Metal–organic
frameworks (MOFs) constructed with mixed ligands
have shown great promise in the generation of materials with improved
sorption, optical, and electronic properties. With an experimental,
spectroscopic, and computational approach, herein, we investigated
how the incorporation of different functionalized ligands within the
structure of MIL-125-NH2 affects its performance in photocatalytic
water reduction. We found that multiligand incorporation within the
MOF structure has an impact on the light absorption spectrum and the
electronic structure. These combined modifications improve the photocatalytic
performance of MIL-125-NH2, thereby increasing the rate
of hydrogen evolution reaction. Of the four nanoparticle/MOF photocatalytic
systems tested, we showed that the Pt/MIL-125-NH2/(OH)2 system (Pt nanoparticle plus MIL-125-NH2 with
amino and dihydroxyl functionalized ligands) outperforms its counterpart
Pt/MIL-125-NH2 system, attributed to the enhanced p−π
conjugation between the lone pairs of O atoms and their aromatic ligands
resulting in a red-shifted absorption spectrum and greater spatial
distribution of electron density.
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