Search

The utilization of fossil fuel has increased atmospheric carbon dioxide (CO2) concentrations drastically over the last few decades. This leads to global warming and climate change, increasing the occurrence of more severe weather around the world. One promising solution to reduce anthropogenic CO2 emissions is methanation. Many researchers and industries are interested in CO2 methanation as a power-to-gas technology and carbon capture and storage (CCS) system. Producing an energy carrier, methane (CH4), via CO2 methanation and water electrolysis is an exceptionally effective method of capturing energy generated by renewables. To enhance methanation efficiency, numerous researches have been conducted to develop catalysts with high activity, CH4 selectivity, and stability against the reaction heat. Therefore, in this mini-review, the characteristics and recent advances of metal-based catalysts in methanation of CO2 is discussed. [ABSTRACT FROM AUTHOR]

In recent years, there has been a growing interest in extending the potential of underground gas storage (UGS) facilities to hydrogen and carbon dioxide storage. However, this transition to hydrogen storage raises concerns regarding potential microbial reactions, which could convert hydrogen into methane. It is crucial to gain a comprehensive understanding of the microbial communities within any UGS facilities designated for hydrogen storage. In this study, underground water samples and water samples from surface technologies from 7 different UGS objects located in the Vienna Basin were studied using both molecular biology methods and cultivation methods. Results from 16S rRNA sequencing revealed that the proportion of archaea in the groundwater samples ranged from 20 to 58%, with methanogens being the predominant. Some water samples collected from surface technologies contained up to 87% of methanogens. Various species of methanogens were isolated from individual wells, including Methanobacterium sp., Methanocalculus sp., Methanolobus sp. or Methanosarcina sp. We also examined water samples for the presence of sulfate-reducing bacteria known to be involved in microbially induced corrosion and identified species of the genus Desulfovibrio in the samples. In the second part of our study, we contextualized our data by comparing it to available sequencing data from terrestrial subsurface environments worldwide. This allowed us to discern patterns and correlations between different types of underground samples based on environmental conditions. Our findings reveal presence of methanogens in all analyzed groups of underground samples, which suggests the possibility of unintended microbial hydrogen-to-methane conversion and the associated financial losses. Nevertheless, the prevalence of methanogens in our results also highlights the potential of the UGS environment, which can be effectively leveraged as a bioreactor for the conversion of hydrogen into methane, particularly in the context of Power-to-Methane technology.

Methanation of CO2 is an important reaction for reducing CO2 emissions in a power-to-gas system. Compared to cobalt supported on gamma-Al2O3, cobalt supported on graphene nanoplatelets (GNPs) showed significantly better performance for CO2 methanation. Cobalt supported on GNPs was capable of 15% conversion of CO2 to CH4 at temperatures below 250°C, compared to 5% for cobalt supported on Al2O3. In situ thermogravimetric analysis (TGA) demonstrated that the Co/GNP catalyst was stable to 400°C. The maximum catalyst mass-specific CH4 yield was obtained at a Co loading of 5wt% on GNPs; however, high Co loading on GNPs deactivated the reactivity of the Co/GNP catalyst. Transmission electron microscopy (TEM) demonstrated that 5wt% Co/GNPs had the smallest and most dispersed cobalt nanoparticles. Excessive loading of cobalt tended to form isolated large Co nanoparticles. X-ray photoelectron spectroscopy (XPS) and Raman spectrometry revealed that more CoO phases were maintained on the surface of 5wt% Co/GNPs, indicating that the interaction between the Co and the GNPs had more of an impact on cobalt’s redox capacity than did particle size, which ultimately affected cobalt’s active phase during the CO2 reduction process. Furthermore, Raman spectrometry demonstrated that Co loading led to an increase in graphene defects. Higher Co loading on GNPs resulted in fewer interfaces between Co and GNPs due to the agglomeration of Co nanoparticles.

A rising interest in a strong hydrogen economy as a part of the future net- zero economy results in an increasing necessity to store hydrogen as a raw material or an energy carrier. Experience and studies show that storing hydrogen in deep underground sites could enable microbial conversion of hydrogen. To predict and examine the loss of hydrogen, laboratory studies, and analysis are essential. A growthmodel is required to interpret batch or chemostat experiments. With this model, the parameters of microbial growth, and the conversion of hydrogen can be specified. This study presents experiments with methanogens and a hydrogen/carbon dioxide gas mixture performed in batch reactors. Further, the microbial growth was modeled by a double Monod model with hydrogen and carbon dioxide as the limiting substrates. As the amount of carbon dioxide dissolved in the water phase can not be neglected, both phases were considered in the proposed model. The mass-transfer rate between the gas and water phase was implemented by a linear relation including the concentrations in both phases and themass-transfer coefficient.With the resulting coupledmodel, it was possible tomatch the pressure behavior in the reactor and conclude themicrobial growth kinetics. Two types of methanogenic species were tested to validate the model. The mass transfer coefficient proves to impact the growth behavior in porous media. The mathematical model and experimental data are necessary to determine the growth rate and yield coefficient. [ABSTRACT FROM AUTHOR]

A rising interest in a strong hydrogen economy as a part of the future net-zero economy results in an increasing necessity to store hydrogen as a raw material or an energy carrier. Experience and studies show that storing hydrogen in deep underground sites could enable microbial conversion of hydrogen. To predict and examine the loss of hydrogen, laboratory studies, and analysis are essential. A growth model is required to interpret batch or chemostat experiments. With this model, the parameters of microbial growth, and the conversion of hydrogen can be specified. This study presents experiments with methanogens and a hydrogen/carbon dioxide gas mixture performed in batch reactors. Further, the microbial growth was modeled by a double Monod model with hydrogen and carbon dioxide as the limiting substrates. As the amount of carbon dioxide dissolved in the water phase can not be neglected, both phases were considered in the proposed model. The mass-transfer rate between the gas and water phase was implemented by a linear relation including the concentrations in both phases and the mass-transfer coefficient. With the resulting coupled model, it was possible to match the pressure behavior in the reactor and conclude the microbial growth kinetics. Two types of methanogenic species were tested to validate the model. The mass transfer coefficient proves to impact the growth behavior in porous media. The mathematical model and experimental data are necessary to determine the growth rate and yield coefficient.

In this study, we investigated Ni supported on polymer-derived ceramics as a new class of catalyst materials. Catalysts have to withstand harsh reaction conditions requiring the use of a support with outstanding thermal and mechanical stability. Polymer-derived ceramics meet these requirements and bring the additional opportunity to realize complex porous structures. Ni-SiOC and La-modified Ni-SiOC catalysts were prepared by wet impregnation methods with target concentrations of 5 wt% for both metal and oxide content. Polymer-derived SiOC supports were produced using a photoactive methyl-silsesquioxane as preceramic polymer. Catalysts were characterized by N2-adsorption-desorption, XRD, SEM, H2-TPR, and in-situ DRIFTS. CO2 methanation was performed as a test reaction to evaluate the catalytic performance of these new materials at atmospheric pressure in the temperature range between 200°C and 400°C. XDR, H2-TPR, and in-situ DRIFTS results indicate both improved dispersion and stability of Ni sites and increased adsorption capacities for CO2 in La-modified samples. Also, modified catalysts exhibited excellent performance in the CO2 methanation with CO2 conversions up to 88% and methane selectivity >99% at 300°C reaction temperature. Furthermore, the pyrolysis temperature of the support material affected the catalytic properties, the surface area, the stability of active sites, and the hydrophobicity of the surface. Overall, the materials show promising properties for catalytic applications.

Three different power-to-methane process chains with grid injection in two scales (1 MWel and 6 MWel) were analysed regarding their investment and operation cost. The process chains were based on biological or catalytic bubbling fluidised bed methanation in combination with proton exchange membrane or solid oxide electrolyser cells. A bottom-up techno-economic analysis showed a cost benefit of around 17–19% lower biomethane production cost for the bubbling fluidised bed technology as less than a third of the reactor volumes is required for catalytic methanation. This cost benefit is only given in combination with PEM electrolysis, as the high-temperature electrolyser stacks currently result in high investment cost. Based on electricity cost of 5 €-ct/kWhel and a plant size of 6 MWel, biomethane production cost of 13.95 €-ct./kWh for catalytic and 17.30 €-ct/kWh for biological methanation could be obtained, both including PEM electrolysis. A significant efficiency increase by integrating the heat of catalytic methanation reaction with the high-temperature electrolysis can be achieved; however investment cost have to decrease below 1000 €/kWel to obtain economically feasible production cost of biomethane. Under current economic and technological circumstances, CO2 methanation using the bubbling fluidised bed technology is the most cost effective.

The flexibilization of bioenergy production has the potential to counteract partly other fluctuating renewable energy sources (such as wind and solar power). As a weather-independent energy source, anaerobic digestion (AD) can offer on-demand energy supply through biogas production. Separation of the stages in anaerobic digestion represents a promising strategy for the flexibilization of the fermentative part of biogas production. Segregation in two reactor systems facilitates monitoring and control of the provision of educts to the second methanogenic stage, thus controlling biogas production. Two-stage operation has proven to reach similar or even higher methane yields and biogas purities than single-stage operation in many different fields of application. It furthermore allows methanation of green hydrogen and an easier combination of material and energy use of many biogenic raw and residual biomass sources. A lot of research has been conducted in recent years regarding the process phase separation in multi-stage AD operation, which includes more than two stages. Reliable monitoring tools, coupled with effluent recirculation, bioaugmentation and simulation have the potential to overcome the current drawbacks of a sophisticated and unstable operation. This review aims to summarize recent developments, new perspectives for coupling processes for energy and material use and a system integration of AD for power-to-gas applications. Thereby, cell physiological and engineering aspects as well as the basic economic feasibility are discussed. As conclusion, monitoring and control concepts as well as suitable separation technologies and finally the data basis for techno-economic and ecologic assessments have to be improved.

Energy-intensive industries still produce high amounts of non-renewable CO2 emissions. These emissions cannot easily be fully omitted in the short- and mid-term by electrification or switching to renewable energy carriers, as they either are of inevitable origin (e.g., mineral carbon in cement production) or require a long-term transition of well-established process chains (e.g., metal ore reduction). Therefore, carbon capture and utilization (CCU) has been widely discussed as an option to reduce net CO2 emissions. In this context, the production of synthetic natural gas (SNG) through power-to-methane (PtM) process is expected to possess considerable value in future energy systems. Considering current low-temperature electrolysis technologies that exhibit electric efficiencies of 60–70%el, LHV and methanation with a caloric efficiency of 82.5%LHV, the conventional PtM route is inefficient. However, overall efficiencies of >80%el, LHV could be achieved using co-electrolysis of steam and CO2 in combination with thermal integration of waste heat from methanation. The present study investigates the techno-economic performance of such a thermally integrated system in the context of different application scenarios that allow for the establishment of a closed carbon cycle. Considering potential technological learning and scaling effects, the assessments reveal that compared to that of decoupled low-temperature systems, SNG generation cost of

The article titled "Current developments in catalytic methanation of carbon dioxide-a review" has been retracted by the journal Frontiers in Energy Research. The retraction was made due to the discovery of undisclosed conflicts of interest that compromised the integrity of the peer review process. As a result, the scientific reliability of the article cannot be guaranteed. The retraction was approved by the Chief Executive Editor of Frontiers, and the authors were notified and given an opportunity to respond. [Extracted from the article]

At the heart of most Power-to-X (PtX) concepts is the utilization of renewable electricity to produce hydrogen through the electrolysis of water. This hydrogen can be used directly as a final energy carrier or it can be converted into, for example, methane, synthesis gas, liquid fuels, electricity, or chemicals. Technical demonstration and systems integration are of major importance for integrating PtX into energy systems. As of June 2020, a total of 220 PtX research and demonstration projects in Europe have either been realized, completed, or are currently being planned. The central aim of this review is to identify and assess relevant projects in terms of their year of commissioning, location, electricity and carbon dioxide sources, applied technologies for electrolysis, capacity, type of hydrogen post-processing, and the targeted field of application. The latter aspect has changed over the years. At first, the targeted field of application was fuel production, for example for hydrogen buses, combined heat and power generation, and subsequent injection into the natural gas grid. Today, alongside fuel production, industrial applications are also important. Synthetic gaseous fuels are the focus of fuel production, while liquid fuel production is severely under-represented. Solid oxide electrolyzer cells (SOECs) represent a very small proportion of projects compared to polymer electrolyte membranes (PEMs) and alkaline electrolyzers. This is also reflected by the difference in installed capacities. While alkaline electrolyzers are installed with capacities between 50 and 5000 kW (2019/20) and PEM electrolyzers between 100 and 6000 kW, SOECs have a capacity of 150 kW. France and Germany are undertaking the biggest efforts to develop PtX technologies compared to other European countries. On the whole, however, activities have progressed at a considerably faster rate than had been predicted just a couple of years ago.

Bioelectrochemical power-to-gas represents a novel solution for electrical energy storage, currently under development. It allows storing renewable energy surplus in the form of methane (CH4), while treating wastewater, therefore bridging the electricity and natural gas (and wastewater) grids. The technology can be coupled with membrane contactors for carbon dioxide (CO2) capture, dissolving the CO2 in wastewater before feeding it to the bioelectrochemical system. This way, the integrated system can achieve simultaneous carbon capture and energy storage objectives, in the scenario of a wastewater treatment plant application. In this study, such technology was developed in a medium-scale prototype (32 L volume), which was operated for 400 days in different conditions of temperature, voltage and CO2 capture rate. The prototype achieved the highest CH4 production rate (147 ± 33 L m–3 d–1) at the lowest specific energy consumption (1.0 ± 0.3 kWh m–3 CH4) when operated at 25°C and applying a voltage of 0.7 V, while capturing and converting 22 L m–3 d–1 of CO2. The produced biogas was nearer to biomethane quality (CH4 > 90% v/v) when CO2 was not injected in the wastewater. Traces of hydrogen (H2) in the biogas, detectable during the periods of closed electrical circuit operation, indicated that hydrogenotrophic methanogenesis was taking place at the cathode. On the other hand, a relevant CH4 production during the periods of open electrical circuit operation confirmed the presence of acetoclastic methanogenic microorganisms in the microbial community, which was dominated by the archaeal genus Methanothrix (Euryarchaeota). Different operational taxonomic units belonging to the bacterial Synergistes phylum were found at the anode and the cathode, having a potential role in organic matter degradation and H2 production, respectively. In the panorama of methanation technologies currently available for power-to-gas, the performances of this bioelectrochemical prototype are not yet competitive, especially in terms of volumetric CH4 production rate and power density demand. However, the possibility to obtain a high-quality biogas (almost reaching biomethane quality standards) at a minimal energy consumption represents a potentially favorable business scenario for this technology.

With the development and prosperity of the global economy, the emission of carbon dioxide (CO2) has become an increasing concern. Its greenhouse effect will cause serious environmental problems, such as the global warming and climate change. Therefore, the worldwide scientists have devoted great efforts to control CO2 emissions through various strategies, such as capture, resource utilization, sequestration, etc. Among these, the catalytic conversion of CO2 to methane is considered as one of the most efficient routes for resource utilization of CO2 owing to the mild reaction conditions and simple reaction device. Pioneer thermodynamic studies have revealed that low reaction temperature is beneficial to the high catalytic activity and CH4 selectivity. However, the low temperature will be adverse to the enhancement of the reaction rate due to kinetic barrier for the activation of CO2. Therefore, the invention of highly efficient catalysts with promising low temperature activities toward CO2 methanation reaction is the key solution. The Ni based catalysts have been widely investigated as the catalysts toward CO2 methanation due to their low cost and excellent catalytic performances. However, the Ni based catalysts usually perform poor low-temperature activities and stabilities. Therefore, the development of highly efficient Ni based catalysts with excellent low-temperature catalytic performances has become the research focus as well as challenge in this field. Therefore, we summarized the recent research progresses of constructing highly efficient Ni based catalysts toward CO2 methanation in this review. Specifically, the strategies on how to enhance the catalytic performances of the Ni based catalysts have been carefully reviewed, which include various influencing factors, such as catalytic supports, catalytic auxiliaries and dopants, the fabrication methods, reaction conditions, etc. Finally, the future development trend of the Ni based catalysts is also prospected, which will be helpful to the design and fabrication of the Ni catalysts with high efficiency toward CO2 methanation process.

Syngas generated by thermal gasification of biomass or coal can be steam reformed and purified into methane, which could be used locally for energy needs, or re-injected in the natural gas grid. As an alternative to chemical catalysis, the main components of the syngas (CO, CO2, and H2) can be used as substrates by a wide range of microorganisms, to be converted into gas biofuels, including methane. This study evaluates the carboxydotrophic (CO-consuming) methanogenic potential present in an anaerobic sludge from an upflow anaerobic sludge bed (UASB) reactor treating waste water, and elucidates the CO conversion routes to methane at 35±3˚C. Kinetic activity tests under CO at partial pressures (pCO) varying from 0.1 to 1.5 atm (0.09-1.31 mmol/L in the liquid phase) showed a significant carboxydotrophic activity potential for growing conditions on CO alone. A maximum methanogenic activity of 1 mmol CH4 per g of volatile suspended solid and per day was achieved at 0.2 atm of CO (0.17 mmol/L), and then the rate decreased with the amount of CO supplied. The intermediary metabolites such as acetate, H2 and propionate started to accumulate at higher CO concentrations. Inhibition experiments with 2-bromoethanesulfonic acid (BES), fluoroacetate, and vancomycin showed that in a mixed culture CO was converted mainly to acetate by acetogenic bacteria, which was further transformed to methane by acetoclastic methanogens, while direct methanogenic CO conversion was negligible. Methanogenesis was totally blocked at high pCO in the bottles (≥ 1 atm). However it was possible to achieve higher methanogenic potential under a 100% CO atmosphere after acclimation of the sludge to CO. This adaptation to high CO concentrations led to a shift in the archaeal population, then dominated by hydrogen-utilizing methanogens, which were able to take over acetoclastic methanogens, while syntrophic acetate oxidizing (SAO) bacteria oxidized acetate into CO2 and H2. The disaggregation of the granular sludge showed a negative impact on their methanogenic activity, confirming that the acetoclastic methanogens were the most sensitive to CO, and a contrario, the advantage of using granular sludge for further development towards large-scale methane production from CO-rich syngas.

Syngas generated by thermal gasification of biomass or coal can be steam reformed and purified into methane, which could be used locally for energy needs, or re-injected in the natural gas grid. As an alternative to chemical catalysis, the main components of the syngas (CO, CO2, and H2) can be used as substrates by a wide range of microorganisms, to be converted into gas biofuels, including methane. This study evaluates the carboxydotrophic (CO-consuming) methanogenic potential present in an anaerobic sludge from an upflow anaerobic sludge bed (UASB) reactor treating waste water, and elucidates the CO conversion routes to methane at 35 ± 3?C. Kinetic activity tests under CO at partial pressures (pCO) varying from 0.1 to 1.5 atm (0.09-1.31 mmol/L in the liquid phase) showed a significant carboxydotrophic activity potential for growing conditions on CO alone. A maximum methanogenic activity of 1 mmol CH4 per g of volatile suspended solid and per day was achieved at 0.2 atm of CO (0.17 mmol/L), and then the rate decreased with the amount of CO supplied. The intermediary metabolites such as acetate, H2, and propionate started to accumulate at higher CO concentrations. Inhibition experiments with 2-bromoethanesulfonic acid (BES), fluoroacetate, and vancomycin showed that in a mixed culture CO was converted mainly to acetate by acetogenic bacteria, which was further transformed to methane by acetoclastic methanogens, while direct methanogenic CO conversion was negligible. Methanogenesis was totally blocked at high pCO in the bottles (≽1 atm). However it was possible to achieve higher methanogenic potential under a 100% CO atmosphere after acclimation of the sludge to CO. This adaptation to high CO concentrations led to a shift in the archaeal population, then dominated by hydrogen-utilizing methanogens, which were able to take over acetoclastic methanogens, while syntrophic acetate oxidizing (SAO) bacteria oxidized acetate into CO2 and H2. The disaggregation of the granular sludge showed a negative impact on their methanogenic activity, confirming that the acetoclastic methanogens were the most sensitive to CO, and a contrario, the advantage of using granular sludge for further development toward large-scale methane production from CO-rich syngas. [ABSTRACT FROM AUTHOR]