Production of H2O2 via Energy Transfer Photocatalysis by Coupling with Furfuryl Alcohol Conversion over an Amide-Functionalized Heptazine Framework
Graphical Abstract
Traditional charge-carrier-based photocatalysis can be switched to a novel energy transfer route for efficient and selective 1O2 generation through amide functionalization to modulate the electronic structure of the photocatalyst, thus providing a promising approach for simultaneous synthesis of H2O2 and conversion of a biomass derivative.
Abstract
Photocatalytic oxygen reduction provides a sustainable approach for hydrogen peroxide (H2O2) synthesis, but the charge carrier-based pathway is severely limited by inefficient charge separation and redox decomposition of the produced H2O2. Energy transfer photocatalysis (EnTP) is an alternative charge-carrier-free route for H2O2 synthesis. Herein, we propose a strategy of killing two birds with one stone to simultaneously realize the synthesis of H2O2 and conversion of a biomass derivative by coupling EnTP with the Achmatowicz reaction. Results show efficient production of H2O2 at a rate of 14.6 mmol gcat−1 h−1 and an apparent quantum yield (AQY) of 44.1% at 420 nm, coupled with the conversion of biomass-derived furfuryl alcohol (FFA) into hydroxy-2H-pyran-3(6H)-one with a high selectivity of 85.9%. Such a performance was attributed to the efficient EnTP over the amide-functionalized heptazine framework photocatalyst for singlet oxygen generation, which induces the FFA conversion and concurrently produces H2O2. A systematic study of the photoexcitation process of the catalysts reveals that the amide functionalization significantly improves the intersystem crossing (ISC) efficiency, as the structural modification optimizes the electronic structure and thus tunes the composition and distribution of energy bands.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.