Abstract
Metal-organic frameworks(MOFs)are highly desirable for promising photocatalytic water splitting,but their practical application is greatly limited due to their unstable chemical properties and insufficient visible light response as well as low charge-carries utilization,espe-cially in photocatalytic O2 production.Herein,we present a post-modification engineering to modulate cerium metal-organic frameworks(Ce-MOFs)for realizing efficient photocatalytic water oxidation to liberate O2 by visible light.The one-step partial oxidation strategy is adopted to modify pristine Ce-MOFs,yielding the new Ce-MOFs(MV-Ce-MOFs)with mixed valence of Ce3+/Ce4+.Creating the Ce nodes of a mixed valence state can effectively extend the optical absorption to the visible region,expose more catalytically active sites and inhibit the recombination of photoinduced charges.Consequently,the MV-Ce-MOFs exhibit high activity for photocatalytic O2 evolution under visible light,manifesting an impressive 1.6%apparent quantum efficiency(AQY)under monochromatic irradiation of 405 nm.The regulation engineering of MOF metal node valence heralds a new paradigm for designing MOF-based photocatalysts.