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A thermochemical study of ceria: exploiting an old material for new modes of energy conversion and CO_2 mitigation

Chueh, William C. and Haile, Sossina M. (2010) A thermochemical study of ceria: exploiting an old material for new modes of energy conversion and CO_2 mitigation. Philosophical Transactions A: Mathematical, Physical and Engineering Sciences, 368 (1923). pp. 3269-3294. ISSN 1364-503X . http://resolver.caltech.edu/CaltechAUTHORS:20100709-144845953

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Abstract

We present a comprehensive thermodynamic and kinetic analysis of the suitability of cerium oxide (ceria) for thermochemical fuel production. Both portions of the two-step cycle, (i) oxygen release from the oxide at 1773 and 1873 K under inert atmosphere, and (ii) hydrogen release upon hydrolysis at 1073 K, are examined theoretically as well as experimentally. We observe gravimetric fuel productivity that is in quantitative agreement with equilibrium, thermogravimetric studies of ceria. Despite the non-stoichiometric nature of the redox cycle, in which only a portion of the cerium atoms change their oxidation state, the fuel productivity of 8.5–11.8 ml of H2 per gram of ceria is competitive with that of other solid-state thermochemical cycles currently under investigation. The fuel production rate, which is also highly attractive, at a rate of 4.6–6.2 ml of H_2 per minute per gram of ceria, is found to be limited by a surface-reaction step rather than by ambipolar bulk diffusion of oxygen through the solid ceria. An evaluation of the thermodynamic efficiency of the ceria-based thermochemical cycle suggests that, even in the absence of heat recovery, solar-to-fuel conversion efficiencies of 16 to 19 per cent can be achieved, assuming a suitable method for obtaining an inert atmosphere for the oxygen release step.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1098/rsta.2010.0114 DOIArticle
http://rsta.royalsocietypublishing.org/content/368/1923/3269PublisherArticle
ORCID:
AuthorORCID
Haile, Sossina M.0000-0002-5293-6252
Additional Information:© 2010 The Royal Society. One contribution of 13 to a Discussion Meeting Issue ‘Energy materials to combat climate change’. This work was funded by the National Science Foundation (CBET-0829114) and eSolar Inc. The authors are grateful for insightful discussions with Prof. Aldo Steinfeld, Dr Philip Gleckman and Dr Francesco Ciucci.
Funders:
Funding AgencyGrant Number
NSFCBET-0829114
eSolar Inc.UNSPECIFIED
Subject Keywords:cerium oxide; thermochemical cycles; hydrogen; water splitting; syngas
Record Number:CaltechAUTHORS:20100709-144845953
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20100709-144845953
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:18977
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:09 Jul 2010 22:35
Last Modified:16 Sep 2015 00:55

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