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Facile Synthesis Approaches for High Li+ ion Conducting Garnet Structures.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Facile Synthesis Approaches for High Li+ ion Conducting Garnet Structures.
Author:	Badami, Pavan Pramod.
Published:	Ann Arbor : ProQuest Dissertations & Theses, 2021
Description:	131 p.
Notes:	Source: Dissertations Abstracts International, Volume: 83-07, Section: B.
Notes:	Advisor: Kannan, Arunachala Mada;Chan, Candace.
Contained By:	Dissertations Abstracts International83-07B.
Subject:	Materials science.
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28721592
ISBN:	9798759962670

Facile Synthesis Approaches for High Li+ ion Conducting Garnet Structures.
Badami, Pavan Pramod.

Facile Synthesis Approaches for High Li+ ion Conducting Garnet Structures. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 131 p.

Source: Dissertations Abstracts International, Volume: 83-07, Section: B.

Thesis (Ph.D.)--Arizona State University, 2021.

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

The current Li-ion batteries with organic liquid electrolytes are limited by their safety and energy density. Therefore, ceramic electrolytes are proposed in developing next-generation, energy-dense Li-metal batteries by replacing organic liquid electrolytes to improve safety and performance. Among numerous ceramic Li-ion conductors, garnet-based solid electrolyte c-Li7La3Zr2O12 (c-LLZO) is considered one of the most promising candidates to enable Li metal batteries due to its high ionic conductivity, chemical stability, and wide electrochemical stability window against Li metal. However, synthesis and processing of c-LLZO through conventional solid-sate reaction methods requires long periods of calcination (> 6 h) at high reaction temperatures (> 1000 °C). The need for high reaction temperature results to attain cubic-LLZO phase results in large aggerated LLZO particles and causes Li-loss from the garnet structure, making them unfavorable to process further as bulk pellets or thin films. To overcome processing challenges with solid-state reaction method, two novel facile synthesis approaches molten salt (flux growth method), and solution combustion are employed to produce submicron-sized LLZO powders at low reaction temperatures (< 1000 °C) in a short time. In the first case, molten salt synthesis method with LiCl-KCl eutectic mixture is employed to produce sub-micron sized Ta-doped LLZO (LLZTO) powders at low temperatures (900 °C, 4 h). In addition, a detailed investigation on effect of sintering medium and sintering additives on the structural, microstructural, chemical, and Li-ion transport behavior of the LLZTO pellets are investigated. Sintered LLZTO pellets prepared using molten salt synthesis route exhibited high Li-ion conductivity up to 0.6 mS cm-1 and high relative density (> 95 %) using Pt-crucible. In the second case, a facile solution-combustion technique using an amide-based fuel source CH6N4O is utilized to produce submicron-sized Al-doped LLZO (Al-LLZO) powders at low reaction temperatures 600-800 °C in a short duration of 4 h. In addition, effect of fuel to oxidizer ratio on phase purity, particle growth size, and formation mechanism of conductive Al-LLZO are reported and discussed. The Al-LLZO pellets sintered at 1100 °C/ 6 h exhibited high Li-ion conductivity up to 0.45 mS cm-1 with relative densities (> 90 %).

ISBN: 9798759962670Subjects--Topical Terms:

221779
Materials science.
Subjects--Index Terms:

Combustion method

Facile Synthesis Approaches for High Li+ ion Conducting Garnet Structures.
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300 $a 131 p.
500 $a Source: Dissertations Abstracts International, Volume: 83-07, Section: B.
500 $a Advisor: Kannan, Arunachala Mada;Chan, Candace.
502 $a Thesis (Ph.D.)--Arizona State University, 2021.
506 $a This item must not be sold to any third party vendors.
520 $a The current Li-ion batteries with organic liquid electrolytes are limited by their safety and energy density. Therefore, ceramic electrolytes are proposed in developing next-generation, energy-dense Li-metal batteries by replacing organic liquid electrolytes to improve safety and performance. Among numerous ceramic Li-ion conductors, garnet-based solid electrolyte c-Li7La3Zr2O12 (c-LLZO) is considered one of the most promising candidates to enable Li metal batteries due to its high ionic conductivity, chemical stability, and wide electrochemical stability window against Li metal. However, synthesis and processing of c-LLZO through conventional solid-sate reaction methods requires long periods of calcination (> 6 h) at high reaction temperatures (> 1000 °C). The need for high reaction temperature results to attain cubic-LLZO phase results in large aggerated LLZO particles and causes Li-loss from the garnet structure, making them unfavorable to process further as bulk pellets or thin films. To overcome processing challenges with solid-state reaction method, two novel facile synthesis approaches molten salt (flux growth method), and solution combustion are employed to produce submicron-sized LLZO powders at low reaction temperatures (< 1000 °C) in a short time. In the first case, molten salt synthesis method with LiCl-KCl eutectic mixture is employed to produce sub-micron sized Ta-doped LLZO (LLZTO) powders at low temperatures (900 °C, 4 h). In addition, a detailed investigation on effect of sintering medium and sintering additives on the structural, microstructural, chemical, and Li-ion transport behavior of the LLZTO pellets are investigated. Sintered LLZTO pellets prepared using molten salt synthesis route exhibited high Li-ion conductivity up to 0.6 mS cm-1 and high relative density (> 95 %) using Pt-crucible. In the second case, a facile solution-combustion technique using an amide-based fuel source CH6N4O is utilized to produce submicron-sized Al-doped LLZO (Al-LLZO) powders at low reaction temperatures 600-800 °C in a short duration of 4 h. In addition, effect of fuel to oxidizer ratio on phase purity, particle growth size, and formation mechanism of conductive Al-LLZO are reported and discussed. The Al-LLZO pellets sintered at 1100 °C/ 6 h exhibited high Li-ion conductivity up to 0.45 mS cm-1 with relative densities (> 90 %).
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653 $a Combustion method
653 $a High ionic conductivity
653 $a LLZO
653 $a Low temperature
653 $a Molten Salt
653 $a Synthesis
653 $a Li+-ion conducting garnets
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690 $a 0546
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