Search results for: methane conversion

Authors: Marcin Dębowski, Marcin Zieliński, Mirosław Krzemieniewski

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As methane fermentation is a complex series of successive biochemical transformations, its subsequent stages are determined, to a various extent, by physical and chemical factors. A specific state of equilibrium is being settled in the functioning fermentation system between environmental conditions and the rate of biochemical reactions and products of successive transformations. In the case of physical factors that influence the effectiveness of methane fermentation transformations, the key significance is ascribed to temperature and intensity of biomass agitation. Among the chemical factors, significant are pH value, type, and availability of the culture medium (to put it simply: the C/N ratio) as well as the presence of toxic substances. One of the important elements which influence the effectiveness of methane fermentation is the pre-treatment of organic substrates and the mode in which the organic matter is made available to anaerobes. Out of all known and described methods for organic substrate pre-treatment before methane fermentation process, the ultrasound disintegration is one of the most interesting technologies. Investigations undertaken on the ultrasound field and the use of installations operating on the existing systems result principally from very wide and universal technological possibilities offered by the sonication process. This physical factor may induce deep physicochemical changes in ultrasonicated substrates that are highly beneficial from the viewpoint of methane fermentation processes. In this case, special role is ascribed to disintegration of biomass that is further subjected to methane fermentation. Once cell walls are damaged, cytoplasm and cellular enzymes are released. The released substances – either in dissolved or colloidal form – are immediately available to anaerobic bacteria for biodegradation. To ensure the maximal release of organic matter from dead biomass cells, disintegration processes are aimed to achieve particle size below 50 μm. It has been demonstrated in many research works and in systems operating in the technical scale that immediately after substrate supersonication the content of organic matter (characterized by COD, BOD5 and TOC indices) was increasing in the dissolved phase of sedimentation water. This phenomenon points to the immediate sonolysis of solid substances contained in the biomass and to the release of cell material, and consequently to the intensification of the hydrolytic phase of fermentation. It results in a significant reduction of fermentation time and increased effectiveness of production of gaseous metabolites of anaerobic bacteria. Because disintegration of Virginia fanpetals biomass via ultrasounds applied in order to intensify its conversion is a novel technique, it is often underestimated by exploiters of agri-biogas works. It has, however, many advantages that have a direct impact on its technological and economical superiority over thus far applied methods of biomass conversion. As for now, ultrasound disintegrators for biomass conversion are not produced on the mass-scale, but by specialized groups in scientific or R&D centers. Therefore, their quality and effectiveness are to a large extent determined by their manufacturers’ knowledge and skills in the fields of acoustics and electronic engineering.

Keywords: ultrasound disintegration, biomass, methane fermentation, biogas, Virginia fanpetals

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Authors: Doo Ki Lee, Kumaresh Selvakumar, Man Young Kim

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Catalytic combustion is an environmentally friendly technique to combust fuels in gas turbines. In this paper, the behavior of surface reaction rate on catalytic combustion is studied with respect to the heterogeneous oxidation of methane-air mixture in a catalytic reactor. Plug flow reactor (PFR), the simplified single catalytic channel assists in investigating the catalytic combustion phenomenon over the Pt catalyst by promoting the desired chemical reactions. The numerical simulation with multi-step elementary surface reactions is governed by the availability of free surface sites onto the catalytic surface and thereby, the catalytic combustion characteristics are demonstrated by examining the rate of the reaction for lean fuel mixture. Further, two different surface reaction mechanisms are adopted and compared for surface reaction rates to indicate the controlling heterogeneous reaction for better fuel conversion. The performance of platinum catalyst under heterogeneous reaction is analyzed under the same temperature condition, where the catalyst with the higher kinetic rate of reaction would have a maximum catalytic activity for enhanced methane catalytic combustion.

Keywords: catalytic combustion, heterogeneous reaction, plug flow reactor, surface reaction rate

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Authors: Lazic Marina, Sugden Scott, Sharma Kanta Hem, Sauvageau Dominic, Stein Lisa

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Methane is a highly potent greenhouse gas mostly released through anthropogenic activities. Methane represents a low-cost and sustainable feedstock used for the biological production of value-added compounds by bacteria known as methanotrophs. In addition to methane, these organisms can utilize methanol, another cheap carbon source that is a common industrial by-product. Alphaproteobacteria methanotrophs can utilize both methane and methanol to produce the biopolymer polyhydroxybutyrate. The goal of this study was to examine the effect of methanol on polyhydroxybutyrate production in Methylocystis sp. Rockwell and to identify the optimal methane: methanol ratio that will improve PHB without reducing biomass production. Three methane: methanol ratios (4, 2.5., and 0.5) and three nitrogen source (ammonium or nitrate) concentrations (10 mM, 1 mM, and 0.1 mM) were combined to generate 18 growing conditions (9 per carbon source). The production of polyhydroxybutyrate and biomass was analyzed at the end of growth. Overall, the methane: methanol ratios that promoted polyhydroxybutyrate synthesis without reducing biomass were 4 and 2.5 and the optimal nitrogen concentration was 1 mM for both ammonium and nitrate. The physiological mechanism behind the beneficial effect of combining methane and methanol as carbon sources remain to be discovered. One possibility is that methanol has a dual role as a carbon source at lower concentrations and as a stringent response trigger at higher concentrations. Nevertheless, the beneficial effect of methanol and optimal nitrogen concentration for PHB production was confirmed, providing a basis for future physiological analysis and conditions for process scale-up.

Keywords: methane, methanol, methanotrophs, polyhydroxybutyrate, methylocystis sp. rockwell, single carbon bioconversions

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Authors: E. Al-Essa, R. Bello-Mendoza, D. G. Wareham

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Anaerobic batch experiments were conducted to investigate the effect of magnetite-supplementation (7 mM) on methane production from digested sludge undergoing two different microbial growth phases, namely fresh sludge (exponential growth phase) and degassed sludge (endogenous decay phase). Three different particle sizes were assessed: small (50 - 150 nm), medium (168 – 490 nm) and large (800 nm - 4.5 µm) particles. Results show that, in the case of the fresh sludge, magnetite significantly enhanced the methane production rate (up to 32%) and reduced the lag phase (by 15% - 41%) as compared to the control, regardless of the particle size used. However, the cumulative methane produced at the end of the incubation was comparable in all treatment and control bottles. In the case of the degassed sludge, only the medium-sized magnetite particles increased significantly the methane production rate (12% higher) as compared to the control. Small and large particles had little effect on the methane production rate but did result in an extended lag phase which led to significantly lower cumulative methane production at the end of the incubation period. These results suggest that magnetite produces a clear and positive effect on methane production only when an active and balanced microbial community is present in the anaerobic digester. It is concluded that, (i) the effect of magnetite particle size on increasing the methane production rate and reducing lag phase duration is strongly influenced by the initial metabolic state of the microbial consortium, and (ii) the particle size would positively affect the methane production if it is provided within the nanometer size range.

Keywords: anaerobic digestion, iron oxide, methanogenesis, nanoparticle

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Authors: Alexander J. Severinsky, Allen L. Sessoms

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Atmospheric carbon dioxide (CO₂) has dominated the discussion about the causes of climate change. This is a reflection of the time horizon that has become the norm adopted by the IPCC as the planning horizon. Recently, it has become clear that a 100-year time horizon is much too long, and yet almost all mitigation efforts, including those in the near-term horizon of 30 years, are geared toward it. In this paper, we show that, for a 30-year time horizon, methane (CH₄) is the greenhouse gas whose radiative forcing exceeds that of CO₂. In our analysis, we used radiative forcing of greenhouse gases in the atmosphere since they directly affect the temperature rise on Earth. In 2019, the radiative forcing of methane was ~2.5 W/m² and that of carbon dioxide ~2.1 W/m². Under a business-as-usual (BAU) scenario until 2050, such forcing would be ~2.8 W/m² and ~3.1 W/m², respectively. There is a substantial spread in the data for anthropogenic and natural methane emissions as well as CH₄ leakages from production to consumption. We estimated the minimum and maximum effects of the reduction of these leakages. Such action may reduce the annual radiative forcing of all CH₄ emissions by between ~15% and ~30%. This translates into a reduction of the RF by 2050 from ~2.8 W/m² to ~2.5 W/m² in the case of the minimum effect and to ~2.15 W/m² in the case of the maximum. Under the BAU, we found that the RF of CO₂ would increase from ~2.1 W/m² nowadays to ~3.1 W/m² by 2050. We assumed a reduction of 50% of anthropogenic emission linearly over the next 30 years. That would reduce radiative forcing from ~3.1 W/m² to ~2.9 W/m². In the case of ‘net zero,’ the other 50% of reduction of only anthropogenic emissions would be limited to either from sources of emissions or directly from the atmosphere. The total reduction would be from ~3.1 to ~2.7, or ~0.4 W/m². To achieve the same radiative forcing as in the scenario of maximum reduction of methane leakages of ~2.15 W/m², then an additional reduction of radiative forcing of CO₂ would be approximately 2.7 -2.15=0.55 W/m². This is a much larger value than in expectations from ‘net zero’. In total, one needs to remove from the atmosphere ~660 GT to match the maximum reduction of current methane leakages and ~270 GT to achieve ‘net zero.’ This amounts to over 900 GT in total.

Keywords: methane leakages, methane radiative forcing, methane mitigation, methane net zero

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Authors: S. H. Nguyen, L. Li, R. S. Hegarty

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Two experiments were conducted assessing the effects of presence or absence of rumen protozoa and dietary nitrate addition on rumen fermentation characteristics and methane production in Brahman heifers. The first experiment assessed changes in rumen fermentation pattern and in-vitro methane production post-refaunation and the second experiment investigated whether addition of nitrate to the incubation would give rise to methane mitigation additional to that contributed by defaunation. Ten Brahman heifers were progressively adapted to a diet containing coconut oil distillate 4.5% (COD) for 18 d and then all heifers were defaunated using sodium 1-(2-sulfonatooxyethoxy) dodecane (Empicol). After 15 d, the heifers were given a second dose of Empicol. Fifteen days after the second dosing, all heifers were allocated to defaunated or refaunated groups by stratified randomisation. On d 48, an oral dose of rumen fluid collected from unrelated faunated cattle was used to inoculate 5 heifers and form a refaunated group so that the effects of re-establishment of protozoa on fermentation characteristics could be investigated. Samples of rumen fluid collected from each animal using oesophageal intubation before feeding on d 48, 55, 62 and 69 were incubated for 23h in-vitro (experiment 1). On day 82, 2% of NO3 (as NaNO3) was included in in-vitro incubations (experiment 2) to test for additivity of NO3 and absence of protozoa effects on fermentation and methane production. It was concluded that increasing protozoal numbers were associated with increased methane production, with methane production rate significantly higher from refaunated heifers than from defaunated heifers 7, 14 and 21 d after refaunation. Concentration and proportions of major VFA, however, were not affected by protozoal treatments. There is scope for further reducing methane output through combining defaunation and dietary nitrate as the addition of nitrate in the defaunated heifers resulted in 86% reduction in methane production in-vitro.

Keywords: defaunation, nitrate, fermentation, methane production

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Authors: Khalid Elbadawi Elshafea, Mahmoud Hassan Onsa

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This paper presents the results of the experiments to measure the impact of pasteurization cows dung on important parameter of anaerobic digestion (retention time) and measure the effect in daily production rate of biogas, were used local materials in these experiments, two experiments were carried out in two bio-digesters (1 and 2) (18.0 L), volume of the mixture 16.0-litre and the mass of dry matter in the mixture 4.0 Kg of cow dung. Pasteurization process has been conducted on the mixture into the digester 2, and put two digesters under room temperature. Digester (1) produced 268.5 liter of methane in period of 49 days with daily methane production rate 1.37L/Kg/day, and digester (2) produced 302.7-liter of methane in period of 26 days with daily methane production rate 2.91 L/Kg/day. This study concluded that the use of system pasteurization cows dung speed up hydrolysis in anaerobic process, because heat to certain temperature in certain time lead to speed up chemical reactions (transfer Protein to Amino acids, Carbohydrate to Sugars and Fat to Long chain fatty acids), this lead to reduce the retention time an therefore increase the daily methane production rate with 212%.

Keywords: methane, cow dung, daily production, pasteurization, increase

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Authors: Assal E. Haddad

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Food waste samples from Irbid were collected from 5 different sources for 12 weeks to characterize their composition in terms of four food categories; rice, meat, fruits and vegetables, and bread. Average food type compositions were 39% rice, 6% meat, 34% fruits and vegetables, and 23% bread. Methane yield was also measured for all food types and was found to be 362, 499, 352, and 375 mL/g VS for rice, meat, fruits and vegetables, and bread, respectively. A representative food waste sample was created to test the actual methane yield and compare it to calculated one. Actual methane yield (414 mL/g VS) was greater than the calculated value (377 mL/g VS) based on food type proportions and their specific methane yield. This study emphasizes the effect of the types of food and their proportions in food waste on the final biogas production. Findings in this study provide representative methane emission factors for Irbid’s food waste, which represent as high as 68% of total Municipal Solid Waste (MSW) in Irbid, and also indicate the energy and economic value within the solid waste stream in Irbid.

Keywords: food waste, solid waste management, anaerobic digestion, methane yield

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Authors: M. Amanipour, J. Towfighi, E. Ganji Babakhani, M. Heidari

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Cylindrical alumina microfiltration membrane (GMITM Corporation, inside diameter=9 mm, outside diameter=13 mm, length= 50 mm) with an average pore size of 0.5 micrometer and porosity of about 0.35 was used as the support for membrane reactor. This support was soaked in boehmite sols, and the mean particle size was adjusted in the range of 50 to 500 nm by carefully controlling hydrolysis time, and calcined at 650 °C for two hours. This process was repeated with different boehmite solutions in order to achieve an intermediate layer with an average pore size of about 50 nm. The resulting substrate was then coated with a thin and dense layer of silica by counter current chemical vapour deposition (CVD) method. A boehmite sol with 10 wt.% of nickel which was prepared by a standard procedure was used to make the catalytic layer. BET, SEM, and XRD analysis were used to characterize this layer. The catalytic membrane reactor was placed in an experimental setup to evaluate the permeation and hydrogen separation performance for a steam reforming reaction. The setup consisted of a tubular module in which the membrane was fixed, and the reforming reaction occurred at the inner side of the membrane. Methane stream, diluted with nitrogen, and deionized water with a steam to carbon (S/C) ratio of 3.0 entered the reactor after the reactor was heated up to 500 °C with a specified rate of 2 °C/ min and the catalytic layer was reduced at presence of hydrogen for 2.5 hours. Nitrogen flow was used as sweep gas through the outer side of the reactor. Any liquid produced was trapped and separated at reactor exit by a cold trap, and the produced gases were analyzed by an on-line gas chromatograph (Agilent 7890A) to measure total CH₄ conversion and H₂ permeation. BET analysis indicated uniform size distribution for catalyst with average pore size of 280 nm and average surface area of 275 m².g^-1. Single-component permeation tests were carried out for hydrogen, methane, and carbon dioxide at temperature range of 500-800 °C, and the results showed almost the same permeance and hydrogen selectivity values for hydrogen as the composite membrane without catalytic layer. Performance of the catalytic membrane was evaluated by applying membranes as a membrane reactor for methane steam reforming reaction at gas hourly space velocity (GHSV) of 10,000 h⁻¹ and 2 bar. CH₄ conversion increased from 50% to 85% with increasing reaction temperature from 600 °C to 750 °C, which is sufficiently above equilibrium curve at reaction conditions, but slightly lower than membrane reactor with packed nickel catalytic bed because of its higher surface area compared to the catalytic layer.

Keywords: catalytic membrane, hydrogen, methane steam reforming, permeance

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Authors: N. Boontian

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Biological conversion of biomass to methane has received increasing attention in recent years. Grasses have been explored for their potential anaerobic digestion to methane. In this review, extensive literature data have been tabulated and classified. The influences of several parameters on the potential of these feedstocks to produce methane are presented. Lignocellulosic biomass represents a mostly unused source for biogas and ethanol production. Many factors, including lignin content, crystallinity of cellulose, and particle size, limit the digestibility of the hemicellulose and cellulose present in the lignocellulosic biomass. Pretreatments have used to improve the digestibility of the lignocellulosic biomass. Each pretreatment has its own effects on cellulose, hemicellulose and lignin, the three main components of lignocellulosic biomass. Solid-state anaerobic digestion (SS-AD) generally occurs at solid concentrations higher than 15%. In contrast, liquid anaerobic digestion (AD) handles feedstocks with solid concentrations between 0.5% and 15%. Animal manure, sewage sludge, and food waste are generally treated by liquid AD, while organic fractions of municipal solid waste (OFMSW) and lignocellulosic biomass such as crop residues and energy crops can be processed through SS-AD. An increase in operating temperature can improve both the biogas yield and the production efficiency, other practices such as using AD digestate or leachate as an inoculant or decreasing the solid content may increase biogas yield but have negative impact on production efficiency. Focus is placed on substrate pretreatment in anaerobic digestion (AD) as a means of increasing biogas yields using today’s diversified substrate sources.

Keywords: anaerobic digestion, lignocellulosic biomass, methane production, optimization, pretreatment

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Authors: A. Alkattib, M. Boumaza

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Steam reforming is industrially important as it is incorporated in several major chemical processes including the production of ammonia, methanol, hydrogen and ox alcohols. Due to the strongly endothermic nature of the process, a large amount of heat is supplied by fuel burning (commonly natural gas) in the furnace chamber. Reaction conversions, tube catalyst life, energy consumption and CO2 emission represent the principal factors affecting the performance of this unit and are directly influenced by the high operating temperatures and pressures. This study presents a simulation of the performance of the reforming of methane in a primary reformer, through a developed empirical relation which enables to investigate the effects of operating parameters such as the pressure, temperature, steam to carbon ratio on the production of hydrogen, as well as the fraction of non-converted methane. It appears from this analysis that the exit temperature Te, the operating pressure as well the steam to carbon ratio has an important effect on the reforming of methane.

Keywords: reforming, methane, performance, hydrogen, parameters

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Authors: Ajay Dwivedi, M. Suresh Kumar, A. N. Vaidya

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The problem of fruit and vegetable waste management is a grave one and with ever increasing need to feed the exponentially growing population, more and more solid waste in the form of fruit and vegetables waste are generated and its management has become one of the key issues in protection of environment. Energy generation from fruit and vegetables waste by dark anaerobic fermentation is a recent an interesting avenue effective management of solid waste as well as for generating free and cheap energy. In the present study 17 vegetables were characterized for their physical as well as chemical properties, these characteristics were used to determine the hydrogen and methane potentials of vegetable from various models, and also lab scale batch experiments were performed to determine their actual hydrogen and methane production capacity. Lab scale batch experiments proved that vegetable waste can be used as effective substrate for bio hydrogen and methane production, however the expected yield of bio hydrogen and methane was much lower than predicted by models, this was due to the fact that other vital experimental parameters such as pH, total solids content, food to microorganism ratio was not optimized.

Keywords: vegetable waste, physico-chemical characteristics, hydrogen, methane

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Authors: Washaya Soul, Mupangwa John, Mapfumo Lizwell, Muchenje Voster

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Ruminant animals contribute a considerable amount of methane to the atmosphere, which is a cause of concern for global warming. Two studies were conducted in beef and goats where the studies aimed to determine the enteric CH₄ levels from a herd of beef cows raised on semi-arid rangelands and to evaluate the effect of supplementing goats with forage legumes: Vigna unguiculata and Lablab purpureus on enteric methane production. A total of 24 cows were selected from Boran and Nguni cows (n = 12 per breed) from two different farms; parity (P1 – P4) and season (dry vs. wet) were considered predictor variables in the first experiment. Eighteen goats (weaners, 9 males, 9 females) were used, in which sex and forage species were predictor variables in the second experiment. Three treatment diets were used in goats. Methane was measured using a Laser methane detector [LMD] for six consecutive days and repeated once after every three months in beef cows and once every week for 6 weeks in goats during the post-adaptation period. Parity and breed had no effects on CH₄ production in beef cows; however, season significantly influenced CH₄ outputs. Methane production was higher (P<0.05) in the dry compared to the wet season, 31.1CH₄/DMI(g/kg) and 28.8 CH₄/DMI(g/kg) for the dry and wet seasons, respectively. In goats, forage species and sex of the animal affected enteric methane production (P<0.05). Animals produce more gas when ruminating than feeding or just standing for all treatments. The control treatment exhibited higher (P<0.05) methane emissions per kg of DMI. Male goats produced more methane compared to females (17.40L/day; 12.46 g/kg DMI and 0.126g/day) versus (15.47L/day, 12.28 g/kg DMI, 0.0109g/day) respectively. It was concluded that cows produce more CH₄/DMI during the dry season, while forage legumes reduce enteric methane production in goats, and male goats produce more gas compared to females. It is recommended to introduce forage legumes, particularly during the dry season, to reduce the amount of gas produced.

Keywords: beef cows, extensive grazing system, forage legumes, greenhouse gases, goats Laser methane detector.

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Authors: Sergey Nikitenko, Vladimir Klishin, Yury Malakhov, Elena Goosen

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Transition to renewable energy sources (solar, wind, bioenergy, etc.) and launching of alternative energy generation has weakened the role of coal as a source of energy. The Paris Agreement and assumption of obligations by many nations to orderly reduce CO₂ emissions by means of technological modernization and climate change adaptation has abridged coal demand yet more. This paper aims to assess current resilience of the coal industry to stress and to define prospects for coal production optimization using high technologies pursuant to global challenges and requirements of energy transition. Our research is based on the resilience concept adapted to the coal industry. It is proposed to divide the coal sector into segments depending on the prevailing value chains (VC). Four representative models of VC are identified in the coal sector. The most promising lines of upgrading VC in the coal industry include: •Elongation of VC owing to introduction of clean technologies of coal conversion and utilization; •Creation of parallel VC by means of waste management; •Branching of VC (conversion of a company’s VC into a production network). The upgrade effectiveness is governed in many ways by applicability of advanced coal processing technologies, usability of waste, expandability of production, entrance to non-rival markets and localization of new segments of VC in receiving regions. It is also important that upgrade of VC by means of formation of agile high-tech inter-industry production networks within the framework of operating surface and underground mines can reduce social, economic and ecological risks associated with closure of coal mines. Such promising route of VC upgrade is application of methanotrophic bacteria to produce protein to be used as feed-stuff in fish, poultry and cattle breeding, or in production of ferments, lipoids, sterols, antioxidants, pigments and polysaccharides. Closed mines can use recovered methane as a clean energy source. There exist methods of methane utilization from uncontrollable sources, including preliminary treatment and recovery of methane from air-and-methane mixture, or decomposition of methane to hydrogen and acetylene. Separated hydrogen is used in hydrogen fuel cells to generate power to feed the process of methane utilization and to supply external consumers. Despite the recent paradigm of carbon-free energy generation, it is possible to preserve the coal mining industry using the differentiated approach to upgrade of value chains based on flexible technologies with regard to specificity of mining companies.

Keywords: resilience, resilience concept, resilience indicator, resilience in the Russian coal industry, value chains

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Authors: S. Jaikeaw, S. Chavadej

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The objective of this study was to determine the effects of COD loading rate on hydrogen and methane production and micronutrient transportation using a two-stage upflow anaerobic sludge blanket (UASB) system under mesophilic temperature (37°C) with a constant recycle ratio of 1:1 (final effluent flow rate: feed flow rate). The first (hydrogen) UASB unit having 4 L liquid holding volume was controlled at pH 5.5 but the second (methane) UASB unit having 24 L liquid holding volume had no pH control. The two-stage UASB system operated at different COD loading rates from 8 to 20 kg/m³d based on total UASB working volume. The results showed that, at the optimum COD loading rate of 13 kg/m³d, the produced gas from the hydrogen UASB unit contained 1.5% H₂, 16.5% CH₄, and 82% CO₂ with H₂S of 252 ppm and also provided a hydrogen yield of 1.66 mL/g COD removed (or 0.56 mL/g COD applied) and a specific hydrogen production rate of 156.85 ml H₂/LRd (or 5.12 ml H₂/g MLVSS d). Under the optimum COD loading rate, the produced gas from the methane UASB unit mainly contained methane and carbon dioxide without hydrogen of 74 and 26%, respectively with hydrogen sulfide of 287 ppm and the system also provided a maximum methane yield of 407.00 mL/g COD removed (or 263.23 mL/g COD applied) and a specific methane production rate of 2081.44 ml CH₄/LRd (or 99.75 ml CH₄/g MLVSS d). Under the optimum COD loading rate, all micronutrients markedly dropped by the sulfide precipitation reactions. The reduction of micronutrients mostly appeared in the methane UASB unit. Under the studied conditions, both Co and Ni were found to be greatly precipitated out, causing the deficiency to microbial activity. It is hypothesized that an addition of both Co and Ni can improve the methanogenic activity.

Keywords: hydrogen and methane production, ethanol wastewater, a two-stage upflow anaerobic blanket (UASB) system, mesophillic temperature, microbial concentration (MLVSS), micronutrients

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Authors: N. Lovanh, J. Loughrin, G. Ruiz-Aguilar

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Animal wastes can serve as the feedstock for biogas production (mainly methane) that could be used as alternative energy source. The green energy derived from animal wastes is considered to be carbon neutral and offsetting those generated from fossil fuels. In this study, an evaluation of system parameters on methane production from anaerobic digesters utilizing poultry rendering plant wastewater was carried out. Anaerobic batch reactors and continuous flow system subjected to different operation conditions (i.e., flow rate, temperature, and etc.) containing poultry rendering wastewater were set up to evaluate methane potential from each scenario. Biogas productions were sampled and monitored by gas chromatography and photoacoustic gas analyzer over six months of operation. The results showed that methane productions increased as the temperature increased. However, there is an upper limit to the increase in the temperature on the methane production. Flow rates and type of systems (batch vs. plug-flow regime) also had a major effect on methane production. Constant biogas production was observed in plug-flow system whereas batch system produced biogas quicker and tapering off toward the end of the six-month study. Based on these results, it is paramount to consider operating conditions and system setup in optimizing biogas production from agricultural wastewater.

Keywords: anaerobic digestion, methane, poultry rendering wastewater, biotechnology

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Authors: Passkorn Khanthongthip, John T. Novak

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Many studies have been reported that the nZVI and MgO NPs were often found in waste activated sludge (WAS). However, little is known about the impact of those NPs on WAS stabilization. The aims of this study were to investigate the effects of both NPs on WAS anaerobic digestion for methane production and to examine the change of metanogenic population under those different environments using qPCR. Four dosages (2, 50, 100, and 200 mg/g-TSS) of MgO NPs were added to four different bottles containing WAS to investigate the impact of MgO NPs on methane production during WAS anaerobic digestion. The effects of nZVI on methane production during WAS anaerobic digestion were also conducted in another four bottles using the same methods described above except that the MgO NPs were replaced by nZVI. A bottle of WAS anaerobic digestion without nanoparticles addition was also operated to serve as a control. It was found that the relative amounts, compared to the control system, of methane production in each WAS anaerobic digestion bottle adding 2, 50, 100, 200 mg/gTSS MgO NPs were 98, 62, 28, and 14 %, respectively. This suggests that higher MgO NPs resulted in lower methane production. The data of batch test for the effects of corresponding released Mg2+ indicated that 50 mg/gTSS MgO NPs or higher could inhibit methane production at least 25%. Moreover, the volatile fatty acid (VFA) concentration was 328, 384, 928, 3,684, and 7,848 mg/L for the control and four WAS anaerobic digestion bottles with 2, 50, 100, 200 mg/gTSS MgO NPs addition, respectively. Higher VFA concentration could reduce pH and subsequently decrease methanogen growth, resulting in lower methane production. The relative numbers of total gene copies of methanogens analyzed from samples taken from WAS anaerobic digestion bottles were approximately 99, 68, 38, and 24 % of control for the addition of 2, 50, 100, and 200 mg/gTSS, respectively. Obviously, the more MgO NPs appeared in sludge anaerobic digestion system, the less methanogens remained. In contrast, the relative amount of methane production found in another four WAS anaerobic digestion bottles adding 2, 50, 100, and 200 mg/gTSS nZVI were 102, 128, 112, and 104 % of the control, respectively. The measurement of methanogenic population indicated that the relative content of methanogen gene copies were 101, 132, 120, and 112 % of those found in control, respectively. Additionally, the cumulative VFA was 320, 234, 308, and 330 mg/L, respectively. This reveals that nZVI addition could assist to increase methanogenic population. Higher amount of methanogen accelerated VFA degradation for greater methane production, resulting in lower VFA accumulation in digesters. Moreover, the data for effects of corresponding released Fe2+ conducted by batch tests suggest that the addition of approximately 50 mg/gTSS nZVI increased methane production by 20%. In conclusion, the presence of MgO NPs appeared to diminish the methane production during WAS anaerobic digestion. Higher MgO NPs dosages resulted in more inhibition on methane production. In contrast, nZVI addition promoted the amount of methanogenic population which facilitated methane production.

Keywords: magnesium oxide nanoparticles, methane production, methanogenic population, nano zerovalent iron

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Authors: T. Topór, A. Derkowski, P. Ziemiański

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Formation of organic matter (OM)-hosted nanopores upon thermal maturation are one of the key factor controlling methane storage potential in unconventional shale-gas reservoirs. In this study, the subcritical CO₂ and N₂ gas adsorption measurements combined with scanning electron microscopy and supercritical methane adsorption have been used to characterize pore system and methane storage potential in black shales from the Baltic Basin (Poland). The samples were collected from a virtually equivalent Llandovery strata across the basin and represent a complete digenetic sequence, from thermally immature to overmature. The results demonstrate that the thermal maturation is a dominant mechanism controlling the formation of OM micro- and mesopores in the Baltic Basin shales. The formation of micro- and mesopores occurs in the oil window (vitrinite reflectance; leavedVR; ~0.5-0.9%) as a result of oil expulsion from kerogenleft OM highly porous. The generated hydrocarbons then turn into solid bitumen causing pore blocking and substantial decrease in micro- and mesopore volume in late-mature shales (VR ~0.9-1.2%). Both micro- and mesopores are regenerated in a middle of the catagenesis range (VR 1.4-1.9%) due to secondary cracking of OM and gas formation. The micropore volume in investigated shales is almost exclusively controlled by the OM content. The contribution of clay minerals to micropore volume is insignificant and masked by a strong contribution from OM. Methane adsorption capacity in the Baltic Basin shales is predominantly controlled by microporous OM with pores < 1.5 nm. The mesopore volume (2-50 nm) and mesopore surface area have no effect on methane sorption behavior. The adsorbed methane density equivalent, calculated as absolute methane adsorption divided by micropore volume, reviled a decrease of the methane loading potential in micropores with increasing maturity. The highest methane loading potential in micropores is observed for OM before metagenesis (VR < 2%), where the adsorbed methane density equivalent is greater than the density of liquid methane. This implies that, in addition to physical adsorption, absorption of methane in OM may occur before metagenesis. After OM content reduction using NaOCl solution methane adoption capacity substantially decreases, suggesting significantly greater adsorption potential for OM microstructure than for the clay minerals matrix.

Keywords: maturation, methane sorption, organic matter, porosity, shales

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Authors: Philip Vercoe, Ali Hardan

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Samples of 29 Australian wild natives and exotic plants were tested in vitro batch rumen culture system for their methanogenic characteristics and potential usage as feed or antimicrobial to enhance sustainable livestock ruminant production system. The plants were tested for their in vitro rumen fermentation end products properties which include: methane production, total gas pressure, concentrations of total volatile fatty acids, ammonia, and acetate to propionate ratio. All of the plants were produced less methane than the positive control (i.e., oaten chaff) in vitro. Nearly 50 % of plants inhibiting methane by over 50% in comparison to the control. Eremophila granitica had the strongest inhibitory effect about 92 % on methane production comparing with oaten chaff. The exotic weed Arctotheca calendula (Capeweed) had the highest concentration of volatile fatty acids production as well as the highest in total gas pressure among all plants and the control. Some of the acacia species have the lowest production of total gas pressure. The majority of the plants produced more ammonia than the oaten chaff control. The plant species that produced the most ammonia was Codonocarpus cotinifolius, producing over 3 times as much methane as oaten chaff control while the lowest was Eremophila galeata. There was strong positive correlation between methane production and total gas production as well as between total gas production and the concentration of VFA produced with R² = 0.74, R² = 0.84, respectively. While there was weak positive correlation between methane production and the acetate to propionate ratio as well as between the concentration of VFA produced and methane production with R² = 0.41, R² = 0.52, respectively.

Keywords: in vitro Rumen Fermentation, methane, wild Australian native plants, forages

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Authors: Yan Bachtiar Muslih, Hangga Wijaya, Trio Fani, Putri Agustin

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Demand of Energy in Indonesia always increases 5-6% a year, but production of conventional energy always decreases 3-5% a year, it means that conventional energy in 20-40 years ahead will not able to complete all energy demand in Indonesia, one of the solve way is using unconventional energy that is gas hydrate, gas hydrate is gas that form by biogenic process, gas hydrate stable in condition with extremely depth and low temperature, gas hydrate can form in two condition that is in pole condition and in deep-sea condition, wherein this research will focus in gas hydrate that association with methane form methane hydrate in deep-sea condition and usually form in depth between 150-2000 m, this research will focus in process of methane hydrate formation that is biogenic process and the important role of deep-sea sediment so can produce accumulation of methane hydrate, methane hydrate usually will be accumulated in find sediment in deep-sea environment with condition high-pressure and low-temperature this condition too usually make methane hydrate change into white nodule, methodology of this research is geology field work and laboratory analysis, from geology field work will get sample data consist of 10-15 samples from Kerek Formation outcrops as random for imagine the condition of deep-sea environment that influence the methane hydrate formation and also from geology field work will get data of measuring stratigraphy in outcrops Kerek Formation too from this data will help to imagine the process in deep-sea sediment like energy flow, supply sediment, and etc, and laboratory analysis is activity to analyze all data that get from geology field work, the result of this research can used to exploration activity of methane hydrate in another prospect deep-sea environment in Indonesia.

Keywords: methane hydrate, deep-sea sediment, kerek formation, sub-basin of kendeng, central java, Indonesia

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Authors: Kumaresh Selvakumar, Man Young Kim

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The presence of a catalyst inside an engine enables complete combustion at lower temperatures which promote desired chemical reactions. The objective of this work is to design and simulate a catalytic combustor by using CHEMKIN with detailed gas and surface chemistries. The simplified approach with single catalyst channel using plug flow reactor (PFR) can be used to predict reasonably well with the effect of various operating parameters such as the inlet temperature, velocity and fuel/air ratios. The numerical results are validated by comparing the surface chemistries in single channel catalytic combustor. The catalytic combustor operates at much lower temperature than the conventional combustor since lean-fuel mixture is used where the complete methane conversion is achieved. The coupling between gas and surface reactions in the catalyst bed is studied by investigating the commencement of flame ignition with respect to the surface site species.

Keywords: catalytic combustion, honeycomb monolith, plug flow reactor, surface reactions

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Authors: Evar C. Umeozor, Experience I. Nduagu, Ian D. Gates

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The energy requirements of carbon dioxide utilization (CDU) technologies/processes are diverse, so also are their environmental footprints. This paper explores the energy and environmental impacts of systems for CO₂ conversion to fuels, chemicals, and materials. Energy needs of the technologies and processes deployable in CO₂ conversion systems are met by one or combinations of hydrogen (chemical), electricity, heat, and light. Likewise, the environmental footprint of any CO₂ utilization pathway depends on the systems involved. So far, evaluation of CDU systems has been constrained to particular energy source/type or a subset of the overall system needed to make CDU possible. This introduces limitations to the general understanding of the energy and environmental implications of CDU, which has led to various pitfalls in past studies. A CDU system has an energy source, CO₂ supply, and conversion units. We apply a holistic approach to consider the impacts of all components in the process, including various sources of energy, CO₂ feedstock, and conversion technologies. The electricity sources include nuclear power, renewables (wind and solar PV), gas turbine, and coal. Heat is supplied from either electricity or natural gas, and hydrogen is produced from either steam methane reforming or electrolysis. The CO₂ capture unit uses either direct air capture or post-combustion capture via amine scrubbing, where applicable, integrated configurations of the CDU system are explored. We demonstrate how the overall energy and environmental impacts of each utilization pathway are obtained by aggregating the values for all components involved. Proper accounting of the energy and emission intensities of CDU must incorporate total balances for the utilization process and differences in timescales between alternative conversion pathways. Our results highlight opportunities for the use of clean energy sources, direct air capture, and a number of promising CO₂ conversion pathways for producing methanol, ethanol, synfuel, urea, and polymer materials.

Keywords: carbon dioxide utilization, processes, energy options, environmental impacts

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Authors: Chetna Mohabeer, Luis Reyes, Lokmane Abdelouahed, Bechara Taouk

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In the transition to sustainability and the increasing use of renewable energy, hydrogen will play a key role as an energy carrier. Biomass has the potential to accelerate the realization of hydrogen as a major fuel of the future. Pyro-gasification allows the conversion of organic matter mainly into synthesis gas, or “syngas”, majorly constituted by CO, H2, CH4, and CO2. A second, condensable fraction of biomass pyro-gasification products are “tars”. Under certain conditions, tars may decompose into hydrogen and other light hydrocarbons. These conditions include two types of cracking: homogeneous cracking, where tars decompose under the effect of temperature ( > 1000 °C), and heterogeneous cracking, where catalysts such as olivine, dolomite or biochar are used. The latter process favors cracking of tars at temperatures close to pyro-gasification temperatures (~ 850 °C). Pyro-gasification of biomass coupled with water-gas shift is the most widely practiced process route for biomass to hydrogen today. In this work, an innovating solution will be proposed for this conversion route, in that all the pyro-gasification products, not only methane, will undergo processes that aim to optimize hydrogen production. First, a heterogeneous cracking step was included in the reaction scheme, using biochar (remaining solid from the pyro-gasification reaction) as catalyst and CO2 and H2O as gasifying agents. This process was followed by a catalytic steam methane reforming (SMR) step. For this, a Ni-based catalyst was tested under different reaction conditions to optimize H2 yield. Finally, a water-gas shift (WGS) reaction step with a Fe-based catalyst was added to optimize the H2 yield from CO. The reactor used for cracking was a fluidized bed reactor, and the one used for SMR and WGS was a fixed bed reactor. The gaseous products were analyzed continuously using a µ-GC (Fusion PN 074-594-P1F). With biochar as bed material, it was seen that more H2 was obtained with steam as a gasifying agent (32 mol. % vs. 15 mol. % with CO2 at 900 °C). CO and CH4 productions were also higher with steam than with CO2. Steam as gasifying agent and biochar as bed material were hence deemed efficient parameters for the first step. Among all parameters tested, CH4 conversions approaching 100 % were obtained from SMR reactions using Ni/γ-Al2O3 as a catalyst, 800 °C, and a steam/methane ratio of 5. This gave rise to about 45 mol % H2. Experiments about WGS reaction are currently being conducted. At the end of this phase, the four reactions are performed consecutively, and the results analyzed. The final aim is the development of a global kinetic model of the whole system in a multi-stage fluidized bed reactor that can be transferred on ASPEN PlusTM.

Keywords: multi-staged fluidized bed reactor, pyro-gasification, steam methane reforming, water-gas shift

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Authors: Wajeeha A. Qazi, Mohammed-Hasham Azam, Umais A. Mehmood, Ghithaa A. Al-Mufragi, Noor-Alhuda Alrawahi, Mohammed F. M. Abushammala

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Municipal Solid Waste (MSW) disposed in landfill sites decompose under anaerobic conditions and produce gases which mainly contain carbon dioxide (CO₂) and methane (CH₄). Methane has the potential of causing global warming 25 times more than CO₂, and can potentially affect human life and environment. Thus, this research aims to determine MSW generation and the annual CH₄ emissions from the generated waste in Oman over the years 1971-2030. The estimation of total waste generation was performed using existing models, while the CH₄ emissions estimation was performed using the intergovernmental panel on climate change (IPCC) default method. It is found that total MSW generation in Oman might be reached 3,089 Gg in the year 2030, which approximately produced 85 Gg of CH₄ emissions in the year 2030.

Keywords: methane, emissions, landfills, solid waste

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Authors: Li Chin Law, Epaminondas Mastorakos, Mohd Roslee Othman, Antonis Trakakis

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The paper introduces an alternative concept of carbon capture for shipping by using pre-combustion carbon capture technology (Pre-CCS), which was proven to be less energy intensive than post-combustion carbon capture from the engine exhaust. Energy assessment on amine-based post-combustion CCS on LNG-fuelled ships showed that the energy efficiency of CCS ships reduced from 48% to 36.6%. Then, an energy assessment was carried out to compare the power and heat requirements of the most used hydrogen production methods and carbon capture technologies. Steam methane reformer (SMR) was found to be 20% more energy efficient and achieved a higher methane conversion than auto thermal reaction and methane decomposition. Next, pressure swing adsorber (PSA) has shown a lower energy requirement than membrane separation, cryogenic separation, and amine absorption in pre-combustion carbon capture. Hence, an integrated system combining SMR and PSA (SMR-PSA) with waste heat integration (WHR) was proposed. This optimized SMR-based integrated system has achieved 65% of CO₂ reduction with less than 7-percentage point of energy penalty (41.7% of energy efficiency). Further integration of post-combustion CCS with the SMR-PSA integrated system improved carbon capture rate to 86.3% with 9-percentage points of energy penalty (39% energy efficiency). The proposed system was shown to be able to meet the carbon reduction targets set by International Maritime Organization (IMO) with certain energy penalties.

Keywords: shipping, decarbonisation, alternative fuels, low carbon, hydrogen, carbon capture

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Authors: Marcin Zieliński, Marcin Dębowski, Mirosław Krzemieniewski

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This publication presents a device designed for mechanical fragmentation of plant substrate before methane fermentation. The device is equipped with a perforated rotary cylindrical drum coated with a thermal layer, connected to a substrate feeder and driven by a motoreducer. The drum contains ball- or cylinder-shaped weights of different diameters, while its interior is mounted with lateral permanent magnets with an attractive force ranging from 100 kg to 2 tonnes per m2 of the surface. Over the perforated rotary drum, an infrared radiation generator is mounted, producing 0.2 kW to 1 kW of infrared radiation per 1 m2 of the perforated drum surface. This design reduces the energy consumption required for the biomass destruction process by 10-30% in comparison to the conventional ball mill. The magnetic field generated by the permanent magnets situated within the perforated rotary drum promotes this process through generation of free radicals that act as powerful oxidants, accelerating the decomposition rate. Plant substrate shows increased susceptibility to biodegradation when subjected to magnetic conditioning, reducing the time required for biomethanation by 25%. Additionally, the electromagnetic radiation generated by the radiator improves substrate destruction by 10% and the efficiency of the process. The magnetic field and the infrared radiation contribute synergically to the increased efficiency of destruction and conversion of the substrate.

Keywords: biomass pretreatment, mechanical fragmentation, biomass, methane fermentation

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Authors: Daniel Fozer

Abstract:

Limiting global warming to 1.5°C to the pre-industrial levels urges the application of efficient and sustainable carbon dioxide removal (CDR) technologies. Microalgae based biorefineries offer scalable solutions for the biofixation of CO2, where the produced biomass can be transformed into value added products by applying thermochemical processes. In this paper we report on the utilization of hydrochar as a blending component in hydrothermal gasification (HTG) process. The effects of blending ratio and hydrochar quality were investigated on the biogas yield and and composition. It is found that co-gasifying the hydrochar and the algae biomass can increase significantly the total gas yield and influence the biogas (H2, CH4, CO2, CO, C2H4, C2H6) composition. It is determined that the carbon conversion ratio, hydrogen and methane selectivity can be increased by influencing the fuel ratio of hydrochar via hydrothermal carbonization. In conclusion, it is found that increasing the synergy between hydrothermal technologies result in elevated conversion efficiency.

Keywords: biogas, CDR, Co-HTG, hydrochar, microalgae

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Authors: Pauline Bredy, Yves Schuurman, David Farrusseng

Abstract:

To fulfill climate objectives, the production of synthetic e-fuels using CO₂ as a raw material appears as part of the solution. In particular, Power-to-Liquid (PtL) concept combines CO₂ with hydrogen supplied from water electrolysis, powered by renewable sources, which is currently gaining interest as it allows the production of sustainable fossil-free liquid fuels. The proposed process discussed here is an upgrading of the well-known Fischer-Tropsch synthesis. The concept deals with two cascade reactions in one pot, with first the conversion of CO₂ into CO via the reverse water gas shift (RWGS) reaction, which is then followed by the Fischer-Tropsch Synthesis (FTS). Instead of using a Fe-based catalyst, which can carry out both reactions, we have chosen the strategy to decouple the two functions (RWGS and FT) on two different catalysts within the same reactor. The FTS shall shift the equilibrium of the RWGS reaction (which alone would be limited to 15-20% of conversion at 250°C) by converting the CO into hydrocarbons. This strategy shall enable optimization of the catalyst pair and thus lower the temperature of the reaction thanks to the equilibrium shift to gain selectivity in the liquid fraction. The challenge lies in maximizing the activity of the RWGS catalyst but also in the ability of the FT catalyst to be highly selective. Methane production is the main concern as the energetic barrier of CH₄ formation is generally lower than that of the RWGS reaction, so the goal will be to minimize methane selectivity. Here we report the study of different combinations of copper-based RWGS catalysts with different cobalt-based FTS catalysts. We investigated their behaviors under mild process conditions by the use of high-throughput experimentation. Our results show that at 250°C and 20 bars, Cobalt catalysts mainly act as methanation catalysts. Indeed, CH₄ selectivity never drops under 80% despite the addition of various protomers (Nb, K, Pt, Cu) on the catalyst and its coupling with active RWGS catalysts. However, we show that the activity of the RWGS catalyst has an impact and can lead to longer hydrocarbons chains selectivities (C₂⁺) of about 10%. We studied the influence of the reduction temperature on the activity and selectivity of the tandem catalyst system. Similar selectivity and conversion were obtained at reduction temperatures between 250-400°C. This leads to the question of the active phase of the cobalt catalysts, which is currently investigated by magnetic measurements and DRIFTS. Thus, in coupling it with a more selective FT catalyst, better results are expected. This was achieved using a cobalt/iron FTS catalyst. The CH₄ selectivity dropped to 62% at 265°C, 20 bars, and a GHSV of 2500ml/h/gcat. We propose that the conditions used for the cobalt catalysts could have generated this methanation because these catalysts are known to have their best performance around 210°C in classical FTS, whereas the iron catalysts are more flexible but are also known to have an RWGS activity.

Keywords: cobalt-copper catalytic systems, CO₂-hydrogenation, Fischer-Tropsch synthesis, hydrocarbons, low-temperature process

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Authors: Ts. Lazarova, V. Tumbalev, S. Atanacova-Vladimirova, G. Ivanov, A. Naydenov, D. Kovacheva

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Methane is a major Greenhouse Gas (GHG) that accounts for 14% of the world’s total amount of GHG emissions, originating mainly from agriculture, Coal mines, land fields, wastewater and oil and gas facilities. Nowadays the problem caused by the methane emissions has been a subject of an increased concern. One of the methods for neutralization of the methane emissions is it's complete catalytic oxidation. The efforts of the researchers are focused on the development of new types of catalysts and optimizing the existing catalytic systems in order to prevent the sintering of the palladium, providing at the same time a sufficient activity at temperatures below 500oC. The aim of the present work is to prepare mixed Cu-Ag-Pd oxide catalysts supported on alumina and to test them for methane complete catalytic oxidation. Cu-Ag-Pd/Al2O3 were prepared on a γ-Al2O3 (BET surface area = 220 m2/g) by the incipient wetness method using the corresponding metal nitrates (Cu:Ag = 90:10, Cu:Pd =97:3, Cu:Ag:Pd= 87:10:3) as precursors. A second set of samples were prepared with addition of urea to the metal nitrate solutions with the above mentioned ratios assuming increased dispersivity of the catalysts. The catalyst samples were dried at 100°C for 3 hours and calcined at 550°C for 30 minutes. Catalysts samples were characterized using X-ray diffraction (XRD), low temperature adsorption of nitrogen (BET) and scanning electron microscopy (SEM). The catalytic activity tests were carried out in a continuous flow type of reactor at atmospheric pressure. The effect of catalyst aging at 500 oC for 120 h on the methane combustion activity was also investigated. The results clearly indicate the synergetic effect of Ag and Pd on the catalytic activity.

Keywords: catalysts, XRD, BET, SEM, catalytic oxidation

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Authors: Kefale W. Yizengaw, Delele Worku Ayele, Jyh-Chiang Jiang

Abstract:

The catalytic co-conversion of CO₂ and CH₄ to value-added compounds has become one of the promising approaches to addressing global climate change by having valuable fossil fuels. Thedirect co-conversion of CO₂ and CH₄ to value-added compounds is attractive but tremendously challenging because of both molecules' thermodynamic stability and kinetic inertness. In the present study, a single iridium atom doped and a single oxygen atom defect hematite (110)surface model catalyst, which can comprehend direct C–O coupling based on simultaneous activation of CO2 and CH4 was studied using density functional theory plus U (DFT + U)calculations. The presence of dual active sites on the Ir/Fe₂O₃(110)-OV surface catalyst enablesCO₂ activation on the Ir site and CH₄ activation at the defect site. The electron analysis for the theco-adsorption of CO₂ and CH₄ deals with the electron redistribution on the surface and clearly shows the synergistic effect for simultaneous CO₂ and CH₄ activation on Ir/α- Fe₂O₃(110)-OVsurface. The microkinetic analysis shows that the dissociation of CH4 to CH3 * and H* plays an excellent role in the C–O coupling. The coverage analysis for the intermediate products of the microkinetic simulation results indicates that C–O coupling is the reaction limiting step. Finally, after the CH₃O* intermediate product species is produced, the radical hydrogen species spontaneously diffuse to the CH3O* intermediate product to form methanol at around 490 [K]. The present work provides mechanistic and kinetic insights into the direct C–O coupling of CO₂and CH₄, which could help design more-efficient catalysts.

Keywords: co-conversion, C–O coupling, doping, oxygen vacancy, microkinetic

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