Safe extended-range cycling of Li4Ti5O12-based anodes for ultra-high capacity thin-film batteries

Siller, V. ; Gonzalez-Rosillo, J. ; Nuñez Eroles, M. ; Stchakovsky, M. ; Arenal, R. ; Morata, A. ; Tarancón, A.

Resumen: Lithium titanium oxide thin films are increasingly popular anode materials in microbatteries and hybrid supercapacitors, due to their improved safety, cost, and cycle lifetime. So far, research efforts have mainly focused on the pure spinel phase Li4Ti5O12 (LTO) and only a small fraction is dedicated to a broader spectrum of titanium-based metal oxide thin films. In this work, pulsed laser deposition is used in a multilayer approach by alternating LTO and Li2O ablations to create a heterogeneous landscape in the titania-based micro-anodes. This rich microstructure enables the safe extension of the accessible electrochemical window down to 0.2 V. This leads to extraordinary high specific capacities of 250–300 mAh/g at 1 C, maintaining a stable discharge capacity of 180 mAh/g at 16 C. Operando spectroscopic ellipsometry and Raman spectroscopy are used to track optical and structural changes as a function of the discharge voltage down to 0.01 V. A kinetically limited degradation mechanism based on the effective trapping of Li-ions at the octahedral 16c positions is proposed when cycling in the range of 0.2–0.01 V. In essence, our work contributes to titania-based nanoshapes as anodes of increased specific capacity due to a higher Li-site occupation, while maintaining their good stability and safety. © 2022 The Author(s)

Idioma: Inglés

DOI: 10.1016/j.mtener.2022.100979

Año: 2022

Publicado en: Materials Today Energy 25, 100979 (2022), [11 pp]
ISSN: 2468-6069

Factor impacto JCR: 9.3 (2022)

Categ. JCR: CHEMISTRY, PHYSICAL rank: 35 / 161 = 0.217 (2022) - Q1 - T1
Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 58 / 343 = 0.169 (2022) - Q1 - T1
Categ. JCR: ENERGY & FUELS rank: 20 / 119 = 0.168 (2022) - Q1 - T1

Factor impacto CITESCORE: 12.5 - Energy (Q1) - Materials Science (Q1)

Factor impacto SCIMAGO: 2.046 - Energy Engineering and Power Technology (Q1) - Fuel Technology (Q1) - Renewable Energy, Sustainability and the Environment (Q1) - Nuclear Energy and Engineering (Q1) - Materials Science (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA/E13-20R
Financiación: info:eu-repo/grantAgreement/EC/H2020/801342/EU/ACCIÓ programme to foster mobility of researchers with a focus in applied research and technology transfer/TECNIOspringINDUSTRY
Financiación: info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ESTEEM3
Financiación: info:eu-repo/grantAgreement/EC/H2020/824072/EU/Energy HarveStorers for Powering the Internet of Things/HARVESTORE
Financiación: info:eu-repo/grantAgreement/ES/MINECO-AEI-FEDER/PID2019-104739GB-I00-AEI-10.13039-501100011033

Tipo y forma: Article (Published version)