Integrated carbon capture and utilisation (ICCU) is a promising technology to mitigate the impact of carbon emissions, as it combines sorbent regeneration and CO2 utilisation. ICCU has been intensively studied for reverse water shift reaction (RWGS), methanation and dry methane reforming (DRM). However, ICCU-RWGS and ICCU-Methanation rely on hydrogen, which compromises economic viability and safety, and the complex synthesis of DFMs for ICCU-DRM, requiring promoters or multilayer structures. To enhance the practicality of ICCU technology, here we investigated carbon-based ICCU (C-ICCU), which utilises the reverse Boudouard reaction with carbon as the reducing agent. In this study, we explored the key operational factors influencing C-ICCU performance, specifically Ni loading, the Ni/graphite mass, and temperature. Our findings indicate that Ni/graphite is a highly effective catalyst for the in-situ conversion of CO2 to CO. Specifically, a Ni loading of 3 wt.% or higher achieved a CO2 conversion greater than 95% at 650°C. Furthermore, in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis revealed the synergistic interactions between graphite and nickel. Specifically, graphite promotes CO2 generation while nickel catalyses its subsequent conversion. Our research demonstrates that the C-ICCU mechanism is a complex synergistic process involving the dynamic evolution of surface species. This work offers a promising, safer, and potentially more economical pathway for industrial carbon capture and utilisation.
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