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Engineering Composite Solid Electrol...

Howell, Benjamin Russell.

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Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries./
Author:	Howell, Benjamin Russell.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2024,
Description:	157 p.
Notes:	Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
Contained By:	Dissertations Abstracts International85-11B.
Subject:	Chemical engineering. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31241335
ISBN:	9798382319384

Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries.
Howell, Benjamin Russell.

Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries. - Ann Arbor : ProQuest Dissertations & Theses, 2024 - 157 p.

Source: Dissertations Abstracts International, Volume: 85-11, Section: B.

Thesis (Ph.D.)--Northeastern University, 2024.

Solid-state lithium-ion batteries (SSLIBs) are widely regarded as the breakthrough technology that will replace conventional liquid electrolyte batteries due to their potential to eliminate the flammability risks of large-format batteries and to greatly increase the energy density of cells. SSLIBs rely on a solid electrolyte (SE) to replace the liquid electrolyte and allow lithium transport throughout the battery. Of the SEs known, polymer SEs are by far the most economical and processable, and so are the most promising candidates for development. Further development of polymer-based SSLIBs requires the successful engineering of the SE itself, as well as the cathode. Traditional liquid electrolyte cathodes are porous composites of active material, conductive additive, and binder that are infiltrated with the ionically conductive liquid electrolyte, which fills pores and provides excellent ionic transport paths. While polymer and composite SEs have been studied extensively and with good results, achieving a good ionic transport network in the cathodes of polymer SSLIBs is a difficult problem that has only recently seen concerted effort. Integrating the SE into the cathode to function as a catholyte is difficult due to several reasons. Internal interfaces between the catholyte and active material particles must be stable and allow for low charge transfer resistance, while also still functioning as a stable binder for the cathode as the active material particles expand and contract during battery cycling. Additionally, the catholyte must allow for a good interface with the SE to provide good transport paths across the SE/cathode interface. Material properties like strength, relative permittivity, binding strength with active materials, and electrochemical stability are all critical to a successful catholyte. This work is about understanding the factors that affect and limit the performance of polymer-based SSLIBs, with regard to both the catholyte, the SE, and their interface. High-conductivity, strong SEs are shown to exacerbate the issue of the cathode/SE interface. Cathodes are analyzed for their electrochemical properties, cycling performance, and microstructure while systematically varying the catholyte content and composition to determine the feasibility of different catholyte materials and the issues preventing their development. Extensive cycling of cathodes combined with electrochemical impedance spectroscopy and SEM imaging reveals large differences in the internal interfaces formed by different catholyte materials with a strong dependence on catholyte content. Systematic variation in cathode thickness combined with multiple types of porosity measurements reveals that porosity is pervasive and a primary limiting factor in achieving higher active material loading for polymer-based SSLIBs. These results serve to inform further development of catholytes and SEs.

ISBN: 9798382319384Subjects--Topical Terms:

560457
Chemical engineering.
Subjects--Index Terms:

Catholytes

Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries.
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245 1 0 $a Engineering Composite Solid Electrolytes and Catholytes for All-Solid-State Lithium Batteries.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2024
300 $a 157 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
500 $a Advisor: Gallaway, Joshua W.
502 $a Thesis (Ph.D.)--Northeastern University, 2024.
520 $a Solid-state lithium-ion batteries (SSLIBs) are widely regarded as the breakthrough technology that will replace conventional liquid electrolyte batteries due to their potential to eliminate the flammability risks of large-format batteries and to greatly increase the energy density of cells. SSLIBs rely on a solid electrolyte (SE) to replace the liquid electrolyte and allow lithium transport throughout the battery. Of the SEs known, polymer SEs are by far the most economical and processable, and so are the most promising candidates for development. Further development of polymer-based SSLIBs requires the successful engineering of the SE itself, as well as the cathode. Traditional liquid electrolyte cathodes are porous composites of active material, conductive additive, and binder that are infiltrated with the ionically conductive liquid electrolyte, which fills pores and provides excellent ionic transport paths. While polymer and composite SEs have been studied extensively and with good results, achieving a good ionic transport network in the cathodes of polymer SSLIBs is a difficult problem that has only recently seen concerted effort. Integrating the SE into the cathode to function as a catholyte is difficult due to several reasons. Internal interfaces between the catholyte and active material particles must be stable and allow for low charge transfer resistance, while also still functioning as a stable binder for the cathode as the active material particles expand and contract during battery cycling. Additionally, the catholyte must allow for a good interface with the SE to provide good transport paths across the SE/cathode interface. Material properties like strength, relative permittivity, binding strength with active materials, and electrochemical stability are all critical to a successful catholyte. This work is about understanding the factors that affect and limit the performance of polymer-based SSLIBs, with regard to both the catholyte, the SE, and their interface. High-conductivity, strong SEs are shown to exacerbate the issue of the cathode/SE interface. Cathodes are analyzed for their electrochemical properties, cycling performance, and microstructure while systematically varying the catholyte content and composition to determine the feasibility of different catholyte materials and the issues preventing their development. Extensive cycling of cathodes combined with electrochemical impedance spectroscopy and SEM imaging reveals large differences in the internal interfaces formed by different catholyte materials with a strong dependence on catholyte content. Systematic variation in cathode thickness combined with multiple types of porosity measurements reveals that porosity is pervasive and a primary limiting factor in achieving higher active material loading for polymer-based SSLIBs. These results serve to inform further development of catholytes and SEs.
590 $a School code: 0160.
650 4 $a Chemical engineering. $3 560457
650 4 $a Polymer chemistry. $3 3173488
650 4 $a Physical chemistry. $3 1981412
653 $a Catholytes
653 $a Composite solid electrolytes
653 $a Cycle stability
653 $a Interfaces
653 $a Solid state batteries
690 $a 0542
690 $a 0495
690 $a 0494
710 2 $a Northeastern University. $b Chemical Engineering. $3 1669259
773 0 $t Dissertations Abstracts International $g 85-11B.
790 $a 0160
791 $a Ph.D.
792 $a 2024
793 $a English
856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31241335