Control of heterogeneity in nanostructured Ce1-xZr xO2 Binary oxides for enhanced thermal stability and water splitting activity

Nicholas D. Petkovich, Stephen G. Rudisill, Luke J. Venstrom, Daniel B. Boman, Jane H. Davidson, Andreas Stein

Research output: Contribution to journalArticlepeer-review

112 Scopus citations

Abstract

To enhance the kinetics and overall production of renewable H2 fuel through a two-step thermochemical water splitting cycle, three-dimensionally ordered macroporous (3DOM) Ce1-xZr xO2 (x = 0, 0.1, 0.2, 0.3, 0.4, and 0.5) materials were synthesized via colloidal crystal templating. The interconnected macropore system in these materials facilitates ready access to a relatively large active surface area (tens of m2/g), which benefits the heterogeneous reaction. Two different synthetic routes were employed, a methanolic solution of metal chloride salts, and a Pechini-type gel. These routes produced significant differences in the compositional homogeneity of the resulting mixed oxide. 3DOM Ce1-xZrxO2 synthesized with methanolic precursors had distinct CeO2- and ZrO2-rich domains, whereas the Pechini samples contained only a single phase. At higher Zr content, heterogeneities present in the samples from the methanolic synthesis increased both the productivity and peak production rates of H2 compared to the single-phase Pechini samples. Increasing the content of Zr in the mixed oxides also stabilized the 3DOM structure at 825 °C. All 3DOM Ce 1-xZrxO2 materials exhibited significantly faster kinetics during water splitting compared to sintered, micrometer-sized CeO2 granules. Pechini-derived 3DOM Ce0.8Zr 0.2O2 maximized both H2 production and peak production rates, offering better catalytic performance over 3DOM CeO 2.

Original languageEnglish (US)
Pages (from-to)21022-21033
Number of pages12
JournalJournal of Physical Chemistry C
Volume115
Issue number43
DOIs
StatePublished - Nov 3 2011

Fingerprint

Dive into the research topics of 'Control of heterogeneity in nanostructured Ce<sub>1-x</sub>Zr <sub>x</sub>O<sub>2</sub> Binary oxides for enhanced thermal stability and water splitting activity'. Together they form a unique fingerprint.

Cite this