Development of Li-based Garnet Electrolytes for All-Solid-State Li Batteries

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dc.contributor.advisorThangadurai, Venkataraman
dc.contributor.authorPalakkathodi Kammampata, Sanoop
dc.contributor.committeememberMarriott, Robert A
dc.contributor.committeememberTrudel, Simon
dc.contributor.committeememberCheng, Yufeng
dc.contributor.committeememberKleinke, Holger
dc.dateSpring Convocation
dc.date.accessioned2022-06-17T20:48:11Z
dc.date.available2022-06-17T20:48:11Z
dc.date.issued2021-04-26
dc.description.abstractAll-solid-state Li batteries employing a ceramic solid electrolyte are considered as the nextgeneration energy storage devices due to their advantages in safety and potentially high energydensity. Garnet-type Li6.5La3-xAxZr1.5-xTax+0.5O12 (A = Ca, Sr, Ba; x = 0, 0.1, 0.3, 0.5) solidelectrolytes were prepared by conventional solid-state synthesis and spark plasma synthesis (SPS).The effect of doping of alkaline earth metals and sintering methods on the structural andelectrochemical properties of the solid electrolytes were investigated in this thesis. Powder X-raydiffraction (PXRD) studies have confirmed the cubic garnet-type structure of the solid electrolytes.Microstructure of the solid electrolytes were analysed by scanning electron microscopy (SEM).The samples prepared by SPS process exhibited higher density than the samples prepared byconventional solid-state route. The AC electrochemical impedance spectroscopy (EIS) was usedto measure the impedance of solid electrolytes. All garnet electrolytes prepared in this thesisshowed bulk conductivity in the range of 10-4 S/cm. Among the alkaline earth metal-doped solidelectrolytes, x = 0.1 (Ca and Sr) members prepared by SPS route showed highest conductivity atroom temperature (4.8 x 10-4 S/cm). Li6.5La2.9Sr0.1Zr1.4Ta0.6O12 prepared by SPS process showedan excellent Li-ion charge transfer resistance of 3.5 ? cm2 at 25 °C and the highest critical currentdensity of 0.6 mA/cm2 among all other samples.X-ray photoelectron spectroscopy (XPS) analyses were conducted on SPS-processedLi6.5La3-xAxZr1.5-xTax+0.5O12 (A = Ca, Sr, Ba; x = 0, 0.1) garnet electrolytes to quantify the impuritylayers on garnet surface. XPS analyses revealed that the surface of these electrolytes is covered byLiOH and Li2CO3-based compounds with a thickness of 4?6 nm within 30 minutes as a result ofthe reaction with traces of H2O and CO2 in an Ar-filled glovebox. Chemical compatibility ofLi7La2.75Ca0.25Zr1.75Ta0.25O12 (LLCZT) with commercial cathode materials and liquid Li-ion electrolytes (LLEs) was investigated using PXRD, SEM and EIS analysis. Hybrid cell consistingof Li metal, LLEs, LLCZT and LiNi0.8Co0.15Al0.05O2 or LiNi0.6Mn0.2Co0.2O2 cathode wereassembled in a coin cell and electrochemical performance was evaluated.
dc.identifier.citationPalakkathodi Kammampata, S. (2021). Development of Li-based Garnet Electrolytes for All-Solid-State Li Batteries (Doctoral thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca.
dc.identifier.doihttp://dx.doi.org/10.11575/PRISM/39839
dc.identifier.urihttp://hdl.handle.net/1880/114751
dc.language.isoenen
dc.language.isoEnglish
dc.publisher.facultyGraduate Studiesen
dc.publisher.facultyScience
dc.publisher.institutionUniversity of Calgaryen
dc.rightsUniversity of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.en
dc.subjectLi batteries
dc.subjectsolid-state electrolytes
dc.subjectLi garnets
dc.subject.classificationPhysical Sciences
dc.titleDevelopment of Li-based Garnet Electrolytes for All-Solid-State Li Batteries
dc.typedoctoral thesis
thesis.degree.disciplineChemistry
thesis.degree.grantorUniversity of Calgaryen
thesis.degree.grantorUniversity of Calgary
thesis.degree.nameDoctor of Philosophy (PhD)
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