【Frontiers in HaiChuan Chemical Technology】Dalian Institute of Chemical Physics develops a new electro-thermal coupled catalytic process for the ultra-dry reforming of methane

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Dalian Institute of Chemical Physics develops new electro-thermal coupled catalytic process for ultra-dry methane reforming. Published on: 2025-04-08. Recently, the Nanoscale and Interface Catalysis Research Group (Group 502) and the Computational and Data-Driven Catalysis Research Group (Group 511) within the Institute’s Key Laboratory of Catalytic Fundamentals have collaborated to develop a new electro-thermal coupled catalytic process that enables the direct production of syngas from ultra-dry methane. China’s maritime areas are rich in oil and gas resources. However, the natural gas extracted from offshore gas fields generally contains high levels of carbon dioxide (CO2) – ranging from 20% to 80% – and is often referred to as \"carbon-rich natural gas\"; CO2 removal is necessary before it can be transported and utilized further. However, the CO2 separation process increases energy consumption and causes entrainment losses of natural gas, raising the costs of extracting and using carbon-rich natural gas resources. Therefore, there is an urgent need to develop new technologies for the direct utilization of carbon-rich natural gas to support the high-quality development of China’s offshore oil and gas industry. Given that the operating temperature of solid oxide electrolyzers (SOECs) – ranging from 600 oC to 850 oC – matches the reaction temperature required for methane dry reforming (DRM), in this study the team developed a new process for the electro-thermally coupled catalytic super-dry reforming of methane based on SOECs. This process involves serially coupling DRM, reverse water-gas shift (RWGS), and water electrolysis reactions to the cathode of the SOEC; the intermediate product water (H2O) is electrochemically reduced in situ to produce hydrogen (H2) and oxygen ions (O2-). Driven by an electric potential difference, these oxygen ions are electrochemically oxidized at the anode of the SOEC through a dense electrolyte membrane to form oxygen (O2), thereby promoting the RWGS reaction to proceed in the forward direction and overcoming the limitations imposed by thermodynamic equilibrium – as a result, the conversion rate of CO2 and the selectivity for H2 are significantly increased. The team induced the in-situ dissolution of stable rhodium (Rh) nanoparticles on the surface of the CeO2-x carrier, thereby creating high-density Ce3+-VO-Rhδ+ interfacial active sites. When the volume ratio of CO2 to methane (CH4) was 4, electro-thermal coupled catalysis achieved a CH4 conversion rate of 94.5% and a CO2 conversion rate of 95.0%; the selectivity for carbon monoxide (CO) and H2 products was close to 100%. The apparent reduction capacity of CH4 was approximately 4.0, reaching the theoretical value. Furthermore, by using high-temperature atmosphere electron microscopy and high-temperature electrochemical in-situ spectroscopy in combination with theoretical calculations, the team revealed that Rhδ+ serves as the active site for methane cracking; the Ce3+-VO-Rhδ+ interface, rich in oxygen vacancies, enables the adsorption and activation of CO2; and it also acts as an active site for the RWGS reaction. Furthermore, the H2 generated by the electrocatalytic reduction of H2O at this interface can further promote the conversion of CO2. The relevant research findings were published in Nature Chemistry under the title “Super-dry reforming of methane using a tandem electro-thermocatalytic system”. The co-first authors of this work are Dr. Lv Houfu and Dr. Li Rongtan from Group 502, and Dr. Dong Xue from Group 511. The above work was supported by projects such as the **Key Research and Development Program**, the National Natural Science Foundation, and the Liaoning Binhai Laboratory.