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Structural and Electrical Properties...

Kafle, Amrit Prasad.

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Structural and Electrical Properties of Garnets and Glasses - Prospective Electrolytes for Alkali-Ion Batteries.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Structural and Electrical Properties of Garnets and Glasses - Prospective Electrolytes for Alkali-Ion Batteries./
Author:	Kafle, Amrit Prasad.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2024,
Description:	228 p.
Notes:	Source: Dissertations Abstracts International, Volume: 85-06, Section: B.
Contained By:	Dissertations Abstracts International85-06B.
Subject:	Physics. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30815194
ISBN:	9798381163162

Structural and Electrical Properties of Garnets and Glasses - Prospective Electrolytes for Alkali-Ion Batteries.
Kafle, Amrit Prasad.

Structural and Electrical Properties of Garnets and Glasses - Prospective Electrolytes for Alkali-Ion Batteries. - Ann Arbor : ProQuest Dissertations & Theses, 2024 - 228 p.

Source: Dissertations Abstracts International, Volume: 85-06, Section: B.

Thesis (Ph.D.)--The Catholic University of America, 2024.

This item must not be sold to any third party vendors.

Liquid and polymer electrolytes, commonly used in in commercial rechargeable Lithium-ion batteries (LiBs), pose safety concerns and create electrochemical instability. Solid electrolytes, such as oxide glasses and garnet-type ceramics, offer enhanced safety, are more durable and possess increased electrochemical stability. Oxide glasses, despite their lower ionic conductivity, provide physical isotropy and compositional flexibility, and make dendrite growth improbable. Garnet-type ceramics, with their broad electrochemical stability range and improved stability when interfacing with lithium metal anodes, hold promise but face challenges, including susceptibility to environmental factors, limited wettability, high impedance at lithium-solid electrolyte interfaces, and the potential for dendrite growth. To address these challenges, a comprehensive examination of the structure-property relationship of oxide glasses and garnet-type solid-state electrolytes is crucial. In this study, we investigate lithium boro-silicate glasses, analyzing their structural variations and electrical properties across various compositions. Raman spectroscopy and Van der Pauw Four-probe method serve as investigative tools, unveiling details of glass structure and electrical conductivity. Notably, we observe significant changes in borate and silicate units as the composition varies, shedding light on the interplay between structure and properties in these glasses. Furthermore, we explore the impact of sintering temperature on the structure and ionic conductivity of Li5-xLa3(NbTa)O12 garnets. Even though the most desirable coordination of Li+ ions for an electrolyte is octahedral, there are reports of Li+ in other coordination states. However, accurate determination of the relative proportions of Li+ in different coordination states is challenging, which we have attempted in this research. We also provide X-ray powder diffraction patterns for references, facilitating future research in the field. Moreover, we examine Li7La3Zr2O12 garnets by substituting Hf, taking advantage of the close atomic radii and similar characteristics of Zr and Hf, which are known as chemical twins due to lanthanoid contraction. We produce a solid solution, Li7La3(Zr1.8Hf0.2)O12, and unveil phase transitions at elevated temperatures. Li7La3(Zr1.8Hf0.2)O12 garnet undergoes a tetragonal-to-cubic transition between 100 and 200 °C due to CO2 absorption. Ionic conductivity measurements and Arrhenius plots pinpoint the transition temperature at approximately 125 °C. Real-time STEM imaging reveals intriguing morphological stability despite the structural shift. The comprehension of structure-property relationships and phase transitions plays a central role in the development of advanced materials for energy conversion and storage applications.

ISBN: 9798381163162Subjects--Topical Terms:

516296
Physics.
Subjects--Index Terms:

Alkali ion batteries

Structural and Electrical Properties of Garnets and Glasses - Prospective Electrolytes for Alkali-Ion Batteries.
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300 $a 228 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-06, Section: B.
500 $a Advisor: Dutta, Biprodas.
502 $a Thesis (Ph.D.)--The Catholic University of America, 2024.
506 $a This item must not be sold to any third party vendors.
520 $a Liquid and polymer electrolytes, commonly used in in commercial rechargeable Lithium-ion batteries (LiBs), pose safety concerns and create electrochemical instability. Solid electrolytes, such as oxide glasses and garnet-type ceramics, offer enhanced safety, are more durable and possess increased electrochemical stability. Oxide glasses, despite their lower ionic conductivity, provide physical isotropy and compositional flexibility, and make dendrite growth improbable. Garnet-type ceramics, with their broad electrochemical stability range and improved stability when interfacing with lithium metal anodes, hold promise but face challenges, including susceptibility to environmental factors, limited wettability, high impedance at lithium-solid electrolyte interfaces, and the potential for dendrite growth. To address these challenges, a comprehensive examination of the structure-property relationship of oxide glasses and garnet-type solid-state electrolytes is crucial. In this study, we investigate lithium boro-silicate glasses, analyzing their structural variations and electrical properties across various compositions. Raman spectroscopy and Van der Pauw Four-probe method serve as investigative tools, unveiling details of glass structure and electrical conductivity. Notably, we observe significant changes in borate and silicate units as the composition varies, shedding light on the interplay between structure and properties in these glasses. Furthermore, we explore the impact of sintering temperature on the structure and ionic conductivity of Li5-xLa3(NbTa)O12 garnets. Even though the most desirable coordination of Li+ ions for an electrolyte is octahedral, there are reports of Li+ in other coordination states. However, accurate determination of the relative proportions of Li+ in different coordination states is challenging, which we have attempted in this research. We also provide X-ray powder diffraction patterns for references, facilitating future research in the field. Moreover, we examine Li7La3Zr2O12 garnets by substituting Hf, taking advantage of the close atomic radii and similar characteristics of Zr and Hf, which are known as chemical twins due to lanthanoid contraction. We produce a solid solution, Li7La3(Zr1.8Hf0.2)O12, and unveil phase transitions at elevated temperatures. Li7La3(Zr1.8Hf0.2)O12 garnet undergoes a tetragonal-to-cubic transition between 100 and 200 °C due to CO2 absorption. Ionic conductivity measurements and Arrhenius plots pinpoint the transition temperature at approximately 125 °C. Real-time STEM imaging reveals intriguing morphological stability despite the structural shift. The comprehension of structure-property relationships and phase transitions plays a central role in the development of advanced materials for energy conversion and storage applications.
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650 4 $a Condensed matter physics. $3 3173567
650 4 $a Physical chemistry. $3 1981412
650 4 $a Materials science. $3 543314
650 4 $a Analytical chemistry. $3 3168300
653 $a Alkali ion batteries
653 $a Electrochemical impedance Spectroscopy
653 $a Garnet type ceramics
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653 $a Solid state electrolytes
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