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Issue 36, 2017
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Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2

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Abstract

Paired charge-compensating doped ceria (PCCD) using trivalent and pentavalent cations are evaluated as redox materials for the thermochemical splitting of H2O and CO2. The oxygen nonstoichiometries of PCCD materials with formulas of Ce0.9A0.05Nb0.05O2 (A = Y, La, Sc) and CexLa(1−x)/2Nb(1−x)/2O2 (x = 0.75, 0.95) were measured in a thermogravimetric analyzer over a range of temperatures (T = 1173–1773 K) and oxygen partial pressures (pO2 = 10−15–10−1 atm). Undoped and single element doped ceria (Ce0.9B0.1O2 where B = Y, La, Nb, Hf) served as a reference. At any given set of T and pO2, the relative reduction extent follows Ce0.9Hf0.1O2 > Ce0.9Sc0.05Nb0.05O2 > Ce0.9Y0.05Nb0.05O2 > CexLa(1−x)/2Nb(1−x)/2O2 > CeO2 > solely trivalent or pentavalent doped ceria. The partial molar reduction enthalpies were determined using Van't Hoff analysis coupled to defect modeling and range from 360 to 410 kJ mol−1. A system efficiency model predicts that these PCCD materials have the potential of achieving high solar-to-fuel energy conversion efficiencies because of their balanced reduction and oxidation properties. Ce0.9Y0.05Nb0.05O2 in particular can outperform undoped ceria and reach efficiency values of 31% and 28% for H2 and CO production, respectively.

Graphical abstract: Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2

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Publication details

The article was received on 05 Jul 2017, accepted on 25 Aug 2017 and first published on 29 Aug 2017


Article type: Paper
DOI: 10.1039/C7TA05824A
Citation: J. Mater. Chem. A, 2017,5, 19476-19484
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    Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2

    M. Hoes, C. L. Muhich, R. Jacot, G. R. Patzke and A. Steinfeld, J. Mater. Chem. A, 2017, 5, 19476
    DOI: 10.1039/C7TA05824A

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