Decoupled Solar Energy Storage and Dark Photocatalysis in a 3D Metal-Organic Framework

Materials enabling solar energy conversion and long-term storage for readily available electrical and chemical energy are key for off-grid energy distribution. Herein, the specific confinement of a rhenium coordination complex in a metal-organic framework (MOF) unlocks a unique electron accumulating property under visible-light irradiation. About 15 C g(MOF)(-1) of electric charges can be concentrated and stored for over four weeks without loss. Decoupled, on-demand discharge for electrochemical reactions and H-2 evolution catalysis is shown and light-driven recharging can be conducted for >10 cycles with approximate to 90% of the initial charging capacity retained. Experimental investigations and theoretical calculations link electron trapping to MOF-induced geometry constraints as well as the coordination environment of the Re-center, highlighting the key role of MOF confinement on molecular guests. This study serves as the seminal report on 3D porous colloids achieving photoaccumulation of long-lived electrons, unlocking dark photocatalysis, and a path toward solar capacitor and solar battery systems.

Automated summary

This study demonstrates the specific confinement of a rhenium coordination complex in a metal-organic framework (MOF) that enables unique electron accumulating property under visible-light irradiation. The material can concentrate and store electric charges for over four weeks without loss. It also allows decoupled, on-demand discharge for electrochemical reactions and H-2 evolution catalysis. Experimental investigations and theoretical calculations reveal the key role of MOF confinement on molecular guests in electron trapping.