Enhanced dry reforming of methane over nickel catalysts supported on zirconia coated mesoporous silica.

Dry reforming of methane (DRM) offers a sustainable route to convert CH and CO into syngas, addressing both greenhouse gas emissions and energy demand. However, catalyst deactivation due to sintering and coking limits practical applications. In this work, we developed a mesoporous Ni-based catalyst (Ni/ZrSBA-15-OH) featuring abundant Ni-ZrO interfaces and small Ni nanoparticles (5.6 nm) confined within a stable silica framework. This catalyst showed excellent performance, achieving 80% CH and 87% CO conversions at 750°C, with minimal coke formation (0.4 mg g h) and high durability (1.3% CH conversion loss over 20 h). Advanced characterizations (X-ray absorption spectroscopy [XAS], transmission electron microscopy [TEM], H-temperature programmed reduction [H-TPR], and temperature-programmed surface reaction [TPSR]) revealed that the metal-oxide interface enhances the activation of reactants and stabilizes active sites. Density functional theory (DFT) calculations confirmed that the Ni-ZrO interface increases the energy barrier for CH∗ dehydrogenation, effectively suppressing carbon deposition. This study provides a rational strategy for designing structurally robust and coke-resistant Ni-based catalysts for efficient DRM.