Metal‐catalysed CO2 hydrogenation is considered a source of methane in serpentinized (hydrated) igneous rocks and a fundamental abiotic process germane to the origin of life. Iron, nickel, chromium and cobalt are the catalysts typically employed in hydrothermal simulation experiments to obtain methane at temperatures >200°C. However, land‐based present‐day serpentinization and abiotic gas apparently develop below 100°C, down to approximately 40–50°C. Here, we document considerable methane production in thirteen CO2 hydrogenation experiments performed in a closed dry system, from 20 to 90°C and atmospheric pressure, over 0.9–122 days, using concentrations of non‐pretreated ruthenium equivalent to those occurring in chromitites in ophiolites or igneous complexes (from 0.4 to 76 mg of Ru, equivalent to the amount occurring approximately in 0.4–760 kg of chromitite). Methane production increased with time and temperature, reaching approximately 87 mg CH4 per gram of Ru after 30 days (2.9 mgCH4/gru/day) at 90°C. At room temperature, CH4 production rate was approximately three orders of magnitude lower (0.003 mgCH4/gru/day). We report the first stable carbon and hydrogen isotope ratios of abiotic CH4 generated below 100°C. Using initial δ13CCO2 of ‐40‰, we obtained room temperature δ13CCH4 values as 13C depleted as −142‰. With time and temperature, the C‐isotope separation between CO2 and CH4 decreased significantly and the final δ13CCH4 values approached that of initial δ13CCO2. The presence of minor amounts of C2‐C6 hydrocarbons is consistent with observations in natural settings. Comparative experiments at the same temperatures with iron and nichel catalysts did not generate CH4. Ru‐enriched chromitites could potentially generate methane at low temperatures on Earth and on other planets.

Hypersaline meromictic lakes are extreme environments in which water stratification is associated with powerful physicochemical gradients and high salt concentrations. Furthermore, their physical stability coupled with vertical water column partitioning makes them important research model systems in microbial niche differentiation and biogeochemical cycling. Here, we compare the prokaryotic assemblages from Ursu and Fara Fund hypersaline meromictic lakes (Transylvanian Basin, Romania) in relation to their limnological factors and infer their role in elemental cycling by matching taxa to known taxon-specific biogeochemical functions. To assess the composition and structure of prokaryotic communities and the environmental factors that structure them, deepcoverage small subunit (SSU) ribosomal RNA (rDNA) amplicon sequencing, community domainspecific quantitative PCR and physicochemical analyses were performed on samples collected along depth profiles. The analyses showed that the lakes harbored multiple and diverse prokaryotic communities whose distribution mirrored the water stratification patterns. Ursu Lake was found to be dominated by Bacteria and to have a greater prokaryotic diversity than Fara Fund Lake that harbored an increased cell density and was populated mostly by Archaea within oxic strata. In spite of their contrasting diversity, the microbial populations indigenous to each lake pointed to similar physiological functions within carbon degradation and sulfate reduction. Furthermore, the taxonomy results coupled with methane detection and its stable C isotope composition indicated the presence of a yet-undescribed methanogenic group in the lakes' hypersaline monimolimnion. In addition, ultrasmall uncultivated archaeal lineages were detected in the chemocline of Fara Fund Lake, where the recently proposed Nanohaloarchaeota phylum was found to thrive.

Abstract. An ensemble Kalman filter (EnKF) has been coupled to the CHIMERE chemical transport model in order to assimilate ozone ground-based measurements on a regional scale. The number of ensembles is reduced to 20, which allows for future operational use of the system for air quality analysis and forecast. Observation sites of the European ozone monitoring network have been classified using criteria on ozone temporal variability, based on previous work by Flemming et al. (2005). This leads to the choice of specific subsets of suburban, rural and remote sites for data assimilation and for evaluation of the reference run and the assimilation system. For a 10-day experiment during an ozone pollution event over Western Europe, data assimilation allows for a significant improvement in ozone fields: the RMSE is reduced by about a third with respect to the reference run, and the hourly correlation coefficient is increased from 0.75 to 0.87. Several sensitivity tests focus on an a posteriori diagnostic estimation of errors associated with the background estimate and with the spatial representativeness of observations. A strong diurnal cycle of both these errors with an amplitude up to a factor of 2 is made evident. Therefore, the hourly ozone background error and the observation error variances are corrected online in separate assimilation experiments. These adjusted background and observational error variances provide a better uncertainty estimate, as verified by using statistics based on the reduced centered random variable. Over the studied 10-day period the overall EnKF performance over evaluation stations is found relatively unaffected by different formulations of observation and simulation errors, probably due to the large density of observation sites. From these sensitivity tests, an optimal configuration was chosen for an assimilation experiment extended over a three-month summer period. It shows a similarly good performance as the 10-day experiment.

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