Coke Accumulation Research Articles

Bi-reforming of model biogas to syngas over ultrasmall Ru/MgO nano-catalysts prepared via soft template-assisted mechanochemical method

The upgrading of renewable biogas into value-added fuel and chemicals via syngas is of great significance. Ru/MgO nano-catalysts were prepared via novel soft template-assisted mechanochemical method. Comprehensive characterizations (XRD, N2 physisorption, ICP-OES, CO-chemisorption, CO2-TPD, XPS, HAADF-STEM, HRTEM, CH4-TPSR/CO2-TPO, TGA and Raman spectroscopy, etc.) were conducted to deeply analyze the fresh/spent catalysts. The 0.2Ru/MgO-0.2CTAB catalyst showed high initial activity in terms of CH4/CO2 conversion (∼94 %/61 %) and maintained catalytic stability over 120 h in bi-reforming of model biogas, at 800 °C under CH4/CO2/N2/H2O molar ratio of 3:2:1:2.6 and weight hourly space velocity of 30960 mL g-1h−1. CTAB and other soft templates were effective in enhancing the dispersion of Ru nanoparticles (NPs), which contribute to the inhibition of the deep cracking of CH4 and coke accumulation. Alkaline MgO oxide was crucial in the activation of CO2 and the production of active O* species, thus promoting the removal of carbonaceous precursor and inhibiting the coke accumulation. Additionally, the strong interaction between ultrafine Ru NPs and the MgO support significantly contributed to its anti-sintering performance. The combined advantages of narrow size distribution of ultra-small Ru NPs, suitable basicity of MgO as well as the interaction between ultrafine Ru NPs and MgO over 0.2Ru/MgO-0.2CTAB catalyst led to satisfying catalytic performance in bi-reforming of model biogas.

Coking and deactivation behavior study of Ce-modified Cs-Nb/Al2O3 in aldol condensation of methyl propionate with formaldehyde

Coke deposition during the aldol condensation of methyl propionate (MP) and formaldehyde (FA) to produce methyl methacrylate (MMA) is a critical factor limiting the long-term stability of catalysts. In this work, Ce-modified Cs-Nb/Al2O3 catalysts with superior catalytic activity and robust coke resistance were achieved during the reaction by enhancing the oxygen vacancy (OV) ratio. With optimal Ce loading of 1 %, the MP conversion of 35.4 % and MMA selectivity of 90.3 % can be achieved. Meanwhile, the coke content of the modified catalyst significantly reduced from the original 10.49 wt% to 5.44 wt%. It was discovered that higher water content in the reaction feedstock promotes the hydrolysis reaction, resulting in a decrease in MMA selectivity. Furthermore, the presence of water can promote the conversion of Lewis acid sites to Brønsted acid sites, while an excess of Brønsted acid sites can accelerate the coke formation. Various characterization techniques confirmed that the coke species on the used catalysts consisted basically of polycyclic aromatic hydrocarbons and aliphatic compounds. Ultimately, the kinetics of coke deposition on Cs-Nb/Al2O3 and Cs-Nb-1Ce/Al2O3 were established using the modified Voorhies equation, offering a reliable method to predict coke accumulation under specific conditions. The higher apparent activation energy of coke formation observed on Cs-Nb-1Ce/Al2O3 is responsible for its robust coke resistance.

Mitigating deactivation in dry methane reforming by lanthanum catalysts for enhanced hydrogen production: A review

Catalyst deactivation in dry methane reforming, resulting from coke accumulation and sintering, has long captivated academic interest due to its negative impact on catalytic performance and hindrance to industrial scalability. Thus, developing efficient catalysts capable of sustaining high reforming activity and stability is crucial. Lately, lanthanum (La) has gained popularity in catalysis for its ability to enhance performance and resist coking, owing to its great basicity, redox capabilities, and high oxygen storage capacity. As a result, diverse strategies for incorporating La into catalysts, including support, promoter, bimetallic combinations, and perovskite formation, have been extensively explored. Herein, this review delves into various advancements in lanthanum-based catalysts and their effectiveness in dry methane reforming while addressing catalyst deactivation and regeneration. Finally, the prospect of La-based catalysts in dry methane reforming is also emphasized in this review.

Transient simulation of conjugate heat transfer of kerosene with thermal oxidative and surface coking reactions at a supercritical pressure

The regenerative cooling technology in aerospace applications often involves supercritical-pressure heat transfer of a hydrocarbon fuel, in which thermal oxidative reactions of the fuel would lead to surface coke accumulation on the cooling channel wall. In this paper, the long-term transient conjugate heat transfer of kerosene has been numerically investigated in a circular mini tube at a supercritical pressure of 3 MPa. The modified chemical mechanism and kinetics of thermal oxidative and surface coking reactions of kerosene are proposed, which, with an additional surface reaction, are capable of treating large coke deposition in regions with sharp temperature gradients. Transient surface coke accumulation and its effect on heat transfer are handled by a dynamic mesh technique. A series of numerical studies are conducted to elucidate the influences of surface heat flux, dissolved oxygen mass fraction, inlet fuel mass flow rate, and coke layer thermal conductivity on the supercritical-pressure heat transfer and thermal oxidative reactions. The effects of different reaction pathways on surface coke accumulation are analyzed comprehensively, and it is revealed that the oxygen-consuming surface coke deposition is initiated only at the high fuel temperature at around 590 K. The present numerical results would enhance fundamental understanding of the long-term transient heat transfer process of a hydrocarbon fuel at supercritical pressures in the regenerative cooling applications.

Lattice-embedded Ni single-atom catalyst on porous Al2O3 nanosheets derived from Ni-doped carbon dots for efficient propane dehydrogenation

The controlled synthesis of highly durable single-atom catalysts (SACs) for high-temperature applications remains a great challenge. Herein, we develop a facile strategy to construct Al2O3 lattice-embedded Ni SAC via thermal treatment of aluminum oxide encapsulated Ni-doped carbon dots (Ni-CDs@Al2O3). Detailed studies reveal that the Ni atoms are released from carbon matrix and simultaneously captured by cation defects formed in situ within a phase transformation of aluminum oxide. Al2O3 stabilized Ni atoms via Ni-O4 coordination are well illustrated by combined characterizations. For propane dehydrogenation, reactivity measurements show that the center of Ni-O ion pairs effectively activates C3H8 and the higher rate of C3H6 formation on Ni SAs than Ni NPs, by a factor of 12, is the result of inhibition of C-C bond cleavage involving side reactions, as identified by density functional calculations. Beyond that, this lattice-embedded Ni SAC exhibits superior stability and recyclability in long-term operation with little coke accumulation.

Highly stable 3D-printed monolithic Al2O3-supported Ni-based structured catalysts for dry reforming of methane

Nickel (Ni)-based powder catalysts with poor stability used in dry reforming of methane (DRM) suffer from severe coking and high bed pressure drop. We successfully prepared a monolithic NiAl2O4/Al2O3 structured catalyst using 3D printed α-Al2O3 topological carrier followed by Ni impregnation and calcination at 1400 oC to improve the stability and decrease the pressure drop. The monolithic Ni/NiAl2O4/Al2O3 structured catalyst reduced from NiAl2O4/Al2O3 could inhibit coke accumulation effectively and exhibit excellent catalytic performance. During the 750-h stability test, monolithic Ni/NiAl2O4/Al2O3 catalyst exhibited 3% CH4 conversion degradation and 0.37 mgC h-1 gcat-1 coke accumulation rate. The formation mechanisms of two different types of cokes were proposed to explain the performance. Monolithic Ni/NiAl2O4/Al2O3 structured catalyst also exhibited a lower pressure drop and superior stability than the powder catalyst. This work serves as a guide for preparing the monolithic Ni-based structured catalyst with outstanding stability and low pressure drop for practical application in DRM.

Maximizing light olefin production via one-pot catalytic cracking of crude waste plastic pyrolysis oil

Energy-efficient processes for converting polyolefinic waste plastics into light olefins are critical for mitigating environmental pollution and reducing carbon emissions. In this study, an alternative recycling scheme, the catalytic cracking of crude waste plastic pyrolysis oil (WPPO) over microspherical P-modified steam-treated ZSM-5 (ms-P-HZSM5-S), was demonstrated and compared to a state-of-the-art commercial scheme, the thermal cracking of a hydrotreated naphtha range of WPPO. The C2–C4 olefins yield achieved by the catalytic WPPO cracking (56.6 wt%) exceeded those achieved by the thermal WPPO cracking (36.1 wt%), thermal naphtha cracking (23.1 wt%), and catalytic naphtha cracking (29.7 wt%), which indicated the superiority of WPPO over naphtha as a feedstock. However, during a deactivation test over ms-P-HZSM5-S, coke accumulation resulted in a rapid decline in the yields of ethylene (from 17.2 to 14.6 wt%), propylene (from 25.8 to 23.6 wt%), and benzene, toluene, and xylenes (from 16.1 to 13.4 wt%) after a reaction time of 810 s (temperature = 680 °C, weight hourly space velocity = 16 h−1). Nevertheless, the catalytic performance was fully restored through regeneration in air at 730 °C, which confirmed the viability of continuous operation involving successive reaction–regeneration cycles. These findings can be leveraged to devise a new approach, the catalytic cracking of WPPO integrated with a continuous regeneration (e.g., circulating fluidized bed reactor) system, which could offer several advantages over the commercial strategy, including the posttreatment-free utilization of the entire WPPO range, higher light olefins yields, continuous coke removal, reduced energy consumption, and non-necessity of H2.

Evaluation of Oxygen Carrier Performance in a Packed‐Bed Reactor during Chemical Looping Hydrogen Generation

AbstractChemical looping hydrogen generation (CLHG) has attracted much attention owing to its simple operation, low carbon capture cost, and high hydrogen purity. The performance of oxygen carrier plays an important role in the CLHG. In this work, considering the variation of internal reaction and coke deposition inside the oxygen carrier during the CLHG process, a packed‐bed reactor model is established. The temperature, gas composition, and coke deposition distribution inside the particle and reactor are explored. The results indicate that the reaction progress of the oxygen carrier near the wall is slightly faster than that at the center. The overall conversion rate and coke accumulation of the oxygen carrier near the wall are greater than those at the center.

A Mini-Review on Lanthanum–Nickel-Based Perovskite-Derived Catalysts for Hydrogen Production via the Dry Reforming of Methane (DRM)

Given that the attempts to head toward a hydrogen economy are gathering pace, the dry reforming of methane (DRM) to produce hydrogen-rich syngas is a reaction that is worthy of investigation. Nickel-based catalysts have been extensively examined as a cost-effective solution for DRM, though they suffer from fast deactivation caused by coke accumulation. However, a number of published studies report high catalytic performance in terms of both activity and stability for La–Ni-based perovskite-derived catalysts used in DRM in comparison to other corresponding materials. In the work presented herein, a thorough analysis regarding the application of La–Ni-based perovskite catalysts for DRM is carried out. LaNiO3 is known for its anti-coking ability owing to the strong interaction between CO2 and La2O3. A further modification to improve the catalytic performance can be achieved by the partial or complete substitution of A or/and B sites of the perovskite catalysts. The latest developments with respect to this topic are also discussed in this manuscript. Even though the low surface area of perovskite catalysts has always been an obstacle for their commercialization, new supported and porous perovskite materials have recently emerged to address, at least partly, the challenge. Finally, conclusions and future outlooks for developing novel perovskite catalysts that may potentially pioneer new technology are included.

The impact of various catalysts on pyrolysis bio-oil characteristics and catalyst coking behavior of corn stover

ABSTRACT Biomass has immense potential to address energy and environmental issues. Catalytic pyrolysis is an effective technology for utilizing biomass. Six catalysts (CaO, Al2O3, Fe2O3, MCM-41, HZSM-5, and red mud(RM)) were used to pyrolyze corn stover in a fixed-bed reactor. Six catalysts (CaO, Al2O3, Fe2O3, MCM-41, HZSM-5, and red mud (RM)) were used in a fixed-bed reactor. The feedstock-to-catalyst (FCR) ratio was adjusted to optimize the catalytic effect. The comprehensive evaluation of the catalysts was carried out by analyzing the deoxygenation effect, liquid yield, and catalyst coke accumulation behavior through TG, GC-MS, SEM/EDS, and XRD techniques. The study revealed that superior deoxygenation performance among the six investigated were HZSM-5, CaO, and RM. At the highest FCR (2:1), the liquid yield and deoxygenation effect of CaO are both at their optimal state simultaneously. The bio-oil yield reached 51.98%, but it has a coke accumulation of 27.07% by TG. MCM-41 and HZSM-5 exhibited more severe coking with coke contents of 8.14% and 8.04%, respectively, along with higher maximum heat loss temperature, upon dichloromethane extraction. The relative peak areas of alkanes in the coke accumulation were more than 50% except for RM, which the main component of the latter was polycyclic aromatic hydrocarbons (78.43%). By comparing the bio-oil characteristics and carbon accumulation behavior of different catalysts, it provides a reference for the study of carbon accumulation in pyrolysis catalysts.

Numerical study on reaction and heat transfer of supercritical aviation kerosene with pyrolysis and steam reforming in a corrugated cooling channel

Coking and heat transfer deterioration of supercritical aviation kerosene pose grave challenges to regenerative cooling of scramjet engines. In the present study, reaction and heat transfer characteristics of supercritical China aviation kerosene No. 3, RP-3 undergoing simultaneous pyrolysis and steam reforming reactions in a corrugated channel are numerically studied. Compared with reacting flow of RP-3 in the smooth channel, temperature and coke deposition are much lower in majority part of the corrugated channel. The maximum temperature difference between the smooth and corrugated channels is up to 300K. The maximum heat transfer coefficient in the corrugated channel is almost three times of that in the smooth channel under the same condition. However, low-velocity and high-temperature zones are formed near the corrugated micro-structures and cause coke accumulation and heat transfer deterioration along the flow direction of the corrugated channel. With the increase of wall heat flux, both temperature and velocity increase significantly in the corrugated channel. The conversion of RP-3 and formation of coke are also enhanced with increasing wall heat flux. Moreover, the total heat transfer coefficient first increases and then decreases with wall heat flux. The maximum total heat transfer coefficient increases from 4000W/m2∙K to 18,000W/m2∙K with wall heat flux increasing from 0.3MW/m2 to 1.8MW/m2. Periodic wavy structures are found at the interface between the corrugated micro-structure and the bulk flow, which is pronounced when wall heat flux is 1.3MW/m2 or above. With the increase of flow time, local turbulent kinetic energy decreases due to the interaction between the corrugated micro-structures and the wavy structures. The interaction between the corrugated structures and complex reaction and heat transfer leads to intersection of the distributions of temperature and coke in the smooth and the corrugated channels. An empirical heat transfer correlation formula is obtained as Nu=0.1Re0.65Pr1.94 for RP-3 reacting flow in the corrugated channel. The study provides better insight into interaction mechanism between chemically reacting flow and micro corrugated structures.

Methane conversion to syngas by chemical looping on La0.8Sr0.2FexCo1-xO3 (x = 0, 0.25, 0.50, 0.75) perovskites with CO2 co-feeding

Partial oxidation of methane (POM) by chemical looping with CO2 co-feeding on La0.8Sr0.2FeO3 (LSF) perovskite catalyst yielded a highly selective operation and enabled to extend the duration of reduction cycle. In this work, the conversion of methane to syngas was studied on La0.8Sr0.2Fe(x)Co(1-x)O3 (x = 0, 0.25, 0.5, 0.75) perovskites in chemical-looping mode, co-feeding CO2 and methane. The reaction was conducted at 850 °C, 15 min reduction (10% methane in N2, 0–3% CO2), and 10 min oxidation (10% O2 in N2) cycles. The perovskites activity decreased with increasing Co content, in the absence of CO2, due to intensified coke deposition on the catalyst. Addition of CO2 during the reduction step (1–3%) reduced coke accumulation. A run conducted on La0.8Sr0.2CoO3 (LSC) with continuous feeding of CO2 and periodical (on–off) methane feeding indicated that CO2 reacts with the accumulated coke in reverse-Boudouard reaction, increasing CO selectivity without affecting the methane conversion. XRD analysis of reduced Co-containing perovskites indicates a decreasing perovskite content. Metallic Co and La2O3 phases increased as the Co content in the fresh perovskite increased, increasing coke deposition. As the Co content increased, the process shifts from POM with oxygen replenishment (LSF) to cracking followed by reverse-Boudouard reaction (LSC).

Experimental and kinetic studies of the advantages of coke accumulation over Beta and Mordenite catalysts according to the pore mouth catalysis hypothesis

Coke formation inside heterogeneous reactors is an important industrial problem that leads to reduced catalyst efficiency. However, this study aims to prove the benefits of coke build-up in improving catalyst performance. The formation and decomposition of coke on six different zeolite structures was studied. The dissociation kinetic model of the spent catalysts during the toluene alkylation with 1-heptene inside a stainless-steel autoclave reactor at different temperatures was carried out. Various techniques (XRD, XRF, TPO, CHNS and TGA-DTG) were used. It was found that the conversion and selectivity of the desired product were higher on the parent H-mordenite and the dealuminated H-beta catalysts with conversions of 85.3% and 84.67%, respectively, at a 360 min reaction time. This was attributed to the reduction of the ratio of hard:soft coke. It is confirmed that the decomposition activation energies of hard coke, 140.1–202.6 kJ/mol, are much higher energies than those of soft coke, 89.9–118.7 kJ/mol. It is also noted that the hypothesis of pore mouth catalysis is dominated by non-polyaromatic coke on the surface of the H-beta catalysts, while the hypothesis is dominated by polyaromatic coke on the surface of the H-mordenite catalysts.

Anti-coking performance of Al/Si/Cr/Ce ceramic coating during naphtha steam cracking applied on Cr25Ni35Nb alloy

To reduce the coke formation, a novel Al/Si/Cr/Ce composite ceramic coating was prepared on the surface of the Cr25Ni35Nb alloy substrate by pack cementation. The microstructure, phase composition, surface morphology and element distribution of substrate and coating were characterized by X-ray diffractometer (XRD), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS). The results reveal that the outer layer of the coating forms a protective layer with a high proportion of AlN and Cr3Si and trace amounts of Ce. The inter-diffusion layer is mainly aluminide coating (AlNi and AlFe) and transition layer contains a small amount of AlN. The anti-coking performance of the coating was assessed using naphtha steam cracking. To study coking behavior, the morphology and microstructure of the coke layer were analyzed and characterized by SEM and Laser Micro-Raman Spectrometer. The coke layer on uncoated sample has a higher focal density and is more likely to spall and peel off when subjected to coking experiment. A large number of filamentous and granular cokes appear on the surface of the uncoated sample, whereas only less granular cokes appear on the surface of the coated sample, and the coke on the uncoated sample has a more disordered and amorphous carbon structure. The coating significantly inhibited the growth of filamentous coke and reduced coke accumulation.

1-Butanol dehydration and oxidation over vanadium phosphate catalysts

The transformation of 1-butanol into either butenes or maleic anhydride was carried out both with and without oxygen, using V/P/O catalysts. With vanadyl pyrophosphate prepared by coprecipitation, at temperature lower than 240 °C and without oxygen, selectivity to butenes was higher than 90%, but a slow deactivation took place. At temperature higher than 300 °C and in the presence of air, maleic and phthalic anhydrides were the prevailing products, with selectivity of 60% and 14%, respectively. Catalytic performance was affected by crystallinity and acidity. αI-VOPO4 showed a poor performance in the absence of air, with a quick deactivation due to coke accumulation; but it displayed an excellent selectivity to butenes (close to 98%) at temperatures lower than 320 °C in the presence of air, with stable performance. At temperature higher than 360 °C, α I-VOPO4 was reduced to vanadyl pyrophosphate and catalyzed the direct oxidation of 1-butanol into maleic anhydride, but with 35% selectivity.

Studies on polyoxymethylene dimethyl ethers production from dimethoxymethane and 1,3,5-trioxane over [formula omitted

Polyoxymethylene dimethyl ethers (OMEs) with physical properties similar to those of diesel has received significant attention as green additives for soot emission suppression. Herein, series of SO42-/ZrO2–TiO2 catalysts were developed for OMEs production from dimethoxymethane (DMM) and 1,3,5-trioxane through sequential formaldehyde monomer insertion into CO bond of DMM. Not Lewis but Brønsted acid sites were identified to be active for the decomposition of 1,3,5-trioxane into formaldehyde unit, however, both of them are effective for the chain propagation of DMM via formaldehyde unit insertion into CO bond. Kinetic studies indicated each chain growth step exhibited the same parameters and activation barrier on corresponding Brønsted and Lewis acid sites due to the same reaction mechanism and very similar chemical structure of OMEs. Also, the catalytic stability investigation suggested the deactivation behavior was derived from the carbon deposition, and the decay factor could be exponentially correlated with the amount of coke accumulation.

Inherently separated syngas production from plastic waste fast pyrolysis integrated with volatile chemical looping conversion with CO2 splitting

To convert plastic waste into high-value products coupled with CO2 utilization, this study proposed a new concept to produce inherently separated syngas through fast pyrolysis integrated with volatile chemical looping CO2 splitting. Three conversion modes, i.e., redox, cracking and redox-cracking mixed modes, were evaluated using different catalyst, and found that cracking mode with Ni/Al2O3 or Ni/MgAl2O4 exhibited better fuel conversion and syngas separation performance than redox and mixed modes (using Ca2Fe2O5 and Ni/Ca2Fe2O5, respectively), achieving nearly full CO-H2 separation from the syngas product. Focusing on the cracking mode, higher temperature facilitated the fuel and coke conversion, due to the endothermic nature of both reaction stages. The syngas separation efficiency increased during 5 cycles and stabilized ∼95% while using Ni/MgAl2O4 catalyst. The redox between Ni0 and Ni2+ was inevitable for both cracking catalysts during multiple cycles due to the Ni-support interaction, limiting the full separation of syngas. The accumulation of low-reactive coke during multiple cycles was another important consideration. Ni/MgAl2O4 possessed weaker Ni-support interaction and less coke accumulation than Ni/Al2O3, thus performed better syngas separation efficiency. Therefore, it is crucial to minimize Ni-support interaction and the generation of high-graphitic coke for optimization.

Distinct coking depth in steam reforming of oxygen-containing organics and hydrocarbons

In steam reforming of organics in a fixed-bed reactor, catalyst particles in varied location of catalyst bed will experience different history of contacting with reactants/products. This may affect accumulation of coke in varied section of catalyst bed, which are investigated in steam reforming of some typical oxygen-containing organics (acetic acid, acetone and ethanol) and hydrocarbons (n-hexane and toluene) in a fixed-bed reactor with double layers of catalyst bed for investigating coking depth at 650 °C over Ni/KIT-6 catalyst in this study. The results indicated that the intermediates derived from the oxygen-containing organics in steam reforming could hardly penetrate the upper-layer catalyst to form coke in the lower-layer catalyst. In converse, they reacted quickly over the upper-layer catalyst via gasification or coking, forming coke almost exclusively in the upper-layer catalyst. The hydrocarbon intermediates from the dissociation of hexane or toluene could easily penetrate and reach the lower-layer catalyst to form even more coke therein than the upper-layer catalyst. The characterization showed that the insufficient gasification of *CxHy species led to their aggregation/integration to form more aromatic coke, especially from n-hexane. The aromatic-ring containing intermediates from toluene tended to integrate with *OH species to form ketones that further involved in coking, forming coke of less aromatic nature than that from n-hexane. Steam reforming of oxygen-containing organics also produced oxygen-containing intermediates and coke of higher aliphatic nature, lower carbon to hydrogen (C/H) ratio, lower crystallinity and thermal stability.

Effect of air introduction on filamentous coke during CO2 reforming of tar with core-shell catalysts

The coke accumulation is the main factor affecting the activity of nickel-based catalysts during the CO2 reforming of tar. In this work, toluene is chosen to study the influence of filamentous coke on the coke-forming mechanism of the Ni/La2O3 @SiO2 catalyst. Two methods are proposed to address the problem of reduced tar conversion of Ni/La2O3 @SiO2 due to coke deposition. The Ni/La2O3 @SiO2 is first modified with cobalt doping to improve the resistance to coke accumulation. The Ni8Co/La2O3 @SiO2 catalyst showed higher carbon conversion (50–75%) and hydrogen conversion (35–55%) than Ni/La2O3 @SiO2 within the 5 h tar reforming process. And the used Ni8Co/La2O3 @SiO2 catalysts had only 0.1 g/g of filamentous coke after reforming reaction. Next, air is introduced to oxidize the deposited coke to address the problem of coke accumulation affecting catalyst activity. An appropriate air flow rate could provide oxidation of the coke and prolong the reaction activity of the catalyst from 5 h to 10 h.

Influence of the textural characteristics and the preparation conditions of the support on coking resistance and performance of Ni/MgAl2O4 catalysts

This study aimed at establishing the influence of the textural properties, interparticle pores in particular, of the support in Ni/MgAl2O4 catalyst on other physicochemical properties and on coke formation during partial oxidation of methane. Ni catalysts were prepared over four different MgAl2O4 supports with different surface area and pore characteristics to establish their impact. Mesoporous MgAl2O4 supports were prepared by modified sol-gel and co-precipitation methods, and were compared with a commercial nano-powder counterpart. The catalysts were characterized by various techniques including powder XRD, XRF, N2 sorption, TEM, CO2-TPD, H2-TPR, DRIFTS, TGA, and Raman spectroscopy. The catalysts over the sol-gel prepared supports showed CH4 conversion around 89%, H2 selectivity close to 100%, H2/CO ratio ∼2.05, and negligible carbon deposits. While the catalyst over the support prepared by coprecipitation showed comparable conversion and products selectivity, it showed a slight decrease in conversion that was referred to the formation of a small amount of carbon deposit. On the other hand, the catalyst based on the commercial MgAl2O4 nano-powder showed conversion ∼84%, H2/CO ratio of 2.2, and large amount of coke deposit that lead to unstable conversion and gradual deactivation. The significantly enhanced coking resistance of the catalysts based on the prepared supports was referred to their larger volume of wider mesopores and their higher density of basic sites. On the other hand, the considerable and rapid coke formation over commercial support-based catalyst was referred to the narrow pores as well as lower pore volume, in addition to the lower density of basic sites, of its support. Narrow pores are expected to get rapidly filled with carbonaceous species blocking some active sites, hindering diffusion of products as well as O2 and CO2 access, and limiting oxidation and removal of these species as they form. The results indicate that the dominance of wide interparticle mesopores (>5 nm) of the support are essential to avoid coke accumulation.