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

Marie Hoes; Christopher L. Muhich; Roger Jacot; Greta R. Patzke; Aldo Steinfeld

doi:10.1039/c7ta05824a

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

Marie Hoes, Christopher L. Muhich, Roger Jacot, Greta R. Patzke, Aldo Steinfeld

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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 Ce_0.9A_0.05Nb_0.05O₂ (A = Y, La, Sc) and Ce_xLa_(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 (p_O₂ = 10^-15-10^-1 atm). Undoped and single element doped ceria (Ce_0.9B_0.1O₂ where B = Y, La, Nb, Hf) served as a reference. At any given set of T and p_O₂, the relative reduction extent follows Ce_0.9Hf_0.1O₂ > Ce_0.9Sc_0.05Nb_0.05O₂ > Ce_0.9Y_0.05Nb_0.05O₂ > Ce_xLa_(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. Ce_0.9Y_0.05Nb_0.05O₂ in particular can outperform undoped ceria and reach efficiency values of 31% and 28% for H₂ and CO production, respectively.

Original language	English (US)
Pages (from-to)	19476-19484
Number of pages	9
Journal	Journal of Materials Chemistry A
Volume	5
Issue number	36
DOIs	https://doi.org/10.1039/c7ta05824a
State	Published - 2017
Externally published	Yes

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

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10.1039/c7ta05824a

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@article{9ddc1ef0cbb74a2e9dbdaa672c1e09f7,

title = "Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2",

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.",

author = "Marie Hoes and Muhich, {Christopher L.} and Roger Jacot and Patzke, {Greta R.} and Aldo Steinfeld",

note = "Publisher Copyright: {\textcopyright} 2017 The Royal Society of Chemistry.",

year = "2017",

doi = "10.1039/c7ta05824a",

language = "English (US)",

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TY - JOUR

T1 - Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2

AU - Hoes, Marie

AU - Muhich, Christopher L.

AU - Jacot, Roger

AU - Patzke, Greta R.

AU - Steinfeld, Aldo

PY - 2017

Y1 - 2017

N2 - 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.

AB - 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.

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DO - 10.1039/c7ta05824a

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EP - 19484

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 36

ER -

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

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