Global estimates of potential mitigation of greenhouse gas emissions by agriculture

Technologies to reduce net emissions of carbon dioxide, methane and nitrous oxide within the agriculture sector were reviewed to estimate the global potential for mitigation of these radiatively active greenhouse gases. Our estimates of the potential reduction of radiative forcing by the agricultural sector range from 1.15-3.3 Gt C equivalents per year. Of the total potential reduction, approximately 32% could result from reduction in CO₂ emissions, 42% of carbon offsets by biofuel production on 15% of existing croplands, 16% from reduced CH₄ emissions and 10% from reduced emissions of N₂O. Agriculture encompasses large regional differences in management practices and rates of potential adoption of mitigation practices. Acceptability of mitigation options will depend on the extent to which sustainable production will be achieved or maintained and benefits will accrue to farmers. Technologies such as no-till farming and strategic fertilizer placement and timing are now being adopted for reasons other than concern for climate change issues. This revised version was published online in August 2006 with corrections to the Cover Date.     

Technical and policy aspects of strategies to decrease greenhouse gas emissions from agriculture

Agricultural activities greatly contribute to the global net flux of CH₄, N₂O and CO₂ from the terrestrial biosphere into the atmosphere. For CH₄ and N₂O, the net contribution is in the order of 40%. Because of this relatively large contribution, there is an urgent need for the implementation of effective strategies to decrease the net flux of CH₄, N₂O and CO₂ from agriculture. The objectives of this paper are to review the various measures that have been proposed so far and to discuss the constraints and challenges. A large number of suggestions for decreasing emissions of CH₄, N₂O and CO₂ from agriculture can be found in literature. Common to most of these abatement measures is that the suggested potentials to decrease the emissions of CO₂, CH₄ and N₂O from agriculture are large. Common to most of the measures is also the `single gas' and `source-oriented' approach. In most papers it has been implicitly assumed that farmers are able and willing to implement the proposed measures. So far, none of the measures has been consciously implemented and tested at farm scale. The major challenge of policy makers is to formulate effective and efficient policies and measures, using the potentials of the abatement measures proposed so far, and in an international setting with still highly uncertain cause–effect relationships. Major constraints for policy makers follow from the complexities and possible feed back and side effects of abatement measures, from the many stakeholders involved, often with contrasting views, and from the unfamiliarity of farmers with the problem of climate change. Because of the many complexities and interactions involved, policy makers should follow two tracks. Priority should be given to chain-oriented measures, i.e. measures that aim at an increased carbon, nitrogen and water use efficiencies in the whole food chain, above source-oriented measures, i.e. measures that aim at decreased emission from specific sources. Chain-oriented measures should fit in with other environmental policies that aim at increasing resource use efficiency, to be effective and efficient. This revised version was published online in August 2006 with corrections to the Cover Date.     

Greenhouse gas emissions from simulated beef and dairy livestock systems in the United States

Computer spreadsheets were developed to evaluate greenhouse gas (GHG) emissions from U.S. beef and dairy livestock systems from nine locations. Of the beef systems the cow-calf herd emitted the most and feedlot cattle the least methane (CH₄) and nitrous oxide (N₂O) per unit product. Carbon dioxide (CO₂) emissions per unit product were the least for the cow-calf and greatest for the feedlot scenarios. In the dairy systems approximately one-half of the total GHG CO₂ equivalents were from CH₄ and one-third from N₂O. Mitigation strategies, such as intensive grazing, reduced GHG emissions by approximately 10%. This revised version was published online in August 2006 with corrections to the Cover Date.     

The significance of agricultural sources of greenhouse gases

The impact of development of land for agriculture and agricultural production practices on emissions of greenhouse gases is reviewed and evaluated within the context of anthropogenic radiative forcing of climate. Combined, these activities are estimated to contribute about 25%, 65%, and 90% of total anthropogenic emissions of CO₂, CH₄, and N₂O, respectively. Agriculture is also a significant contributor to global emissions of NH₃, CO, and NO. Over the last 150 y, cumulative emissions of CO₂ associated with land clearing for agriculture are comparable to those from combustion of fossil fuel, but the latter is the major source of CO₂ at present and is projected to become more dominant in the future. Ruminant animals, rice paddies, and biomass burning are principal agricultural sources of CH₄, and oxidation of CH₄ by aerobic soils has been reduced by perturbations to natural N cycles. Agricultural sources of N₂O have probably been substantially underestimated due to incomplete analysis of increased N flows in the environment, especially via NH₃ volatilization from animal manures, leaching of NO ₃ ^- , and increased use of biological N fixation.The contribution of agriculture to radiative forcing of climate is analyzed using data from the Intergovernmental Panel on Climate Change (IPCC)(base case) and cases where the global warming potential of CH₄, and agricultural emissions of N₂O are doubled. With these scenarios, agriculture, including land clearing, is estimated to contribute between 28–33% of the radiative forcing created over the next 100yr by 1990 anthropogenic emissions of CO₂, CH₄, and N₂O. Analyses of the sources of agriculturally generated radiative climate forcing show that 80% is associated with tropical agriculture and that two-thirds comes from non-soil sources of greenhouse gases. The importance of agriculture to radiative forcing created by different countries varies widely and is illustrated by comparisons between the USA, India, and Brazil. Some caveats to these analyses include inadequate evaluations of the net greenhouse effects of agroecosystems, uncertainties in global fluxes of greenhouse gases, and incomplete understanding of tropospheric chemical processes.Extension of the analytical approach to projected future emissions of greenhouse gases (IPCC moderate growth scenario) indicates that agriculture will become a less important source of radiative forcing in the future. Technological approaches to mitigation of agricultural sources of greenhouse gases will probably focus on CH₄ and N₂O because emissions of CO₂ are essentially associated with the socio-political issue of tropical deforestation. Available technologies include dietary supplements to reduce CH₄ production by ruminant animals and various means of improving fertilizer N management to reduce N₂O emissions. Increased storage of C in soil organic matter is not considered to be viable because of slow accretion rates and misconceptions about losses of soil organic matter from agricultural soils.     

Effect of climate change on greenhouse gas emissions from arable crop rotations

The DAISY soil–plant–atmosphere model was used to simulate crop production and soil carbon (C) and nitrogen (N) turnover for three arable crop rotations on a loamy sand in Denmark under varying temperature, rainfall, atmospheric CO₂ concentration and N fertilization. The crop rotations varied in proportion of spring sown crops and use of N catch crops (ryegrass). The effects on CO₂ emissions were estimated from simulated changes in soil C. The effects on N₂O emissions were estimated using the IPCC methodology from simulated amounts of N in crop residues and N leaching. Simulations were carried out using the original and a revised parameterization of the soil C turnover. The use of the revised model parameterization increased the soil C and N turnover in the topsoil under baseline conditions, resulting in an increase in crop N uptake of 11 kg N ha^–1 y^–1 in a crop rotation with winter cereals and a reduction of 16 kg N ha^–1 y^–1 in a crop rotation with spring cereals and catch crops. The effect of increased temperature, rainfall and CO₂ concentration on N flows was of the same magnitude for both model parameterizations. Higher temperature and rainfall increased N leaching in all crop rotations, whereas effects on N in crop residues depended on use of catch crops. The total greenhouse gas (GHG) emission increased with increasing temperature. The increase in total GHG emission was 66–234 kg CO₂-eq ha^–1 y^–1 for a temperature increase of 4°C. Higher rainfall increased total GHG emissions most in the winter cereal dominated rotation. An increase in rainfall of 20% increased total GHG emissions by 11–53 kg CO₂-eq ha^–1 y^–1, and a 50% increase in atmospheric CO₂ concentration decreased emissions by 180–269 kg CO₂-eq ha^–1 y^–1. The total GHG emissions increased considerably with increasing N fertilizer rate for a crop rotation with winter cereals, but remained unchanged for a crop rotation with spring cereals and catch crops. The simulated increase in GHG emissions with global warming can be effectively mitigated by including more spring cereals and catch crops in the rotation.     

Possible CO2 mitigation via addition of charcoal to coking coal blends

Processes involving biomass oxidation are considered to be CO₂ neutral since the replenishing of the biomass by normal growth will remove CO₂ from the atmosphere. Thus the use of charcoal in the production of metallurgical coke, to be used as a reducing agent in the formation of iron, would be a strategy for the reduction of CO₂ in the overall ironmaking process. This paper describes experimental attempts to produce industrial grade coke from coking coal blends to which are added amounts of charcoal up to 10%. Coking experiments were carried out partly in a 30 lb coke oven and partly in a sole heated oven. The influence of blend composition, heating rates and charcoal particle size was investigated. Cokes made using fine charcoal addition (− 60 mesh) were considerably weaker than cokes made from the base blend. This is interpreted to be the effect of the ash constituents in the charcoal which, among other things, contains much higher calcium than the coals used. However, carefully sized fractions of coarse charcoal (− 3/8 + 1/4 in) produced much higher quality coke, possibly the result of a different dispersion of the charcoal mineral components.     

Enhancing the carbon sink in European agricultural soils: including trace gas fluxes in estimates of carbon mitigation potential

The possibility that the carbon sink in agricultural soils can be enhanced has taken on great political significance since the Kyoto Protocol was finalised in December 1997. The Kyoto Protocol allows carbon emissions to be offset by demonstrable removal of carbon from the atmosphere. Thus, forestry activities (Article 3.3) and changes in the use of agricultural soils (Article 3.4) that are shown to reduce atmospheric CO₂levels may be included in the Kyoto emission reduction targets. The European Union is committed to a reduction in CO₂ emissions to 92% of baseline (1990) levels during the first commitment period (2008–2012). We have shown recently that there are a number of agricultural land-management changes that show some potential to increase the carbon sink in agricultural soils and others that allow alternative forms of carbon mitigation (i.e. through fossil fuel substitution), but the options differ greatly in their potential for carbon mitigation. The changes examined were, (a) switching all animal manure use to arable land, (b) applying all sewage sludge to arable land, (c) incorporating all surplus cereal straw, (d) conversion to no-till agriculture, (e) use of surplus arable land to de-intensify 1/3 of current intensive crop production (through use of 1/3 grass/arable rotations), (f) use of surplus arable land to allow natural woodland regeneration, and (g) use of surplus arable land for bioenergy crop production. In this paper, we attempt for the first time to assess other (non-CO₂) effects of these land-management changes on (a) the emission of the other important agricultural greenhouse gases, methane and nitrous oxide, and (b) other aspects of the ecology of the agroecosystems. We find that the relative importance of trace gas fluxes varies enormously among the scenarios. In some such as the sewage sludge, woodland regeneration and bioenergy production scenarios, the inclusion of trace gases makes only a small (<10%) difference to the CO₂-C mitigation potential. In other cases, for example the no-till, animal manure and agricultural de-intensification scenarios, trace gases have a large impact, sometimes halving or more than doubling the CO₂-C mitigation potential. The scenarios showing the greatest increase when including trace gases are those in which manure management changes significantly. In the one scenario (no-till) where the carbon mitigation potential was reduced greatly, a small increase in methane oxidation was outweighed by a sharp increase in N₂O emissions. When these land-management options are combined to examine the whole agricultural land area of Europe, most of the changes in mitigation potential are small, but depending upon assumptions for the animal manure scenario, the total mitigation potential either increases by about 20% or decreases by about 10%, shifting the mitigation potential of the scenario from just above the EU's 8% Kyoto emission reduction target (98.9 Tg C y⁻¹) to just below it. Our results suggest that (a) trace gas fluxes may change the mitigation potential of a land management option significantly and should always be considered alongside CO₂-C mitigation potentials and (b) agricultural management options show considerable potential for carbon mitigation even after accounting for trace gas fluxes. This revised version was published online in August 2006 with corrections to the Cover Date.     

Nitrate accumulation and greenhouse gas emissions during compost storage

Greenhouse gases (CO₂, CH₄ and N₂O) are emitted during livestock manure handling, including composting, storage and land application. However, published data on emission rates of these gases during storage are sparse. In this study, the levels of GHG emissions and N levels during compost storage were investigated. The compost materials were produced by composting livestock manure for 133 d with 0, 10, 20 and 30% phosphogypsum (PG) or 10, 20 and 30% sand amendment. These compost materials were then stored on a clay pad for 233 d. Results from this study indicated that TN content did not change but mineral N content increased significantly during the 233 d storage for all treatments. The higher mineral N content in compost increases its agronomic value. There were only trace amounts of CH₄ and N₂O emissions. The C loss during storage was mainly as CO₂ and accounted for about 2.9 to 10% of total C initially in the compost. This information is vital to livestock manure life cycle analysis, and can be used to develop best manure management strategies that reduce GHG emissions from livestock production. The LRC Contribution No. 387-06006.     

Modified CaO-based sorbent looping cycle for CO2 mitigation

CaO-based sorbent looping cycle, i.e. cyclic calcination/carbonation, is one of the most interesting technologies for CO₂ capture during coal combustion and gasification processes. In order to improve the durability of limestone during the multiple calcination/carbonation cycles, modified limestone with acetic acid solution was proposed as an CO₂ sorbent. The cyclic carbonation conversions of modified limestone and original one were investigated in a twin fixed bed reactor system. The modified limestone shows the optimum carbonation conversion at the carbonation temperature of 650 °C and achieves a conversion of 0.5 after 20 cycles. The original limestone exhibits the maximum carbonation conversion of 0.15 after 20 cycles. Conversion of the modified limestone decreases slightly as the calcination temperature increases from 920 °C to 1100 °C with the number of cycles, while conversion of the original one displays a sharp decay at the same reaction conditions. The durability of the modified limestone is significantly better than the original one during the multiple cycles because mean grain size of CaO derived from the modified limestone is lower than that from the original one at the same reaction conditions. The calcined modified limestone shows higher surface area and pore volume than the calcined original one with the number of cycles, and pore size distribution of the modified limestone is superior to the original one after the same number of calcinations.     

Toward Improved Coefficients for Predicting Direct N<Subscript>2</Subscript>O Emissions from Soil in Canadian Agroecosystems

Agricultural soils emit nitrous oxide (N₂O), a potent greenhouse gas. Predicting and mitigating N₂O emissions is not easy. To derive national coefficients for N₂O emissions from soil, we collated over 400 treatment evaluations (measurements) of N₂O fluxes from farming systems in various ecoregions across Canada. A simple linear coefficient for fertilizer-induced emission of N₂O in non-manured soils (1.18% of N applied) was comparable to that used by the Intergovernmental Panel on Climate Change (IPCC) (1.25% of N applied). Emissions were correlated to soil and crop management practices (manure addition, N fertilizer addition and inclusion of legumes in the rotation) as well as to annual precipitation. The effect of tillage on emissions was inconsistent, varying among experiments and even within experiments from year to year. In humid regions (e.g., Eastern Canada) no-tillage tended to enhance N₂O emissions; in arid regions (e.g., Western Prairies) no-tillage sometimes reduced emissions. The variability of N₂O fluxes shows that we cannot yet always distinguish between potential mitigation practices with small (e.g., <10%) differences in emission. Our analysis also emphasizes the need for developing consistent experimental approaches (e.g., ‘control’ treatments) and methodologies (i.e. measurement period lengths) for estimating N₂O emissions.     

Effects of matrix moisture on gas diffusion and flow in coal

Gas production from coal is a complex process whereby gas, initially adsorbed in the coal matrix, desorbs and diffuses through the matrix into the cleat and eventually flows through the cleat system into a production well or a drainage borehole. Hence, the gas production rate is mainly controlled by the gas diffusivity in the matrix and gas permeability in the cleat system. Moisture in the coal matrix has significant impact on gas adsorption capacity and would also play a key role in desorption and migration of gas. However, how moisture affects gas desorption and diffusion in the coal matrix is still poorly understood. In this work, experimental study is performed to investigate effects of moisture on gas sorption rate for an Australian coal. Coal seam gases, CH₄ and CO₂, are used in the study. The experimental results show that moisture content in the matrix has significant impact on the gas sorption rate and the impact of moisture content on the diffusion rate is stronger for CH₄ than CO₂. Moreover, the impact of moisture on gas diffusivity in pores with different size is different, suggested from the modelling results using the bidisperse approach. Furthermore, moisture in coal matrix would cause coal swelling/shrinkage and mechanical properties change that could impact on coal permeability under reservoir conditions. Experimental measurements of coal matrix swelling and Young’s modulus on the same coal sample show that matrix moisture content has significant impact on those properties and may have significant implications on coalbed methane recovery and CO₂ storage in coal.     

Life cycle emissions of greenhouse gas for ammonia scrubbing technology

It is thought that the CO₂ emissions from coal-fired power plants contribute greatly to the total anthropogenic CO₂ emissions. Ammonia solvent can be used to absorb the CO₂, called ammonia scrubbing. However, as has been pointed out, the production of ammonia would emit CO₂; therefore, the effectiveness of ammonia scrubbing is doubted. The paper focuses on the problem. Two systems are defined in the paper. System I is CO₂ absorption by ammonia scrubbing, and system II is industrial production of ammonium bicarbonate. The total CO₂ emissions of the two systems are calculated by means of life cycle assessment. The paper shows that the total CO₂ emissions of ammonia scrubbing are less than that of the industrial production of fertilizer ammonium bicarbonate. It can be concluded that ammonia scrubbing is an effective way to reduce the anthropogenic CO₂ emissions. This work was presented at the 6 ^th Korea-China Workshop on Clean Energy Technology held at Busan, Korea, July 4–7, 2006.     

CO2 capture using oxygen enhanced combustion strategies for natural gas power plants

This paper describes a series of experiments conducted with natural gas in air and in mixtures of oxygen and recycled flue gas, termed O₂/CO₂ recycle combustion. The objective is to enrich the flue gas with CO₂ to facilitate its capture and sequestration. Detailed measurements of gas composition, flame temperature and heat flux profiles were taken inside CANMET's 0.3 MWth down-fired vertical combustor fitted with a proprietary pilot scale burner. Flue gas composition was continuously monitored. The effects of burner operation, including swirling of secondary stream and air staging, on flame characteristics and NO_x emissions were also studied. The results of this work indicate that oxy-gas combustion techniques based on O₂/CO₂ combustion with flue gas recycle offer excellent potential for retrofit to conventional boilers for CO₂ emission abatement. Other benefits of the technology include considerable reduction and even elimination of NO_x emissions, improved plant efficiency due to lower gas volume and better operational flexibility.     

A multi-scale model for CO2 sequestration enhanced coalbed methane recovery

This paper presents a multi-scale model to simulate the multicomponent gas diffusion and flow in bulk coals for CO₂ sequestration enhanced coalbed methane recovery. The model is developed based on a bi-dispersed structure model by assuming that coal consists of microporous micro-particles, meso/macro-pores and open microfractures. The bi-disperse diffusion theory and the Maxwell-Stefan approach were incorporated in the model, providing an improved simulation of the CH₄-CO₂/CH₄-N₂ counter diffusion dynamics. In the model, the counter diffusion process is numerically coupled with the flow of the mixture gases occurring within macro-pores or fractures in coal so as to account for the interaction between diffusion and flow in gas transport through coals. The model was validated by both experimental data from literature and our CO₂ flush tests, and shows an excellent agreement with the experiments. The results reveal that the gas diffusivities, in particular the micro-pore diffusivities are strongly concentration-dependent.     

Overwinter greenhouse gas fluxes in two contrasting agricultural habitats

Mid-day field fluxes of nitrous oxide (N₂O), carbon dioxide (CO₂) and methane (CH₄) were measured during late winter/early spring in an arable field and an adjacent fallow in southern Germany. On the arable field, 2 dm high ridges, drawn as seed-beds for potato, were exposed to mild, partly diurnal freezing–thawing. Substantially elevated N₂O emission rates (6–750 µg N₂O-N m^–2 h^–1) were observed throughout the investigation period which coincided with freezing–thawing events in the surface soil (0–5 cm). Soil temperatures in the densely vegetated fallow were more isothermal due to an insulating snow/ice cover, resulting in much lower N₂O emission rates (0–57 µg N₂O-N m^–2 h^–1). CH₄ uptake rates were low in both habitats during soil frost (+2 to –7.5 µg CH₄-C m^–2 h^–1) but increased markedly in the fallow after spring thaw. Our data suggest that N₂O emission peaks may occur recurrently throughout the winter when soils are subjected to diurnal surface thawing. We concluded that microclimatic conditions strongly control N₂O winter loss, thus overriding ecosystem-level differences in off-season nutrient cycling. To further characterize winter-time nutrient cycling and habitat functioning in our sites, we determined NO₃ ^– and NH₄ ⁺ contents, fumigation-extractable carbon (C_mic) and nitrogen (N_mic) and enumerated protozoa and nematoda throughout the investigation period. C_mic and microbial C:N ratios in the fallow were higher in winter than during the rest of the year as indicated by a 2-year study, reflecting favorable conditions for microbial C assimilation at low temperatures in the absence of freeze–thaw perturbation. In the arable soil, C_mic contents were significantly reduced during soil freezing but recovered quickly upon warming of the soil. Dynamics of C_mic in the arable soil were paralleled by protozoan biomass and transient shifts in functional composition of the nematode community, indicating that microfaunal predation played an important role in nutrient cycling after freeze–thaw perturbation. Only minor microfaunal dynamics were observed in the climatically more stable fallow, essentially confirming the absence of perturbation at this site. Our findings provide strong evidence that overwinter N₂O formation is regulated by both the physical freeze–thaw susceptibility of the soil and the ecological functioning of the habitat.     

Selective oxidation of methane to methanol and formaldehyde over V2O5/SiO2 catalysts. Role of NO in the gas phase

The role of nitric oxide incorporation into the reaction feed for the partial oxidation of methane to C₂-hydrocarbons and C₂-oxygenates is evaluated. The addition of NO increases the conversion of methane under all the experimental conditions studied and has a strong effect on the product distribution. At low NO concentration the catalysts yield mainly C₂H_n hydrocarbons, but at higher NO concentrations, carbon oxides dominate. Amongst the C₁-oxygenates produced, methanol is the major compound observed and its proportion increases with increasing NO concentration. The highest C₁-oxygenates yield was 7% at atmospheric pressure. This revised version was published online in July 2006 with corrections to the Cover Date.     

Modification of ABS Membrane by PEG for Capturing Carbon Dioxide from CO2/N2 Streams

Carbon dioxide capture and storage (CCS) has been propounded as an important issue in greenhouse gas emissions control. In this connection, in the present article, the advantages of using polymeric membrane for separation of carbon dioxide from CO₂/N₂ streams have been discussed. A novel composition for fabrication of a blend membrane prepared from acrylonitrile-butadiene-styrene (ABS) terpolymer and polyethylene glycol (PEG) has been suggested. The influence of PEG molecular weight (in the range of 400 to 20000) on membrane characteristics and gas separation performance, the effect of PEG content (0–30 wt%) on gas transport properties, and the effect of feed side pressure (ranging from 1 to 8 bar) on CO₂ permeability have been studied. The results show that CO₂ permeability increases from 5.22 Barrer for neat ABS to 9.76 Barrer for ABS/PEG20000 (10 wt%) while the corresponding CO₂/N₂ selectivity increases from 25.97 to 44.36. Furthermore, it is concluded that this novel membrane composition has the potential to be considered as a commercial membrane.     

Study on the influence of SDS and THF on hydrate-based gas separation performance

Hydrate additives can be used to mitigate hydrate formation conditions, promote hydrate growth rate and improve separation efficiency. CO₂ + N₂ and CO₂ + CH₄ systems with presence of sodium dodecyl sulfate (SDS) or tetrahydrofuran (THF) are studied to analyze the effect of hydrate additives on gas separation performance. The experiment results show that CO₂ can be selectively enriched in the hydrate phase. SDS can speed up the hydrate growth rate by facilitating gas molecules solubilization. When SDS concentration increases, split and loss fraction increase initially and then decrease slightly, resulting in a decreased separation factor. The optimum concentration of SDS exists at the range of 100–300 ppm. As THF can be easily encaged in hydrate cavities, hydrate formation condition can be mitigated greatly with its existence. Additionally, THF can also strengthen hydrate formation. The THF effect on separation performance is related to feed gas components. CO₂ occupies the small cavities of type II hydrate prior to N₂. But the competitiveness of CO₂ and CH₄ to occupy cavities are quite fair. The variations of split fraction, loss fraction and separation factor depend on the concentration of THF added. The work in this paper has a positive role in flue gas CO₂ capture and natural gas de-acidification.     

Carbon dioxide reforming of methane to synthesis gas over hexaaluminate ANiAl11O19-delta (A = Ca, Sr, Ba and La) catalysts

A series of A‐modified hexaaluminates, ANiAl₁₁O_19-δ (A = Ca, Sr, Ba and La) as new catalysts for carbon dioxide reforming of methane to synthesis gas, were prepared by decomposition of nitrates and calcination at high temperature. Nickel ions as active component were inlayed in the hexaaluminate lattices to substitute part of Al ions. The structure and properties of these samples were characterized using XRD, XPS, TPR and TGA techniques. The series of hexaaluminates exhibited significantly catalytic activity and stability at high temperature, for instance at 780°C for 18 h, the conversion of CH₄ and CO₂ was kept over 91.0 and 93.7%, respectively, meanwhile no Ni sintering, phase transformation and catalyst deactivation due to carbon deposition were found. Besides, the modifier A in the mirror plane layer of the lattices showed different effects on reducibility and catalytic activity of transition metal Ni in the hexaaluminate lattices. This revised version was published online in July 2006 with corrections to the Cover Date.     

Synthesis gas production using steam hydrogasification and steam reforming

Experimental work has been carried out on the mixed reforming reaction, i.e., simultaneous steam and CO₂ reforming of methane under a wide range of feed compositions and four different reaction temperatures from 700 °C to 850 °C using a commercial steam reforming catalyst. The experiments were conducted for a CO₂/CH₄ ratio from 0 to 2 and a steam to methane ratio from 3 to 5. The effect of CO₂/CH₄ ratio on the exit H₂/CO ratio and the conversions of the reactants indicate that the dry reforming reaction is dominant under increased carbon dioxide in the feed. Steam reforming of typical steam hydrogasification product gas consisting of CO, H₂ and CO₂ in addition to steam and methane has also been investigated. The H₂/CO ratio of the product synthesis gas varies from 4.3 to 3.7 and from 4.8 to 4.1 depending on the feed composition and reaction temperature. The CO/CO₂ ratios of the synthesis gas varied from 1.9 to 2.9 and 2.0 to 3.3. The results are compared with simulation results obtained through the Aspen Plus process simulation tool. The results demonstrate that a coupled steam hydrogasification and reforming process can generate a synthesis gas with a flexible H₂/CO ratio from carbon-containing feedstocks.