Integration of 3D macroscopic reduced graphene oxide aerogel with DUT-67 for selective CO2 photoreduction to CO in Gas-Solid reaction

Herein, DUT-67/RGO aerogel photocatalysts with three-dimensional (3D) macroscopic morphology were first prepared by a facile hydrothermal and freeze-drying process. It was observed that DUT-67 endowed aerogels with strong adsorption/activation capacity for CO2 molecules. Besides, RGO not only dispersed DUT-67 as a macroscopic carrier, but also improved the utilization rate of light energy. The high conductivity of RGO and the strong interaction with DUT-67 enhanced the electron coupling effect, which was conducive to the separation of carriers. 15D/R achieved near 99.6% selectivity at the gas-solid interface for UV-Vis light-driven CO2 reduction to CO, with a rate of 42.41 mu mol.g(-1). The adsorption behavior of products at the interface and formation process of intermediates were monitored based on CO-TPD and in situ Fourier transform infrared spectra. The extremely high selectivity for CO came from the weak adsorption of CO on the surface of 15D/R and formation of CH4 required more complex intermediates.

Automated summary

DUT-67/RGO aerogel photocatalysts with 3D macroscopic morphology were prepared by a hydrothermal and freeze-drying process. The aerogels exhibited strong adsorption/activation capacity for CO2 molecules, and the addition of RGO improved light energy utilization. The high selectivity and rate of CO2 reduction to CO were achieved at the gas-solid interface.