Enhancing <sup>1</sup>O<sub>2</sub> Production with Biomimetic Pt Catalysts through Electronic Structure Modification
Zhenjiang Liu, Jie Qin, Hailong Chen, Yuan Xue, Zedong Wang, Bingqing Shen, Ming Li, Yanguo Guo, Longhua Li, Yuanbo Li, Chengzhou Zhu
Abstract
Singlet oxygen ( 1 O 2 ) is an excellent reactive oxygen species in the biomedical disinfection field; however, efficient and selective generation of 1 O 2 remains challenging. Herein, we design bioinspired Pt@UiO-66-X catalysts (X = −NH 2, −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 1 O 2 generation. The results demonstrate that the electron-withdrawing functionalized Pt@UiO-66-Br can significantly improve the production efficiency of 1 O 2, which is 1.5 and 2.5 times higher than those of Pt@UiO-66 and Pt@UiO-66-NH 2, 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–O ads 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.