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Title: Copper cluster size effect in methanol synthesis from CO2

Journal Article · · Journal of Physical Chemistry. C

Here, size-selected Cun catalysts (n = 3, 4, 20) were synthesized on Al2O3 thin films using mass-selected cluster deposition. A systematic study of size and support effects was carried out for CO2 hydrogenation at atmospheric pressure using a combination of in situ grazing incidence X-ray absorption spectroscopy, catalytic activity measurement, and first-principles calculations. The catalytic activity for methanol synthesis is found to strongly vary as a function of the cluster size; the Cu4/Al2O3 catalyst shows the highest turnover rate for CH3OH production. With only one atom less than Cu4, Cu3 showed less than 50% activity. Density functional theory calculations predict that the activities of the gas-phase Cu clusters increase as the cluster size decreases; however, the stronger charge transfer interaction with Al2O3 support for Cu3 than for Cu4 leads to remarkably reduced binding strength between the adsorbed intermediates and supported Cu3, which subsequently results in a less favorable energetic pathway to transform carbon dioxide to methanol.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1372481
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 19 Vol. 121; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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