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

Ryan D. Bayliss; Stuart N. Cook; David O. Scanlon; Sarah Fearn; Jordi Cabana; Colin Greaves; John A. Kilner; Stephen J. Skinner

doi:10.1039/c4ta04299a

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

Ryan D. Bayliss, Stuart N. Cook, David O. Scanlon, Sarah Fearn, Jordi Cabana, Colin Greaves, John A. Kilner, Stephen J. Skinner

Research output: Contribution to journal › Article › peer-review

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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

Original language	English (US)
Pages (from-to)	17919-17924
Number of pages	6
Journal	J. Mater. Chem. A
Volume	2
Issue number	42
DOIs	https://doi.org/10.1039/c4ta04299a
State	Published - Sep 24 2014
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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

abstract = "{\textcopyright} 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",

author = "Bayliss, {Ryan D.} and Cook, {Stuart N.} and Scanlon, {David O.} and Sarah Fearn and Jordi Cabana and Colin Greaves and Kilner, {John A.} and Skinner, {Stephen J.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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doi = "10.1039/c4ta04299a",

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AU - Bayliss, Ryan D.

AU - Cook, Stuart N.

AU - Scanlon, David O.

AU - Fearn, Sarah

AU - Cabana, Jordi

AU - Greaves, Colin

AU - Kilner, John A.

AU - Skinner, Stephen J.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2014/9/24

Y1 - 2014/9/24

N2 - © 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

AB - © 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

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JF - J. Mater. Chem. A

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ER -

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

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