Header

UZH-Logo

Maintenance Infos

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


Hoes, Marie; Muhich, Christopher L; Jacot, Roger; Patzke, Greta R; Steinfeld, Aldo (2017). Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2. Journal of Materials Chemistry A, 5(36):19476-19484.

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.

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.

Statistics

Citations

Dimensions.ai Metrics
1 citation in Web of Science®
1 citation in Scopus®
1 citation in Microsoft Academic
Google Scholar™

Altmetrics

Downloads

4 downloads since deposited on 09 Feb 2018
4 downloads since 12 months
Detailed statistics

Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 University Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Language:English
Date:2017
Deposited On:09 Feb 2018 07:55
Last Modified:18 Apr 2018 11:49
Publisher:Royal Society of Chemistry
ISSN:2050-7488
Funders:SNF Project REDOX – Grant No. 200021_16243, Swiss State Secretariat for Education, Research and Innovation (Grant No. 15.0330), ERC Project SUNFUELS – Grant No. 32054
OA Status:Hybrid
Publisher DOI:https://doi.org/10.1039/C7TA05824A
Project Information:
  • : FunderH2020
  • : Grant ID654408
  • : Project TitleSUN-to-LIQUID - SUNlight-to-LIQUID: Integrated solar-thermochemical synthesis of liquid hydrocarbon fuels
  • : FunderSNSF
  • : Grant ID
  • : Project TitleSNF Project REDOX – Grant No. 200021_16243
  • : Funder
  • : Grant ID
  • : Project TitleSwiss State Secretariat for Education, Research and Innovation (Grant No. 15.0330)
  • : Funder
  • : Grant ID
  • : Project TitleERC Project SUNFUELS – Grant No. 32054

Download

Download PDF  'Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H2O and CO2'.
Preview
Content: Published Version
Filetype: PDF
Size: 1MB
View at publisher
Licence: Creative Commons: Attribution 4.0 International (CC BY 4.0)