Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 115, Issue 43, Pages 21022-21033Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp2071315
Keywords
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Funding
- University of Minnesota Initiative for Renewable Energy and the Environment
- National Science Foundation [EFRI-1038307, DMR-0704312]
- University of Minnesota
- Emerging Frontiers & Multidisciplinary Activities
- Directorate For Engineering [1038307] Funding Source: National Science Foundation
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To enhance the kinetics and overall production of renewable H-2 fuel through a two-step thermochemical water splitting cycle, three-dimensionally ordered macroporous (3DOM) Ce1-xZrxO2 (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 m(2)/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 H-2 compared to the single-phase Pechini samples. Increasing the content of Zr in the mixed oxides also stabilized the 3DOM structure at 825 degrees C. All 3DOM Ce1-xZrxO2 materials exhibited significantly faster kinetics during water splitting compared to sintered, micrometer-sized CeO2 granules. Pechini-derived 3DOM Ce0.8Zr0.2O2 maximized both H-2 production and peak production rates, offering better catalytic performance over 3DOM CeO2.
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