In Situ Reconstruction Regenerates Sinter-Degraded NiO-Based Monolithic Ceramic Catalysts for Efficient Methane Oxidation in Ventilation Air

Monolithic ceramic catalysts are a key technology for the industrial treatment of coal mine ventilation air methane (VAM). The preparation of straight-channel NiO/CeO₂ monolithic ceramic catalysts via phase inversion addresses critical bottlenecks for industrial VAM abatement. However, high-temperature sintering leads to irreversible NiO agglomeration and coarsening, severely reducing catalytic activity. In this study, an in situ reduction–oxidation reconstruction method is developed to regenerate sinter-degraded NiO. The reconstructed catalyst increases methane conversion from below 70% after sintering to over 95% at 550 °C and achieves full conversion at 600 °C. The catalyst maintains near 100% conversion during 400 h of continuous operation at 600 °C and shows no performance degradation over 15 thermal cycles. Moreover, the reconstructed catalyst exhibits excellent steam tolerance with fully reversible deactivation. The reconstructed catalyst presents a refined porous structure with BET surface area rising from 4.5 to 11.4 m² g⁻¹, an elevated Ni³⁺/Ni²⁺ ratio (1.47 to 1.97), a higher surface adsorbed oxygen proportion (36.8% to 48.7%) and significantly strengthened NiO-CeO₂ interfacial interaction. This work provides a facile and efficient in situ regeneration strategy, greatly enhancing the VAM oxidation activity and stability of sinter-degraded monolithic ceramic catalysts.