Bimetallic Exsolved Heterostructures of Controlled Composition with Tunable Catalytic Properties.

Autor: Tsiotsias AI; Institut für Anorganische und Angewandte Chemie, Universität Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany.; Department of Chemical Engineering, University of Western Macedonia, 50100 Koila, Kozani, Greece., Ehrhardt B; Institut für Anorganische und Angewandte Chemie, Universität Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany., Rudolph B; Institut für Anorganische und Angewandte Chemie, Universität Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany., Nodari L; Department of Chemical Science, University of Padua, Via F. Marzolo, 1, 35122 Padova, Italy.; Institute of Condensed Matter Chemistry and Technologies for Energy, National Research Council. C.so Stati Uniti 4, 35127 Padova, Italy., Kim S; Department of Materials Science and Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea., Jung W; Department of Materials Science and Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea., Charisiou ND; Department of Chemical Engineering, University of Western Macedonia, 50100 Koila, Kozani, Greece., Goula MA; Department of Chemical Engineering, University of Western Macedonia, 50100 Koila, Kozani, Greece., Mascotto S; Institut für Anorganische und Angewandte Chemie, Universität Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany.
Jazyk: angličtina
Zdroj: ACS nano [ACS Nano] 2022 Jun 28; Vol. 16 (6), pp. 8904-8916. Date of Electronic Publication: 2022 Jun 16.
DOI: 10.1021/acsnano.1c11111
Abstrakt: In this paper, we show how the composition of bimetallic Fe-Ni exsolution can be controlled by the nature and concentration of oxygen vacancies in the parental matrix and how this is used to modify the performance of CO 2 -assisted ethane conversion. Mesoporous A-site-deficient La 0.4 Sr 0.6-α Ti 0.6 Fe 0.35 Ni 0.05 O 3±δ (0 ≤ α ≤ 0.2) perovskites with substantial specific surface area (>40 m 2 /g) enabled fast exsolution kinetics ( T < 500 °C, t < 1 h) of bimetallic Fe-Ni nanoparticles of increasing size (3-10 nm). Through the application of a multitechnique approach we found that the A-site deficiency determined the concentration of oxygen vacancies associated with iron, which controlled the Fe reduction. Instead of homogeneous bimetallic nanoparticles, the increasing Fe fraction from 37 to 57% led to the emergence of bimodal Fe/Ni 3 Fe systems. Catalytic tests showed superior stability of our catalysts with respect to commercial Ni/Al 2 O 3 . Ethane reforming was found to be the favored pathway, but an increase in selectivity toward ethane dehydrogenation occurred for the systems with a low metallic Fe fraction. The chance to control the reduction and growth processes of bimetallic exsolution offers interesting prospects for the design of advanced catalysts based on bimodal nanoparticle heterostructures.
Databáze: MEDLINE