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Comment on "Activation of methane to CH₃ ⁺: A selective industrial route to methanesulfonic acid".

ABSTRACT: Díaz-Urrutia and Ott (Reports, 22 March 2019, p. 1326) report a selective conversion of methane to methanesulfonic acid that is proposed to occur by a cationic chain reaction in which CH₃ ⁺ adds to sulfur trioxide (SO₃) to form CH₃-S(O)₂O⁺ This mechanism is not plausible because of the solvent reactivity of CH₃ ⁺, the non-nucleophilicity of the sulfur atom of SO₃, and the high energy of CH₃-S(O)₂O^.

SUBMITTER: Roytman VA

PROVIDER: S-EPMC8530155 | biostudies-literature | 2019 May

REPOSITORIES: biostudies-literature

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Comment on "Activation of methane to CH3 +: A selective industrial route to methanesulfonic acid".

Roytman Vladislav A VA Singleton Daniel A DA

Science (New York, N.Y.) 20190501 6440

Díaz-Urrutia and Ott (Reports, 22 March 2019, p. 1326) report a selective conversion of methane to methanesulfonic acid that is proposed to occur by a cationic chain reaction in which CH3 + adds to sulfur trioxide (SO3) to form CH3-S(O)2O+ This mechanism is not plausible because of the solvent reactivity of CH3 +, the non-nucleophilicity of the sulfur atom of SO3, and the high energy of CH3</s ...[more]

PMID: 31073043

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Project description:The recent interest in measuring methane (CH4) emissions from abandoned oil and gas wells has resulted in five methods being typically used. In line with the US Federal Orphaned Wells Program's (FOWP) guidelines and the American Carbon Registry's (ACR) protocols, quantification methods must be able to measure minimum emissions of 1 g of CH4 h-1 to within ±20%. To investigate if the methods meet the required standard, dynamic chambers, a Hi-Flow (HF) sampler, and a Gaussian plume (GP)-based approach were all used to quantify a controlled emission (Qav; g h-1) of 1 g of CH4 h-1. After triplicate experiments, the average accuracy (Ar; %) and the upper (Uu; %) and lower (Ul; %) uncertainty bounds of all methods were calculated. Two dynamic chambers were used, one following the ACR guidelines, and a second "mobile" chamber made from lightweight materials that could be constructed around a source of emission on a well head. The average emission calculated from the measurements made using the dynamic chamber (Qav = 1.01 g CH4 h-1, Ar = +0.9%), the mobile chamber (Qav = 0.99 g CH4 h-1, Ar = -1.4%), the GP approach (Qav = 0.97 g CH4 h-1, Ar = -2.6%), and the HF sampler (Qav = 1.02 g CH4 h-1, Ar = +2.2%) were all within ±3% of 1 g of CH4 h-1 and met the requirements of the FOWP and ACR protocols. The results also suggest that the individual measurements made using the dynamic chamber can quantify emissions of 1 g of CH4 h-1 to within ±6% irrespective of the design (material, number of parts, geometrical shape, and hose length), and changes to the construction or material specifications as defined via ACR make no discernible difference to the quantification uncertainty. Our tests show that a collapsible chamber can be easily constructed around the emission source on an abandoned well and be used to quantify emissions from abandoned wells in remote areas. To our knowledge, this is the first time that methods for measuring the CH4 emissions of 1 g of CH4 h-1 have been quantitively assessed against a known reference source and against each other.

Project description:Greenhouse gas (GHG) emissions from Arctic permafrost soils create a positive feedback loop of climate warming and further GHG emissions. Active methane uptake in these soils can reduce the impact of GHG on future Arctic warming potential. Aerobic methane oxidizers are thought to be responsible for this apparent methane sink, though Arctic representatives of these organisms have resisted culturing efforts. Here, we first used in situ gas flux measurements and qPCR to identify relative methane sink hotspots at a high Arctic cytosol site, we then labeled the active microbiome in situ using DNA Stable Isotope Probing (SIP) with heavy 13CH4 (at 100 ppm and 1000 ppm). This was followed by amplicon and metagenome sequencing to identify active organisms involved in CH4 metabolism in these high Arctic cryosols. Sequencing of 13C-labeled pmoA genes demonstrated that type II methanotrophs (Methylocapsa) were overall the dominant active methane oxidizers in these mineral cryosols, while type I methanotrophs (Methylomarinovum) were only detected in the 100 ppm SIP treatment. From the SIP-13C-labeled DNA, we retrieved nine high to intermediate quality metagenome-assembled genomes (MAGs) belonging to the Proteobacteria, Gemmatimonadetes, and Chloroflexi, with three of these MAGs containing genes associated with methanotrophy. A novel Chloroflexi MAG contained a mmoX gene along with other methane oxidation pathway genes, identifying it as a potential uncultured methane oxidizer. This MAG also contained genes for copper import, synthesis of biopolymers, mercury detoxification, and ammonia uptake, indicating that this bacterium is strongly adapted to conditions in active layer permafrost and providing new insights into methane biogeochemical cycling. In addition, Betaproteobacterial MAGs were also identified as potential cross-feeders with methanotrophs in these Arctic cryosols. Overall, in situ SIP labeling combined with metagenomics and genome binning demonstrated to be a useful tool for discovering and characterizing novel organisms related to specific microbial functions or biogeochemical cycles of interest. Our findings reveal a unique and active Arctic cryosol microbial community potentially involved in CH4 cycling.

Dataset Information

Comment on "Activation of methane to CH₃ ⁺: A selective industrial route to methanesulfonic acid".

Publications

Comment on "Activation of methane to CH<sub>3</sub> <sup>+</sup>: A selective industrial route to methanesulfonic acid".

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