TY - JOUR
T1 - Atomic-scale investigation of cation doping and defect clustering in the anti-perovskite Na3OCl sodium-ion conductor
AU - Goldmann, Benedek A.
AU - Clarke, Matt J.
AU - Dawson, James A.
AU - Islam, M. Saiful
N1 - Funding Information:
The authors thank the Faraday Institution CATMAT project (EP/ S003053/1, FIRG016) and the Bath URS studentship scheme for nancial support, and the HEC Materials Chemistry Consortium (EP/R029431) for Archer high-performance computing facilities. JAD also acknowledges Newcastle University for funding through a Newcastle Academic Track (NUAcT) Fellowship.
PY - 2022/2/7
Y1 - 2022/2/7
N2 - Solid-state batteries present potential advantages over their liquid-based electrolyte equivalents, including enhanced safety and increased energy density. In the search for novel solid electrolytes, the anti-perovskite family of materials are attracting growing interest. However, while there is significant work on Li-rich anti-perovskites, their Na-based counterparts and the atomistic effects of aliovalent doping on these materials are not fully characterised. Here, we investigate the effects on Na-ion conductivity of doping with divalent (Mg, Ca, Sr and Ba) and trivalent cations (Al and Ga), and of possible dopant-vacancy clustering in the anti-perovskite Na3OCl by employing atomistic simulation techniques. Our results highlight the potential of Mg2+, Ca2+, Al3+ and Ga3+ doping due to their favourable incorporation and increased Na-ion vacancy concentration. Local defect clustering and binding energies are analysed, and such effects inhibit Na-ion conductivity in the doped Na3OCl solid electrolyte at operating temperatures. These results provide a framework to guide future work on anti-perovskites to enhance their solid electrolyte properties. This journal is
AB - Solid-state batteries present potential advantages over their liquid-based electrolyte equivalents, including enhanced safety and increased energy density. In the search for novel solid electrolytes, the anti-perovskite family of materials are attracting growing interest. However, while there is significant work on Li-rich anti-perovskites, their Na-based counterparts and the atomistic effects of aliovalent doping on these materials are not fully characterised. Here, we investigate the effects on Na-ion conductivity of doping with divalent (Mg, Ca, Sr and Ba) and trivalent cations (Al and Ga), and of possible dopant-vacancy clustering in the anti-perovskite Na3OCl by employing atomistic simulation techniques. Our results highlight the potential of Mg2+, Ca2+, Al3+ and Ga3+ doping due to their favourable incorporation and increased Na-ion vacancy concentration. Local defect clustering and binding energies are analysed, and such effects inhibit Na-ion conductivity in the doped Na3OCl solid electrolyte at operating temperatures. These results provide a framework to guide future work on anti-perovskites to enhance their solid electrolyte properties. This journal is
UR - http://www.scopus.com/inward/record.url?scp=85124418414&partnerID=8YFLogxK
U2 - 10.1039/d1ta07588h
DO - 10.1039/d1ta07588h
M3 - Article
AN - SCOPUS:85124418414
VL - 10
SP - 2249
EP - 2255
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 5
ER -