Entropy-Controlled Exsolution of Highly Dispersed Nickel-Based Active Metals From Spinel Oxide via Optimizing Metal-Support Interaction for Dry Reforming of Methane

Abstract

Sintering and coking are critical barriers to achieving high performance in dry reforming of methane (DRM) catalysts. A finely dispersed and thermostable Ni-based catalyst is the key to address these issues. By leveraging the intrinsic superiorities of high-entropy oxides in high-temperature stability and low atomic diffusivity, in this study, a highly dispersed Ni-based catalyst is synthesized via an entropy-controlled exsolution of active components. By increasing the number of transition-metal elements in spinel oxides, the active metal-support interaction (MSI) can be continuously strengthened, which controls the exsolution and thermal stability of Ni-based active metal in harsh reaction conditions of DRM. An optimized medium-entropy spinel (Mg_0.4Ni_0.2Co_0.2Zn_0.2)Al₂O₄ with the exsolution of finely dispersed Ni–Co nanoparticles displayed superior activity and stability in thermal DRM at 800°C and photothermal DRM. This entropy-controlled MSI and exsolution principle provides a significant strategy for designing robust catalysts resistant to sintering and coking for high-temperature reactions like DRM in thermal and photothermal systems.

Keywords

dry reforming of methane / exsolution / high-entropy / Ni catalyst / spinel

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