Covalently Bonded Interfaces with Delocalized π Electrons in MOF-in-MOF Heterojunction for Efficient Gas-Solid Phase CO2 Photoreduction

Abstract

The interfaces in heterostructure photocatalysts play an important role on charge migration, but the rational controllable interfacial construction remains a challenge. Herein, a covalently bonded interface with delocalized π bonds was controllably constructed via the encapsulation of UiO-66-NH2 nanoparticles into MUV-10 skeletons. The UiO-66-NH2/MUV-10 heterojunction enables both efficient capture and conversion of CO2 and H2O. The delocalized π bond in the covalent interface efficiently accelerates interfacial charge migration, suppress carrier recombination, and reduce work function for electronic effusion. As a consequence, the UiO-66-NH2/MUV-10 exhibited superior CO2 photoreduction activity with H2O under visible light irradiation in gas-solid phase. The CO evolution rate reached as highly as 38.7 μmol g-1 h-1, which surpassed most commonly reported gas-solid phase photocatalysts. This work not only provides a feasible strategy for the controllable construction of interfaces, but also demonstrates great potentials of interfacial engineering for efficient photocatalysis and the other related areas.