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A Supported Bismuth Halide Perovskite Photocatalyst for Selective Aliphatic and Aromatic C–H Bond Activation
Author(s) -
Dai Yitao,
Poidevin Corentin,
OchoaHernández Cristina,
Auer Alexander A.,
Tüysüz Harun
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201915034
Subject(s) - halide , photocatalysis , catalysis , photochemistry , chemistry , perovskite (structure) , selectivity , bismuth , mesoporous material , nanoparticle , inorganic chemistry , materials science , organic chemistry , nanotechnology
Direct selective oxidation of hydrocarbons to oxygenates by O 2 is challenging. Catalysts are limited by the low activity and narrow application scope, and the main focus is on active C−H bonds at benzylic positions. In this work, stable, lead‐free, Cs 3 Bi 2 Br 9 halide perovskites are integrated within the pore channels of mesoporous SBA‐15 silica and demonstrate their photocatalytic potentials for C−H bond activation. The composite photocatalysts can effectively oxidize hydrocarbons (C 5 to C 16 including aromatic and aliphatic alkanes) with a conversion rate up to 32900 μmol g cat −1 h −1 and excellent selectivity (>99 %) towards aldehydes and ketones under visible‐light irradiation. Isotopic labeling, in situ spectroscopic studies, and DFT calculations reveal that well‐dispersed small perovskite nanoparticles (2–5 nm) possess enhanced electron–hole separation and a close contact with hydrocarbons that facilitates C(sp 3 )−H bond activation by photoinduced charges.