Enhancing coke resistance of Ni-based spinel-type oxides by tuning the configurational entropy

[Display omitted] •High-entropy spinel-type (NiMgCaZnCo)Al10Ox exhibited optimal activity and stability in DRM reaction at 800 ℃ and 650 ℃.•Doping with Co and Zn stabilizes the high-entropy spinel structure and dilutes the active Ni sites.•Doping with alkaline earth metal elements Ca and Mg generates additional oxygen defects to eliminate carbon deposition. The reforming of CH4 and CO2 into syngas is a highly relevant technology for energy conservation and reducing greenhouse gas emissions, attracting widespread attention in the industry. Inspired by this, this work proposes a general criterion for coke-resistant nickel-based catalysts. By leveraging the high-entropy effect and the lattice distortion of the structure, a high-entropy (NiCaMgZnCo)Al10Ox catalyst was synthesized. The high-entropy oxide exhibited good activity and stability during the DRM reaction over 100 h at 800°C and 650°C, producing only a minimal amount of easily removable carbon deposition. O2-TPO, CO2-TPD, CH4-TPSR, CO2-TPSR, DFT and in situ DRIFT were employed to investigate the mechanism of carbon deposition elimination on the surface of the high-entropy catalyst. Then, a high-entropy strategy for designing coke-resistant catalysts was proposed. This strategy may soon inspire the development of catalysts with enhanced stability and anti-coke deposition properties for various catalytic applications.