Unprecedented stepwise electron transfer and photocatalysis in supramolecular assembly derived hybrid single-layer two-dimensional nanosheets in water

Abstract

Herein, a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid (TSA) inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks (Q[10]-SOFs) in water. Importantly, the 2D Q[10]-SOFs can further serve as light harvesting antenna, achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation, resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature. Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process, due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.