Modifying the Substrate-Dependent Pd/Fe 2 O 3 Catalyst-Support Synergism with ZnO Atomic Layer Deposition.

Autor: Shultz-Johnson LR; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States.; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States., Rahmani A; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States.; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States., Frisch J; Department Interface Design, Helmholtz-Zentrum Berlin Für Materialien und Energie GmbH (HZB), 12489 Berlin, Germany.; Energy Materials In-Situ Laboratory Berlin (EMIL), HZB, 12489 Berlin, Germany., Hsieh TE; Department Interface Design, Helmholtz-Zentrum Berlin Für Materialien und Energie GmbH (HZB), 12489 Berlin, Germany.; Energy Materials In-Situ Laboratory Berlin (EMIL), HZB, 12489 Berlin, Germany., Hu L; Department of Materials Science and Engineering, UCF, Orlando 32816, Florida, United States., Sosa J; NanoScience and Technology Center (NSTC), UCF, Orlando 32816, Florida, United States., Davy M; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States., Xie S; Department of Civil, Environmental, and Construction Engineering, UCF, Orlando 32816, Florida, United States., Beazley MJ; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States., Gao Z; Department of Materials Science and Engineering, UCF, Orlando 32816, Florida, United States., Golvari P; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States., Wang TH; Institute of Chemistry, Academia Sinica, Taipei 11529, Taiwan, Republic of China.; School of Environmental and Chemical Engineering, Zhaoqing University, Zhaoqing 526061, Guangdong, P. R. China., Ong TG; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States.; Institute of Chemistry, Academia Sinica, Taipei 11529, Taiwan, Republic of China., Rudawski NG; Herbert Wertheim College of Engineering Research Service Centers, University of Florida, Gainesville 32611, Florida, United States., Liu F; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States.; NanoScience and Technology Center (NSTC), UCF, Orlando 32816, Florida, United States.; Department of Civil, Environmental, and Construction Engineering, UCF, Orlando 32816, Florida, United States.; Department of Chemical and Environmental Engineering, University of California, Riverside 92521, California, United States., Banerjee P; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States.; Department of Materials Science and Engineering, UCF, Orlando 32816, Florida, United States.; NanoScience and Technology Center (NSTC), UCF, Orlando 32816, Florida, United States., Feng X; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States.; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States.; Department of Materials Science and Engineering, UCF, Orlando 32816, Florida, United States.; NanoScience and Technology Center (NSTC), UCF, Orlando 32816, Florida, United States.; Department of Physics, UCF, Orlando 32816, Florida, United States., Bär M; Department Interface Design, Helmholtz-Zentrum Berlin Für Materialien und Energie GmbH (HZB), 12489 Berlin, Germany.; Energy Materials In-Situ Laboratory Berlin (EMIL), HZB, 12489 Berlin, Germany.; Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (HI ERN), Albert-Einstein-Str. 15, 12489 Berlin, Germany.; Department of Chemistry and Pharmacy, Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Egerlandstr. 3, 91058 Erlangen, Germany., Jurca T; Department of Chemistry, University of Central Florida (UCF), Orlando 32816, Florida, United States.; Renewable Energy and Chemical Transformations Cluster (REACT), UCF, Orlando 32816, Florida, United States.; NanoScience and Technology Center (NSTC), UCF, Orlando 32816, Florida, United States.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2024 Jul 31; Vol. 16 (30), pp. 39387-39398. Date of Electronic Publication: 2024 Jul 20.
DOI: 10.1021/acsami.4c01528
Abstrakt: Low-loading Pd supported on Fe 2 O 3 nanoparticles was synthesized. A common nanocatalyst system with previously reported synergistic enhancement of reactivity that is attributed to the electronic interactions between Pd and the Fe 2 O 3 support. Fe 2 O 3 -selective precoalescence overcoating with ZnO atomic layer deposition (ALD), using Zn(CH 2 CH 3 ) 2 and H 2 O as precursors, dampens competitive hydrogenation reactivity at Fe 2 O 3 -based sites. The result is enhanced efficiency at the low-loading but high reactivity Pd sites. While this increases catalyst efficiency toward most aqueous redox reactions tested, it suppresses reactivity toward polyaromatic core substrates. X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) show minimal electronic impacts for the ZnO overcoat on the Pd particles, implying a predominantly physical site blocking effect as the reason for the modified reactivity. This serves as a proof-of-concept of not only stabilizing supported nanocatalysts but also altering reactivity with ultrathin ALD overcoats. The results point to a facile ALD route for selective enhancement of reactivity for low-loading Pd-based supported nanocatalysts.
Databáze: MEDLINE