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Photoredox‐Promoted Co‐Production of Dihydroisoquinoline and H<sub>2</sub>O<sub>2</sub> over Defective Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub>

Juanjuan Luo, Xinfa Wei, Qiao Yang, Chenyao Wu, Lanxin Li, Lisong Chen, Jianlin Shi

2023Advanced Materials187 citationsDOIOpen Access PDF

Abstract

Abstract One of the most sustainable and promising approaches for hydrogen peroxide (H 2 O 2 ) production in a low‐cost and environment‐friendly way is photosynthesis, which, however, suffers from poor carrier utilization and low H 2 O 2 productivity. The addition of proton donors such as isopropanol or ethanol can increase H 2 O 2 production, which, unfortunately, will inevitably elevate the entire cost while wasting the oxidizing power of holes (h + ). Herein, the tetrahydroisoquinolines (THIQs) is employed as a distinctive proton donor for the thermodynamically feasible and selective semi‐dehydrogenation reaction to highly valuable dihydroisoquinolines (DHIQs), and meanwhile, to couple with and promote H 2 O 2 generation in one photoredox reaction under the photocatalysis by dual‐functional Zn 3 In 2 S 6 photocatalyst. Surprisingly, the suitably defective Zn 3 In 2 S 6 offers an excellent and near‐stoichiometric co‐production performance of H 2 O 2 and DHIQs at unprecedentedly high rates of 66.4 and 62.1 mmol h ‐1 g ‐1 under visible light (λ ≥ 400 nm), respectively, which outperforms all the previously available reports even though sacrificial agents were employed in those reports. Additionally, photocatalytic redox reaction mechanism demonstrates that H 2 O 2 can be generated through multiple pathways, highlighting the synergistic effect among ROS (·O 2 ‐ and 1 O 2 ), h + and proton donor, which has been ignored in previous studies.

Topics & Concepts

Oxidizing agentDehydrogenationPhotocatalysisMaterials scienceHydrogen peroxideRedoxProtonHydrogen productionPhotochemistryNanotechnologyCatalysisChemistryOrganic chemistryQuantum mechanicsMetallurgyPhysicsAdvanced Photocatalysis TechniquesSulfur-Based Synthesis TechniquesCopper-based nanomaterials and applications
Photoredox‐Promoted Co‐Production of Dihydroisoquinoline and H<sub>2</sub>O<sub>2</sub> over Defective Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub> | Litcius