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Title: Titania-Supported Single-Atom Platinum Catalyst for Water-Gas Shift Reaction

 [1];  [1]
  1. University of South Carolina, Department of Chemical Engineering, 301 South Main Street 29208 Columbia, South Carolina USA
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Journal Article: Publisher's Accepted Manuscript
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Journal Volume: 89; Journal Issue: 10; Related Information: CHORUS Timestamp: 2017-10-20 15:52:42; Journal ID: ISSN 0009-286X
Wiley Blackwell (John Wiley & Sons)
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Citation Formats

Ammal, Salai Cheettu, and Heyden, Andreas. Titania-Supported Single-Atom Platinum Catalyst for Water-Gas Shift Reaction. Germany: N. p., 2017. Web. doi:10.1002/cite.201700046.
Ammal, Salai Cheettu, & Heyden, Andreas. Titania-Supported Single-Atom Platinum Catalyst for Water-Gas Shift Reaction. Germany. doi:10.1002/cite.201700046.
Ammal, Salai Cheettu, and Heyden, Andreas. 2017. "Titania-Supported Single-Atom Platinum Catalyst for Water-Gas Shift Reaction". Germany. doi:10.1002/cite.201700046.
title = {Titania-Supported Single-Atom Platinum Catalyst for Water-Gas Shift Reaction},
author = {Ammal, Salai Cheettu and Heyden, Andreas},
abstractNote = {},
doi = {10.1002/cite.201700046},
journal = {Chemie-Ingenieur-Technik},
number = 10,
volume = 89,
place = {Germany},
year = 2017,
month = 9

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This content will become publicly available on September 5, 2018
Publisher's Accepted Manuscript

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  • WGS reaction has been investigated on catalysts based on platinum supported over CeO{sub 2}, TiO{sub 2} and Ce-modified TiO{sub 2}. XPS and XANES analyses performed on calcined catalysts revealed a close contact between Pt precursors and cerium species on CeO{sub 2} and Ce-modified TiO{sub 2} supports. TPR results corroborate the intimate contact between Pt and cerium entities in the Pt/Ce-TiO{sub 2} catalyst that facilitates the reducibility of the support at low temperatures while the Ce-O-Ti surface interactions established in the Ce-modified TiO{sub 2} support decreases the reduction of TiO{sub 2} at high temperature. The changes in the support reducibility leadsmore » to significant differences in the WGS activity of the studied catalysts. Pt supported on Ce-modified TiO{sub 2} support exhibits better activity than those corresponding to individual CeO{sub 2} and TiO{sub 2}-supported catalysts. Additionally, the Ce-TiO{sub 2}-supported catalyst displays better stability at reaction temperatures higher than 573 K that observed on pure TiO{sub 2}-supported counterpart. Activity measurements, when coupled with the physicochemical characterization of catalysts suggest that the modifications in the surface reducibility of the support play an essential role in the enhancement of activity and stability observed when Pt is supported on the Ce-modified TiO{sub 2} substrate.« less
  • This study was focused to investigate the roles of Cu and Pd in CuPd/CeO2 bimetallic catalysts containing 20-30 wt% Cu and 0.5-1 wt% Pd used in the oxygen-assisted water-gas shift (OWGS) reaction employing a combined bulk and surface characterization techniques such as XRD, TPR, CO chemisorption, and in-situ XPS. The catalytic activity for CO conversion and the stability of catalyst during on-stream operation increased by the addition of Cu to Pd/CeO2 or Pd to Cu/CeO2 monometallic catalysts, especially when the OWGS reaction was performed under low temperatures, below 200oC. The bimetallic catalyst after leaching with nitric acid retained about 60%more » of its original activity. The TPR of monometallic Cu/CeO2 showed reduction of CuO supported on CeO2 in two distinct regions, around 150 and 250oC. The high temperature peak disappeared and reduction occurred in a single step around 150oC upon Pd addition. The Pd dispersion decreased from 38.5% for Pd/CeO2 to below 1% for CuPd/CeO2 bimetallic catalyst. In-situ XPS studies showed a shift in Cu 2p peaks toward lower binding energy (BE) with concommitant shift in the Pd 3d peaks toward higher BE. Addition of Pd decreased the surface Cu concentration while the concentration of Pd remained unaltered. All these observations indicated the formation of Cu-Pd surface alloy. The valence band XP spectra collected below 10 eV corroborated the core level XP spectra and indicated that Cu is mainly involved in the catalytic reaction. The improved catalytic activity and stability of CuPd/CeO2 bimetallic catalyst was attributed to the alloy formation.« less
  • Selective hydrogenation of [alpha],[beta]-unsaturated aldehydes into allylic alcohols remains a difficult task to achieve, especially in the gas phase, when working with heterogeneous catalysts. Crotonaldehyde hydrogenation is a complex reaction that has been modeled using results from a standard gas flow system. The obtained results give rise to the formation of a reaction network and an elementary step mechanism derived from steady-state kinetics. The selectivity of the system to give crotyl alcohol is explained in terms of the surface electronic gas model.
  • We report a new method for stabilizing appreciable loadings (~1 wt %) of isolated gold atoms on titania and show that these catalyze the low-temperature water-gas shift reaction. The method combines a typical gold deposition/precipitation method with UV irradiation of the titania support suspended in ethanol. Dissociation of H 2O on the thus-created Au–O–TiO x sites is facile. At higher gold loadings, nanoparticles are formed, but they were shown to add no further activity to the atomically bound gold on titania. Removal of this “excess” gold by sodium cyanide leaching leaves the activity intact and the atomically dispersed gold stillmore » bound on titania. The new materials may catalyze a number of other reactions that require oxidized active metal sites.« less