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

• High-entropy spinel-type (NiMgCaZnCo)Al 10 O x 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 CH 4 and CO 2 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)Al 10 O x 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. O 2 -TPO, CO 2 -TPD, CH 4 -TPSR, CO 2 -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.