Abstract
Generation of singlet oxygen (1O2) with metal-organic frameworks (MOFs) is limited by either poor light harvesting ability of type I MOFs or low availability of type II MOFs. Herein, we report a facile and widely applicable strategy, post-synthetic modification of type I MOFs with photo-redox active acetylacetone (AA) via a diazo coupling reaction, to enhance the visible-light-driven generation of 1O2 by MOFs. The introduction of AA to MOFs with variant metal nodes, such as Zr, Ti, Al, and Cr clusters, leads to intraligand charge transfer (ILCT), which not only strengthens the ligand to metal cluster charge transfer (LCCT) but also expands the photo-responsive edge of MOFs. Via the coupled ILCT and LCCT processes, UiO-66-AA functions as a hybrid type I-type II MOFs, which can efficiently generate 1O2 even at indoor lighting conditions. This work would open an avenue for the synthesis of MOFs towards diverse visible-light photocatalysis.
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