期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 3, 页码 1216-1219出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201913309
关键词
chromium; heterogeneous catalysis; methane; single atoms; synergistic catalysis
资金
- National Basic Research Program of China (973 Program) [2018YFA0208504, 2018YFA0703503, 2018YFA0208504] Funding Source: Medline
- Youth Innovation Promotion Association of the Chinese Academy of Sciences [2017049] Funding Source: Medline
- Key Programme [21932006, 21573245] Funding Source: Medline
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 H2O2 as oxidant under mild conditions. The highest yield for C1 oxygenated products can be reached as 57.9molmol(Cr)(-1) with selectivity of around 93% at 50 degrees C for 20h, 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 TiO2 support. Combining catalytic kinetics, electron paramagnetic resonance, and control experiment results, the methane conversion mechanism was proposed as a methyl radical pathway to form CH3OH and CH3OOH first, and then the generated CH3OH is further oxidized to HOCH2OOH and HCOOH.
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