Lithium-ion Mobility in Li6B18(Li3N) and Li Vacancy Tuning in the Solid Solution Li6B18(Li3N)1−x(Li2O)x

Tassilo M.F. Restle; Lavinia Scherf; Jasmin V. Dums; Alexander G. Mutschke; Robert J. Spranger; Holger Kirchhain; Antti J. Karttunen; Leo van Wüllen; Thomas F. Fässler

doi:10.1002/anie.202213962

Lithium-ion Mobility in Li₆B₁₈(Li₃N) and Li Vacancy Tuning in the Solid Solution Li₆B₁₈(Li₃N)_1−x(Li₂O)_x

Tassilo M.F. Restle
, Lavinia Scherf
, Jasmin V. Dums
, Alexander G. Mutschke
, Robert J. Spranger
, Holger Kirchhain
, Antti J. Karttunen
, Leo van Wüllen
, Thomas F. Fässler^*

^*Tämän työn vastaava kirjoittaja

Technical University of Munich
TUMInt.Energy Research GmbH
University of Augsburg

Tutkimustuotos: Lehtiartikkeli › Article › Scientific › vertaisarvioitu

9 Sitaatiot (Scopus)

64 Lataukset (Pure)

Abstrakti

All-solid-state batteries are promising candidates for safe energy-storage systems due to non-flammable solid electrolytes and the possibility to use metallic lithium as an anode. Thus, there is a challenge to design new solid electrolytes and to understand the principles of ion conduction on an atomic scale. We report on a new concept for compounds with high lithium ion mobility based on a rigid open-framework boron structure. The host–guest structure Li₆B₁₈(Li₃N) comprises large hexagonal pores filled with (Formula presented.) Li₇N] strands that represent a perfect cutout from the structure of α-Li₃N. Variable-temperature ⁷Li NMR spectroscopy reveals a very high Li mobility in the template phase with a remarkably low activation energy below 19 kJ mol⁻¹ and thus much lower than pristine Li₃N. The formation of the solid solution of Li₆B₁₈(Li₃N) and Li₆B₁₈(Li₂O) over the complete compositional range allows the tuning of lithium defects in the template structure that is not possible for pristine Li₃N and Li₂O.

Alkuperäiskieli	Englanti
Artikkeli	e202213962
Sivumäärä	9
Julkaisu	Angewandte Chemie - International Edition
Vuosikerta	62
Numero	10
DOI - pysyväislinkit	https://doi.org/10.1002/anie.202213962
Tila	Julkaistu - 1 maalisk. 2023
OKM-julkaisutyyppi	A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

Rahoitus

The authors are grateful to the Bavarian Ministry of Economic Affairs, Regional Development, and Energy for funding their research in the project “Industrialisierbarkeit von Festkörperelektrolytzellen”. A.J.K. thanks CSC—the Finnish IT Center for Science for computational resources. Open Access funding enabled and organized by Projekt DEAL. The authors are grateful to the Bavarian Ministry of Economic Affairs, Regional Development, and Energy for funding their research in the project “Industrialisierbarkeit von Festkörperelektrolytzellen”. A.J.K. thanks CSC—the Finnish IT Center for Science for computational resources. Open Access funding enabled and organized by Projekt DEAL.

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Pääsy asiakirjaan

10.1002/anie.202213962Lisenssi: CC BY

CHEM_Restle_et_al_Lithium‐ion_Mobility_2023_Angewandte_Chemie_Int_EdFinal published version, 3,1 MBLisenssi: CC BY

Muut tiedostot ja linkit

Linkki julkaisuun Scopuksessa

CCDC 2207446: Experimental Crystal Structure Determination
Restle, T. M. F. (Creator), Scherf, L. (Creator), Dums, J. V. (Creator), Spranger, R. J. (Creator), Mutschke, A. (Creator), Kirchhain, H. (Creator), Karttunen, A. J. (Creator), van Wüllen, L. (Creator) & Fässler, T. F. (Creator), Cambridge Crystallographic Data Centre , 2023
DOI - pysyväislinkki: 10.5517/ccdc.csd.cc2d30yh, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2d30yh&sid=DataCite
Tietoaineisto: Dataset
CCDC 2207443: Experimental Crystal Structure Determination
Restle, T. M. F. (Creator), Scherf, L. (Creator), Dums, J. V. (Creator), Spranger, R. J. (Creator), Mutschke, A. (Creator), Kirchhain, H. (Creator), Karttunen, A. J. (Creator), van Wüllen, L. (Creator) & Fässler, T. F. (Creator), Cambridge Crystallographic Data Centre , 2023
DOI - pysyväislinkki: 10.5517/ccdc.csd.cc2d30vd, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2d30vd&sid=DataCite
Tietoaineisto: Dataset
CCDC 2207445: Experimental Crystal Structure Determination
Restle, T. M. F. (Creator), Scherf, L. (Creator), Dums, J. V. (Creator), Spranger, R. J. (Creator), Mutschke, A. (Creator), Kirchhain, H. (Creator), Karttunen, A. J. (Creator), van Wüllen, L. (Creator) & Fässler, T. F. (Creator), Cambridge Crystallographic Data Centre , 2023
DOI - pysyväislinkki: 10.5517/ccdc.csd.cc2d30xg, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2d30xg&sid=DataCite
Tietoaineisto: Dataset

Technical University Munich (TU Munich) Reports Findings in Science [Lithium-ion Mobility in Li6 B18 (Li3 N) and Li Vacancy Tuning in the Solid Solution Li6 B18 (Li3 N)1-x (Li2 O)x]
Karttunen, A.
07/02/2023
1 kohde/ Medianäkyvyys
Lehdistö/media: Esiintyminen mediassa

Siteeraa tätä

Restle, T. M. F., Scherf, L., Dums, J. V., Mutschke, A. G., Spranger, R. J., Kirchhain, H., Karttunen, A. J., van Wüllen, L., & Fässler, T. F. (2023). Lithium-ion Mobility in Li₆B₁₈(Li₃N) and Li Vacancy Tuning in the Solid Solution Li₆B₁₈(Li₃N)_1−x(Li₂O)_x. Angewandte Chemie - International Edition, 62(10), Artikkeli e202213962. https://doi.org/10.1002/anie.202213962

@article{e667e803caa5483bb59cd8d6bf87efc4,

title = "Lithium-ion Mobility in Li6B18(Li3N) and Li Vacancy Tuning in the Solid Solution Li6B18(Li3N)1−x(Li2O)x",

abstract = "All-solid-state batteries are promising candidates for safe energy-storage systems due to non-flammable solid electrolytes and the possibility to use metallic lithium as an anode. Thus, there is a challenge to design new solid electrolytes and to understand the principles of ion conduction on an atomic scale. We report on a new concept for compounds with high lithium ion mobility based on a rigid open-framework boron structure. The host–guest structure Li6B18(Li3N) comprises large hexagonal pores filled with (Formula presented.) Li7N] strands that represent a perfect cutout from the structure of α-Li3N. Variable-temperature 7Li NMR spectroscopy reveals a very high Li mobility in the template phase with a remarkably low activation energy below 19 kJ mol−1 and thus much lower than pristine Li3N. The formation of the solid solution of Li6B18(Li3N) and Li6B18(Li2O) over the complete compositional range allows the tuning of lithium defects in the template structure that is not possible for pristine Li3N and Li2O.",

keywords = "Boride, Host Guest System, Ion Conduction, Lithim, Nitride",

author = "Restle, \{Tassilo M.F.\} and Lavinia Scherf and Dums, \{Jasmin V.\} and Mutschke, \{Alexander G.\} and Spranger, \{Robert J.\} and Holger Kirchhain and Karttunen, \{Antti J.\} and \{van W{\"u}llen\}, Leo and F{\"a}ssler, \{Thomas F.\}",

note = "Funding Information: The authors are grateful to the Bavarian Ministry of Economic Affairs, Regional Development, and Energy for funding their research in the project “Industrialisierbarkeit von Festk{\"o}rperelektrolytzellen”. A.J.K. thanks CSC—the Finnish IT Center for Science for computational resources. Open Access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

year = "2023",

month = mar,

day = "1",

doi = "10.1002/anie.202213962",

language = "English",

volume = "62",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "Wiley",

number = "10",

}

TY - JOUR

T1 - Lithium-ion Mobility in Li6B18(Li3N) and Li Vacancy Tuning in the Solid Solution Li6B18(Li3N)1−x(Li2O)x

AU - Restle, Tassilo M.F.

AU - Scherf, Lavinia

AU - Dums, Jasmin V.

AU - Mutschke, Alexander G.

AU - Spranger, Robert J.

AU - Kirchhain, Holger

AU - Karttunen, Antti J.

AU - van Wüllen, Leo

AU - Fässler, Thomas F.

N1 - Funding Information: The authors are grateful to the Bavarian Ministry of Economic Affairs, Regional Development, and Energy for funding their research in the project “Industrialisierbarkeit von Festkörperelektrolytzellen”. A.J.K. thanks CSC—the Finnish IT Center for Science for computational resources. Open Access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

PY - 2023/3/1

Y1 - 2023/3/1

N2 - All-solid-state batteries are promising candidates for safe energy-storage systems due to non-flammable solid electrolytes and the possibility to use metallic lithium as an anode. Thus, there is a challenge to design new solid electrolytes and to understand the principles of ion conduction on an atomic scale. We report on a new concept for compounds with high lithium ion mobility based on a rigid open-framework boron structure. The host–guest structure Li6B18(Li3N) comprises large hexagonal pores filled with (Formula presented.) Li7N] strands that represent a perfect cutout from the structure of α-Li3N. Variable-temperature 7Li NMR spectroscopy reveals a very high Li mobility in the template phase with a remarkably low activation energy below 19 kJ mol−1 and thus much lower than pristine Li3N. The formation of the solid solution of Li6B18(Li3N) and Li6B18(Li2O) over the complete compositional range allows the tuning of lithium defects in the template structure that is not possible for pristine Li3N and Li2O.

AB - All-solid-state batteries are promising candidates for safe energy-storage systems due to non-flammable solid electrolytes and the possibility to use metallic lithium as an anode. Thus, there is a challenge to design new solid electrolytes and to understand the principles of ion conduction on an atomic scale. We report on a new concept for compounds with high lithium ion mobility based on a rigid open-framework boron structure. The host–guest structure Li6B18(Li3N) comprises large hexagonal pores filled with (Formula presented.) Li7N] strands that represent a perfect cutout from the structure of α-Li3N. Variable-temperature 7Li NMR spectroscopy reveals a very high Li mobility in the template phase with a remarkably low activation energy below 19 kJ mol−1 and thus much lower than pristine Li3N. The formation of the solid solution of Li6B18(Li3N) and Li6B18(Li2O) over the complete compositional range allows the tuning of lithium defects in the template structure that is not possible for pristine Li3N and Li2O.

KW - Boride

KW - Host Guest System

KW - Ion Conduction

KW - Lithim

KW - Nitride

UR - https://www.scopus.com/pages/publications/85146389460

U2 - 10.1002/anie.202213962

DO - 10.1002/anie.202213962

M3 - Article

C2 - 36588091

AN - SCOPUS:85146389460

SN - 1433-7851

VL - 62

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 10

M1 - e202213962

ER -

Lithium-ion Mobility in Li6B18(Li3N) and Li Vacancy Tuning in the Solid Solution Li6B18(Li3N)1−x(Li2O)x

Abstrakti

Rahoitus

YK:n kestävän kehityksen tavoitteet

Pääsy asiakirjaan

Muut tiedostot ja linkit

Sormenjälki

Tietoaineistot

CCDC 2207446: Experimental Crystal Structure Determination

CCDC 2207443: Experimental Crystal Structure Determination

CCDC 2207445: Experimental Crystal Structure Determination

Lehtileikkeet

Technical University Munich (TU Munich) Reports Findings in Science [Lithium-ion Mobility in Li6 B18 (Li3 N) and Li Vacancy Tuning in the Solid Solution Li6 B18 (Li3 N)1-x (Li2 O)x]

Siteeraa tätä

Lithium-ion Mobility in Li₆B₁₈(Li₃N) and Li Vacancy Tuning in the Solid Solution Li₆B₁₈(Li₃N)_1−x(Li₂O)_x