348</p>


2019 ◽  
Vol 30 (5) ◽  
pp. 893-907
Author(s):  
Qianwen Li ◽  
Xiongqi Pang ◽  
Ling Tang ◽  
Wei Li ◽  
Kun Zhang ◽  
...  

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