Biomethane Energy Production Using Orange Hydrogen Coupled With CO₂ Sequestration and Utilization

Abstract

The escalating concerns of global warming have intensified the global demand for clean energy solutions, coupled with effective carbon management strategies. Biomethanation offers a promising approach by producing energy-dense biomethane (bCH₄) while simultaneously reducing carbon dioxide (CO₂) emissions. However, the potential to leverage in-situ generated “orange hydrogen (H₂)” from geochemical reactions as a more efficient and integrated electron donor for this process remains largely unexplored. This study explored the efficacy of CO₂ biomethanation using orange H₂ generated from water-olivine-CO₂ interactions and externally supplied green H₂. Results showed that the orange H₂-assisted biomethanation strategy achieved H₂ to bCH₄ conversion efficiency of up to ~84.47%, which is approximately 12% higher than that of green H₂ to bCH₄ under identical experimental conditions. Molecular analysis (16S rRNA and mcrA gene sequencing) identified Methanothermobacter as the key archaeon driving the hydrogenotrophic conversion of CO₂ to bCH₄. In addition to biotic CO₂ utilization via biomethanation, experimental characterization combined with atomistic simulations revealed that carbonate mineral formation (e.g., siderite and magnesite) serves as an abiotic sink for CO₂ sequestration. This integrated approach highlights the dual CO₂ reduction potential of biomethanation using orange H₂ for both sustainable energy production and long-term carbon management, advancing the vision of a clean and green future.

Keywords

biomethanation / carbon dioxide mineralization / hydrogen conversion efficiency / orange hydrogen

References

[1] M. Ali, A. Isah, N. Yekeen, et al., “Recent Progress in Underground Hydrogen Storage,” Energy & Environmental Science 18, no. 12 (2025): 5740–5810.

[2] J. Li, M. Luo, K. Wang, G. Li, and G. Zhang, “Review of Carbon Dioxide Mineralization of Magnesium-Containing Materials,” Carbon Neutralization 2, no. 5 (2023): 574–584.

[3] Y. Yan, Y. X. Pang, X. Luo, et al., “Carbon Dioxide-Focused Greenhouse Gas Emissions From Petrochemical Plants and Associated Industries: Critical Overview, Recent Advances and Future Prospects of Mitigation Strategies,” Process Safety and Environmental Protection 188 (2024): 406–421.

[4] K. R. Shivanna, “Climate Change and Its Impact on Biodiversity and Human Welfare,” Proceedings of the Indian National Science Academy 88, no. 2 (2022): 160–171.

[5] L. Grant, I. Vanderkelen, L. Gudmundsson, E. Fischer, S. I. Seneviratne, and W. Thiery, “Global Emergence of Unprecedented Lifetime Exposure to Climate Extremes,” Nature 641, no. 8062 (2025): 374–379.

[6] K. Liu, M. A. Nawaz, and G. Liao, “Progress and Future Challenges in Designing High-Performance Ni/CeO₂ Catalysts for CO₂ Methanation: A Critical Review,” Carbon Neutralization 4, no. 1 (2025): e190.

[7] J. M. S. Oliveira, L. D. M. Ottosen, and M. V. W. Kofoed, “Continuous Biomethanation of Flue Gas-Carbon Dioxide Using Bio-Integrated Carbon Capture and Utilization,” Bioresource Technology 399 (2024): 130506.

[8] L. Hu, J. Yang, Q. Xia, J. Zhang, H. Zhao, and Y. Lu, “Chemico-Biological Conversion of Carbon Dioxide,” Journal of Energy Chemistry 89 (2024): 371–387.

[9] M. Kazmi, M. Irfan, L. Zhou, et al., “Electron Donors and Mediators in the Thermodynamics and Kinetics of CO₂ Bioreduction,” Renewable and Sustainable Energy Reviews 156 (2022): 111997.

[10] N. J. Claassens, C. A. R. Cotton, D. Kopljar, and A. Bar-Even, “Making Quantitative Sense of Electromicrobial Production,” Nature Catalysis 2, no. 5 (2019): 437–447.

[11] M. U. Sieborg, A. K. H. Nielsen, L. D. M. Ottosen, K. Daasbjerg, and M. V. W. Kofoed, “Bio-Integrated Carbon Capture and Utilization: at the Interface Between Capture Chemistry and Archaeal CO₂ Reduction,” Nature Communications 15, no. 1 (2024): 7492.

[12] J. Zabranska and D. Pokorna, “Bioconversion of Carbon Dioxide to Methane Using Hydrogen and Hydrogenotrophic Methanogens,” Biotechnology Advances 36, no. 3 (2018): 707–720.

[13] M. Vítězová, V. Onderka, I. Urbanová, et al., “In Situ Field Experiment Shows the Potential of Methanogenic Archaea for Biomethane Production From Underground Gas Storage in Natural Rock Environment,” Environmental Technology & Innovation 32 (2023): 103253.

[14] L. Wu, Z. Hou, Z. Luo, et al., “Efficiency Assessment of Underground Biomethanation With Hydrogen and Carbon Dioxide in Depleted Gas Reservoirs: A Biogeochemical Simulation,” Energy 283 (2023): 128539.

[15] G. Strobel, B. Hagemann, T. M. Huppertz, and L. Ganzer, “Underground Bio-Methanation: Concept and Potential,” Renewable and Sustainable Energy Reviews 123 (2020): 109747.

[16] R. Farajzadeh, B. P. Lomans, H. Hajibeygi, and J. Bruining, “Exergy Return on Exergy Investment and CO₂ Intensity of the Underground Biomethanation Process,” ACS Sustainable Chemistry & Engineering 10, no. 31 (2022): 10318–10326.

[17] C. J. Ballentine, R. Karolytė, A. Cheng, B. Sherwood Lollar, J. G. Gluyas, and M. C. Daly, “Natural Hydrogen Resource Accumulation in the Continental Crust,” Nature Reviews Earth & Environment 6, no. 5 (2025): 342–356.

[18] F. Osselin, C. Soulaine, C. Fauguerolles, E. C. Gaucher, B. Scaillet, and M. Pichavant, “Orange Hydrogen Is the New Green,” Nature Geoscience 15, no. 10 (2022): 765–769.

[19] S. Brunauer, P. H. Emmett, and E. Teller, “Adsorption of Gases in Multimolecular Layers,” Journal of the American Chemical Society 60, no. 2 (1938): 309–319.

[20] L. Zhou, J. Gao, L.-G. Chen, et al., “Bioconversion of CO₂ to Methane Energy by Methanococcus Maripaludis in Newly-Designed Bioreactor System: Kinetic Characteristics, Parameter Optimization and Grid-Quality Production,” Bioresource Technology 439 (2025): 133283.

[21] B. J. Callahan, P. J. McMurdie, M. J. Rosen, A. W. Han, A. J. A. Johnson, and S. P. Holmes, “DADA2: High-Resolution Sample Inference From Illumina Amplicon Data,” Nature Methods 13, no. 7 (2016): 581–583.

[22] C. Quast, E. Pruesse, P. Yilmaz, et al., “The Silva Ribosomal RNA Gene Database Project: Improved Data Processing and Web-Based Tools,” Nucleic Acids Research 41, no. D1 (2012): D590–D596.

[23] P. E. Galand, H. Juottonen, H. Fritze, and K. Yrjälä, “Methanogen Communities in a Drained Bog: Effect of Ash Fertilization,” Microbial Ecology 49, no. 2 (2005): 209–217.

[24] J.-F. Liu, S. M. Mbadinga, X.-B. Sun, et al., “Microbial Communities Responsible for Fixation of CO₂ Revealed by Using mcrA, cbbM, cbbL, fthfs, fFefe-Hydrogenase Genes as Molecular Biomarkers in Petroleum Reservoirs of Different Temperatures,” International Biodeterioration & Biodegradation 114 (2016): 164–175.

[25] J. H. Lee, J. C. Kim, J. Lee, et al., “Theoretical and Mechanistic Insights Into Control Factor-Assisted CO₂ Mineralization With Olivine,” Journal of Industrial and Engineering Chemistry 122 (2023): 241–250.

[26] G. A. W. Sudiartha, T. Imai, and A. Reungsang, “Syntrophic Relationship Among Microbial Communities Enhance Methane Production During Temperature Transition From Mesophilic to Thermotolerant Conditions,” Journal of Environmental Chemical Engineering 12, no. 6 (2024): 114903.

[27] Y. Xiong, Z. Hou, H. Xie, J. Zhao, X. Tan, and J. Luo, “Microbial-Mediated CO₂ Methanation and Renewable Natural Gas Storage in Depleted Petroleum Reservoirs: A Review of Biogeochemical Mechanism and Perspective,” Gondwana Research 122 (2023): 184–198.

[28] A. Al-Yaseri, M. Desouky, M. S. Aljawad, and A. Hassanpouryouzband, “Evidence of Hydrogen Release During CO₂ Sequestration in Basalt,” International Journal of Hydrogen Energy 101 (2025): 1183–1190.

[29] V. Awosiji, S. Graham, and T. Mukerji, “The Concept of a Blind Hydrogen System,” International Journal of Hydrogen Energy 158 (2025): 150492.

[30] C. Truong, N. Gaudu, O. Farr, et al., “Fe2+ Disproportionation Within Iron-Rich Alkaline Vent Analogues Reveals Proto-Bioenergetic Systems,” Nature Communications 16, no. 1 (2025): 10682.

[31] X. Y. Liu, J. Y. Ma, M. Y. Liu, et al., “Light-Independent Fe₃O₄-Methanosarcina Acetivorans Biohybrid Enhances Nitrogen Fixation and Methanogenesis,” Journal of the American Chemical Society 147, no. 9 (2025): 7694–7702.

[32] Y. Zheng, H. Wang, Y. Liu, et al., “Electrochemically Coupled CH4 and CO₂ Consumption Driven by Microbial Processes,” Nature Communications 15, no. 1 (2024): 3097.

[33] V. Helmbrecht, R. Reichelt, D. Grohmann, and W. D. Orsi, “Simulated Early Earth Geochemistry Fuels a Hydrogen-Dependent Primordial Metabolism,” Nature Ecology & Evolution 9, no. 5 (2025): 769–778.

[34] M. Irfan, L. Zhou, J.-H. Ji, et al., “Enhanced Energy Generation and Altered Biochemical Pathways in an Enrichment Microbial Consortium Amended With Natural Iron Minerals,” Renewable Energy 159 (2020): 585–594.

[35] M. Irfan, L. Zhou, J.-H. Ji, et al., “Energy Recovery From the Carbon Dioxide for Green and Sustainable Environment Using Iron Minerals as Electron Donor,” Journal of Cleaner Production 277 (2020): 124134.

[36] T. Uchiyama, K. Ito, K. Mori, H. Tsurumaru, and S. Harayama, “Iron-Corroding Methanogen Isolated From a Crude-Oil Storage Tank,” Applied and Environmental Microbiology 76, no. 6 (2010): 1783–1788.

[37] L.-G. Chen, L. Zhou, B.-W. Wang, et al., “Microbial Assembly and Metabolic Restructuring Following CO₂ Injection in Subsurface Oil Reservoir,” AMB Express (2026).

[38] M. Irfan, L. Zhou, Y. Bai, et al., “Insights Into the Hydrogen Generation From Water-Iron Rock Reactions at Low Temperature and the Key Limiting Factors in the Process,” International Journal of Hydrogen Energy 44, no. 33 (2019): 18007–18018.

[39] L. Ma, L. Zhou, S. M. Mbadinga, J.-D. Gu, and B.-Z. Mu, “Accelerated CO₂ Reduction to Methane for Energy by Zero Valent Iron in Oil Reservoir Production Waters,” Energy 147 (2018): 663–671.

[40] C. Hellerschmied, J. Schritter, N. Waldmann, et al., “Hydrogen Storage and Geo-Methanation in a Depleted Underground Hydrocarbon Reservoir,” Nature Energy 9, no. 3 (2024): 333–344.

[41] R. Mushabe, N. Liu, N. Dopffel, G. Ersland, and M. A. Fernø, “Impact of Specific Surface Area on Anaerobic Microbial Hydrogen Consumption by a Sulfate Reducer: A Sand Pack Study,” International Journal of Hydrogen Energy 166 (2025): 150861.

[42] L. Wu, Z. Hou, and Z. Luo, “Impacts of Microbial Competition on Underground Bio-Methanation of Hydrogen and Carbon Dioxide: Insights From Biogeochemical Simulations,” Renewable Energy 251 (2025): 123458.

[43] H. Dong, L. Huang, L. Zhao, et al., “A Critical Review of Mineral–Microbe Interaction and Co-Evolution: Mechanisms and Applications,” National Science Review 9, no. 10 (2022): nwac128.

[44] Y. Wu, S. Wang, D. Liang, and N. Li, “Conductive Materials in Anaerobic Digestion: From Mechanism to Application,” Bioresource Technology 298 (2020): 122403.

[45] D. Xu, T. Gu, and D. R. Lovley, “Microbially Mediated Metal Corrosion,” Nature Reviews Microbiology 21, no. 11 (2023): 705–718.

[46] D. E. Holmes, H. Tang, T. Woodard, et al., “Cytochrome-Mediated Direct Electron Uptake From Metallic Iron by Methanosarcina acetivorans,” mLife 1, no. 4 (2022): 443–447.

[47] N. Kamala Ilango, H. Nguyen, M. Alzeer, F. Winnefeld, and P. Kinnunen, “Stabilization of Nesquehonite for Application in Carbon Capture Utilization and Storage,” Materials Advances 6, no. 2 (2025): 552–556.

[48] M. J. Abdolhosseini Qomi, Q. R. S. Miller, S. Zare, H. T. Schaef, J. P. Kaszuba, and K. M. Rosso, “Molecular-Scale Mechanisms of CO₂ Mineralization in Nanoscale Interfacial Water Films,” Nature Reviews Chemistry 6, no. 9 (2022): 598–613.

[49] U. Geymond, L. Truche, O. Sissmann, D. Kubániová, N. Recham, and I. Martinez, “Mineralogical Changes and H₂ Generation Yield During Hydrothermal Alteration of a Magnetite-Siderite Assemblage,” Journal of Geophysical Research: Solid Earth 130, no. 8 (2025): e2024JB030724.

[50] J. Wang, R. Sekiai, R. Tamura, and N. Watanabe, “CO₂ Capture, Geological Storage, and Mineralization Using Biobased Biodegradable Chelating Agents and Seawater,” Science Advances 10, no. 46 (2024): eadq0515.

[51] A. Alqahtani, M. Addassi, H. Hoteit, and E. Oelkers, “Rapid CO₂ Mineralization by Zeolite via Cation Exchange,” Scientific Reports 15, no. 1 (2025): 958.

[52] X. Zhou, Y.-S. Wu, H. Chen, et al., “Review of Carbon Dioxide Utilization and Sequestration in Depleted Oil Reservoirs,” Renewable and Sustainable Energy Reviews 202 (2024): 114646.

[53] A. Fontana, P. G. Kougias, L. Treu, et al., “Microbial Activity Response to Hydrogen Injection in Thermophilic Anaerobic Digesters Revealed by Genome-Centric Metatranscriptomics,” Microbiome 6, no. 1 (2018): 194.

[54] D. R. Lovley, “Electrotrophy: Other Microbial Species, Iron, and Electrodes as Electron Donors for Microbial Respirations,” Bioresource Technology 345 (2022): 126553.

[55] M. Orthofer, W. Hofmann, S. K. M. R. Rittmann, and C. Paulik, “A High-Pressure Bioreactor System for the Cultivation of Methanothermobacter marburgensis on Advanced Growth Media for Sustainable Energy Applications,” Scientific Reports 15, no. 1 (2025): 35519.

[56] R. L. Tyne, P. H. Barry, M. Lawson, et al., “Rapid Microbial Methanogenesis During CO₂ Storage in Hydrocarbon Reservoirs,” Nature 600, no. 7890 (2021): 670–674.

[57] D. Mayumi, H. Tamaki, S. Kato, et al., “Hydrogenotrophic Methanogens Overwrite Isotope Signals of Subsurface Methane,” Science 386, no. 6728 (2024): 1372–1376.

[58] R. L. Tyne, P. H. Barry, M. Lawson, et al., “Identifying and Understanding Microbial Methanogenesis in CO₂ Storage,” Environmental Science & Technology 57, no. 26 (2023): 9459–9473.

[59] H. T. Dinh, J. Kuever, M. Mußmann, A. W. Hassel, M. Stratmann, and F. Widdel, “Iron Corrosion by Novel Anaerobic Microorganisms,” Nature 427, no. 6977 (2004): 829–832.

[60] M. Noussan, V. Negro, M. Prussi, and D. Chiaramonti, “The Potential Role of Biomethane for the Decarbonization of Transport: An Analysis of 2030 Scenarios in Italy,” Applied Energy 355 (2024): 122322.

[61] S. Alafnan, “Factors Influencing Hydrogen Migration in Cap Rocks: Establishing New Screening Criteria for the Selection of Underground Hydrogen Storage Locations,” International Journal of Hydrogen Energy 83 (2024): 1099–1106.

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