Metal‐Organic Frameworks Enable Spontaneous Singlet Oxygen Generation Without Light Irradiation

Singlet oxygen (1O2) is a widely used reactive oxygen species (ROS), making the development of new materials capable of efficiently generating it highly important. In this work, we report a series of isostructural MOFs (named JNU‐300) that can spontaneously generate 1O2 by directly activating triplet oxygen (3O2) from the air without the need for additional light irradiation. The highly selective generation of 1O2 by JNU‐300 is verified by electron paramagnetic resonance (EPR) spectroscopy and probe experiments for 1O2. The generated 1O2 can be employed for aerobic oxidation of sulfide and antibacterial application. Mechanism studies revealed that the framework structure, and the adsorption and polarization of O2 by the coordination units of JNU‐300, are crucial for the 1O2 generation. To the best of our knowledge, MOFs JNU‐300 are the first MOF material capable of producing 1O2 by activating 3O2 in the absence of light at room temperature. This work provides new insights into the design and construction of functional MOF materials capable of generating 1O2 via activating 3O2 without light irradiation, opening new possibilities for their application in specialized fields that require 1O2 in the dark.