Robust Hollow Spheres Consisting of Alternating Titania Nanosheets and Graphene Nanosheets with High Photocatalytic Activity for CO₂ Conversion into Renewable Fuels

Abstract

Abstract Robust hollow spheres consisting of molecular‐scale alternating titania (Ti 0.91 O 2 ) nanosheets and graphene (G) nanosheets are successfully fabricated by a layer‐by‐layer assembly technique with polymer beads as sacrificial templates using a microwave irradiation technique to simultaneously remove the template and reduce graphene oxide into graphene. The molecular scale, 2D contact of Ti 0.91 O 2 nanosheets and G nanosheets in the hollow spheres is distinctly different from the prevenient G‐based TiO 2 nanocomposites prepared by simple integration of TiO 2 and G nanosheets. The nine times increase of the photocatalytic activity of G‐Ti 0.91 O 2 hollow spheres relative to commercial P25 TiO 2 is confirmed with photoreduction of CO 2 into renewable fuels (CO and CH 4 ). The large enhancement in the photocatalytic activity benefits from: 1) the ultrathin nature of Ti 0.91 O 2 nanosheets allowing charge carriers to move rapidly onto the surface to participate in the photoreduction reaction; 2) the sufficiently compact stacking of ultrathin Ti 0.91 O 2 nanosheets with G nanosheets allowing the photogenerated electron to transfer fast from the Ti 0.91 O 2 nanosheets to G to enhance lifetime of the charge carriers; and 3) the hollow structure potentially acting as a photon trap‐well to allow the multiscattering of incident light for the enhancement of light absorption.