Effect of cerium incorporation into zirconia on the activity ofCu/ZrO2 for methanol synthesis via CO hydrogenation

PDF Version Also Available for Download.

Description

The effects of Ce incorporation into ZrO2 on the catalyticperformance of Cu/ZrO2 for the hydrogenation of CO have beeninvestigated. A Ce0.3Zr0.7O2 solid solution was synthesized by forcedhydrolysis at low pH. After calcination at 873 K, XRD and Ramanspectroscopy characterization indicated that the Ce0.3Zr0.7O2 had a t''crystal structure. 1.2 wt percent Cu/Ce0.3Zr0.7O2 exhibited H2consumption peaks at low temperature (<473 K) during H2-TPRindicating a significant fraction (~; 70 percent) of Ce4+ is reduced toCe3+. 1.2 wt percent Cu/Ce0.3Zr0.7O2 is 2.7 times more active formethanol synthesis than 1.2 wt percent Cu/m-ZrO2 at 3.0 MPa attemperatures between 473 and 523 K and exhibits a ... continued below

Creation Information

Pokrovski, Konstantin A.; Rhodes, Michael D. & Bell, Alexis T. August 24, 2005.

Context

This article is part of the collection entitled: Office of Scientific & Technical Information Technical Reports and was provided by UNT Libraries Government Documents Department to Digital Library, a digital repository hosted by the UNT Libraries. More information about this article can be viewed below.

Who

People and organizations associated with either the creation of this article or its content.

Provided By

UNT Libraries Government Documents Department

Serving as both a federal and a state depository library, the UNT Libraries Government Documents Department maintains millions of items in a variety of formats. The department is a member of the FDLP Content Partnerships Program and an Affiliated Archive of the National Archives.

Contact Us

What

Descriptive information to help identify this article. Follow the links below to find similar items on the Digital Library.

Description

The effects of Ce incorporation into ZrO2 on the catalyticperformance of Cu/ZrO2 for the hydrogenation of CO have beeninvestigated. A Ce0.3Zr0.7O2 solid solution was synthesized by forcedhydrolysis at low pH. After calcination at 873 K, XRD and Ramanspectroscopy characterization indicated that the Ce0.3Zr0.7O2 had a t''crystal structure. 1.2 wt percent Cu/Ce0.3Zr0.7O2 exhibited H2consumption peaks at low temperature (<473 K) during H2-TPRindicating a significant fraction (~; 70 percent) of Ce4+ is reduced toCe3+. 1.2 wt percent Cu/Ce0.3Zr0.7O2 is 2.7 times more active formethanol synthesis than 1.2 wt percent Cu/m-ZrO2 at 3.0 MPa attemperatures between 473 and 523 K and exhibits a higher selectivity tomethanol. In-situ infrared spectroscopy shows that, analogous toCu/m-ZrO2, the primary surface species on Cu/Ce0.3Zr0.7O2 during COhydrogenation are formate and methoxide species. A shift in the bandposition of the bridged methoxide species indicated that some of thesegroups were bonded to both Zr4+ and Ce3+ cations. For both catalysts, therate-limiting step for methanol synthesis is the reductive elimination ofmethoxide species. The higher rate of methanol synthesis onCu/Ce0.3Zr0.7O2 relative to Cu/m-ZrO2 was primarily due to a ~; 2.4 timeshigher apparent rate constant, kapp, for methoxide hydrogenation, whichis attributed to the higher surface concentration of H atoms on theformer catalyst. The increased capacity of the Ce-containing catalyst isattributed to interactions of H atoms with Ce-O pairs present at thesurface of the oxide phase.

Source

  • Journal Name: Journal of Catalysis; Journal Volume: 235; Related Information: Journal Publication Date: 2005

Language

Item Type

Identifier

Unique identifying numbers for this article in the Digital Library or other systems.

  • Report No.: LBNL--57002
  • Grant Number: DE-AC02-05CH11231
  • DOI: 10.1016/j.jcat.2005.09.002 | External Link
  • Office of Scientific & Technical Information Report Number: 900698
  • Archival Resource Key: ark:/67531/metadc883794

Collections

This article is part of the following collection of related materials.

Office of Scientific & Technical Information Technical Reports

What responsibilities do I have when using this article?

When

Dates and time periods associated with this article.

Creation Date

  • August 24, 2005

Added to The UNT Digital Library

  • Sept. 22, 2016, 2:13 a.m.

Description Last Updated

  • Sept. 29, 2016, 2:27 p.m.

Usage Statistics

When was this article last used?

Yesterday: 0
Past 30 days: 1
Total Uses: 4

Interact With This Article

Here are some suggestions for what to do next.

Start Reading

PDF Version Also Available for Download.

Citations, Rights, Re-Use

Pokrovski, Konstantin A.; Rhodes, Michael D. & Bell, Alexis T. Effect of cerium incorporation into zirconia on the activity ofCu/ZrO2 for methanol synthesis via CO hydrogenation, article, August 24, 2005; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc883794/: accessed September 26, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.