High-purity hydrogen production by sorption-enhanced methanol steam reforming over a combination of Cu–Zn–CeO2–ZrO2/MCM-41 catalyst and (Li–Na–K) NO3·MgO adsorbent

In this study, sorption-enhanced methanol steam reforming (SEMSR) was applied to generate high-purity hydrogen. The mesoporous MCM-41 as support and CuO, ZnO, CeO₂, ZrO₂ as active agents and promoters were employed for the catalyst preparation. In addition, (Li–Na–K) NO₃·MgO as a CO₂ adsorbent was prepared by the wet mixing method. The fresh and used catalysts were characterized by XRD, BET, FTIR, FESEM, TEM, H₂-TPR and TGA analyses. Also, the CO₂ sorbent was studied by XRD, BET, FESEM, TEM and TGA analyses before and after the reaction. The SEMSR performances of the synthesized catalyst and adsorbent were evaluated experimentally in a fixed-bed reactor. The effect of various conditions such as temperature, WHSV, feed molar ratio and sorbent/catalyst ratio were investigated. The best results were obtained at 300 °C, a feed molar ratio (water/methanol) of 2:1, a WHSV of 1.62 h^?1, and the sorbent/catalyst ratio of 8:1, which produced 99.8% hydrogen, 25% more than the hydrogen production during conventional methanol steam reforming. Moreover, the cyclic stability of the catalyst and the sorbent was studied for 10 cycles.     

The operation types and operation window for high-purity hydrogen production for the sorption enhanced steam methane reforming in a fixed-bed reactor

The operation types and operation window for high-purity H₂ production for the sorption enhanced steam methane reforming (SE-SMR) with Ni/Al₂O₃ catalyst and CaO sorbent in a fixed-bed reactor are investigated by an experimentally verified 2D numerical method. Four chemical reactions including steam reforming, water gas shift, global steam reforming, and CO₂ sorption are considered. The operation window is defined as the H₂ and CO molar fractions at outlet satisfying both y_H2,out ≥ 90% and y_CO,out ≤ y_CO,allow (= 1%, 2% or 3%) in dry base. Under the conditions of y_H2,out and y_CO,allow, there are six operation types, of which 2 types are within the operation window and 4 types are not within the operation window as the temperature, weight hourly space velocity (WHSV) and steam to methane (S/C) molar ratio vary. For a common case of S/C = 3, the operation windows for y_CO,allow = 3% at WHSV = 8.5 h^?1 and 42.5 h^?1 are located at 570–670 °C and 640–690 °C respectively, based on the parameters in this work. The operation window of temperature is wider with decreasing WHSV, and it becomes wider remarkably as the S/C ratio increases. The lowest temperature inside the operation window is 550 °C. The effects of the temperature, WHSV and S/C ratio on the operating types, y_H2,out and y_CO,out are also presented and discussed in details.     

Dry reforming of methane over Ni/MgO–Al2O3 catalysts: Thermodynamic equilibrium analysis and experimental application

In this study, dry reforming of methane (DRM) employing a Ni/MgO–Al₂O₃ catalyst was undertaken to evaluate the effects of temperature (650, 700 and 750 °C), weight hourly space velocity (7.5, 15 and 30 L h⁻¹ g_cat⁻¹) and catalyst MgO content (3, 5 and 10 wt%) on catalytic activity and coke-resistance. The catalysts were prepared by the wet impregnation method and were characterized by wavelength dispersive X-ray fluorescence (XRF), N₂ physisorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR-H₂), temperature-programmed desorption (TPD-NH₃), H₂ chemisorption, thermogravimetric/derivative thermogravimetry analysis (TG/DTG) and scanning electron microscopy (SEM). The best conversions of methane (CH₄) and carbon dioxide (CO₂) and lower coke formation were obtained using higher temperatures, lower WHSV and 5 wt% MgO in the catalyst. The H₂/CO molar ratios obtained were within the expected range for the DRM reaction. The experimental yields of H₂ and CO differed from chemical equilibrium, mainly due to occurrence of the reverse water-gas shift reaction. Thermodynamic analysis of the reaction system, based on minimization of the Gibbs free energy, was performed in order to compare the experimental results with the optimal values for chemical equilibrium conditions, which has indicated that the DRM reaction was favored by higher temperature, lower pressure, and lower CH₄/CO₂ molar ratio.     

A novel catalyst–sorbent system for an efficient H2 production with in-situ CO2 capture

This paper presents an experimental investigation for an improved process of sorption-enhanced steam reforming of methane in an admixture fixed bed reactor. A highly active Rh/Ce_αZr_1−αO₂ catalyst and K₂CO₃-promoted hydrotalcite are utilized as novel catalyst/sorbent materials for an efficient H₂ production with in situ CO₂ capture at low temperature (450–500 °C). The process performance is demonstrated in response to temperature (400–500 °C), pressure (1.5–6.0 bar), and steam/carbon ratio (3–6). Thus, direct production of high H₂ purity and fuel conversion >99% is achieved with low level of carbon oxides impurities (<100 ppm). A maximum enhancement of 162% in CH₄ conversion is obtained at a temperature of 450 °C and a pressure of 6 bar using a steam/carbon molar ratio of 4. The high catalyst activity of Rh yields an enhanced CH₄ conversion using much lower catalyst/sorbent bed composition and much smaller reactor size than Ni-based sorption enhanced processes at low temperature. The cyclic stability of the process is demonstrated over a series of 30 sorption/desorption cycles. The sorbent exhibited a stable performance in terms of the CO₂ working sorption capacity and the corresponding CH₄ conversion obtained in the sorption enhanced process. The process showed a good thermal stability in the temperature range of 400–500 °C. The effects of the sorbent regeneration time and the purge stream humidity on the achieved CH₄ conversion are also studied. Using steam purge is beneficial for high degree of CO₂ recovery from the sorbent.     

Catalytic steam reforming of bio-oil aqueous fraction for hydrogen production over Ni–Mo supported on modified sepiolite catalysts

Hydrogen will be an important energy carrier in the future and hydrogen production has drawn a great deal of attention to its advantages in efficiency and environmental benefit. Catalytic steam reforming in this study was carried out in a fixed bed tubular reactor with sepiolite catalysts. Sepiolite catalysts modified with nickel (Ni) and molybdenum (Mo) were prepared using the precipitation method. Influential parameters such as temperature, catalyst, steam to carbon ratio (S/C), the feeding space velocity (WHSV), reforming length, and activity of catalyst were investigated and the yields of H₂, CO, CH₄, and CO₂ were obtained. The result of this experiment shows that the acidified sepiolite catalyst with addition of the Ni and Mo greatly improves the activities of catalyst and effectively increases the yield of hydrogen. The favorable reaction condition is as follows: reaction temperature is 700–800 °C; S/C is 16–18; the feeding space velocity is 1.5–2.2 h⁻¹, respectively.     

Si-MCM-41 obtained from different sources of silica and its application as support for nickel catalysts used in dry reforming of methane

Si-MCM-41 molecular sieves are attractive for use as catalytic supports in reforming processes, requiring the development of catalysts that combine low cost, high activity and resistance to coking for viable conversion of biogas (CH₄ + CO₂) into higher added value products such as synthesis gas (H₂ + CO). In this work was synthesized Si-MCM-41 from a waste material (rice husk ash - RHA) and compared with Si-MCM-41 synthesized from a commercial silica source (tetraethylorthosilicate - TEOS). Both were evaluated as catalytic support in dry reforming of methane (DRM). Calcined Si-MCM-41 supports were wet impregnated with 10, 20 and 50% of nickel. DRM reactions were performed in a continuous-flow tubular reactor using a 1:1 CH₄:CO₂ molar mixture, at 700 and 800 °C, and WHSV of 30 L.h⁻¹g_cat⁻¹. The results confirmed that the Si-MCM-41 structure was successfully synthesized by the different methods. The best DRM results were obtained with the 20%Ni/Si-MCM-41_TEOS catalyst.     

An experimental and theoretical approach for the biogas steam reforming reaction

An experimental and theoretical study for the biogas steam reforming reaction over 5%Ru/Al₂O₃ catalyst have been performed. An apparatus was constructed for the conduction of the experiments, the core of which was a tube reactor, filled with the catalyst in form of pellets. The inlet gas mixture consisted of CH₄ and CO₂ in various composition ratios as a model biogas and steam. A theoretical model of the process was developed. The experimental reactor was modelled as an isothermal pseudo homogeneous fixed bed reactor. Internal and external transport phenomena were neglected and appropriate effectiveness factors were employed instead. A physical properties model was used for the calculation of the physicochemical properties of the real mixture. Five reactant species, CH₄, CO₂, H₂O, CO and H₂, were included in the model, whereas the feed consisted of the first three. Steam reforming and water gas shift were the main reactions. Experimental results and theoretical predictions match closely, stability of the catalyst was assured and an optimal operational window was identified, at GHSV = 10,000–20,000 h⁻¹, T = 700–800 °C, CH₄/CO₂ = 1.0–1.5 and H₂O/CH₄ = 3.0–5.0.     

Hydrogen by glycerol steam reforming on a nickel–alumina catalyst: Deactivation processes and regeneration

Hydrogen energy has attracted considerable attention because of its efficiency and environmental benefits, and the increasing demand requires finding renewable sources of raw materials to produce it. Glycerol, by-product of biodiesel production and coming from renewable raw materials, could be a bio-renewable substrate to produce hydrogen. The glycerol steam reforming to obtain hydrogen was evaluated using a 5.1 wt% Ni impregnated on Al₂O₃ catalyst, characterized by nitrogen adsorption, XRD, and FTIR. Deactivation processes were analyzed in successive cycles of reaction at 700 °C, atmospheric pressure, 5 h⁻¹ WHSV, and 3:1 water:glycerol molar ratio, during 12 h. Between reaction cycles, regenerating took place using a He/Air stream. Hydrogen was the main product on the fresh catalyst, following by CO and CH₄; during reaction, carbonaceous deposits deactivated catalyst, decreasing H₂ and increasing both CO and CH₄. Carbonaceous deposits were characterized by TPO, showing a main peak centered at 690 °C; the carbon content reached 11.9%.     

Improvement of steam methane reforming via in-situ CO2 sorption over a nickel-calcium composite catalyst

Optimization of steam methane reforming (SMR) reaction by CO₂ sorption enhancement was investigated. In this study, the sorption-enhanced steam methane reforming reaction (SESMR) was conducted to maximize hydrogen production via suitable adjustments in the operating conditions of the reaction, which include the molar ratio of steam to CH₄, space velocity, and temperature. The reforming catalysts were prepared by a physical mixture of 20 wt% Ni/Al₂O₃ and CaO. The results reveal that there are significant differences in CH₄ conversion between the SMR and the SESMR from 18% to 108%; this conversion strongly depended on the reaction conditions. High-purity H₂ products (98.9%) with <0.1 ppmv CO were obtained by SESMR under the suitable conditions of 2600 cm³/g/h, steam/CH₄ molar ratio of 4 and 823 K. This implies that the high-quality H₂ produced through the SESMR process could be directly used for the proton-exchange membrane fuel cell.     

Combined pre-reformer/reformer system utilizing monolith catalysts for hydrogen production

The pre-reforming of higher hydrocarbon, propane, was performed to generate hydrogen from LPG without carbon deposition on the catalysts. A Ru/Ni/MgAl₂O₄ metallic monolith catalyst was employed to minimize the pressure drop over the catalyst bed. The propane pre-reforming reaction conditions for the complete conversion of propane with no carbon formation were identified to be the following: space velocities over 2400 h⁻¹ and temperatures between 400 and 450 °C with a H₂O/C₁ ratio of 3. The combined pre-reformer and the main reformer system with the Ru/Ni/MgAl₂O₄ metallic monolith catalyst was employed to test the conversion propane to syngas where the reaction heat was provided by catalytic combustors. Propane was converted in the pre-reformer to 52.5% H₂, 27.0% CH₄, 17.5% CO, and 3.0% CO₂ with a 331 °C inlet temperature and a 482 °C catalyst outlet temperature. The main steam reforming reactor converted the methane from the pre-reformer with a conversion of higher than 99.0% with a 366 °C inlet temperature and an 824 °C catalyst outlet temperature. With a total of 912 cc of the Ru/Ni/MgAl₂O₄ metallic monolith catalyst in the main reformer, the H₂ production from the propane reached an average of 3.25 Nm³h⁻¹ when the propane was fed at 0.4 Nm³h⁻¹.     

Influence of catalyst and temperature on gasification performance of pig compost for hydrogen-rich gas production

The catalytic steam gasification of pig compost (PC) for hydrogen-rich gas production was conducted in a fixed-bed reactor. The influence of the catalyst and reactor temperature on yield and product composition was studied at the temperature range of 700–850 °C, for weight hourly space velocity (WHSV) in the range of 0.30–0.60 h⁻¹. The results indicate that the developed NiO on modified dolomite (NiO/MD) catalyst reveals better catalytic performance on the tar elimination and hydrogen yield than calcined MD or NiO/γ-Al₂O₃ catalyst. Meanwhile, the lower WHSV and higher reactor temperature can contribute to more hydrogen production and gas yield. Moreover, the char from catalytic steam gasification of PC has a highest ash content of 75.84% at 850 °C. In conclusion, pig compost is a potential candidate for hydrogen gas production through catalytic steam gasification technology.     

Biogas reforming for hydrogen production over a Ni–Co bimetallic catalyst: Effect of operating conditions

A Ni–Co bimetallic catalyst, Ni–Co/La₂O₃/Al₂O₃, was prepared by conventional incipient wetness impregnation. It shows a high level of activity and excellent stability for biogas reforming. This work examines how operating conditions, such as the reaction temperature, operating pressure, feed ratio, gas hourly space velocity (GHSV), and CO₂ excessive coefficient, affect the catalytic performances of the catalyst. The experimental biogas is simulated with CH₄ and CO₂ at a molar ratio of 1, without any dilute gas. The catalyst was also characterized by XRD, BET, TEM and TG-DSC. In a stability test of 510 h under the conditions of 800 °C, 1 atm, and a GHSV of 6000 ml g_cat⁻¹ h⁻¹, the average coking rate over the catalyst was only about 0.0374 mg g_cat⁻¹ h⁻¹. The experimental results also indicate that the dynamic equilibrium between the deposition and gasification of carbon deposited on the surface of the catalyst can be established during the reaction. The aggregation of metallic Ni/Co and the formation of filamentous carbon over the surface of the catalyst can be inhibited effectively. During the last 50 h of the 510 h stability test, the average conversion of CH₄ and CO₂, the selectivity to H₂ and CO, and ratio of H₂/CO were 95.2%, 96.7%, 95.0%, 98.3%, and 0.96, respectively.     

Tri-reforming of methane over Ni@SiO2 catalyst

A nickel-silica core@shell catalyst was applied for a methane tri-reforming process in a fixed-bed reactor. To determine the optimal condition of the tri-reforming process for production of syngas appropriate for methanol synthesis the effect of reaction temperature (550–750 °C), CH₄:H₂O molar ratio (1:0–3.0) and CH₄:O₂ molar ratio (1:0–0.5) in the feedstock was investigated. CH₄ conversion rate and H₂/CO ratio in the produced syngas were influenced by the feedstock composition. Increasing the amount of steam above the proportion of CH₄:H₂O 1:0.5 reduced the H₂:CO molar ratio in produced syngas to ∼1.5. Increasing oxygen partial pressure improved methane conversion to 90% at 750 °C. At low ∼550 °C reaction temperature the tri-reforming process was not effective with low hydrogen production (H₂ yield ∼20%) and very low <5% CO₂ conversion. Increasing reaction temperature increased hydrogen yield to ∼85% at 750 °C. From all the tested reaction conditions the optimal for tri-reforming over the 11%Ni@SiO₂ catalyst was: feed composition with molar ratio CH₄:CO₂:H₂O:O₂:He 1:0.5:0.5:0.1:0.4 at T = 750 °C. The results were explained in the context of characterisation of the catalysts used. The obtained results showed that the tri-reforming process can be applied for production of syngas with composition suitable for methanol synthesis.     

Sorbent enhanced hydrogen production from steam gasification of coal integrated with CO2 capture

In this work, CO₂ capture and H₂ production during the steam gasification of coal integrated with CO₂ capture sorbent were investigated using a horizontal fixed bed reactor at atmospheric pressure. Four different temperatures (650, 675, 700, and 750 °C) and three sorbent-to-carbon ratios ([Ca]/[C] = 0, 1, 2) were studied. In the absence of sorbent, the maximum molar fraction of H₂ (64.6%) and conversion of coal (71.3%) were exhibited at the highest temperature (750 °C). The experimental results verified that the presence of sorbent in the steam gasification of coal enhanced the molar fraction of H₂ to more than 80%, with almost all CO₂ was fixed into the sorbent structure, and carbon monoxide (CO) was converted to H₂ and CO₂ through the water gas shift reaction. The steam gasification of coal integrated with CO₂ capture largely depended on the reaction temperature and exhibited optimal conditions at 675 °C. The maximum molar fraction of H₂ (81.7%) and minimum CO₂ concentration (almost 0%) were obtained at 675 °C and a sorbent-to-carbon ratio of 2.     

Hydrogen production by glycerol steam-reforming over nickel and nickel-cobalt impregnated on alumina

Hydrogen is a clean energy carrier, and its utilization will reduce environmental problems related to fossil fuels one. Biomass is an inexhaustible renewable source to generate biocompounds. Glycerol, obtained from a crescent biodiesel industry, is an abundant bio-substrate to produce hydrogen. The steam reforming of glycerol was studied employing 4Ni/Al₂O₃, 4Co–4Ni/Al₂O₃, and 12Co–4Ni/Al₂O₃ catalysts at 300, 500, and 700 °C, 1 atm, 10 h⁻¹ WHSV, 6:1 water:glycerol molar ratio (WGMR), 0.17 ml min⁻¹ glycerol solution feed flow rate and time-on-stream 8 h. The main product obtained was H₂, followed by CO₂, CO, and CH₄ in smaller proportion. Co promotes H₂ production and unfavors CO₂ generation when temperature decreases; CH₄ formation is observed at higher temperature. A low Co loading produces the largest H₂ and CO₂ amounts at the lowest temperature. A high Co loading improves H₂ production at lower temperature, but this does not occur at high temperature.     

Hydrogen rich fuel gas production by gasification of wet biomass using a CO2 sorbent

Hydrogen rich fuel gas production by gasification of wet biomass accompanied by CO₂ absorption is proposed. The paper addressed this topic, and experiments were conducted to investigate the effects of the moisture content (M), the molar ratio of Ca(OH)₂ to carbon in the biomass ([Ca]/[C]) and the reactor temperature (T) on hydrogen production and CO₂ absorption by CaO. Measurement of the calcium compounds in solid residues was carried out with XRD and SEM. The results show that directly gasifying of wet biomass not only favors hydrogen production but also promotes CO₂ absorption by CaO. For the experiment with wet biomass (M = 0.90), the H₂ yield is increased by 51.5% while the CO₂ content is decreased by 28.4% than that for experiments with dry biomass (M = 0.09). CaO plays the dual role of catalyst and sorbent. It is noteworthy that CaO reveals a stronger effect on the water gas shift reaction than on the steam reforming of methane. The increase of the reactor temperature contributes to produce more H₂, but goes against CO₂ absorption by CaO. XRD spectrum and SEM image of the solid residues further confirmed that high temperature is unfavorable to CO₂ absorption by CaO. For the new method, the optimal operating temperature is in the 923–973 K range.     

Operation of Rh/Ce0.75Zr0.25O2-δ-ƞ-Al2O3/FeCrAl wire mesh honeycomb catalytic modules in diesel steam and autothermal reforming

The Rh/Ce_0·75Zr_0·25O_2–δ-ƞ-Al₂O₃/FeCrAl structured catalytic blocks of length 10, 20, and 60 mm were prepared and tested in the reactions of steam and autothermal reforming of n-hexadecane. It was found in a series of experiments on hexadecane steam reforming with the catalyst heating solely through the reactor wall that the complete conversion of hexadecane at a furnace temperature below 750 °C was not achieved even at GHSV = 10,000 h⁻¹. Under these conditions, the formation of carbon on the catalyst surface was observed. At the reactor wall temperature of 800 °C, the complete conversion of hexadecane was achieved even in the 10 mm long catalytic block (GHSV = 60,000 h⁻¹), accompanied by the formation of various intermediate light hydrocarbons. To achieve complete conversion of these intermediate compounds (mainly 1-alkenes), it is necessary to carry out the steam reforming reaction at GHSV = 10,000 h⁻¹. At hexadecane autothermal reforming, heat is supplied to the reaction zone by exothermic oxidation reaction, which makes this process more efficient. In experiments with the use of additional external heat supply through the reactor wall, complete conversion of hexadecane occurred at GHSV = 120,000 h⁻¹. To convert all by-products (mainly 1-alkenes) and achieve a nearly thermodynamic equilibrium distribution of the main reaction products (H₂, CO, CO₂), the reaction should be carried out at GHSV = 20,000 h⁻¹. Without external heat supply, hexadecane conversion decreased, while the content of light hydrocarbons in the reaction products increased. An increase in the inlet amount of oxygen helps to compensate the heat losses in the reactor and to increase the efficiency of hexadecane autothermal reforming. The performed experiments allow better understanding of the processes which occur during the steam and autothermal reforming of diesel.     

Transient reaction phenomena of sorption-enhanced steam methane reforming in a fixed-bed reactor

The transient chemical reaction phenomena of the sorption-enhanced steam methane reforming (SE-SMR) by using Ni/Al₂O₃ catalyst and CaO sorbent in a tubular fixed-bed reactor were numerically investigated by an experimentally verified unsteady 2D model. Four chemical reactions are involved in SE-SMR including steam reforming (SR), water gas shift (WGS), global steam reforming (GSR), and CO₂ sorption. The reaction process in time is divided into period 1, transient period, and period 2. The high-purity H₂ is produced in period 1 which is defined as the outlet molar fractions of H₂ ≥ 90% and CO ≤ 1% (dry basis) in this work. In the first half of period 1, the endothermic reaction rates of SR and GSR are dominant in the entrance region of catalyst/sorbent bed. The WGS and CO₂ sorption reactions are triggered by SR and GSR reactions. The heat transfer from the wall plays an important role. Higher CaO conversion, temperature, and reaction rates appear first near the wall region, then they gradually expand to the central region.In the second half of period 1, a sharp wave-shaped curve of strong CO₂ sorption reaction occurred in downstream becomes dominant and it moves to downstream almost at a constant speed, as time progresses. The peak value of the CO₂ sorption reaction is more than twice larger than that of SR or WGS. The SR and WGS reaction rates are significantly enhanced by CO₂ sorption reaction. The great sorption, WGS, and SR reactions result in a high-purity H₂ production with the outlet molar fractions of 95.8% H₂, 0.998% CO, and 0.73% CO₂ at the end of period 1, based on the parameters used in this work such as reactor temperature of 600 °C. The maximum CaO conversion is about 76% in end of period 1 and the average CaO conversion in the reactor is 51%. The 2D distributions of CaO conversion, temperature, and reaction rates are also presented and discussed.     

Metal foam-supported Pd–Rh catalyst for steam methane reforming and its application to SOFC fuel processing

Pd–Rh/metal foam catalyst was studied for steam methane reforming and application to SOFC fuel processing. Performance of 0.068 wt% Pd–Rh/metal foam catalyst was compared with 13 wt% Ni/Al₂O₃ and 8 wt% Ru/Al₂O₃ catalysts in a tubular reactor. At 1023 K with GHSV 2000 h⁻¹ and S/C ratio 2.5, CH₄ conversion and H₂ yield were 96.7% and 3.16 mol per mole of CH₄ input for Pd–Rh/metal foam, better than the alumina-supported catalysts. In 200 h stability test, Pd–Rh/metal foam catalyst exhibited steady activity. Pd–Rh/metal foam catalyst performed efficiently in a heat exchanger platform reactor to be used as prototype SOFC fuel processor: at 983 K with GHSV 1200 h⁻¹ and S/C ratio 2.5, CH₄ conversion was nearly the same as that in the tubular reactor, except for more H₂ and CO₂ yields. Used Pd–Rh/metal foam catalyst was characterized by SEM, TEM, BET and CO chemisorption measurements, which provided evidence for thermal stability of the catalyst.     

Response surface optimization of syngas production from greenhouse gases via DRM over high performance Ni–W catalyst

The process parameters for dry reforming of methane (DRM) over Ni–W/Al₂O₃–MgO catalyst are optimized using response surface methodology (RSM). The Ni–W bimetallic catalyst is synthesized by co-precipitation method followed by impregnation. The catalysts are characterized by BET, XRD, FESEM, EDX and TEM; to study physicochemical properties, morphology, composition, crystallite size and deposited carbon. The effect of process parameters, i.e., reaction temperature (600^oC–800 °C) and feed gas ratio (0.5–1.5) on the CH₄, CO₂ conversions and syngas ratio are studied. A temperature of 777.29 °C with CH₄: CO₂ of 1.11 at GHSV of 36,000 cm³gm.cat^?1h^?1, delivered the CH₄ and CO₂ conversions of 87.6% and 93.3%, respectively along with H₂:CO of 1. The predicted process parameters were verified through actual experimental analysis at the optimized conditions, and results agreed with CCD of the RSM model with insignificant error. The MWCNT formed during DRM avoided catalyst deactivation and delivered stable performance over 12 h of reaction test at the optimized conditions.