Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions

0510109 - ÚFCH JH 2020 RIV US eng J - Článek v odborném periodiku
Yang, B. - Yu, X. - Halder, A. - Zhang, X. - Zhou, X. - Mannie, G. J. A. - Tyo, E. C. - Pellin, M. J. - Seifert, S. - Su, D. - Vajda, Štefan
Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions.
ACS Sustainable Chemistry & Engineering. Roč. 7, č. 17 (2019), s. 14435-14442. ISSN 2168-0485. E-ISSN 2168-0485
GRANT EU: European Commission(XE) 810310
Institucionální podpora: RVO:61388955
Klíčová slova: oxygen reduction reaction * carbon-dioxide * active-sites * catalysts * hydrogenation * cu * clusters * water * xps * interface * CO2 conversion
Obor OECD: Physical chemistry
Impakt faktor: 7.632, rok: 2019
Způsob publikování: Omezený přístup

Atomically precise subnanometer catalysts are of significant interest because of their remarkable efficiency in a variety of catalytic reactions. However, the dynamic changes of active sites under reaction conditions, in particular, the transition of cluster-oxide interface structure have not yet been well-elucidated, lacking in situ measurements. By using multiple state-of-the-art in situ characterizations, here we show a dynamic interplay between copper tetramers and iron oxides in a single-size Cu-4/Fe2O3 catalyst, yielding an enrichment of surface Cu-4-Fe2+ species under reaction conditions that boosts CO2 hydrogenation at near-atmospheric pressures. During reaction, Cu-4 clusters facilitate the reduction of Fe2O3 producing surface-rich Fe2+ species in the proximate sites. The as-formed Fe2+ species in return promotes CO2 activation and transformation over Cu4 cluster, resulting in strikingly high methanol synthesis at low temperatures and C-1/C-3 hydrocarbon production in a high-temperature regime. The discovery of highly active Cu-4-Fe2+ sites thus provides new insights for the atomic-level design of copper catalyst toward high-efficiency CO2 conversion under mild conditions.
Trvalý link: http://hdl.handle.net/11104/0300660