Unlocking Potential for Low-Carbon Hydrogen Production from U.S. Natural Gas Resources.

Hydrogen will potentially play a key role while transitioning to a net-zero economy. This study addresses resource, environmental, economic, policy, and societal issues related to low-carbon hydrogen production by steam methane reforming with carbon capture and storage in Wyoming and other natural-gas-rich states. For low-carbon hydrogen produced from natural gas and electricity supplies and which stores CO2 in saline reservoirs in Wyoming, the levelized cost of hydrogen (LCOH) ranges from $1.62-2.00/kg H2, and the life cycle emissions range from 3.85-5.74 kg CO2-eq/kg H2. If claimed, the 45Q tax credit decreases the LCOH by 19%. Although the supplies of renewable natural gas feedstock and zero- or low-carbon electricity can lower the carbon footprint to make hydrogen projects qualified for the 45V tax credit, the 45Q tax credit is still a stronger economic incentive. To reduce the supply cost, a hydrogen cluster can be developed in the state by leveraging the colocation and coavailability of multiple natural resources and transport infrastructure. Developing a hydrogen cluster can directly create several thousand construction jobs and several hundred permanent jobs in Wyoming. Low-carbon hydrogen production can also be scaled up in other states across the nation.

Oxygen Species Involved in Complete Oxidation of CH4 by SrFeO3-δ in Chemical Looping Reforming of Methane.

Compared with conventional methane reforming technologies, chemical looping reforming (CLR) has the advantages of self-elimination of coke, a suitable syngas ratio for certain down-stream processes, and a pure H2 or CO stream. In the reduction step of CLR, methane combustion has to be inhibited, which could be achieved by designing appropriate oxygen carriers and/or optimizing the operating conditions. To gain a further understanding of the combustion reaction, methane oxidation by perovskite (SrFeO3-δ) at 900 °C and 1 atm in a pulse mode was investigated in this work. The oxygen non-stoichiometry of SrFeO3-δ prepared by a Pechini-type polymerizable complex method is 0.14 at ambient conditions, and it increases to 0.25 and subsequently to 0.5 when heating from 100 to 900 °C in argon that contains 2 ppmv of molecular oxygen. The activation energies of the first and second transitions are 294 and 177 kJ/mol, respectively. The presence of 0.99 vol.% hydrogen in argon significantly reduces the amount CO2 produced. At a pulse interval of 10 min, the amount of CO2 produced in the absence of hydrogen is one order of magnitude greater than that in the presence of hydrogen. In the former case, the amount of CO2 produced dramatically decreases first and then gradually approaches a constant, and the oxygen species involved in methane combustion can be partially replenished by extending the pulse interval, e.g., 82.5% of this type of oxygen species is replenished when the pulse interval is extended to 60 min. The restored species predominantly originate from those that reside in the surface layer or even in the bulk.

Tri-reforming of methane over Ni/ZrO2 catalyst derived from Zr-MOF for the production of synthesis gas.

The increasing concentration of CO2 and CH4 in the environment is a global concern. Tri-reforming of methane (TRM) is a promising route for the conversion of these two greenhouse gases to more valuable synthesis gas with an H2/CO ratio of 1.5-2. In this study, a series of Zr-MOF synthesized via the solvothermal method and impregnation technique was used to synthesize the nickel impregnated on MOF-derived ZrO2 catalyst. The catalyst was characterized by various methods, including N2-porosimetry, X-ray diffraction (XRD), temperature programmed reduction (TPR), CO2-temperature programmed desorption (CO2-TPD), thermo-gravimetric analysis (TGA), chemisorption, field-emission scanning electron microscopy (FE-SEM), and high-resolution transmission electron microscopy (HR-TEM). Characterization results confirmed the formation of the Zr-MOF and nickel metal dispersed on MOF-derived ZrO2. Further, the tri-reforming activity of the catalyst developed was evaluated in a downflow-packed bed reactor. The various catalysts were screened for TRM activity at different temperatures (600-850 °C). Results demonstrated that TRM was highly favorable over the NZ-1000 catalyst due to its desirable physicochemical properties, including nickel metal surface area (2.3 m2/gcat-1), metal dispersion (7.1%), and nickel metal reducibility (45%), respectively. Over the NZ-1000 catalyst, an optimum H2/CO ratio of ~ 1.6-2 was achieved at 750 °C, and it was stable for a longer period of time.

One-dimensional modeling of heterogeneous catalytic chemical looping steam methane reforming in an adiabatic packed bed reactor.

Hydrogen production via chemical looping steam methane reforming (CL-SMR) is among the most promising current technologies. This work presents the development in gPROMS Model Builder 4.1.0® of a 1D model of an adiabatic packed bed reactor used for chemical looping reforming (CLR). The catalyst used for this process was 18 wt. % NiO with the support of Al2O3. A brief thermodynamic analysis using Chemical Equilibrium Application (CEA) was carried out to identify the optimum operating conditions. The model was simulated for 10 complete CL-SMR cycles. The effects of variations in temperature, pressure, gas mass velocity, nickel oxide concentration, reactor length, and particle diameter were studied to investigate the performance of the CL-SMR process under these variations. A parametric analysis was carried out for different ranges of conditions: temperatures from 600 to 1,000 K, pressure from 1 to 5 bar, gas mass velocity between 0.5 and 0.9 kg·m-2 s-1, nickel oxide concentration values between 0.1 and 1 mol·m-3, particle diameters between 0.7 and 1 mm, and fuel reactor (FR) lengths between 0.5 and 1.5 m. At the optimum temperature (950 K), pressure (1 bar), and steam-to-carbon molar ratio (3/1), with an increase in particle diameter from 0.7 to 1 mm, an 18% decrease in methane conversion and a 9.5% increase in hydrogen yield were observed. Similarly, with an increase in FR length from 0.5 m to 1.5 m, a delay in the temperature drop was observed.

Improving the Coke Resistance of Ni-Ceria Catalysts for Partial Oxidation of Methane to Syngas: Experimental and Computational Study.

The synthesis of syngas (H2 : CO=2) via catalytic partial oxidation of methane (CPOM) is studied over noble metal doped Ni-CeO2 bimetallic catalysts for CPOM reaction. The catalysts were synthesized via a controlled deposition approach and were characterized using XRD, BET-surface area analysis, H2 -TPR, TEM, Raman and TGA analysis. The catalysts were experimentally and computationally studied for their activity, selectivity, and long-term stability. Although the pure 5Ni/CeO2 catalyst showed high initial activity (∼90%) of CH4 conversion, it rapidly deactivates around 20% of its initial activity within 140 hours of TOS. Doping of Ni/CeO2 catalyst with noble metal was found to be coke resistant with the best-performing Ni-Pt/CeO2 catalyst showed ∼95% methane conversion with >90% selectivity at a temperature of 800 °C, having exceptional stability for about 300 hours of time-on-stream (TOS). DFT studies were performed to calculate the activation barrier for the C-H activation of methane over the Ni, Ni3 Pt, Ni3 Pd, and Ni3 Ru (111) surfaces showed nearly equal activation energy over all the studied surfaces. DFT studies showed high coke formation tendency of the pure Ni (111) having a very small C-C coupling activation barrier (14.2 kJ/mol). In contrast, the Ni3 Pt, Ni3 Pd, and Ni3 Ru (111) surfaces show appreciably higher C-C coupling activation barrier (∼70 kJ/mol) and hence are more resistant against coke formation as observed in the experiments. The combined experimental and DFT study showed Ni-Pt/CeO2 as a promising CPOM catalyst for producing syngas with high conversion, selectivity and long-term stability suited for future industrial applications.

Influence of Lanthanum Precursor on the Activity of Nickel Catalysts in the Mixed-Methane Reforming Process.

This work investigated the influence of the catalytic support precursor on the activity of nickel catalysts 20%Ni/5%La2O3-95%Al2O3 in the mixed methane reforming process. The activity tests were carried out at a temperature of 750 °C. The research showed that the catalyst prepared from the precursor containing chloride exhibited very low conversions of methane and carbon dioxide. The poisoned catalyst system before and after the calcination process was subjected to Temperature Programmed Surface Reaction tests to determine whether the thermal treatment causes a decrease in the amount of chlorine in the system. To determine the decomposition temperature of the LaCl3 precursor and the nickel chloride NiCl2 compound, the samples were analyzed by Thermogravimetry. Finally, the catalytic samples were tested by Time-of-Flight Secondary Ion Mass Spectrometry analysis to confirm the presence of nickel-chlorine bonds on the surface of the catalytic system.

Using greenhouse gases in the synthesis gas production processes: Thermodynamic conditions.

The work concerns the thermodynamic analysis of CH4 reforming with various oxidants (CO2, H2O, O2) in the technological variants DRM (Dry Reforming of Methane) and TRM (Tri-reforming of Methane) technological variants. Both processes of synthesis gas production (raw material for the production of value-added products) are problematic in terms of environmental protection. In the process, two components of greenhouse gases are used as a substrate: CO2 and CH4. The influence of temperature, pressure, and the molar ratio of oxidants to methane on the efficiency of both processes was analyzed using the deterministic method: raw material conversion, product efficiency and selectivity - H2 and CO, and the value of the H2/CO ratio characterizing the suitability of the synthesis gas for various syntheses. The problem of carbon deposition tendency in DRM was minimized through the selection of operational process conditions, and in the case of TRM, it was fully reduced. The deterministic method of non-linear programming by defining the objective function with constraints helped formulate allowed one the values of TRM parameters: complete reduction of the coking problem, maintaining the H2/CO ratio at the desired level - 2 and CO2 conversion equal to 90%, led to a hydrogen efficiency of over 90%. This efficiency can be obtained at the process temperature T = 273 K, with a pressure of 1 atm, and the molar ratios of oxidants to methane: CH4/CO2/H2O/O2 = 1/0.36/0.77/0.01.

Nanocomposite Catalyst for High-Performance and Durable Intermediate-Temperature Methane-Fueled Metal-Supported Solid Oxide Fuel Cells.

CH4-fueled metal-supported solid oxide fuel cells (CH4-MS-SOFCs) are propitious as CH4 is low-priced and readily available, and its renewable production is possible, such as biomethane. However, the current CH4-MS-SOFCs suffer from either poor power density or short durable operation, which is ascribed to the low catalytic activity and poor coking tolerance of the metallic anode support. Herein, we have deliberately designed and synthesized a highly active nanocomposite catalyst, Sm-doped CeO2-supported Ni, as the internal steam methane reforming catalyst, to optimize CH4-MS-SOFCs. Both power densities and durability of optimized CH4-MS-SOFCs have been dramatically enhanced compared to the pristine CH4-MS-SOFCs. The optimized CH4-MS-SOFCs deliver the highest performances among all zirconia-based CH4-MS-SOFCs. Furthermore, the operating temperature has been reduced to 600 °C. At 600 °C, a viable peak power density of >350 mW/cm2 is achieved, which is more than three times as high as the pristine CH4-MS-SOFCs. Furthermore, the optimized CH4-MS-SOFC achieves >1000 h of stable operation.

A General Route to Flame Aerosol Synthesis and In Situ Functionalization of Mesoporous Silica.

Mesoporous silica is a versatile material for energy, environmental, and medical applications. Here, for the first time, we report a flame aerosol synthesis method for a class of mesoporous silica with hollow structure and specific surface area exceeding 1000 m2 g-1 . We show its superior performance in water purification, as a drug carrier, and in thermal insulation. Moreover, we propose a general route to produce mesoporous nanoshell-supported nanocatalysts by in situ decoration with active nanoclusters, including noble metal (Pt/SiO2 ), transition metal (Ni/SiO2 ), metal oxide (CrO3 /SiO2 ), and alumina support (Co/Al2 O3 ). As a prototypical application, we perform dry reforming of methane using Ni/SiO2 , achieving constant 97 % CH4 and CO2 conversions for more than 200 hours, dramatically outperforming an MCM-41 supported Ni catalyst. This work provides a scalable strategy to produce mesoporous nanoshells and proposes an in situ functionalization mechanism to design and produce flexible catalysts for many reactions.

Improving Anti-Coking Properties of Ni/Al2O3 Catalysts via Synergistic Effect of Metallic Nickel and Nickel Phosphides in Dry Methane Reforming.

A series of NiP-x/Al2O3 catalysts containing different ratio of metallic nickel to nickel phosphides, prepared by varying Ni/P molar ratio of 4, 3, 2 through a co-impregnation method, were employed to investigate the synergistic effect of metallic nickel-nickel phosphides in dry methane reforming reaction. The Ni/Al2O3 catalyst indicates good activity along with severe carbon deposition. The presence of phosphorus increases nickel dispersion as well as the interaction between nickel and alumina support, which results in smaller nickel particles. The co-existence of metallic nickel and nickel phosphides species is confirmed at all the P contained catalysts. Due to the relative stronger CO2 dissociation ability, the NiP-x/Al2O3 catalysts indicate obvious higher resistance of carbon deposition. Furthermore, because of good balance between CH4 dissociation and CO2 dissociation, NiP-2/Al2O3 catalyst exhibits best resistance of carbon deposition, few carbon depositions were formed after 50 h of dry methane reforming.

Life cycle flaring emissions mitigation potential of a novel Fischer-Tropsch gas-to-liquid microreactor technology for synthetic crude oil production.

This paper compares the environmental impacts of the operation of a novel Gas-to-Liquid (GtL) process for synthetic crude oil production with conventional crude oil production. This process uses novel microreactor technology (NetMIX) applied in Steam Methane Reforming and Fischer-Tropsch (FT-SMR) for the conversion of associated gas originated on offshore Oil and Gas exploration. Data from literature for Oil and Gas extraction together with data obtained from Aspen Plus ® simulations was used to build the life cycle inventory. An attributional Life Cycle Assessment (LCA) was performed to compare the FT-SMR pathway to conventional crude oil production, using 1 MJ LHV as the functional unit. An additional assessment was also conducted by reporting the impact to 1 barrel. This is done to assess the effect that the add-on technology may have on the impact of current crude production. Converting associated gas using the FT-SMR pathway produces a synthetic crude with negative net GWP impacts. This is because the amount of avoided emissions is larger than the emissions due to the operation of the pathway. The remaining impact categories increase since the FT-SMR has additional intermediary steps, with added fuel energy needs, and additional process emissions. Moreover, the amount of natural gas required to produce 1 MJ of synthetic crude oil (abbreviated in the text as syncrude) results in larger impacts in the extraction phase, than those associated with the extraction of 1 MJ of conventional crude. The obtained syncrude has a GWP impact of -0.34 [-0.62, -0.14] kg CO2 eq/MJ, in comparison to 0.012 [0.009, 0.017] kg CO2 eq/MJ of conventional crude. A reduction of 8% to the impacts per daily barrel of crude (70.3 kg CO2 eq/barrel and 64.6 kg CO2 eq/barrel before and after using the FT-SMR pathway) was observed for a reduction of 34% of the total flared gas mass.

The Influence of High-Energy Faceted TiO2 Supports on Co and Co-Ru Catalysts for Dry Methane Reforming.

The reforming of methane from biogas has been proposed as a promising method of CO2 utilization. Co-based catalysts are promising candidates for dry methane reforming. However, the main constraints limiting the large-scale use of Co-based catalysts are deactivation through carbon deposition (coking) and sintering due to weak metal-support interaction. We studied the structure-function properties and catalytic behavior of Co/TiO2 and Co-Ru/TiO2 catalysts using two different types of TiO2 supports, commercial TiO2 and faceted non-stoichiometric rutile TiO2 crystals (TiO2 *). The Co and Ru metal particles were deposited on TiO2 supports using a wet-impregnation method with the percentage weight loading of Co and Ru of 5% and 0.5%, respectively. The materials were characterized using SEM, STEM-HAADF, XRD, XPS and BET. The catalytic performance was studied using the CH4 : CO2 ratio of 3 : 2 to mimic the methane-rich biogas composition. Our results indicate that the addition of Ru to Co catalysts supported on TiO2 * reduces carbon deposition and influences oxygen mobility. Co and Co-Ru catalysts supported on TiO2 * has superior activity with the highest conversion of CO2 and CH4 of 34.7% and 23.5%, respectively. Despite the improved performance, the Co-Ru/TiO2 * catalyst has limited stability due to the proliferation of nanoparticle growth and TiOx layers on the surface of the nanoparticles indicating the prevalence of the strong-metal support interaction.

Effect of Ruthenium and Cerium Oxide (IV) Promotors on the Removal of Carbon Deposit Formed during the Mixed Methane Reforming Process.

This work investigates the effect of the addition of Ru and CeO2 on the process of gasification of carbon deposits formed on the surface of a nickel catalyst during the mixed methane reforming process. Activity studies of the mixed methane reforming process were carried out on (Ru)-Ni/CeO2-Al2O3 catalysts at the temperature of 650-750 °C. The ruthenium-promoted catalyst exhibited the highest activity. Carbonized post-reaction catalyst samples were tested with the TOC technique to investigate the carbonization state of the samples. The bimetallic catalyst had the lowest amount of carbon deposit (1.5%) after reaction at 750 °C. The reactivity of the carbon species was assessed in mixtures of oxygen, hydrogen, carbon dioxide, and water. Regardless of the gasifying agent used, the carbon deposit was removed from the surface of the catalytic system. The overall mechanism of mixed methane reforming over Ru and CeO2 was shown.

Development of Gas Sensor Array for Methane Reforming Process Monitoring.

The article presents a new method of monitoring and assessing the course of the dry methane reforming process with the use of a gas sensor array. Nine commercially available TGS chemical gas sensors were used to construct the array (seven metal oxide sensors and two electrochemical ones). Principal Component Regression (PCR) was used as a calibration method. The developed PCR models were used to determine the quantitative parameters of the methane reforming process: Inlet Molar Ratio (IMR) in the range 0.6-1.5, Outlet Molar Ratio (OMR) in the range 0.6-1.0, and Methane Conversion Level (MCL) in the range 80-95%. The tests were performed on model gas mixtures. The mean error in determining the IMR is 0.096 for the range of molar ratios 0.6-1.5. However, in the case of the process range (0.9-1.1), this error is 0.065, which is about 6.5% of the measured value. For the OMR, an average error of 0.008 was obtained (which gives about 0.8% of the measured value), while for the MCL, the average error was 0.8%. Obtained results are very promising. They show that the use of an array of non-selective chemical sensors together with an appropriately selected mathematical model can be used in the monitoring of commonly used industrial processes.

A review on the computational studies of the reaction mechanisms of CO2 conversion on pure and bimetals of late 3d metals.

Despite series of experimental studies that reveal unique activities of late 3d transition metals and their role in microorganisms known for CO2 conversion, these surfaces are not industrially viable yet. An insight into the elementary steps of surface catalytic processes is crucial for effective surface modification and design. The mechanisms of CO2 transformation into CO, through the reverse water gas shift and methane reforming, are being studied. Mechanisms of CO2 methanation is also being explored by the Sabatier reaction into methane. This review covers both experimental and theoretical studies into the mechanisms of CO2 reduction into CO and methane, on single metals and bimetals of late 3d transition metals, i.e. Fe, Co, Ni, Cu and Zn. This paper highlights progress and gaps still existing in our knowledge of the reaction mechanisms. These mechanistic studies reveal CO2 activation and reduction mechanisms are specific to both composition and surface facet. Surfaces with least CO2 binding potential are seen to favour CO and O binding and provide higher barriers to dissociation. No direct correlation has been seen between binding strength of CO2 and its degree of activation. Hydrogen-assisted dissociation is seen to be generally favoured kinetically on Cu and Ni surfaces over direct dissociation except on the Ni (211) surface. Methane production on Cu and Ni surfaces is seen to occur via the non-formate pathway. Hydrogenation reactions have focused on Cu and Ni, and more needs to be done on other surfaces, i.e. Co, Fe and Zn.

Revisiting the role of steam methane reforming with CO2 capture and storage for long-term hydrogen production.

Road transport is associated with high greenhouse gas emissions due to its current dependence on fossil fuels. In this regard, the implementation of alternative fuels such as hydrogen is expected to play a key role in decarbonising the transport system. Nevertheless, attention should be paid to the suitability of hydrogen production pathways as low-carbon solutions. In this work, an energy systems optimisation model for the prospective assessment of a national hydrogen production mix was upgraded in order to unveil the potential role of grey hydrogen from steam methane reforming (SMR) and blue hydrogen from SMR with CO2 capture and storage (CCS) in satisfying the hydrogen demanded by fuel cell electric vehicles in Spain from 2020 to 2050. This was done by including CCS retrofit of SMR plants in the energy systems model, as a potential strategy within the scope of the European Hydrogen Strategy. Considering three hypothetical years for banning hydrogen from fossil-based plants without CCS (2030, 2035, and 2040), it was found that SMR could satisfy the whole demand for hydrogen for road transport in the short term (2020-2030), while being substituted by water electrolysis in the medium-to-long term (2030-2050). Furthermore, this trend was found to be associated with an appropriate prospective behaviour in terms of carbon footprint.

Potential of microbial protein from hydrogen for preventing mass starvation in catastrophic scenarios.

Human civilization's food production system is currently unprepared for catastrophes that would reduce global food production by 10% or more, such as nuclear winter, supervolcanic eruptions or asteroid impacts. Alternative foods that do not require much or any sunlight have been proposed as a more cost-effective solution than increasing food stockpiles, given the long duration of many global catastrophic risks (GCRs) that could hamper conventional agriculture for 5 to 10 years. Microbial food from single cell protein (SCP) produced via hydrogen from both gasification and electrolysis is analyzed in this study as alternative food for the most severe food shock scenario: a sun-blocking catastrophe. Capital costs, resource requirements and ramp up rates are quantified to determine its viability. Potential bottlenecks to fast deployment of the technology are reviewed. The ramp up speed of food production for 24/7 construction of the facilities over 6 years is estimated to be lower than other alternatives (3-10% of the global protein requirements could be fulfilled at end of first year), but the nutritional quality of the microbial protein is higher than for most other alternative foods for catastrophes. Results suggest that investment in SCP ramp up should be limited to the production capacity that is needed to fulfill only the minimum recommended protein requirements of humanity during the catastrophe. Further research is needed into more uncertain concerns such as transferability of labor and equipment production. This could help reduce the negative impact of potential food-related GCRs.

Comparative life cycle sustainability assessment of renewable and conventional hydrogen.

Hydrogen is gaining interest as a strategic element towards a sustainable economy. In this sense, sound decision-making processes in the field of hydrogen energy require thorough analyses integrating economic, environmental and social indicators from a life-cycle perspective. For this purpose, Life Cycle Sustainability Assessment (LCSA) constitutes an appropriate methodology jointly handling indicators related to the three traditional dimensions of the sustainability concept. In this work, the sustainability performance of renewable hydrogen from both wind-powered electrolysis and biomass gasification was benchmarked against that of conventional hydrogen from steam methane reforming under a set of five life-cycle indicators: global warming, acidification, levelised cost, child labour, and health expenditure. The results led to identify the stage of driving-energy/biomass production as the main source of impact. When compared to conventional hydrogen, the life-cycle sustainability performance of renewable hydrogen was found to underperform under social and economic aspects. Nevertheless, the expected enhancement in process efficiency would significantly improve the future performance of renewable hydrogen in each of the three main sustainability dimensions.

Prospective carbon footprint comparison of hydrogen options.

The Life Cycle Assessment methodology is often used to evaluate the environmental performance of hydrogen energy systems. However, even though hydrogen is usually seen as a strategic energy carrier for the future energy sector, there is a lack of case studies assessing its prospective life-cycle performance. In order to contribute to filling this gap, this work addresses a carbon footprint comparison of hydrogen options from a prospective standpoint. Four relevant hydrogen production pathways (steam methane reforming, grid-powered alkaline electrolysis, wind-powered alkaline electrolysis, and biomass gasification) under three time scenarios (reference, year 2030, and year 2050) are assessed, taking into account the expected evolution of key technical parameters such as efficiencies, lifespans, and the grid electricity mix. The results show a favourable carbon footprint of renewable hydrogen from biomass gasification and wind electrolysis, with a relatively steady near-zero carbon footprint. Despite the unfavourable carbon footprint results of conventional hydrogen from steam methane reforming and hydrogen from grid electrolysis, the latter is associated with a rapid trend towards a suitable long-term carbon footprint.

Influence of Nature Support on Methane and CO2 Conversion in a Dry Reforming Reaction over Nickel-Supported Catalysts.

A promising method to reduce global warming has been methane reforming with CO2, as it combines two greenhouse gases to obtain useful products. In this study, Ni-supported catalysts were synthesized using the wet impregnation method to obtain 5%Ni/Al2O3(SA-5239), 5%Ni/Al2O3(SA-6175), 5%Ni/SiO2, 5%Ni/MCM41, and 5%Ni/SBA15. The catalysts were tested in dry reforming of methane at 700 °C, 1 atm, and a space velocity of 39,000 mL/gcat h, to study the interaction of Ni with the supports, and evaluation was based on CH4 and CO2 conversions. 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2 gave the highest conversion of CH4 (78 and 75%, respectively) and CO2 (84 and 82%, respectively). The catalysts were characterized by some techniques. Ni phases were identified by X-ray diffraction patterns. Brunauer-Emmett-Teller analysis showed different surface areas of the catalysts with the least being 4 m2/g and the highest 668 m2/g belonging to 5%Ni/Al2O3(SA-5239) and 5%Ni/SBA15, respectively. The reduction profiles revealed weak NiO-supports interaction for 5%Ni/Al2O3(SA-5239), 5%Ni/MCM41, and 5%Ni/SBA15; while strong interaction was observed in 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2. The 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2 were close with respect to performance; however, the former had a higher amount of carbon deposit, which is mostly graphitic, according to the conducted thermal analysis. Carbon deposits on 5%Ni/SiO2 were mainly atomic in nature.