A Highly Stable Copper-Based Catalyst for Clarifying the Catalytic Roles of Cu0 and Cu+ Species in Methanol Dehydrogenation.
Angew Chem Int Ed Engl
; 57(7): 1836-1840, 2018 02 12.
Article
in En
| MEDLINE
| ID: mdl-29314496
ABSTRACT
Identification of the active copper species, and further illustration of the catalytic mechanism of Cu-based catalysts is still a challenge because of the mobility and evolution of Cu0 and Cu+ species in the reaction process. Thus, an unprecedentedly stable Cu-based catalyst was prepared by uniformly embedding Cu nanoparticles in a mesoporous silica shell allowing clarification of the catalytic roles of Cu0 and Cu+ in the dehydrogenation of methanol to methyl formate by combining isotope-labeling experiment, inâ
situ spectroscopy, and DFT calculations. It is shown that Cu0 sites promote the cleavage of the O-H bond in methanol and of the C-H bond in the reaction intermediates CH3 O and H2 COOCH3 which is formed from CH3 O and HCHO, whereas Cu+ sites cause rapid decomposition of formaldehyde generated on the Cu0 sites into CO and H2 .
Full text:
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Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
Angew Chem Int Ed Engl
Year:
2018
Type:
Article