期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 24, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202204116
关键词
Methane; Oxygenates; Reaction Mechanisms; Selective Oxidation; Tandem Catalysis
资金
- Natural Science Foundation of China [91945301]
- National Key RAMP
- D Program of China [2021YFF0500702]
- Program of Shanghai Academic/Technology Research Leader [20XD1404000]
- Key Research Program of Frontier Sciences of the Chinese Academy of Sciences [QYZDB-SSW-SLH035]
- Transformational Technologies for Clean Energy and Demonstration of CAS [XDA21020600]
- Strategic Priority Research Program of CAS [XDA21020600]
- Youth Innovation Promotion Association of CAS
A bimetallic catalyst PdCu/Z-5 was developed for the selective oxidation of methane to oxygenates at low temperature, achieving high yield and selectivity through the synergistic effect of PdO nanoparticles and Cu single atoms.
Selective oxidation of methane to oxygenates with O-2 under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O-2 in the presence of H-2 at low temperature (120 degrees C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g(Pd)(-1) h(-1) (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %. Control experiments and mechanistic studies revealed that PdO nanoparticles promoted the in situ generation of H2O2 from O-2 and H-2, while Cu single atoms not only accelerated the activation of H2O2 for the generation of abundant hydroxyl radicals (OH)-O-center dot) from H2O2 decomposition, but also enabled the homolytic cleavage of CH4 by (OH)-O-center dot to methyl radicals ((CH3)-C-center dot). Subsequently, the (OH)-O-center dot reacted quickly with the (CH3)-C-center dot to form CH3OH with high selectivity.
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