Journal
ENERGY & FUELS
Volume 28, Issue 6, Pages 4088-4095Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ef500610n
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Funding
- National Science Foundation [EFRI-1038307]
- University of Minnesota Initiative for Renewable Energy and the Environment
- National Science Foundation Graduate Research Fellowship Program (NSF-GRFP) [00039202]
- Directorate For Engineering
- Emerging Frontiers & Multidisciplinary Activities [1038307] Funding Source: National Science Foundation
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The present work considers the convergence of two approaches for syngas production: solar fuels via the cerium oxide (ceria) redox cycle and the partial oxidation of methane. The chemical thermodynamics of the ceria-methane system reveal that coupling the reduction of ceria to the partial oxidation of methane enables isothermal cycling at temperatures as low as 1223 K with the additional production of high-quality syngas during the reduction step. The equilibrium non-stoichiometry of the oxidation step has a substantial impact on the conversion of the oxidizer to fuel, with important implications for cycle efficiency. A model of the process thermodynamics is used to evaluate the efficiency of the cycle and its sensitivity to oxidation non-stoichiometry, temperature, and concentration ratio. Reduction with methane enables significant gains in efficiency over other proposed approaches, with plausible solar-to-fuel efficiencies reaching 40% without any heat recovery.
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