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Dynamical Properties of a Ru/MgAl_(2)O_4 Catalyst during Reduction and Dry Methane Reforming

Kehres, Jan and Jakobsen, Jon Geest and Andreasen, Jens Wenzel and Wagner, Jakob B. and Liu, Haihua and Molenbroek, Alfons and Sehested, Jens and Chorkendorff, Ib and Vegge, Tejs (2012) Dynamical Properties of a Ru/MgAl_(2)O_4 Catalyst during Reduction and Dry Methane Reforming. Journal of Physical Chemistry C, 116 (40). pp. 121407-21415. ISSN 1932-7447.

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Combined in situ small- and wide-angle X-ray scattering (SAXS/WAXS) studies were performed in a new laboratory setup to investigate the dynamical properties of a ruthenium/spinel ( Ru/MgAl_2O_4) catalyst, w(Ru) = 4 wt %, during the reduction and subsequent dry methane reforming. The Ru particles in the fresh catalyst sample were found to be partially oxidized. High-resolution transmission electron microscopy (HRTEM) indicated a coexistence of pure Ru and RuO_2 nanoparticles. Reduction in hydrogen occurred at a temperature between 373 and 393 K. The mean particle diameter as refined from SAXS of the size regime attributed to scattering from Ru/RuO_2-particles decreases slightly by about 0.2 nm during the reduction. Dry methane reforming experiments were performed in a temperature interval from 723 to 1023 K by applying a gas mixture of carbon dioxide and methane in molar ratio of 3:1. The catalyst did not show any deactivation during the experiment of overall 32 h, indicated by stable turnover frequencies for methane. The mean Ru-particle diameter remained constant during the dry methane reforming experiments, revealing a high sintering stability of the Ru/MgAl_2O_4 catalyst.

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Additional Information:© 2012 American Chemical Society. Received: July 13, 2012; Revised: September 12, 2012; Published: September 18, 2012. We thank Steen Bang, Ove Rasmussen, Torben Kjær, and Jens Borchsenius for maintenance of the equipment and technical support during the implementation of the in situ laboratory setup, Hjalte Sylvest Jacobsen for improvement of the WAXS 1D data transformation, Henning Engelbrecht for guidance regarding LabVIEW and data acquisition during the implementation of the sample gas system, and the Copenhagen Graduate School for Nanoscience and Nanotechnology (C:O:N:T) and Haldor Topsøe A/S for financial support.
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Copenhagen Graduate School for Nanoscience and NanotechnologyUNSPECIFIED
Issue or Number:40
Record Number:CaltechAUTHORS:20121112-112231131
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Official Citation:Dynamical Properties of a Ru/MgAl2O4 Catalyst during Reduction and Dry Methane Reforming Jan Kehres, Jon Geest Jakobsen, Jens Wenzel Andreasen, Jakob B. Wagner, Haihua Liu, Alfons Molenbroek, Jens Sehested, Ib Chorkendorff, and Tejs Vegge The Journal of Physical Chemistry C 2012 116 (40), 21407-21415
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:35411
Deposited By: Jason Perez
Deposited On:12 Nov 2012 22:46
Last Modified:03 Oct 2019 04:28

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