CH-π interaction boosts photocatalytic CO2 reduction activity of a molecular cobalt catalyst anchored on carbon nitride

Abstract

The construction of efficient noble-metal-free systems for visible-light-driven CO 2 reduction still remains a key challenge. Here, we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g -C 3 N 4 dye surface via CH-π interactions. This hybrid material achieves high turnover numbers (TONs) and turnover frequencies (TOFs) for visible light reduction of CO 2 to CO of 533 and 95 h −1 that are within the best reported up to now. The improved performance is rationalized in terms of the electronic coupling that takes place with the π system of the pyrene group with both the g -C 3 N 4 surface and the Co-pyridyl moiety of the catalysts. CH-π interactions used to anchor a cobalt catalyst for CO 2 photoreduction Delocalized π system of pyrene functionality boost reactivity Very high CO 2 photoreduction turnover number for a molecular/g-C 3 N 4 system Efficient noble-metal-free systems for CO 2 reduction using visible light remains a key challenge. Wang et al. present a pyrene-functionalized, Co-based molecular catalyst immobilized onto an organic conjugated semiconductor using CH-π interactions that is used for selective CO generation.