Enhancing 1O2 Production with Biomimetic Pt Catalysts through Electronic Structure Modification.

Singlet oxygen (1O2) is an excellent reactive oxygen species in the biomedical disinfection field; however, efficient and selective generation of 1O2 remains challenging. Herein, we design bioinspired Pt@UiO-66-X catalysts (X = -NH2, -H, -Br), with Pt nanoparticles as active centers and metal-organic framework (MOF) nanocavities as biomimetic binding pockets, to form a tailored electronic microenvironment for enhancing 1O2 generation. The results demonstrate that the electron-withdrawing functionalized Pt@UiO-66-Br can significantly improve the production efficiency of 1O2, which is 1.5 and 2.5 times higher than those of Pt@UiO-66 and Pt@UiO-66-NH2, respectively. Ab initio calculations reveal that electron-withdrawing functional groups can reduce the local electron density of Pt, thereby leading to a decrease in antibonding-orbital occupancy in Pt-Oads and subsequently facilitating the formation of *OO. Importantly, the Pt@UiO-66-Br catalyst shows good antibacterial properties both in vitro and in vivo. This work provides a promising prospect for the rational design of high-performance biomimetic catalysts for antibacterial application.