Methane Supply Research Articles

Flexibility provision in the Swiss integrated power, hydrogen, and methane infrastructure

The renewable energy transition hinges on balancing energy supply and demand across seasons. This paper investigates the potential flexibility of Switzerland’s integrated power, hydrogen, and methane infrastructure to balance temporal mismatches while complying with national energy policies for sustainability and security. It develops an optimization method for energy system expansion and operation planning, filling crucial research gaps by (1) explicitly modeling power and gas transmission networks to guide technology placement and pinpoint network expansions, and (2) incorporating flexibility in power demand via shedding and shifting and in hydrogen and methane demands via price elasticity. The findings suggest that a 6.7-fold capacity expansion of variable renewables (i.e., photovoltaic, wind, run-of-river) by 2050 offsets nuclear phase-out and demand growth. The winter power gap is filled by power imports, hydropower generation, and gas turbines fueled by cost-effective hydrogen or methane imports. However, fuel embargoes escalate winter hydrogen and methane prices, reducing demand by 3.8%–10.4% and increasing domestic fuel production from biomass and excess renewable power in summer. To bridge the seasonal hydrogen and methane supply–demand gaps, up to 1.9 terawatt-hours of gas cavern storage is deployed in geologically viable locations, while costly tank storage plays a minor role. Power-to-gas requirements and power trade restrictions necessitate further renewable expansion, including 8.0 to 9.5 gigawatts of wind installations.

Disorder-dominated and scattering-dominated thermal transport in clathrate hydrates

Methane hydrate (MH) is an ice-like compound where methane molecules are encased within a lattice of water molecules. Found abundantly on ocean floors, MHs can influence future methane supplies, ocean floor stability, and climate change. In this study, a high-precision deep neural network interatomic potential for MHs is developed using ab initio molecular dynamics. Our findings reveal a transition between disorder-dominated and scattering-dominated lattice thermal transport in partially filled MHs, which are the most common form in real-world conditions. Although guest methane molecules have a minimal effect on the anharmonicity of the host lattice and the phonon band structure, they significantly increase the scattering rate of host lattice phonons by enlarging their anharmonic scattering phase space. Spectral phonon analysis further shows that methane guest molecules scatter low-frequency phonons associated with water molecule vibrations, considerably reducing the thermal conductivity of filled MHs.

Single cell protein production from methane in a gas-delivery membrane bioreactor

Single cell protein (SCP, or microbial protein) is one of the emerging alternative protein sources to address the global challenge of food insecurity. Recently, the SCP produced from methane has attracted substantial attention since methane is a renewable resource attainable from anaerobic digestion. However, the supply of methane, an insoluble gas in water, is one of the major challenges in producing methane-based SCP. This work developed a novel bioreactor configuration, in which hollow fiber membrane was used for efficient methane supply while microorganisms were growing in the suspended form favourable for the biomass harvest. Over a 312-day operation, the impacts of three critical parameters on the SCP production were investigated, including the ratio of methane loading to ammonium loading, the ratio of methane loading to oxygen loading, and the sludge retention time (SRT). Under the condition of 4 g CH4/g NH4+, 4 g O2/g CH4, and SRT of 4 days, the highest SCP production yield was observed and determined to be 1.36 g SCP/g CH4 and 5.05 g SCP/g N, respectively. The protein content was up to 67 %, which is higher than the majority of reported values to date. Moreover, the methane and ammonium utilization efficiencies were both close to 100 %, suggesting the highly efficient utilization of substrates in this new bioreactor configuration. A high relative abundance of essential amino acids (EAA) above 42 % was achieved, representing the highest EAA content reported. These findings provide valuable insights into SCP production using methane as a feedstock.

Lipidomic diversity and proxy implications of archaea from cold seep sediments of the South China Sea

Cold seeps on the continental margins are characterized by intense microbial activities that consume a large portion of methane by anaerobic methanotrophic archaea (ANME) through anaerobic oxidation of methane (AOM). Although ANMEs are known to contain unique ether lipids that may have an important function in marine carbon cycling, their full lipidomic profiles and functional distribution in particular cold-seep settings are still poorly characterized. Here, we combined the 16S rRNA gene sequencing and lipidomic approaches to analyze archaeal communities and their lipids in cold seep sediments with distinct methane supplies from the South China Sea. The archaeal community was dominated by ANME-1 in the moderate seepage area with strong methane emission. Low seepage area presented higher archaeal diversity covering Lokiarchaeia, Bathyarchaeia, and Thermoplasmata. A total of 55 core lipids (CLs) and intact polar lipids (IPLs) of archaea were identified, which included glycerol dialkyl glycerol tetraethers (GDGTs), hydroxy-GDGTs (OH-GDGTs), archaeol (AR), hydroxyarchaeol (OH-AR), and dihydroxyarchaeol (2OH-AR). Diverse polar headgroups constituted the archaeal IPLs. High concentrations of dissolved inorganic carbon (DIC) with depleted δ13CDIC and high methane index (MI) values based on both CLs (MICL) and IPLs (MIIPL) indicate that ANMEs were active in the moderate seepage area. The ANME-2 and ANME-3 clades were characterized by enhanced glycosidic and phosphoric diether lipids production, indicating their potential role in coupling carbon and phosphurus cycling in cold seep ecosystems. ANME-1, though representing a smaller proportion of total archaea than ANME-2 and ANME-3 in the low seepage area, showed a positive correlation with MIIPL, indicating a different mechanism contributing to the IPL-GDGT pool. This also suggests that MIIPL could be a sensitive index to trace AOM activities performed by ANME-1. Overall, our study expands the understanding of the archaeal lipid composition in the cold seep and improves the application of MI using intact polar lipids that potentially link to extent ANME activities.

Effects of wax on the formation of methane hydrate in oil-dominate systems: Experiments and molecular dynamics simulations

Hydrate formation and wax deposition in underwater multiphase pipelines have become two vital problems affecting the flow assurance safety. Experiments and molecular dynamics (MD) simulations were performed to investigate the effect of wax crystals on hydrate nucleation and growth. Our experimental results showed that wax crystals had an inhibitory effect on hydrate growth, but played a dual role in methane hydrate nucleation (promotion and inhibition). The addition of wax could decrease mass transfer coefficient of methane by increasing viscosity of oil phase, which lower methane supply from the oil bulk phase to the oil–water interface. The simulation results revealed that the wax crystals at the interface influenced the mass transfer of methane molecules instead of providing heterogeneous nucleation sites. Small wax crystal adjacent to the oil–water interface accelerated methane supersaturation dissolution and restricted gas diffusion in the aqueous phase because of adsorption to methane, which promoted hydrate nucleation and shifted the nucleation position toward the oil–water interface. While the large wax crystal could effectively block the methane mass transfer from oil phase to aqueous phase by covering the oil–water surface, which reduced the concentration of methane in the aqueous phase and prolonged the induction time of hydrate formation. These results of this work would provide a better understanding of the interaction mechanism between hydrate and wax.

Experimental Demonstration of the Electric Efficiency with BZYb based Protonic Ceramic Fuel Cell

Protonic Ceramic Fuel Cell (PCFC) is expected to be the next-generation fuel cell for its higher energy conversion efficiency and lower operation temperature. BaZrO3 based oxide are potential materials as PCFC electrolyte because they have a high chemical stability under CO2 condition and high proton conductivity. We have developed PCFC using BaZr0.8Yb0.2Ox (BZYb) as the electrolyte and performed max power density 0.49 W cm–2 at 873 K. For practical use of PCFC, it is needed to conduct the higher electric efficiency and to improve the durability. Especially, improving the electric efficiency of PCFC might be difficult due to the internal current leakage by the hole creation.In this work, we have evaluated the electric efficiency using a Φ60mm anode supported PCFC (active electrode area: Φ45mm, 15.9 cm2). Thin and dense BZYb electrolyte is supported on porous Ni-BZYb cermet anode and La0.6Sr0.4CoOx cathode. The effect of fuel utilization on PCFC cell was examined and the electric efficiency of PCFC was calculated as follows:η = V / (-ΔH / nF) × Ufwhere the n and F are the mole number and the Faraday constant, respectively. ΔH is the standard combustion enthalpy of hydrogen or methane. The value of -ΔH / nF is 1.24 V or 1.04 V in the case of hydrogen supply or methane supply respectively. V is the cell voltage and Uf is the fuel utilization.Φ60mm anode supported PCFC was fabricated by tape-casting process used for the industrial production of ceramic electronic devices. NiO-BZYb anode slurry and BZYb electrolyte slurry were prepared by mixing the powder, binder, solvents and plasticizer. And then, these slurries were tape-casted respectively. The anode green sheets and the electrolyte green sheets were stacked and pressed. The anode electrolyte half-cell was obtained by firing this laminate at 1673–1773 K for 2 h. La0.6Sr0.4CoO3-δ (LSC) paste was applied to the surface of the half-cell by screen–printing, and then, fired at 1223 K for 2 h to form a cathode.The electrochemical performance of the Φ60mm anode supported PCFC was investigated at 873 K under the conditions of a humid fuel gas (i.e., 3% H2O, 48.5% N2 and 48.5% H2) and a humid air (i.e. 3% H2O and 97% air). Fuel flow rate were determined by the operational current and the fuel utilization (Uf), and air flow rate were constant at 264 cc min–1, which the air utilization (Uair) was 30% at the current of 0.3 A cm–2.Figure 1 shows the comparison of the current-voltage (I-V) and current-power (I-P) characteristics of Φ60mm and Φ20mm BZYb cell. Fuel flow rate was 100 cc min–1 at this experiment. The same electrochemical performance was observed, and the maximum power reached 7 W at 12.9 A in the case of the Φ60mm cell.Figure 2 shows the cell performance of 0.3 A cm–2 current density under the various Uf condition. The theoretical voltage line was also drawn in the figure, which was calculated by Nernst equation used the PH2 in the anode outlet gas, PO2 and PH2O in the cathode outlet gas. Cell voltage followed the same path as the theoretical voltage in the low Uf condition (Uf≦70%). On the other hand, the gap between the cell voltage and theoretical one was larger in the higher Uf condition (Uf≧80%). Anode gas diffusion overvoltage might be increased by PH2 decreasing in anode gas or the imbalanced gas flow due to decreasing the anode gas flow rate. We demonstrated that BZYb based PCFC could be operated at high Uf condition (i.e., Uf=90%) and the maximum electric efficiency was 55% (DC). This presentation is partially based on results obtained from a project, JPNP20003, commissioned by the New Energy and Industrial Technology Development Organization (NEDO). Figure 1

Origins of sediments and fluids in submarine mud volcanoes off Tanegashima Island, northern Ryukyu Trench, Japan

Mud volcanoes are topographic features through which over-pressurized sediments are intruded upward and erupted, transporting fluids and sediments from the deep subsurface to the surface/seafloor. To understand material and biogeochemical cycling through mud volcanoes, we investigated the origins of sediments and fluids erupted by four submarine mud volcanoes off Tanegashima Island, along the northern Ryukyu Trench: MV#1–3 and MV#14. We estimated the ages of the source sequences of the mud volcano sediments to be middle to late Miocene based on nannofossils and 10Be ages. The sediments were characteristically enriched in illite. The similar mineral compositions and vitrinite reflectance values (0.42%–0.45%) of sediments erupted by the mud volcanoes strongly suggest that each is rooted in the same source sequence. Pore waters had Cl− concentrations ∼40% that of seawater and were proportionally enriched in 18O and depleted in D, indicating the addition of freshwater from the dehydration of clay minerals. However, the smectite and illite contents (<40%) in the clay size fraction ruled out in situ smectite dewatering as the cause of the pore water Cl− dilution. Thus, fluids derived from clay dewatering must have originated from deeper than the source sequence of the mud volcano sediments. Vertical Cl− profiles indicate that the upward fluid advection rate and eruption frequency decrease from MV#3 to MV#2, MV#1, and MV#14 (MV#14 being dormant). At the active mud volcanoes, the C1/C2 ratios (<100) and methane δ13C values (−56‰ to −42‰) indicate that hydrocarbon gases are mostly derived from the thermal decomposition of organic matter in deep sediments where the in situ temperature exceeds 80°C. At the dormant MV#14, high C1/C2 ratios (700–4,000) and low methane δ13C values (ca. −75‰) suggest the limited supply of thermogenic methane and the subsequent shallow methanogenesis. Because vitrinite reflectance values indicate that the source sediments are too immature to produce thermogenic hydrocarbons, the hydrocarbon gases, like the fluids derived from clay dewatering, were probably supplied from deeper than the source strata. The supply of deep fluids into the source sequence might be a universal phenomenon in subduction zones, and may play an important role in mud volcanism and associated biogeochemical cycling.

Carbon dioxide removal from the oceans: Carbon dioxide emission and techno-economic analyses of producing renewable synthetic methane

The capture of carbon dioxide from ocean water and utilizing the captured carbon as a stock for carbon-neutral renewable methane production may reduce a considerable amount of carbon in the atmosphere. However, given the lack of comprehensive analyses to reveal the potential, the examination proceeded through techno-economic and carbon dioxide emission analyses with several possible options of carbon dioxide extraction, location, electricity sources, and transport media. Through the economic analysis, the unit methane supply costs range from 3.5 to 7.5 $ kgCH4−1 according to the different options, and the majority of the total cost is found to be the electrolysis for generating hydrogen. The results of the emission analysis indicate cumulative emissions of the considered pathways which are highly negative values of around −80,000 tonCO2 y−1 due to the utilization of carbon by extraction. However, the utilization of synthesized methane in the natural gas power plant makes the final cumulative emission amount become highly positive values of more than 70,000 tonCO2 y−1. Here, the required capture rates in the power plant are suggested for the respective pathways to achieve carbon neutrality. A capture rate of 54.44 % is required for the pathway using column and OTEC, while 77.62 % is required for the pathway using BPMED and PV. Thus, given that it could be verified that the suggested pathways are competitive in the environmental aspect if the carbon capture in the utilization plant is possible, which can take advantage of the rate less than the common existing rate, a significant reduction in the cost, especially the levelized cost of electricity, will be crucial for the pathways to attaining competitiveness in the economic aspect as well.

Development of Membrane Reactor Coupling Hydrogen and Syngas Production.

Simultaneous syngas and pure hydrogen production through partial oxidation of methane and water splitting, respectively, were demonstrated by using mixed ionic-electronic conductors. Tubular ceramic membranes prepared from La0.5Sr0.5FeO3 perovskite were successfully utilized in a 10 M lab scale reactor by applying a radial arrangement. The supply of methane to the middle area of the reaction zone was shown to provide a uniform distribution of the chemical load along the tubes' length. A steady flow of steam feeding the inner part of the membranes was used as oxidative media. A described configuration was found to be favorable to maintaining oxygen permeability values exceeding 1.1 mL∙cm-2∙min-1 and long-term stability of related functional characteristics. Methane's partial oxidation reaction assisted by 10%Ni@Al2O3 catalyst proceeded with selectivity values above 90% and conversion of almost 100%. The transition from a laboratory model of a reactor operating on one tubular membrane to a ten-tube one resulted in no losses in the specific performance. The optimized supply of gaseous fuel opens up the possibility of scaling up the reaction zone and creating a promising prototype of a multitubular reaction zone with a simplified sealing procedure.

Life Cycle Assessment of Biomethane vs. Fossil Methane Production and Supply

Considering the current geopolitical situation that has hindered the gas supply gas from Russia, Europe’s main supplier, it is necessary to find alternative routes to guarantee the Italian gas stocks in winter at a reasonable cost. Such energetic strategies should consider the environmental sustainability of the different available options, fitting the targets of the EU environmental policy. With the aim of supplying a quantitative tool to support the European green transition, this paper reports the entire life cycle assessment (LCA) of three different options for the production and supply of natural gas/methane in Italy: the production of biomethane from biogas (considering a real-scale plant in Italy), the use of liquefied natural gas (LNG) supplied by Qatar by vessel, and the use of compressed gas delivered from Algeria via pipeline. The application of the LCA standardized method allowed for the quantification of the environmental benefit provided by the first option, against all the considered impact categories, thanks to a combination of several advantages: (a) its low-impact anaerobic production, (b) its exploitation of a waste product from the food/agriculture industries, and (c) its production of valuable by-products, which can be considered environmental credits. The results proved the possible environmental gain resulting from an integrated energy supply system that would be able to enhance the economic fabric of specific areas.

Simultaneous control of combustion instabilities and NOx emissions in a lean premixed flame using linear genetic programming

Combustion instabilities have been a plaguing challenge in lean-conditioned propulsion systems. An open-loop control system was developed using machine learning to suppress pressure fluctuations and NOx emissions simultaneously. The open-loop control is realized by regulating the solenoid valve to modulate the methane supply. Control laws comprising the multi-frequency forcing are generated via the linear genetic programming (LGP), before being converted into square waves with different frequencies and duty cycles to activate the solenoid valve. The cost function is intended to evaluate and rank individuals of each generation, so as to select candidates for evolution. Optimized periodic forcing (OPF) with different duty cycles (d) and frequencies (fP) is set to provide a comparison with the superiority of multi-frequency forcing of LGP. Three stages of pressure oscillations and NOx emissions have been found as d increases from 0.5 to 1.0: high level, transition, and low level, revealing the transition of the combustion mode. After ten generations of development, the pressure amplitude and NOx emissions are reduced by 67.1% and 36.9% under the optimal control law identified by LGP, respectively. The flame structure images and Rayleigh index maps indicate that the convective movement of the flame, which may be the key factor driving combustion instabilities, can be suppressed by the optimal control law. Furthermore, the proximity graph of the similarity between control laws is introduced to depict the machine learning process, with the steepest descent lines visualizing its ridgeline topology. With the evolution process, individuals are found moving closer to the top right-hand corner of the map, and two main search pathways gradually become clear.

"Sea Water" Supplemented with Calcium Phosphate and Magnesium Sulfate in a Long-Term Miller-Type Experiment Yields Sugars, Nucleic Acids Bases, Nucleosides, Lipids, Amino Acids, and Oligopeptides.

The standard approach to exploring prebiotic chemistry is to use a small number of highly purified reactants and to attempt to optimize the conditions required to produce a particular end product. However, purified reactants do not exist in nature. We have previously proposed that what drives prebiotic evolution are complex chemical ecologies. Therefore, we have begun to explore what happens if one substitutes "sea water", with its complex mix of minerals and salts, for distilled water in the classic Miller experiment. We have also adapted the apparatus to permit it to be regassed at regular intervals so as to maintain a relatively constant supply of methane, hydrogen, and ammonia. The "sea water" used in the experiments was created from Mediterranean Sea salt with the addition of calcium phosphate and magnesium sulfate. Tests included several types of mass spectrometry, an ATP-monitoring device capable of measuring femtomoles of ATP, and a high-sensitivity cAMP enzyme-linked immunoadsorption assay. As expected, amino acids appeared within a few days of the start of the experiment and accumulated thereafter. Sugars, including glucose and ribose, followed as did long-chain fatty acids (up to C20). At three-to-five weeks after starting the experiment, ATP was repeatedly detected. Thus, we have shown that it is possible to produce a "one-pot synthesis" of most of the key chemical prerequisites for living systems within weeks by mimicking more closely the complexity of real-world chemical ecologies.

Reactivated biofilm coupling n-DAMO with anammox achieved high-rate nitrogen removal in membrane aerated moving bed biofilm reactor

As a promising technology, the combination of nitrate/nitrite-dependent anaerobic methane oxidation (n-DAMO) with Anammox offers a solution to achieve effective and sustainable wastewater treatment. However, this sustainable process faces challenges to accumulate sufficient biomass for reaching practical nitrogen removal performance. This study developed an innovative membrane aerated moving bed biofilm reactor (MAMBBR), which supported sufficient methane supply and excellent biofilm attachment, for cultivating biofilms coupling n-DAMO with Anammox. Biofilms were developed rapidly on the polyurethane foam with the supply of ammonium and nitrate, achieving the bioreactor performance of 275 g N m−3 d−1 within 102 days. After the preservation at −20 °C for 8 months, the biofilm was successfully reactivated and achieved 315 g N m−3 d−1 after 188 days. After reactivation, MAMBBR was applied to treat synthetic sidestream wastewater. Up to 99.9% of total nitrogen was removed with the bioreactor performance of 4.0 kg N m−3 d−1. Microbial community analysis and mass balance calculation demonstrated that n-DAMO microorganisms and Anammox bacteria collectively contributed to nitrogen removal in MAMBBR. The MAMBBR developed in this study provides an ideal system of integrating n-DAMO with Anammox for sustainable wastewater treatment.

Numerical modeling of methane pyrolysis in a bubble column of molten catalysts for clean hydrogen production

Methane pyrolysis using molten catalysts in a bubble column reactor (BCR) has recently been proposed to produce hydrogen with separable carbon particles as byproducts. In this study, a numerical model of the BCR of molten catalysts for methane pyrolysis was developed and validated using experimental data. Based on a non-isothermal 1-D simplification, continuous liquid and discrete bubble phases were considered by incorporating submodels for bubble behaviors, catalytic and homogeneous reactions, heat/mass transfer, and a submerged orifice for methane supply. The initial bubble diameter was predicted using the correlation derived from measurements. When applied to experiments with Ni(27)Bi(73) and mixtures of KCl–MnCl2, the model accurately reproduced the methane conversion at different temperatures and column heights. Furthermore, detailed information on the key phenomena was acquired, including the profiles of the bubble diameter, rise velocity, reaction rates, temperature, and gas composition. A sensitivity analysis confirmed that the uncertainties regarding the physical properties of molten catalysts had a negligible impact. A comparison of the performances of Ni(27)Bi(73) and KCl(50)MnCl2(50) under the same reaction conditions revealed a favorable influence of the catalyst density on methane conversion because of the increased pressure. The proposed model would be useful in reactor optimization and scale-up with high hydrogen productivity.

Methane supply drives prokaryotic community assembly and networks at cold seeps of the South China Sea.

Marine cold seeps are unique chemosynthetic habitats fuelled by deeply sourced hydrocarbon-rich fluids discharged at the seafloor. Through oxidizing methane and other hydrocarbons, microorganisms inhabiting cold seeps supply subsurface-derived energy to higher trophic levels, sustaining highly productive oases of life in the deep sea. Despite the central role of microbiota in mediating biogeochemical cycles, the factors that govern the assembly and network of prokaryotic communities in cold seeps remain poorly understood. Here we analysed the geochemical and microbiological profiles of 11 different sediment cores from two spatially distant cold seeps of the South China Sea. We show that prokaryotic communities belonging to the same methane-supply regimes (high-methane-supply, low-methane-supply and non-seep control sediments) had a highly similar community structure, regardless of geographical location, seep-associated biota (mussel, clam, microbial mat) and sediment depth. Methane supply appeared to drive the niche partitioning of anaerobic methanotrophic archaea (ANME) at the regional scale, with ANME-1 accounting for >60% sequence abundance of ANME in the high-methane-supply sediments, while ANME-2 dominated (>90%) the low-methane-supply sediments. Increasing methane supply enhanced the contribution of environmental selection but lessened the contributions of dispersal limitation and drift to overall community assembly. High methane supply, moreover, promoted a more tightly connected, less stable prokaryotic network dominated by positive correlations. Together, these results provide a potentially new framework for understanding the niches and network interplay of prokaryotic communities across different methane seepage regimes in cold-seep sediments.

Towards sustainable methane supply from local bioresources: Anaerobic digestion, gasification, and gas upgrading

Methane is a versatile and storable energy carrier, which is likely to play an important role in the European transition towards a low fossil carbon energy sector. We investigate the potentials for meeting regional methane demands through conversion of local residual bioresources for supply of bio-based CH4. We have developed a tiered assessment framework involving i) allocation of residual and constrained bioresources to conversion pathways based on physical and biochemical properties, ii) life cycle assessment (LCA) of technology conversion pathways through process-oriented parameterisation of the LCA model, and iii) LCA modelling of system-level technology implementation scenarios for quantification of regional potentials for bio-based CH4 supply and environmental savings, in view of current uses of the same bioresources. Two main technology conversion pathways are included: gasification and anaerobic digestion, both with hydrogen enhancement. The latter was also considered with water scrubbing upgrading. The framework is implemented for the French region, Occitania, with a residual bioresource potential of 48 TWh·y−1 (distributed on 41 different bioresources), and an annual methane demand of 17.5 TWh·y−1, currently supplied by natural gas. The assessment results clearly demonstrate that utilisation of available residual bioresources has tremendous potential both for covering current gas demands in the region (up to about seven times in some scenarios) but also for a reduction in climate change impacts from the region (up to about 37%).

Abiotic passive nitrogen and methane enrichment during exhumation of subducted rocks: Primary multiphase fluid inclusions in high‐pressure rocks from the Cabo Ortegal Complex, NW Spain

AbstractPrimary multiphase fluid inclusions (MFI) were studied in one eclogite and two granulites from the Cabo Ortegal Complex (COC, NW Spain) by means of Raman imaging, Scanning Electron Microscopy with Energy Dispersive Spectroscopy (SEM‐EDS) and Focused Ion Beam ‐ Scanning Electron Microscopy (FIB)‐SEM. Complementary, secondary MFI in pyroxenites from COC were also investigated. MFI hosted in eclogite and granulites occur along growth zones or in 3D clusters in garnet porphyroblasts suggesting a primary origin at high‐pressure (HP) metamorphic conditions. The mineral assemblage of MFI is mainly composed of Fe‐Mg‐Ca‐carbonates and phyllosilicates ± graphite ± quartz ± corundum ± pyrite ± apatite ± rutile and a fluid phase composed of nitrogen ± methane ± carbon‐dioxide. The mineral proportions vary among the lithologies. Dominant carbonates and hydrous silicates are interpreted as step‐daughter minerals (crystals formed in the MFI after entrapment as a result of fluid–host interaction), whereas apatite, quartz and rutile are considered in part as accidentally trapped minerals since they also occur as crystal inclusions together with MFI in each rock type. Quartz and corundum occur together in MFI in ultramafic granulite and are regarded as step‐daughter minerals in this lithology. These observations suggest that the MFI are products of post‐entrapment reactions of a homogeneous COHN fluid system with the host mineral. Thermodynamic calculations in the CaFMAS‐COHN system confirmed that bulk composition of the MFI in eclogite is similar to the host garnet+COHN composition except for a potential lost of H2O. Carbonation and hydration reaction between the host (i.e. garnet or pyroxene) and the fluid inclusion results in the consumption of all CO2 and part of the H2O from the fluid phase producing Ca‐Fe‐Mg‐carbonates and hydrous step‐daughter minerals, mostly pyrophyllite and chlorite. Nitrogen content of the originally trapped COHN fluid in eclogite was estimated to have a maximum value of 10 mol% at peak HP conditions and 30–40 mol% at retrograde conditions that is within the range of the observed MFI in the residual fluid (13–68 mol%). Pseudosection modelling confirmed the stability of the phase assemblage in the MFI in a specific low‐pressure, low‐temperature stability field (between 300°C and 400°C at pressures < 1 GPa), caused by H2O‐ and CO2‐consuming reactions possibly in a single step. Our findings indicate that such processes in the exhuming HP units may play a role in global nitrogen and carbon cycling as well as potentially contributing to nitrogen and methane supply to subsurface–surface environments during devolatilization in the forearc regions of convergent plate margins.

Methane-Dependent Extracellular Electron Transfer at the Bioanode by the Anaerobic Archaeal Methanotroph "Candidatus Methanoperedens".

Anaerobic methanotrophic (ANME) archaea have recently been reported to be capable of using insoluble extracellular electron acceptors via extracellular electron transfer (EET). In this study, we investigated EET by a microbial community dominated by “Candidatus Methanoperedens” archaea at the anode of a bioelectrochemical system (BES) poised at 0 V vs. standard hydrogen electrode (SHE), in this way measuring current as a direct proxy of EET by this community. After inoculation of the BES, the maximum current density was 274 mA m–2 (stable current up to 39 mA m–2). Concomitant conversion of 13CH4 into 13CO2 demonstrated that current production was methane-dependent, with 38% of the current attributed directly to methane supply. Based on the current production and methane uptake in a closed system, the Coulombic efficiency was about 17%. Polarization curves demonstrated that the current was limited by microbial activity at potentials above 0 V. The metatranscriptome of the inoculum was mined for the expression of c-type cytochromes potentially used for EET, which led to the identification of several multiheme c-type cytochrome-encoding genes among the most abundant transcripts in “Ca. Methanoperedens.” Our study provides strong indications of EET in ANME archaea and describes a system in which ANME-mediated EET can be investigated under laboratory conditions, which provides new research opportunities for mechanistic studies and possibly the generation of axenic ANME cultures.

Efficient nitrogen removal from mainstream wastewater through coupling Partial Nitritation, Anammox and Methane-dependent nitrite/nitrate reduction (PNAM)

The application of partial nitritation and anammox to remove nitrogen from mainstream wastewater is of great interest because of the potential to reduce energy cost and carbon dosage. However, this process confronts a dilemma of relatively high effluent nitrogen concentration (>10 mg N/L), owning to the unwanted prevalence of nitrite-oxidizing bacteria (NOB) and the intrinsic nitrate production by anammox bacteria. Here, a novel technology, named the one-stage PNAM, that integrates Partial Nitritation, Anammox and Methane-dependent nitrite/nitrate reduction reactions, was developed in a single membrane biofilm reactor (MBfR). With feeding of synthetic mainstream wastewater containing ∼50 mg NH4+-N/L at a hydraulic retention time of 12 h, more than 95% nitrogen was removed in the established one-stage PNAM process at a practically useful rate of 0.1 kg N/m3/d. Microbial community characterization and in-situ batch tests revealed a sophisticated microbial structure consisting of ammonia-oxidizing bacteria (AOB), anammox bacteria, nitrite/nitrate-dependent anaerobic methane oxidation (n-DAMO) bacteria and archaea, and a small fraction of NOB and aerobic methanotrophs. The role of methane in removing nitrate was confirmed by switching on/off the methane supply, which relaxed the requirement for NOB suppression. In addition, the established system was relatively robust against temperature variations, evidenced by a total nitrogen removal efficiency above 80% at temperature as low as 14 ℃. The results provide a promising alternative for efficient nitrogen removal from domestic wastewater using methane as the sole carbon source.

Insight into temperature impact of Ta filaments on high-growth-rate diamond (100) films by hot-filament chemical vapor deposition

To improve the growth rate of diamond films, we grew single-crystalline (100) diamond films by hot-filament chemical vapor deposition (HFCVD), and investigated their growth mechanism. The methane/hydrogen concentration (CH4/H2) dependence of the growth rate was evaluated at a filament temperature of 3000 °C. The growth rate reached 17.9 μm/h at CH4/H2 = 5% and saturated at higher CH4/H2. We then investigated the filament-temperature dependence of the CH4 reaction rate at CH4/H2 = 5% (at which the methane supply is sufficient). The growth rate decreased with inverse filament temperature, indicating that the growth rate is governed by reactions on the filament surface. From the Arrhenius plot, the activation energy of diamond growth was estimated as 440 kJ/mol, close to that of CH4 → CH3⁎ + H⁎ decomposition. This result indicates that decomposition of CH4 and the formation of CH3 by the filament surface affect the growth rate of HFCVD-grown diamond.