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Ceria Doped with Zirconium and Lanthanide Oxides to Enhance Solar Thermochemical Production of Fuels

Call, Friedemann and Roeb, Martin and Schmücker, Martin and Sattler, Christian and Pitz-Paal, Robert (2015) Ceria Doped with Zirconium and Lanthanide Oxides to Enhance Solar Thermochemical Production of Fuels. Journal of Physical Chemistry C, 119, pp. 6929-6938. ACS Publications. DOI: 10.1021/jp508959y ISSN 1932-7447

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Official URL: http://pubs.acs.org/doi/pdf/10.1021/jp508959y

Abstract

Developing an efficient redox material is crucial for thermochemical cycles that produce solar fuels (e.g., H2 and CO), enabling a sustainable energy supply. In this study, the effects of varying the rare-earth content y in Ce0.85‑yZr0.15REyO2−0.5y with RE = Y, La, Sm and Gd on the fuel productivity and long-term stability were investigated. Compared to the none-RE-doped reference material, Ce0.85Zr0.15O2, none of the compositions exhibits higher performances. However, long-term cycling of more than 80 cycles reveals enhanced performance due to rare-earth doping. Ce0.85Zr0.15O2 suffers from linear degradation of the yields and of the CO:O2 ratio r, which is attributed to declining oxidation kinetics, whereas for instance Ce0.82Zr0.15Sm0.03O1.99 features stable yields and kinetics. The suggested rationale behind is found in a vacancy-depleted region that occurs in the grains of Ce0.85Zr0.15O2. While cycling, the specific surface decreases and the impact of these regions on the reaction rate increases which leads to declining oxidation kinetics. In contrast, Ce0.82Zr0.15Sm0.03O1.99 displays structural vacancies corresponding to the Sm3+, which remain during oxidation. Because of these structural vacancies the oxygen bulk transport is enhanced resulting in a constant reaction rate. Because of the long-term cycling, rare-earth doping is in particular beneficial for the oxidation kinetics and hence, important for the technical realization of the process.

Item URL in elib:https://elib.dlr.de/97848/
Document Type:Article
Title:Ceria Doped with Zirconium and Lanthanide Oxides to Enhance Solar Thermochemical Production of Fuels
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Call, Friedemannfriedemann.call (at) dlr.deUNSPECIFIED
Roeb, MartinMartin.roeb (at) dlr.deUNSPECIFIED
Schmücker, MartinMartin.Schmuecker (at) dlr.deUNSPECIFIED
Sattler, Christianchristian.sattler (at) dlr.deUNSPECIFIED
Pitz-Paal, Robertrobert.pitz-paal (at) dlr.deUNSPECIFIED
Date:10 February 2015
Journal or Publication Title:Journal of Physical Chemistry C
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:119
DOI :10.1021/jp508959y
Page Range:pp. 6929-6938
Publisher:ACS Publications
ISSN:1932-7447
Status:Published
Keywords:Solar fuels, thermochemical, Ceria doped Zirconia, Fuels production
HGF - Research field:Energy
HGF - Program:Renewable Energies
HGF - Program Themes:Concentrating Solar Systems (old)
DLR - Research area:Energy
DLR - Program:E SF - Solar research
DLR - Research theme (Project):E - Solar Process Technology (old)
Location: Köln-Porz
Institutes and Institutions:Institute of Solar Research > Solare Verfahrenstechnik
Institute of Materials Research > Keramische Strukturwerkstoffe
Deposited By: Sattler, Prof. Dr. Christian
Deposited On:17 Aug 2015 13:22
Last Modified:06 Sep 2019 15:22

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