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Single Chromium Atoms Supported on Titanium Dioxide Nanoparticles for Synergic Catalytic Methane Conversion under Mild Conditions
Author(s) -
Shen Qikai,
Cao Changyan,
Huang Runkun,
Zhu Lei,
Zhou Xin,
Zhang Qinghua,
Gu Lin,
Song Weiguo
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201913309
Subject(s) - catalysis , methane , chemistry , selectivity , titanium dioxide , chromium , yield (engineering) , electron paramagnetic resonance , photochemistry , inorganic chemistry , anaerobic oxidation of methane , titanium , heterogeneous catalysis , chemical engineering , organic chemistry , materials science , metallurgy , engineering , physics , nuclear magnetic resonance
Direct conversion of methane to value‐added chemicals with high selectivity under mild conditions remains a great challenge in catalysis. Now, single chromium atoms supported on titanium dioxide nanoparticles are reported as an efficient heterogeneous catalyst for direct methane oxidation to C1 oxygenated products with H 2 O 2 as oxidant under mild conditions. The highest yield for C1 oxygenated products can be reached as 57.9 mol mol Cr −1 with selectivity of around 93 % at 50 °C for 20 h, which is significantly higher than those of most reported catalysts. The superior catalytic performance can be attributed to the synergistic effect between single Cr atoms and TiO 2 support. Combining catalytic kinetics, electron paramagnetic resonance, and control experiment results, the methane conversion mechanism was proposed as a methyl radical pathway to form CH 3 OH and CH 3 OOH first, and then the generated CH 3 OH is further oxidized to HOCH 2 OOH and HCOOH.