Hydrogen peroxide (H2O2) is one of the key chemical feedstocks in various industries. H2O2 is currently produced by the anthraquinone process which requires energy-demanding multi-operations and an expensive metal catalyst. Although solar photocatalysis offers an environmentally friendly strategy for H2O2 production, the design of advanced materials in photocatalysis remains insufficient to meet the industrial level. Herein, we report an alternative reaction design for solar H2O2 production using organic photooxidation with a metal-free photocatalyst. In the photooxidation reaction, H2O2 and aldehyde were coproduced via auto- and photocatalytic alcohol oxidation pathways with a polymeric photocatalyst (CTF-Ph). Light-triggered excitation of organic molecules led to produce significant amounts of H2O2 and aldehyde without the addition of the photocatalysts, demonstrating a crucial role of autocatalysis for H2O2 production. In the presence of CTF-Ph, the overall production of H2O2 and aldehyde was further boosted. The fine modulation of the water-alcohol-solvent mixture enhanced the photocatalytic O2 reduction, resulting in an unprecedented H2O2 production rate of 46.9 mmol h-1 g-1 with a solar-to-chemical conversion efficiency of 1.1% under simulated sunlight. To show the feasibility of the designed reaction system, the solar-driven production was continuously operated for 50 h, leading to generate highly concentrated H2O2 solution up to 10488 ppm. Energy-efficient membrane filtration was applied to purify the obtained H2O2 solution which can be used in a large-scale water purification as a proof-of-the-concept. This study demonstrates a new reaction design of organic working solution for the coproduction of H2O2 and aldehyde under sunlight irradiation, which paves a way to bring the photocatalysis closer to industrial standards.

Solar H2O2 production via synergetic auto- and photocatalytic oxidation

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