Understanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theory

Handle URI:
http://hdl.handle.net/10754/600129
Title:
Understanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theory
Authors:
Bayliss, Ryan D.; Cook, Stuart N.; Scanlon, David O.; Fearn, Sarah; Cabana, Jordi; Greaves, Colin; Kilner, John A.; Skinner, Stephen J.
Abstract:
© the Partner Organisations 2014. Recent reports of remarkably high oxide ion conduction in a new family of strontium silicates have been challenged. It has recently been demonstrated that, in the nominally potassium substituted strontium germanium silicate material, the dominant charge carrier was not the oxygen ion, and furthermore that the material was not single phase (R. D. Bayliss et. al., Energy Environ. Sci., 2014, DOI: 10.1039/c4ee00734d). In this work we re-investigate the sodium-doped strontium silicate material that was reported to exhibit the highest oxide ion conductivity in the solid solution, nominally Sr0.55Na0.45SiO2.775. The results show lower levels of total conductivity than previously reported and sub-micron elemental mapping demonstrates, in a similar manner to that reported for the Sr0.8K0.2Si0.5Ge0.5O2.9 composition, an inhomogeneous chemical distribution correlating with a multiphase material. It is also shown that the conductivity is not related to protonic mobility. A density functional theory computational approach provides a theoretical justification for these new results, related to the high energetic costs associated with oxygen vacancy formation. This journal is
Citation:
Bayliss RD, Cook SN, Scanlon DO, Fearn S, Cabana J, et al. (2014) Understanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theory. J Mater Chem A 2: 17919–17924. Available: http://dx.doi.org/10.1039/c4ta04299a.
Publisher:
Royal Society of Chemistry (RSC)
Journal:
J. Mater. Chem. A
Issue Date:
24-Sep-2014
DOI:
10.1039/c4ta04299a
Type:
Article
ISSN:
2050-7488; 2050-7496
Sponsors:
The authors thank Dr Ron Smith for assistance with the rapid NPD data collection (XB 1390067) via the GEM Xpress access route at ISIS, Rutherford Appleton Laboratories, Chilton, Didcot, UK. Xpress Access neutron beam time on GEM was provided by the UK Science and Technology Facilities Council (STFC). RDB would like to thank the King Abdullah University of Science and Technology for providing resources to complete the work. The UCL/Diamond work presented here made use of the UCL Legion HPC Facility, the IRIDIS cluster provided by the EPSRC funded Centre for Innovation (EP/K000144/1 and EP/K000136/1), and the ARCHER supercomputer through membership of the UK's HPC Materials Chemistry Consortium, which is funded by EPSRC grant EP/L000202.
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Full metadata record

DC FieldValue Language
dc.contributor.authorBayliss, Ryan D.en
dc.contributor.authorCook, Stuart N.en
dc.contributor.authorScanlon, David O.en
dc.contributor.authorFearn, Sarahen
dc.contributor.authorCabana, Jordien
dc.contributor.authorGreaves, Colinen
dc.contributor.authorKilner, John A.en
dc.contributor.authorSkinner, Stephen J.en
dc.date.accessioned2016-02-28T06:43:18Zen
dc.date.available2016-02-28T06:43:18Zen
dc.date.issued2014-09-24en
dc.identifier.citationBayliss RD, Cook SN, Scanlon DO, Fearn S, Cabana J, et al. (2014) Understanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theory. J Mater Chem A 2: 17919–17924. Available: http://dx.doi.org/10.1039/c4ta04299a.en
dc.identifier.issn2050-7488en
dc.identifier.issn2050-7496en
dc.identifier.doi10.1039/c4ta04299aen
dc.identifier.urihttp://hdl.handle.net/10754/600129en
dc.description.abstract© the Partner Organisations 2014. Recent reports of remarkably high oxide ion conduction in a new family of strontium silicates have been challenged. It has recently been demonstrated that, in the nominally potassium substituted strontium germanium silicate material, the dominant charge carrier was not the oxygen ion, and furthermore that the material was not single phase (R. D. Bayliss et. al., Energy Environ. Sci., 2014, DOI: 10.1039/c4ee00734d). In this work we re-investigate the sodium-doped strontium silicate material that was reported to exhibit the highest oxide ion conductivity in the solid solution, nominally Sr0.55Na0.45SiO2.775. The results show lower levels of total conductivity than previously reported and sub-micron elemental mapping demonstrates, in a similar manner to that reported for the Sr0.8K0.2Si0.5Ge0.5O2.9 composition, an inhomogeneous chemical distribution correlating with a multiphase material. It is also shown that the conductivity is not related to protonic mobility. A density functional theory computational approach provides a theoretical justification for these new results, related to the high energetic costs associated with oxygen vacancy formation. This journal isen
dc.description.sponsorshipThe authors thank Dr Ron Smith for assistance with the rapid NPD data collection (XB 1390067) via the GEM Xpress access route at ISIS, Rutherford Appleton Laboratories, Chilton, Didcot, UK. Xpress Access neutron beam time on GEM was provided by the UK Science and Technology Facilities Council (STFC). RDB would like to thank the King Abdullah University of Science and Technology for providing resources to complete the work. The UCL/Diamond work presented here made use of the UCL Legion HPC Facility, the IRIDIS cluster provided by the EPSRC funded Centre for Innovation (EP/K000144/1 and EP/K000136/1), and the ARCHER supercomputer through membership of the UK's HPC Materials Chemistry Consortium, which is funded by EPSRC grant EP/L000202.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.titleUnderstanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theoryen
dc.typeArticleen
dc.identifier.journalJ. Mater. Chem. Aen
dc.contributor.institutionUniversity of Illinois at Chicago, Chicago, United Statesen
dc.contributor.institutionImperial College London, London, United Kingdomen
dc.contributor.institutionMassachusetts Institute of Technology, Cambridge, United Statesen
dc.contributor.institutionDepartment of Chemistry, London, United Kingdomen
dc.contributor.institutionHarwell Science and Innovation Campus, Didcot Oxfordshire, United Kingdomen
dc.contributor.institutionUniversity of Birmingham, Birmingham B15 2TT, United Kingdomen
dc.contributor.institutionNishi-ku, Fukuoka 819-0395, Japanen
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