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[en] Highlights: • Data on long term operation of a system supplied with real biogas are presented. • Ex-situ biological methanation is feasible for biogas upgrading. • Gas quality obtained complies with strictest direct grid injection criteria. • Biomethane can act as flexible storage for renewable surplus electricity. - Abstract: The current study reports on biological biogas upgrading by means of hydrogen addition to obtain biomethane. A mesophilic (37 °C) 0.058 m"3 trickle-bed reactor with an immobilized hydrogenotrophic enrichment culture was operated for a period of 8 months using a substrate mix of molecular hydrogen (H_2) and biogas (36–42% CO_2). Complete CO_2 conversion (> 96%) was achieved up to a H_2 loading rate of 6.5 m_n"3 H_2/m"3_r_e_a_c_t_o_r _v_o_l_. × d, corresponding to 2.3 h gas retention time. The optimum H_2/CO_2 ratio was determined to be between 3.67 and 4.15. CH_4 concentrations above 96% were achieved with less than 0.1% residual H_2. This gas quality complies even with tightest standards for grid injection without the need for additional CO_2 removal. If less rigid standards must be fulfilled H_2 loading rates can be almost doubled (10.95 versus 6.5 m_n"3 H_2/m"3_r_e_a_c_t_o_r _v_o_l_. × d) making the process even more attractive. At this H_2 loading the achieved methane productivity was 2.52 m_n"3 CH_4/m"3_r_e_a_c_t_o_r _v_o_l_. × d. In terms of biogas this corresponds to an upgrading capacity of 6.9 m_n"3 biogas/m"3_r_e_a_c_t_o_r _v_o_l_. × d. The conducted experiments demonstrate that biological methanation in an external reactor is well feasible for biogas upgrading under the prerequisite that an adequate H_2 source is available.
[en] Highlights: •A novel bio-methanation reactor was designed and evaluated. •A biofilm consisting of mixed anaerobic consortia served as the biocatalyst. •High rate methanogenesis was observed without gas-liquid agitation. •Gas conversion was successfully de-coupled from energy consumption. -- Abstract: The performance of a novel biofilm plug flow reactor containing a mixed anaerobic microbial culture was investigated for the conversion of CO2/H2 to CH4. Unlike conventional gas-liquid contactors that depend on agitation, gas diffusion was decoupled from power consumption for mixing by increasing the gas phase inside the reaction space whilst increasing the gas residence time. The mixed mesophilic culture exhibited good biofilm formation and metabolic activity. Within 82 days of operation, 99% and 90% CH4 conversion efficiencies were achieved at total gas throughputs of 100 and 150 v/v/d, respectively. At a gas input rate of 230 v/v/d, methane evolution rates reached 40 v/v/d, which are the highest to date achieved by fixed film biomethanation systems. Significant gas transfer related parasitic energy savings can be achieved when using the novel plug flow design as compared to a CSTR. The results and modelling parameters of the study can aid the development of high rate, low parasitic energy biological methanation technologies for biogas upgrading and renewable power conversion and storage systems. The study has also established a reactor system which has the potential of accelerating biotechnology developments and deployment of other novel C1 gas routes to low carbon products.
[en] Since the publication in July 2006 of the new purchase tariff of electricity produced by biogas, the methanation channel is increasing. In the past ten years the number of biogas plants from domestic wastes, passed from 1 to 20. This document presents an economic analysis of the different sources of biogas, the performances and the injection of biogas in the public network of the gas utilities. (A.L.B.)
[en] Using the ASED-MO (Atom Superposition and Electron Delocalization-Molecular Orbital) theory, we investigated carbon formation and carbon hydrogenation for CO_2 methanation on the Ni (111) surface. For carbon formation mechanism, we calculated the following activation energies, 1.27 eV for CO_2 dissociation, 2.97 eV for the CO, 1.93 eV for 2CO dissociation, respectively. For carbon methanation mechanism, we also calculated the following activation energies, 0.72 eV for methylidyne, 0.52 eV for methylene and 0.50 eV for methane, respectively. We found that the calculated activation energy of CO dissociation is higher than that of 2CO dissociation on the clean surface and base on these results that the CO dissociation step are the ratedetermining of the process. The C-H bond lengths of CH_4 the intermediate complex are 1.21 A, 1.31 A for the C···H_(_1_), and 2.82 A for the height, with angles of 105 .deg. for H_(_1_)CH and 98 .deg. for H_(_1_)CH_(_1_)
[en] It could be shown, that the direct methanation of CO2, as described by the Sabatier-reaction, CO2 + 4H2 <-> CH4 + 2H2O, can be done in laboratory and in an industrial scale under a variation of different process parameters. The Sabatier reaction is accelerated by catalysts. Different commercially available nickel and ruthenium-based catalysts were reviewed for their use in methanation and compared with self-prepared catalysts. Relevant parameters for the activity of a catalyst are the conversion of CO2, the yield of CH4 and the selectivity regarding the Sabatier-reaction. A conversion and yield of above 90% and a selectivity of nearly 100% were measured in the laboratory-set-up. Optimal parameters for the process were studied by variation of temperature, quantity of the reactants, amount of catalyst and pressure inside the reactor. An additional approach was the reaction with synthetic and real flue gases (Oxyfuel, CCS) and in this regard, a dilution of the CO2 with nitrogen and oxygen and the role of known contaminations like sulfur and nitrogen oxides that can poison the catalyst. A relation between the amount of sulfur contamination, the temperature and the decrease in activity could be determined. It was possible to discern single reaction mechanism due to the formation of carbon monoxide during the reaction. Results in the laboratory have been used for the construction of a pilot-plant that represents an upscale of 5000 in gas quantity. A number of experiments were repeated in the pilot-plant. Here, it was possible to convert nearly 250 kg/day CO2 from flue gases to methane. The pilot plant was integrated into a power plant and therefore measurements with real flue gas could be conducted. Without additional cleaning of the flue gas, a conversion rate of up to 90% was achieved. A complex temperature distribution and an increase in the temperature of the reactor up to 600 C lead to a decrease in conversion to 60%. Equilibrium between the produced and removed heat is reached at those temperatures. The resulting gas has a low energy density and is classified as a lean gas that could be used for a reconversion to electric power. The methanation of CO2 represents a possibility to store the CO2 into a loop of conversion and reconversion of energy (Power-to-Gas) and therefore it is possible to reduce the emission of greenhouse gases. The produced methane is a chemical energy storage and contributes to the stabilization of the electric grid.
[en] The Brandenburg University of Technology (BTU) has developed a double stage dry-wet fermentation process for fast and safe anaerobic degradation. Originally designed for treatment of organic wastes, this process allows using a wide variety of solid biodegradable materials. The dividing of hydrolysis and methanation in this process, allows an optimization of the different steps of biogas generation separately. The main advantages of the process are the optimum process control, an extremely stable process operation and a high gas productivity and quality. Compared to conventional processes, the retention times within the percolation stage (hydrolysis) are reduced considerably. In cooperation with the engineering and consulting company GICON, the technology was qualified further to an industrial scale. In 2007 a pilot plant, and, simultaneously, an industrial plant were built by GICON based on this double stage technology. Based on practical experience from the operation of laboratory fermentation plants, the commissioning of the pilot plant was planned, controlled and monitored by our institution. The start-up of a biogas plant of this type focuses mainly on the inoculation the of methane reactor. The growth of microbial populations and generation of a stable biocenosis within the methane reactor is essential and affects the duration of starting period as well as the methanation efficiency a long time afterwards. This paper concerns with start-up of a pilot biogas plant and discusses particular occurrences and effects during this period. (author)
[en] The review addresses direct methane oxidation — an important fundamental problem, which has attracted much attention of researchers in recent years. Analysis of the available results on biomimetic and bio-inspired methane oxygenation has demonstrated that assimilating of the experience of Nature on oxidation of methane and other alkanes significantly enriches the arsenal of chemistry and can radically change the character of the entire chemical production, as well as enables the solution of many material, energetic and environmental problems. The bibliography includes 310 references.
[en] It is a central aim of the German government to significantly reduce the emission of greenhouse gases in the next years. One possibility to reach this aim is the substitution of fossil fuels, especially natural gas, by fuels from biogenic sources (Bio-SNG). However, it is a drawback of Bio-SNG that the production costs are considerably higher than those of fossil natural gas. This work provides an approach to reduce the production costs of Bio-SNG. It is the aim to reduce the process parameters of the methane synthesis. At the same time, it has to be ensured that high methane yields are achieved even at those mild conditions. A procedure for the optimization of the methanation catalyst activity will be presented. If the catalyst is as active as possible even at mild conditions, it will be possible to produce Bio-SNG cost efficient even in small, decentralized scale.
[en] In the fuel cycle system of a fusion reactor, tritium is extracted from exhaust gas and reused. When graphite materials are used in a part of plasma facing components, tritiated methane is contained in exhaust gas. Plasma decomposition is one of the techniques for extracting hydrogen from hydrocarbon. In order to evaluate direct decomposition of methane using helium RF plasma, a flow-type plasma reactor utilizing capacitively coupled plasma was developed and direct decomposition of methane was demonstrated. The decomposition rate of methane by helium plasma was proportional to the supplied RF power. However, it became small when total pressure of gas was high. A part of hydrogen generated from methane was retained in carbon deposits on the electrode. However, the accumulated hydrogen and carbon were effectively removed by the discharge-cleaning with oxygen plasma.