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Facilitated Photocatalytic CO<sub>2</sub>Reduction in Aerobic Environment on a Copper‐Porphyrin Metal–Organic Framework

Shijie Xie, Chaoyuan Deng, Qing Huang, Chuang Zhang, Chuncheng Chen, Jincai Zhao, Hua Sheng

2023Angewandte Chemie International Edition97 citationsDOIOpen Access PDF

Abstract

Abstract Herein, we fabricated a π–π stacking hybrid photocatalyst by combining two two‐dimensional (2D) materials: g‐C 3 N 4 and a Cu‐porphyrin metal–organic framework (MOF). After an aerobic photocatalytic pretreatment, this hybrid catalyst exhibited an unprecedented ability to photocatalytically reduce CO 2 to CO and CH 4 under the typical level (20 %) of O 2 in the air. Intriguingly, the presence of O 2 did not suppress CO 2 reduction; instead, a fivefold increase compared with that in the absence of O 2 was observed. Structural analysis indicated that during aerobic pretreatment, the Cu node in the 2D‐MOF moiety was hydroxylated by the hydroxyl generated from the reduction of O 2 . Then the formed hydroxylated Cu node maintained its structure during aerobic CO 2 reduction, whereas it underwent structural alteration and was reductively devitalized in the absence of O 2 . Theoretical calculations further demonstrated that CO 2 reduction, instead of O 2 reduction, occurred preferentially on the hydroxylated Cu node.

Topics & Concepts

PorphyrinMoietyPhotocatalysisCopperStackingCatalysisChemistryPhotochemistryMetalMetal-organic frameworkReduction (mathematics)Inorganic chemistryOrganic chemistryGeometryMathematicsAdsorptionCO2 Reduction Techniques and CatalystsAdvanced Photocatalysis TechniquesMetal-Organic Frameworks: Synthesis and Applications
Facilitated Photocatalytic CO<sub>2</sub>Reduction in Aerobic Environment on a Copper‐Porphyrin Metal–Organic Framework | Litcius