Enabling photocatalytic hydrogen production over Fe-based MOFs by refining band structure with dye sensitization

Fe-based metal-organic frameworks (MOFs) have shown promising applications in photocatalysis, yet they are incapable of photocatalytic H 2 production due to their inappropriate conduction band (CB) position and large overpotential for H 2 evolution. Herein, we present a facile strategy enabling the photocatalytic H 2 production over Fe-based MOFs through dye sensitization. A combination of characterization techniques with theoretical simulation reveals that dye sensitization can effectively inject energetic electrons into Fe-MOFs and elevate their quasi-Fermi level under light irradiation, overcoming the surface overpotential for H 2 production from water. Furthermore, deposition of Pt nanoparticles on Fe-MOFs can lower the overpotential for H 2 evolution toward further enhanced photocatalytic activity. This work provides insights into MOF band structure engineering at electronic level, and proves a concept that harnesses MOF materials for targeted photocatalytic applications they are originally not fit for.