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Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions
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SYSNO ASEP 0510109 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions Author(s) Yang, B. (CN)
Yu, X. (CN)
Halder, A. (US)
Zhang, X. (CN)
Zhou, X. (CN)
Mannie, G. J. A. (CN)
Tyo, E. C. (US)
Pellin, M. J. (US)
Seifert, S. (US)
Su, D. (CN)
Vajda, Štefan (UFCH-W) RID, ORCIDSource Title ACS Sustainable Chemistry & Engineering. - : American Chemical Society - ISSN 2168-0485
Roč. 7, č. 17 (2019), s. 14435-14442Number of pages 8 s. Language eng - English Country US - United States Keywords oxygen reduction reaction ; carbon-dioxide ; active-sites ; catalysts ; hydrogenation ; cu ; clusters ; water ; xps ; interface ; CO2 conversion Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry Method of publishing Limited access Institutional support UFCH-W - RVO:61388955 UT WOS 000484071600015 EID SCOPUS 85070542684 DOI 10.1021/acssuschemeng.9b01561 Annotation 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. Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2020 Electronic address http://hdl.handle.net/11104/0300660
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