Copper cluster size effect in methanol synthesis from CO2

Yang, Bing; Liu, Cong; Halder, Avik; Tyo, Eric C.; Martinson, Alex B. F.; Seifert, Sonke; Zapol, Peter; Curtiss, Larry A.; Vajda, Stefan

doi:10.1021/acs.jpcc.7b01835

Title: Copper cluster size effect in methanol synthesis from CO₂

Journal Article · 07 May 2017 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.7b01835 · OSTI ID:1372481

Yang, Bing ^[1]; Liu, Cong ^[1]; Halder, Avik ^[1]; Tyo, Eric C. ^[1];

^[1]; Seifert, Sonke ^[1];

^[1];

^[1]

Argonne National Lab. (ANL), Lemont, IL (United States)

Here, size-selected Cu_n 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.

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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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Title: Copper cluster size effect in methanol synthesis from CO₂