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Investigation of Structure and Li Dy...

Inglis, Kenneth Kazuya.

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Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy./
Author:	Inglis, Kenneth Kazuya.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2020,
Description:	188 p.
Notes:	Source: Dissertations Abstracts International, Volume: 82-06, Section: B.
Contained By:	Dissertations Abstracts International82-06B.
Subject:	Nuclear chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28209121
ISBN:	9798684626678

Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy.
Inglis, Kenneth Kazuya.

Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy. - Ann Arbor : ProQuest Dissertations & Theses, 2020 - 188 p.

Source: Dissertations Abstracts International, Volume: 82-06, Section: B.

Thesis (M.Phil.)--The University of Liverpool (United Kingdom), 2020.

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

Developing solid state ionic conductors to replace liquid electrolytes for next generation Li+ ion battery technologies are of high interest due to their major impact resulting from the combination of increased safety, lifetime and power output. Potential candidates are constantly studied by research groups worldwide to obtain such material, however issues such as electrochemical stability with lithium and low ionic conductivity hinder the target to be achieved.Solid state nuclear magnetic resonance (NMR) spectroscopy is an invaluable technique in solid state ionic conductor research with its ability to investigate both local structure and follow the dynamics of the charge carrier. It has been used widely to identify Li+ dynamics and diffusion pathways on time scales inaccessible by other experimental techniques, allowing deeper understanding in what key features are present in achieving high performance Li+ ion conductors.In this thesis, the solid state NMR investigation of three Li+ ion conductors from three distinct crystallographic families are reported. 1. A new class of ABO3 perovskite with composition La3Li3W2O12 is identified, it is the first perovskite material where Li is present on both A- and B-sites. Solid state NMR deduced the ratio of the two sites as 1:2, consistent with DFT calculations. The activation barrier for Li+ diffusion between neighbouring sites was found to be ~0.29 eV and is comparable to the best oxide based Li+ ion conductors reported.2. The effect of Ca2+ doping in the NASICON Li+ ion conductor LiTaAl(PO4)3 to increase Li+ content was studied. Doping resulted in slower Li+ dynamics compared to the undoped material with significantly higher activation barrier to Li+ diffusion. The anisotropic nature of the thermal expansion of the NASICON framework and Li+ diffusion are also observed by variable temperature 7Li NMR spectroscopy. 3. A new structural family of sulfide Li+ ion conductors with compositions Li4.4Al0.4Ge0.6S4 and Li4.4Al0.4Sn0.6S4 were identified. These new phases consisted of a two-dimensional Li+ diffusion pathway with activation barriers as low as ~0.17 eV, similar to the Li10GeP2S12 family, the best solid state sulfide Li+ ion conductor series reported. These findings signify the importance of solid state NMR as a technique complementary to other methods to understanding the properties of newly synthesised phases.

ISBN: 9798684626678Subjects--Topical Terms:

643077
Nuclear chemistry.
Subjects--Index Terms:

NMR spectroscopy

Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy.
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245 1 0 $a Investigation of Structure and Li Dynamics in New Li Ion Conductors Using Solid State NMR Spectroscopy.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2020
300 $a 188 p.
500 $a Source: Dissertations Abstracts International, Volume: 82-06, Section: B.
500 $a Advisor: Rosseinsky, Matthew;Blanc, Frederic.
502 $a Thesis (M.Phil.)--The University of Liverpool (United Kingdom), 2020.
506 $a This item must not be sold to any third party vendors.
520 $a Developing solid state ionic conductors to replace liquid electrolytes for next generation Li+ ion battery technologies are of high interest due to their major impact resulting from the combination of increased safety, lifetime and power output. Potential candidates are constantly studied by research groups worldwide to obtain such material, however issues such as electrochemical stability with lithium and low ionic conductivity hinder the target to be achieved.Solid state nuclear magnetic resonance (NMR) spectroscopy is an invaluable technique in solid state ionic conductor research with its ability to investigate both local structure and follow the dynamics of the charge carrier. It has been used widely to identify Li+ dynamics and diffusion pathways on time scales inaccessible by other experimental techniques, allowing deeper understanding in what key features are present in achieving high performance Li+ ion conductors.In this thesis, the solid state NMR investigation of three Li+ ion conductors from three distinct crystallographic families are reported. 1. A new class of ABO3 perovskite with composition La3Li3W2O12 is identified, it is the first perovskite material where Li is present on both A- and B-sites. Solid state NMR deduced the ratio of the two sites as 1:2, consistent with DFT calculations. The activation barrier for Li+ diffusion between neighbouring sites was found to be ~0.29 eV and is comparable to the best oxide based Li+ ion conductors reported.2. The effect of Ca2+ doping in the NASICON Li+ ion conductor LiTaAl(PO4)3 to increase Li+ content was studied. Doping resulted in slower Li+ dynamics compared to the undoped material with significantly higher activation barrier to Li+ diffusion. The anisotropic nature of the thermal expansion of the NASICON framework and Li+ diffusion are also observed by variable temperature 7Li NMR spectroscopy. 3. A new structural family of sulfide Li+ ion conductors with compositions Li4.4Al0.4Ge0.6S4 and Li4.4Al0.4Sn0.6S4 were identified. These new phases consisted of a two-dimensional Li+ diffusion pathway with activation barriers as low as ~0.17 eV, similar to the Li10GeP2S12 family, the best solid state sulfide Li+ ion conductor series reported. These findings signify the importance of solid state NMR as a technique complementary to other methods to understanding the properties of newly synthesised phases.
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650 4 $a Molecular chemistry. $3 1071612
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710 2 $a The University of Liverpool (United Kingdom). $3 1684840
773 0 $t Dissertations Abstracts International $g 82-06B.
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791 $a M.Phil.
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856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28209121