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FEMS Microbiology Letters Sep 2020Methanogenesis is the final step in the anaerobic degradation of organic matter. The most important substrates of methanogens are hydrogen plus carbon dioxide and...
Methanogenesis is the final step in the anaerobic degradation of organic matter. The most important substrates of methanogens are hydrogen plus carbon dioxide and acetate, but also the use of methanol, methylated amines, and aromatic methoxy groups appears to be more widespread than originally thought. Except for most members of the family Methanosarcinaceae, all methylotrophic methanogens require external hydrogen as reductant and therefore compete with hydrogenotrophic methanogens for this common substrate. Since methanogenesis from carbon dioxide consumes four molecules of hydrogen per molecule of methane, whereas methanogenesis from methanol requires only one, methyl-reducing methanogens should have an energetic advantage over hydrogenotrophic methanogens at low hydrogen partial pressures. However, experimental data on their hydrogen threshold is scarce and suffers from relatively high detection limits. Here, we show that the methyl-reducing methanogens Methanosphaera stadtmanae (Methanobacteriales), Methanimicrococcus blatticola (Methanosarcinales), and Methanomassiliicoccus luminyensis (Methanomassiliicoccales) consume hydrogen to partial pressures < 0.1 Pa, which is almost one order of magnitude lower than the thresholds for M. stadtmanae and M. blatticola reported in the only previous study on this topic. We conclude that methylotrophic methanogens should outcompete hydrogenotrophic methanogens for hydrogen and that their activity is limited by the availability of methyl groups.
Topics: Euryarchaeota; Hydrogen; Methane
PubMed: 32821944
DOI: 10.1093/femsle/fnaa137 -
Waste Management & Research : the... May 2023System modelling of sewage sludge (SS) treatment attracts a growing interest for better comparison and optimisation of technologies. However, SS parameters need to be... (Review)
Review
System modelling of sewage sludge (SS) treatment attracts a growing interest for better comparison and optimisation of technologies. However, SS parameters need to be generalised to be used in holistic assessments, since scattered data may inhibit the development and interpretation of system models. A review of the literature on SS parameters relevant to modelling SS treatment systems revealed 208 datasets published in 162 publicly available scientific papers. We treated thickened and dewatered sludge in the same data analysis, but in some cases, this was an incorrect assumption. The compositional data showed significant variations, but most of the data subscribed to a lognormal distribution, albeit with varying levels of significance. On average, the thickened sludge contained 3.3 ± 1.7% total solid (TS), and the dewatered sludge contained 21.0 ± 6.7% TS. For the combined data, the average Ash content was 32.4 ± 11.8% of TS. Other characteristic parameters were the lower heating value (LHV) of 22.1 ± 2.1 MJ kg volatile solid (VS) and the biochemical methane potential (BMP) of 0.25 ± 0.11 m CH kg VS. Fertiliser-related elements were on average 53.3 ± 9.3% C in VS, 6.8 ± 2.2% N in VS, 6.7 ± 2.4% P in Ash and 1.7 ± 1.3% K in Ash. The data reviewed herein provide a good basis for assessing the generality of individual SS data and for selecting key parameters for modelling SS treatment systems. However, the review reveals a need for the better characterisation of SS in the future.
Topics: Sewage; Methane; Fertilizers
PubMed: 36482728
DOI: 10.1177/0734242X221139171 -
Microbiology Spectrum Dec 2023Cold seeps occur in continental margins worldwide and are deep-sea oases. Anaerobic oxidation of methane is an important microbial process in the cold seeps and plays an...
Cold seeps occur in continental margins worldwide and are deep-sea oases. Anaerobic oxidation of methane is an important microbial process in the cold seeps and plays an important role in regulating methane content. This study elucidates the diversity and potential activities of major microbial groups in dependent anaerobic methane oxidation and sulfate-dependent anaerobic methane oxidation processes and provides direct evidence for the occurrence of nitrate-/nitrite-dependent anaerobic methane oxidation (Nr-/N-DAMO) as a previously overlooked microbial methane sink in the hydrate-bearing sediments of the South China Sea. This study provides direct evidence for occurrence of Nr-/N-DAMO as an important methane sink in the deep-sea cold seeps.
Topics: Anaerobiosis; Geologic Sediments; Methane; RNA, Ribosomal, 16S; Oxidation-Reduction; Nitrates; China
PubMed: 37916811
DOI: 10.1128/spectrum.02505-23 -
Nature Communications Jul 2022Oxidative carbene organocatalysis, inspired from Vitamin B1 catalyzed oxidative activation from pyruvate to acetyl coenzyme A, have been developed as a versatile...
Oxidative carbene organocatalysis, inspired from Vitamin B1 catalyzed oxidative activation from pyruvate to acetyl coenzyme A, have been developed as a versatile synthetic method. To date, the α-, β-, γ-, δ- and carbonyl carbons of (unsaturated)aldehydes have been successfully activated via oxidative N-heterocyclic carbene (NHC) organocatalysis. In comparison with chemical redox or photoredox methods, electroredox methods, although widely used in mechanistic study, were much less developed in NHC catalyzed organic synthesis. Herein, an iodide promoted electroredox NHC organocatalysis system was developed. This system provided general solutions for electrochemical single-electron-transfer (SET) oxidation of Breslow intermediate towards versatile transformations. Radical clock experiment and cyclic voltammetry results suggested an anodic radical coupling pathway.
Topics: Aldehydes; Iodides; Methane; Promoter Regions, Genetic
PubMed: 35780238
DOI: 10.1038/s41467-022-31453-7 -
PloS One 2023From wellhead to burner tip, each component of the natural gas process chain has come under increased scrutiny for the presence and magnitude of methane leaks, because...
From wellhead to burner tip, each component of the natural gas process chain has come under increased scrutiny for the presence and magnitude of methane leaks, because of the large global warming potential of methane. Top-down measures of methane emissions in urban areas are significantly greater than bottom-up estimates. Recent research suggests this disparity might in part be explained by gas leaks from one of the least understood parts of the process chain: behind the gas meter in homes and buildings. However, little research has been performed in this area and few methods and data sets exist to measure or estimate them. We develop and test a simple and widely deployable closed chamber method that can be used for quantifying indoor methane emissions with an order-of-magnitude precision which allows for screening of indoor large volume ("super-emitting") leaks. We also perform test applications of the method finding indoor leaks in 90% of the 20 Greater Boston buildings studied and indoor methane emissions between 0.02-0.51 ft3 CH4 day-1 (0.4-10.3 g CH4 day-1) with a mean of 0.14 ft3 CH4 day-1 (2.8 g CH4 day-1). Our method provides a relatively simple way to scale up indoor methane emissions data collection. Increased data may reduce uncertainty in bottom-up inventories, and can be used to find super-emitting indoor emissions which may better explain the disparity between top-down and bottom-up post-meter emissions estimates.
Topics: Methane; Air Pollutants; Natural Gas; Boston; Data Collection
PubMed: 38032978
DOI: 10.1371/journal.pone.0295055 -
Environmental Science & Technology Jan 2021Unburned methane entrained in exhaust from natural gas-fired compressor engines ("combustion slip") can account for a substantial portion of station-level methane...
Unburned methane entrained in exhaust from natural gas-fired compressor engines ("combustion slip") can account for a substantial portion of station-level methane emissions. A novel in-stack, tracer gas method was coupled with Fourier transform infrared (FTIR) species measurements to quantify combustion slip from natural gas compressor engines at 67 gathering and boosting stations owned or managed by nine "study partner" operators in 11 U.S. states. The mean methane emission rate from 63 four-stroke, lean-burn (4SLB) compressor engines was 5.62 kg/h (95% CI = 5.15-6.17 kg/h) and ranged from 0.3 to 12.6 kg/h. The mean methane emission rate from 39 four-stroke, rich-burn (4SRB) compressor engines was 0.40 kg/h (95% CI = 0.37-0.42 kg/h) and ranged from 0.01 to 4.5 kg/h. Study results for 4SLB engines were lower than both the U.S. EPA compilation of air pollutant emission factors (AP-42) and Inventory of U.S. Greenhouse Gas Emissions and Sinks (GHGI) by 8 and 9%, respectively. Study results for 4SRB engines were 43% of the AP-42 emission factor and 8% of the GHGI emission factor, the latter of which does not distinguish between engine types. Total annual combustion slip from the U.S. natural gas gathering and boosting sector was modeled using measured emission rates and compressor unit counts from the U.S. EPA Greenhouse Gas Reporting Program. Modeled results [328 Gg/y (95% CI = 235-436 Gg/y) of unburned methane] would account for 24% (95% CI = 17-31%) of the 1391 Gg of methane emissions for "Gathering and Boosting Stations", or 6% of the net emissions for "Natural Gas Systems" (5598 Gg) as reported in the 2020 U.S. EPA GHGI. Gathering and boosting combustion slip emissions reported in the 2020 GHGI (374 Gg) fall within the uncertainty of this model.
Topics: Air Pollutants; Greenhouse Gases; Methane; Natural Gas; United States; Vehicle Emissions
PubMed: 33410668
DOI: 10.1021/acs.est.0c05492 -
Molecules (Basel, Switzerland) Feb 2020The direct C-H functionalization reaction is one of the most efficient strategies by which to introduce new functional groups into small organic molecules. Over time,... (Review)
Review
The direct C-H functionalization reaction is one of the most efficient strategies by which to introduce new functional groups into small organic molecules. Over time, iron complexes have emerged as versatile catalysts for carbine-transfer reactions with diazoalkanes under mild and sustainable reaction conditions. In this review, we discuss the advances that have been made using iron catalysts to perform C-H functionalization reactions with diazoalkanes. We give an overview of early examples employing stoichiometric iron carbene complexes and continue with recent advances in the C-H functionalization of C(sp)-H and C(sp)-H bonds, concluding with the latest developments in enzymatic C-H functionalization reactions using iron-heme-containing enzymes.
Topics: Biocatalysis; Cyclization; Esters; Hydrogen Bonding; Iron; Methane; Stereoisomerism
PubMed: 32079259
DOI: 10.3390/molecules25040880 -
Molecules (Basel, Switzerland) Nov 2022-heterocyclic carbene (NHC) has been widely used as an organocatalyst for both umpolung and non-umpolung chemistry. Previous works mainly focus on species including... (Review)
Review
-heterocyclic carbene (NHC) has been widely used as an organocatalyst for both umpolung and non-umpolung chemistry. Previous works mainly focus on species including Breslow intermediate, azolium enolate intermediate, homoenolate intermediate, alkenyl acyl azolium intermediate, etc. Notably, the NHC-bound alkynyl acyl azolium has emerged as an effective intermediate to access functionalized cyclic molecular skeleton until very recently. In this review, we summarized the generation and reactivity of the NHC-bound alkynyl acyl azolium intermediates, which covers the efforts and advances in the synthesis of achiral and axially chiral cyclic scaffolds via the NHC-bound alkynyl acyl azolium intermediates. In particular, the mechanism related to this intermediate is discussed in detail.
Topics: Catalysis; Methane
PubMed: 36432089
DOI: 10.3390/molecules27227990 -
FEMS Microbiology Ecology Oct 2022The methane-rich areas, the Loki's Castle vent field and the Jan Mayen vent field at the Arctic Mid Ocean Ridge (AMOR), host abundant niches for anaerobic...
The methane-rich areas, the Loki's Castle vent field and the Jan Mayen vent field at the Arctic Mid Ocean Ridge (AMOR), host abundant niches for anaerobic methane-oxidizers, which are predominantly filled by members of the ANME-1. In this study, we used a metagenomic-based approach that revealed the presence of phylogenetic and functional different ANME-1 subgroups at AMOR, with heterogeneous distribution. Based on a common analysis of ANME-1 genomes from AMOR and other geographic locations, we observed that AMOR subgroups clustered with a vent-specific ANME-1 group that occurs solely at vents, and with a generalist ANME-1 group, with a mixed environmental origin. Generalist ANME-1 are enriched in genes coding for stress response and defense strategies, suggesting functional diversity among AMOR subgroups. ANME-1 encode a conserved energy metabolism, indicating strong adaptation to sulfate-methane-rich sediments in marine systems, which does not however prevent global dispersion. A deep branching family named Ca. Veteromethanophagaceae was identified. The basal position of vent-related ANME-1 in phylogenomic trees suggests that ANME-1 originated at hydrothermal vents. The heterogeneous and variable physicochemical conditions present in diffuse venting areas of hydrothermal fields could have favored the diversification of ANME-1 into lineages that can tolerate geochemical and environmental variations.
Topics: Arctic Regions; Geologic Sediments; Hydrothermal Vents; Methane; Phylogeny; Sulfates
PubMed: 36190327
DOI: 10.1093/femsec/fiac117 -
Philosophical Transactions. Series A,... Jan 2022We report methane isotopologue data from aircraft and ground measurements in Africa and South America. Aircraft campaigns sampled strong methane fluxes over tropical...
We report methane isotopologue data from aircraft and ground measurements in Africa and South America. Aircraft campaigns sampled strong methane fluxes over tropical papyrus wetlands in the Nile, Congo and Zambezi basins, herbaceous wetlands in Bolivian southern Amazonia, and over fires in African woodland, cropland and savannah grassland. Measured methane C isotopic signatures were in the range -55 to -49‰ for emissions from equatorial Nile wetlands and agricultural areas, but widely -60 ± 1‰ from Upper Congo and Zambezi wetlands. Very similar C signatures were measured over the Amazonian wetlands of NE Bolivia (around -59‰) and the overall C signature from outer tropical wetlands in the southern Upper Congo and Upper Amazon drainage plotted together was -59 ± 2‰. These results were more negative than expected. For African cattle, C values were around -60 to -50‰. Isotopic ratios in methane emitted by tropical fires depended on the C3 : C4 ratio of the biomass fuel. In smoke from tropical C3 dry forest fires in Senegal, C values were around -28‰. By contrast, African C4 tropical grass fire C values were -16 to -12‰. Methane from urban landfills in Zambia and Zimbabwe, which have frequent waste fires, had C around -37 to -36‰. These new isotopic values help improve isotopic constraints on global methane budget models because atmospheric C values predicted by global atmospheric models are highly sensitive to the C isotopic signatures applied to tropical wetland emissions. Field and aircraft campaigns also observed widespread regional smoke pollution over Africa, in both the wet and dry seasons, and large urban pollution plumes. The work highlights the need to understand tropical greenhouse gas emissions in order to meet the goals of the UNFCCC Paris Agreement, and to help reduce air pollution over wide regions of Africa. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 2)'.
Topics: Agriculture; Air Pollution; Animals; Cattle; Methane; Seasons; Wetlands
PubMed: 34865533
DOI: 10.1098/rsta.2021.0112