Reaction‐Induced Dual Metal‐Oxide Interfaces in Ni/MgAl ₂ O ₄ @BN Catalyst Enable Durable Dry Reforming of Methane

Abstract Dry reforming of methane (DRM) has emerged as a promising route for syngas production through synergistic utilization of CO ₂ and CH ₄ , yet its industrial application is hindered by rapid catalyst deactivation caused by sintering and coking. Herein, this challenge is addressd by engineering dual metal‐oxide interfaces in supported Ni‐based catalyst via strong metal‐support interaction (SMSI). Reaction‐induced dynamic formation and migration of BO _x onto surface of Ni nanoparticles (NPs) supported on boron nitride (BN)‐coated MgAl ₂ O ₄ spinel (MAS) produces the dual interfaces. An upper BO _x /Ni interface inhibits sintering of Ni NPs and suppresses coking. A lower Ni/MAS interface prevents sintering of Ni NPs and enhances CO ₂ adsorption. As a result, the dual‐interface‐locked Ni/MAS@BN catalyst delivers a CH ₄ conversion rate of 0.015 mol/g _cat /min with H ₂ /CO ratio of 1.1 under 750 °C, and maintains stable for 500 h with negligible carbon deposition (0.7 wt.%). This performance exceeds that of Ni/MAS (CH ₄ conversion rate < 2.4 × 10 ⁻⁴ mol/g _cat /min after 80 h) and Ni/ h ‐BN (CH ₄ conversion rate < 1.2 × 10 ⁻³ mol/g _cat /min after 20 h), both of which deactivate rapidly within 80 h. This study proposes an innovative dual‐interface engineering strategy for designing high‐performance DRM catalysts with enhanced resistance to sintering and coking.