Binder-Mediated Regulation of Coating Structure over Monolithic Catalyst and Its Performance in CH4-CO2 Reforming

• • The m-NCM-Al-sol catalyst, using inorganic aluminum sol as binder, achieves superior coating adhesion and forms a (Ni-Mg)AlxO4 composite structure via elemental diffusion, leading to the best catalytic activity and stability in DRM, with strong resistance to carbon deposition. • • In contrast, silica sol (Si-sol) binder results in coating cracks and detachment after calcination due to weak interactions, causing activity loss; organic binder (HEC) is oxidized and removed, yielding poor adhesion and severe particle agglomeration, resulting in the poorest performance. • • Coating adhesion strength, mesoporous confinement, and strong metal-support interactions (SMSI) are identified as key factors determining DRM performance; the Al-sol-derived mesoporous Al2O3 network effectively regulates charge transfer around metal sites, promoting C-H bond activation. • • Optimization of aluminum sol coating parameters (binder content, active component dosage, coating cycles) achieves a balance between coating thickness and mass transfer, enabling the integrated catalyst to exhibit excellent DRM performance.