Published
2025-10-10
Issue
Section
Original Research Article
License
Copyright (c) 2025 Ali Khalid Mohsen*, Tahseen A. Al-Hattab

This work is licensed under a Creative Commons Attribution 4.0 International License.
The Author(s) warrant that permission to publish the article has not been previously assigned elsewhere.
Author(s) shall retain the copyright of their work and grant the Journal/Publisher right for the first publication with the work simultaneously licensed under:
OA - Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0). This license allows for the copying, distribution and transmission of the work, provided the correct attribution of the original creator is stated. Adaptation and remixing are also permitted.

This license intends to facilitate free access to, as well as the unrestricted reuse of, original works of all types for non-commercial purposes.
How to Cite
A novel hybrid reforming reactor for enhanced CO₂ conversion and hydrogen production: A CFD analysis
Ali Khalid Mohsen
University of Babylon, College of Engineering, Chemical Engineering department, Bail, Hilla, 51001, Iraq
Tahseen A. Al-Hattab
University of Babylon, College of Engineering, Chemical Engineering department, Bail, Hilla, 51001, Iraq
DOI: https://doi.org/10.59429/ace.v8i4.5761
Keywords: Methane reforming; H2 production; Pd-Ru membrane; carbonate dual-phase membrane; CO2 utilization
Abstract
The use of hydrogen as an energy carrier has gained significant attention due to its environmentally friendly characteristics. Among various production methods, steam reforming of natural gas (CH₄) remains the most cost-effective and widely adopted technique. To enhance the efficiency and carbon utilization of this process, a novel hybrid steam and dry reforming reactor has been proposed, which utilizes the CO₂ produced from steam reforming within a dry reforming zone.
In this study, a two-dimensional axisymmetric hybrid catalytic membrane reactor (CMR) model was developed for the production of pure hydrogen from natural gas, employing a Pd–Ru metallic membrane and a carbonate dual-phase membrane, integrated with Ni/Al₂O₃ and Rh/Al₂O₃ catalysts. A computational fluid dynamics (CFD) approach was employed to investigate the reactor’s performance in terms of methane conversion and hydrogen production under various operating conditions. These include reaction temperatures of 700, 800, 900, and 1000 K, a gas hourly space velocity (GHSV) of 1000 h⁻¹, and a sweep gas Reynolds number (Re) of 100.
Simulation results revealed that the CMR achieved a high hydrogen permeation rate on the permeate (tube) side, along with a maximum CH₄ conversion of approximately 99.9% at 1000 K on the retentate side within the steam reforming zone. Furthermore, the reactor demonstrated effective syngas production with near-complete CO₂ reduction on the dry reforming side, where CO₂ concentrations at the reactor outlet approached zero at 1000 K. These findings highlight the promising potential of the hybrid combined membrane reactor (CMR) system for efficient hydrogen production and near-complete carbon utilization.
References
[1]. Saimon, N. N., Jusoh, M., Kamarudin, M. J., Arsad, A., & Zakaria, Z. Y. (2017). Thermodynamic analysis of hydrogen production from methanol-ethanol-glycerol mixture through dry reforming. Chemical Engineering Transactions, 56, 967–972. https://doi.org/10.3303/CET1756162
[2]. Mazloomi, K., & Gomes, C. (2012). Hydrogen as an energy carrier: Prospects and challenges. In Renewable and Sustainable Energy Reviews (Vol. 16, Issue 5, pp. 3024–3033). https://doi.org/10.1016/j.rser.2012.02.028
[3]. Fang, X., Zhang, X., Guo, Y., Chen, M., Liu, W., Xu, X., Peng, H., Gao, Z., Wang, X., & Li, C. (2016). Highly active and stable Ni/Y2Zr2O7 catalysts for methane steam reforming: On the nature and effective preparation method of the pyrochlore support. International Journal of Hydrogen Energy, 41(26), 11141–11153. https://doi.org/10.1016/j.ijhydene.2016.04.038
[4]. Yurdakul, M., Ayas, N., Bizkarra, K., el Doukkali, M., & Cambra, J. F. (2016). Preparation of Ni-based catalysts to produce hydrogen from glycerol by steam reforming process. International Journal of Hydrogen Energy, 41(19), 8084–8091. https://doi.org/10.1016/j.ijhydene.2015.11.178
[5]. Kho, E. T., Scott, J., & Amal, R. (2016). Ni/TiO2 for low temperature steam reforming of methane. Chemical Engineering Science, 140, 161–170. https://doi.org/10.1016/j.ces.2015.10.021
[6]. Yang, X., Da, J., Yu, H., & Wang, H. (2016). Characterization and performance evaluation of Ni-based catalysts with Ce promoter for methane and hydrocarbons steam reforming process. Fuel, 179, 353–361. https://doi.org/10.1016/j.fuel.2016.03.104
[7]. Buelens, L. C., Galvita, V. V., Poelman, H., Detavernier, C., & Marin, G. B. (2016). Super-dry reforming of methane intensifies CO2 utilization via Le Chateliers principle. Science, 354(6311), 449–452. https://doi:10.1126/science.aah7161
[8]. le Saché, E., Pastor-Pérez, L., Watson, D., Sepúlveda-Escribano, A., & Reina, T. R. (2018). Ni stabilised on inorganic complex structures: superior catalysts for chemical CO2 recycling via dry reforming of methane. Applied Catalysis B: Environmental, 236, 458–465. https://doi.org/10.1016/j.apcatb.2018.05.051
[9]. Pappacena, A., Razzaq, R., de Leitenburg, C., Boaro, M., & Trovarelli, A. (2018). The role of neodymium in the optimization of a Ni/CeO2 and Ni/CeZrO2 Methane dry reforming catalyst. Inorganics, 6(2). https://doi.org/10.3390/inorganics6020039
[10]. Littlewood, P., Xie, X., Bernicke, M., Thomas, A., & Schomäcker, R. (2015). Ni0.05Mn0.95O catalysts for the dry reforming of methane. Catalysis Today, 242(Part A), 111–118. https://doi.org/10.1016/j.cattod.2014.07.054
[11]. Chen, L., Gangadharan, P., & Lou, H. H. (2018). Sustainability assessment of combined steam and dry reforming versus tri-reforming of methane for syngas production. Asia-Pacific Journal of Chemical Engineering, 13(2). https://doi.org/10.1002/apj.2168
[12]. Behroozsarand, A., & Pour, A. N. (2014). Modeling of microreactor for methane dry reforming: Comparison of Langmuir-Hinshelwood kinetic and microkinetic models. Journal of Natural Gas Science and Engineering, 20, 99–108. https://doi.org/10.1016/j.jngse.2014.06.011
[13]. Kassi, A. H., & Al-Hattab, T. A. (2024). A CFD model of natural gas steam reforming in a catalytic membrane reactor: Effect of various operating parameters on the performance of CMR. International Journal of Hydrogen Energy, 56, 780–796. https://doi.org/10.1016/j.ijhydene.2023.12.156
[14]. Fedotov, A. S., Antonov, D. O., Uvarov, V. I., & Tsodikov, M. v. (2018). Original hybrid membrane-catalytic reactor for the Co-Production of syngas and ultrapure hydrogen in the processes of dry and steam reforming of methane, ethanol and DME. International Journal of Hydrogen Energy, 43(14), 7046–7054. https://doi.org/10.1016/j.ijhydene.2018.02.060
[15]. Tosti, S., Borgognoni, F., & Santucci, A. (2010). Multi-tube Pd-Ag membrane reactor for pure hydrogen production. International Journal of Hydrogen Energy, 35(20), 11470–11477. https://doi.org/10.1016/j.ijhydene.2010.06.102
[16]. Basile, A., Iulianelli, A., Longo, T., Liguori, S., & de Falco, M. (2011). Pd-based Selective Membrane State-of-the-Art. In Membrane Reactors for Hydrogen Production Processes (pp. 21–55). Springer London. https://doi.org/10.1007/978-0-85729-151-6_2
[17]. Lee, S., & Lim, H. (2020). Utilization of CO2 arising from methane steam reforming reaction: Use of CO2 membrane and heterotic reactors. Journal of Industrial and Engineering Chemistry, 91, 201–212. https://doi.org/10.1016/j.jiec.2020.08.001
[18]. Chen, T., Yu, B., Zhao, Y., Li, Y., & Lin, Y. S. (2017). Carbon dioxide permeation through ceramic-carbonate dual-phase membrane-effects of sulfur dioxide. Journal of Membrane Science, 540, 477–484. https://doi.org/10.1016/j.memsci.2017.06.063
[19]. Richardson, J. T., & Paripatyadar, S. A. (1990). Carbon Dioxide Reforming of Methane with Supported Rhodium. In Applied Catalysis. Elsevier Science Publishers B.V.
[20]. Lee, S., & Lim, H. (2020). The effect of changing the number of membranes in methane carbon dioxide reforming: A CFD study. Journal of Industrial and Engineering Chemistry, 87, 110–119. https://doi.org/10.1016/j.jiec.2020.03.020.
[21]. Lim, Y., Lee, C. J., Jeong, Y. S., Song, I. H., Lee, C. J., & Han, C. (2012). Optimal design and decision for combined steam reforming process with dry methane reforming to reuse CO 2 as a raw material. Industrial and Engineering Chemistry Research, 51(13), 4982–4989. https://doi.org/10.1021/ie200870m
[22]. Xu, J., & Froment, G. F. (1989). Methane steam reforming, methanation and water‐gas shift: I. Intrinsic kinetics. AIChE journal, 35(1), 88-96.
[23]. Anzelmo, B., Wilcox, J., & Liguori, S. (2018). Hydrogen production via natural gas steam reforming in a Pd-Au membrane reactor. Comparison between methane and natural gas steam reforming reactions. Journal of Membrane Science, 568, 113–120. https://doi.org/10.1016/j.memsci.2018.09.054
[24]. Chompupun, T., Limtrakul, S., Vatanatham, T., Kanhari, C., & Ramachandran, P. A. (2018). Experiments, modeling and scaling-up of membrane reactors for hydrogen production via steam methane reforming. Chemical Engineering and Processing - Process Intensification, 134, 124–140. https://doi.org/10.1016/j.cep.2018.10.007
[25]. Nayebossadri, S., Speight, J. D., & Book, D. (2019). Hydrogen separation from blended natural gas and hydrogen by Pd-based membranes. International Journal of Hydrogen Energy, 44(55), 29092–29099. https://doi.org/10.1016/j.ijhydene.2019.03.044
[26]. Gangadharan, P., Kanchi, K. C., & Lou, H. H. (2012). Evaluation of the economic and environmental impact of combining dry reforming with steam reforming of methane. Chemical Engineering Research and Design, 90(11), 1956–1968. https://doi.org/10.1016/j.cherd.2012.04.008
[27]. Lee, J., Kim, B., & Han, M. (2019). Spatially Patterned Catalytic Reactor for Steam-CO2 Reforming of Methane. Industrial and Engineering Chemistry Research, 58(40), 18731–18741. https://doi.org/10.1021/acs.iecr.9b03091
[28]. Ullah, K. S., Omer, A., Rashid, K., Rehman ,N. U., Rahimipetroudi, I., Kim, S. D., & Dong, S. K. (2023). Modeling and comprehensive analysis of hydrogen production in a newly designed steam methane reformer with membrane system. Computers & Chemical Engineering, 175, 108278
[29]. Su, B., Wang, Y., Xu, Z., Han, W., Jin, H., & Wang, H. (2022). Novel ways for hydrogen production based on methane steam and dry reforming integrated with carbon capture. Energy Conversion and Management, 270. https://doi.org/10.1016/j.enconman.2022.116199
[30]. Jabbour, K. (2020). Tuning combined steam and dry reforming of methane for “metgas” production: A thermodynamic approach and state-of-the-art catalysts. In Journal of Energy Chemistry (Vol. 48, pp. 54–91). Elsevier B.V. https://doi.org/10.1016/j.jechem.2019.12.017
[31]. Shakouri, M., Hu, Y., Lehoux, R., & Wang, H. (2021). CO2 conversion through combined steam and CO2 reforming of methane reactions over Ni and Co catalysts. Canadian Journal of Chemical Engineering, 99(1), 153–165. https://doi.org/10.1002/cjce.23828
[32]. Ghasem, N. (2022). A Review of the CFD Modeling of Hydrogen Production in Catalytic Steam Reforming Reactors. In International Journal of Molecular Sciences (Vol. 23, Issue 24). MDPI. https://doi.org/10.3390/ijms232416064








