A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Reducing the Irreducible : Dispersed Metal Atoms Facilitate Reduction of Irreducible Oxides (2022)

Korpelin, V., Melander, M. M., & Honkala, K. (2022). Reducing the Irreducible : Dispersed Metal Atoms Facilitate Reduction of Irreducible Oxides. Journal of Physical Chemistry C, 126(2), 933-945. https://doi.org/10.1021/acs.jpcc.1c08979

JYU-tekijät tai -toimittajat

Korpelin, Ville
Melander, Marko
Honkala, Karoliina

Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Korpelin, Ville; Melander, Marko M.; Honkala, Karoliina

Lehti tai sarja: Journal of Physical Chemistry C

ISSN: 1932-7447

eISSN: 1932-7455

Julkaisuvuosi: 2022

Ilmestymispäivä: 10.01.2022

Volyymi: 126

Lehden numero: 2

Artikkelin sivunumerot: 933-945

Kustantaja: American Chemical Society (ACS)

Julkaisumaa: Yhdysvallat (USA)

Julkaisun kieli: englanti

DOI: https://doi.org/10.1021/acs.jpcc.1c08979

Julkaisun avoin saatavuus: Avoimesti saatavilla

Julkaisukanavan avoin saatavuus: Osittain avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/79312

Rinnakkaistallenteen verkko-osoite (pre-print): https://chemrxiv.org/engage/chemrxiv/article-details/614c375ab1d4a6c2ea917354

Tiivistelmä

Oxide reducibility is a central concept quantifying the role of the support in catalysis. While reducible oxides are often considered catalytically active, irreducible oxides are seen as inert supports. Enhancing the reducibility of irreducible oxides has, however, emerged as an effective way to increase their catalytic activity while retaining their inherent thermal stability. In this work, we focus on the prospect of using single metal atoms to increase the reducibility of a prototypical irreducible oxide, zirconia. Based on extensive self-consistent DFT+U calculations, we demonstrate that single metal atoms significantly improve and tune the surface reducibility of zirconia. Detailed analysis of the observed single atom induced reducibility allows us to attribute the enhanced reducibility to strong interactions between the metal atom and the electrons trapped in the vacancy and d–p orbital interactions between the metal atom and oxygen. This analysis enables transferring the obtained theoretical understanding to other irreducible oxides as well. The detailed understanding of how oxide reducibility can be tuned offers precise control over the catalytic properties of metal oxides.

YSO-asiasanat: katalyysi; hapetus-pelkistysreaktio; oksidit; zirkoniumoksidi; metallit; adsorptio; pintakemia