Products Cited in Publications Worldwide Singlet-Oxygen-Driven Cooperative Photocatalytic Coupling of Biomass Valorization and Hydrogen Peroxide Production Using Covalent Organic Frameworks

Singlet-Oxygen-Driven Cooperative Photocatalytic Coupling of Biomass Valorization and Hydrogen Peroxide Production Using Covalent Organic Frameworks

Xue, Qiang; Li, Hanxi; Jin, Peng; Zhou, Xukai; Wang, Feng

DOI: PMID:

Abstract

Traditional H2O2 photocatalysis primarily depends on photoexcited electrons and holes to drive oxygen reduction and water oxidation, respectively. However, singlet oxygen (1O2), often underappreciated, plays a pivotal role in H2O2 production. Meanwhile, photocatalytic biomass conversion has attracted attention, yet studies combining H2O2 synthesis with biomass valorization remain rare and typically yield low-value products. Herein, we report a strategy of photocatalytic valorization of furfuryl alcohol (FFA) coupled with the efficient co-production of H2O2, enabled by covalent organic frameworks (COFs) induced, 1O2-participated Achmatowicz rearrangement. This study introduces polyimide-based COF-N0-3 with tailored nitrogen content, representing an unprecedently efficient platform for 1O2 production. Remarkably, reducing the nitrogen content of the COF enhances 1O2 production, significantly boosting the H2O2 generation rate. In FFA, the primary pathway for H2O2 production is Achmatowicz rearrangement, achieving a rate ten times higher than that reliant on oxygen reduction reaction in pure water, reaching 4549 μmol g -1 h -1. Mechanism studies revealed 1O2 selectively engaged FFA, bypassing hole oxidation to trigger the Achmatowicz rearrangement, producing valuable 6-hydroxy-(2H)-pyranone with 99% conversion and 92% selectivity. This work establishes a coupling strategy for simultaneoues synthesis of H2O2 and biochemicals, offering a transformative approach to sustainable photocatalysis.

Keywords

covalent organic frameworks ; hydrogen peroxide photosynthesis ; biomass valorization coupling ; singlet oxygen

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2-Furoic acid

A11754988-14-295%

2-Furoic acid

12.0/100g

Detail

A96766935436-57-897%

6-Hydroxy-2H-pyran-3(6H)-one

42.0/250mg

Detail