Dynamic Interplay between Copper Tetramers and Iron
Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons
under Mild Conditions
Version 2 2020-04-09, 23:43Version 2 2020-04-09, 23:43
Version 1 2019-07-29, 17:23Version 1 2019-07-29, 17:23
Posted on 2020-04-09 - 23:43
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 Cu4/Fe2O3 catalyst,
yielding an enrichment of surface Cu4–Fe2+ species under reaction conditions that boosts CO2 hydrogenation
at near-atmospheric pressures. During reaction, Cu4 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 C1/C3 hydrocarbon production in a high-temperature regime. The
discovery of highly active Cu4–Fe2+ sites
thus provides new insights for the atomic-level design of copper catalyst
toward high-efficiency CO2 conversion under mild conditions.
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Yang, Bing; Yu, Xin; Halder, Avik; Zhang, Xiaoben; Zhou, Xiong; Mannie, Gilbère J. A.; et al. (2019). Dynamic Interplay between Copper Tetramers and Iron
Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons
under Mild Conditions. ACS Publications. Collection. https://doi.org/10.1021/acssuschemeng.9b01561