Density functional theory studies on Li metal electrode/garnet‐type Li 7 La 3 Zr 2 O 12 solid electrolyte interfaces for application in all‐solid‐state batteries

Measures to improve the cycling performance and stability of bulk-type all-solid-state batteries (SSBs) are currently being developed with the goal of substituting conventional Li-ion battery (LIB) technology. As known from liquid electrolyte based LIBs, layered oxide cathode materials undergo volume changes upon (de)lithiation, causing mechanical degradation due to particle fracture, among others. Unlike solid electrolytes, liquid electrolytes are somewhat capable of accommodating morphological changes. In SSBs, the rigidity of the materials used typically leads to adverse contact loss at the interfaces of cathode material and solid electrolyte during cycling. Hence, designing zero- or low-strain electrode materials for application in next-generation SSBs is desirable. In the present work, we report on novel Co-rich NCMs, NCM361 (60% Co) and NCM271 (70% Co), showing minor volume changes up to 4.5 V vs Li+/Li, as determined by operando X-ray diffraction and pressure measurements of LIB pouch and pelletized SSB cells, respectively. Both cathode materials exhibit good cycling performance when incorporated into SSB cells using argyrodite Li6PS5Cl solid electrolyte, albeit their morphology and secondary particle size have not yet been optimized.

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Rational Design of Quasi Zero-Strain NCM Cathode Materials for Minimizing Volume Change Effects in All-Solid-State Batteries

10.26434/chemrxiv.10000751 ◽

2019 ◽

Author(s):

Florian Strauss ◽

Lea de Biasi ◽

A-Young Kim ◽

Jonas Hertle ◽

Simon Schweidler ◽

...

Keyword(s):

Solid State ◽

Solid Electrolyte ◽

Cathode Materials ◽

Rational Design ◽

Electrode Materials ◽

Cycling Performance ◽

Mechanical Degradation ◽

Volume Changes ◽

Solid State Batteries ◽

All Solid State Batteries

Measures to improve the cycling performance and stability of bulk-type all-solid-state batteries (SSBs) are currently being developed with the goal of substituting conventional Li-ion battery (LIB) technology. As known from liquid electrolyte based LIBs, layered oxide cathode materials undergo volume changes upon (de)lithiation, causing mechanical degradation due to particle fracture, among others. Unlike solid electrolytes, liquid electrolytes are somewhat capable of accommodating morphological changes. In SSBs, the rigidity of the materials used typically leads to adverse contact loss at the interfaces of cathode material and solid electrolyte during cycling. Hence, designing zero- or low-strain electrode materials for application in next-generation SSBs is desirable. In the present work, we report on novel Co-rich NCMs, NCM361 (60% Co) and NCM271 (70% Co), showing minor volume changes up to 4.5 V vs Li+/Li, as determined by operando X-ray diffraction and pressure measurements of LIB pouch and pelletized SSB cells, respectively. Both cathode materials exhibit good cycling performance when incorporated into SSB cells using argyrodite Li6PS5Cl solid electrolyte, albeit their morphology and secondary particle size have not yet been optimized.

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Polymorphs of Rb3ScF6: X-ray and Neutron Diffraction, Solid-State NMR, and Density Functional Theory Calculations Study

Inorganic Chemistry ◽

10.1021/acs.inorgchem.1c00485 ◽

2021 ◽

Vol 60 (8) ◽

pp. 6016-6026

Author(s):

Aydar Rakhmatullin ◽

Maxim S. Molokeev ◽

Graham King ◽

Ilya B. Polovov ◽

Konstantin V. Maksimtsev ◽

...

Keyword(s):

Density Functional Theory ◽

Solid State ◽

Neutron Diffraction ◽

Solid State Nmr ◽

Density Functional ◽

Density Functional Theory Calculations ◽

Functional Theory ◽

X Ray

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Study on Li0.33La0.55TiO3 Solid Electrolyte with High Ionic Conductivity and Its Application in Flexible All Solid-State Battery

Nanoscale ◽

10.1039/d1nr02427b ◽

2021 ◽

Author(s):

Feihu Tan ◽

Hua An ◽

Ning Li ◽

Jun Du ◽

Zhengchun Peng

Keyword(s):

Solid State ◽

Ionic Conductivity ◽

Solid Electrolyte ◽

High Ionic Conductivity ◽

Energy Sources ◽

Solid State Battery ◽

Solid State Batteries ◽

All Solid State Batteries

As flexible all-solid-state batteries are highly safe and lightweight, they can be considered as candidates for wearable energy sources. However, their performance needs to be first improved, which can be...

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Hydrated Alkali-B11H14 Salts as Potential Solid-State Electrolytes†

Journal of Materials Chemistry A ◽

10.1039/d1ta01551f ◽

2021 ◽

Author(s):

Diego Holanda Pereira de Souza ◽

Kasper T. Møller ◽

Stephen A. Moggach ◽

Terry D Humphries ◽

Anita D’Angelo ◽

...

Keyword(s):

Solid State ◽

Ionic Conductivity ◽

Solid Electrolyte ◽

High Ionic Conductivity ◽

Solid State Batteries ◽

All Solid State Batteries ◽

Solid State Electrolytes

Metal boron-hydrogen compounds are considered as promising solid electrolyte candidates for the development of all-solid-state batteries (ASSB), owing to the high ionic conductivity exhibited by closo- and nido-boranes. In this...

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Spectroscopic, X-ray Diffraction and Density Functional Theory Study of Intra- and Intermolecular Hydrogen Bonds in Ortho-(4-tolylsulfonamido)benzamides

Molecules ◽

10.3390/molecules26040926 ◽

2021 ◽

Vol 26 (4) ◽

pp. 926

Author(s):

Malose J. Mphahlele ◽

Eugene E. Onwu ◽

Marole M. Maluleka

Keyword(s):

Density Functional Theory ◽

Solid State ◽

Hydrogen Bonds ◽

Density Functional ◽

Tetrahedral Geometry ◽

Hindered Rotation ◽

Hydrogen Bond Acceptor ◽

Functional Theory ◽

Vis Spectroscopy ◽

Hydrogen Bonded

The conformations of the title compounds were determined in solution (NMR and UV-Vis spectroscopy) and in the solid state (FT-IR and XRD), complemented with density functional theory (DFT) in the gas phase. The nonequivalence of the amide protons of these compounds due to the hindered rotation of the C(O)–NH2 single bond resulted in two distinct resonances of different chemical shift values in the aromatic region of their 1H-NMR spectra. Intramolecular hydrogen bonding interactions between the carbonyl oxygen and the sulfonamide hydrogen atom were observed in the solution phase and solid state. XRD confirmed the ability of the amide moiety of this class of compounds to function as a hydrogen bond acceptor to form a six-membered hydrogen bonded ring and a donor simultaneously to form intermolecular hydrogen bonded complexes of the type N–H···O=S. The distorted tetrahedral geometry of the sulfur atom resulted in a deviation of the sulfonamide moiety from co-planarity of the anthranilamide scaffold, and this geometry enabled oxygen atoms to form hydrogen bonds in higher dimensions.

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Iron(II) complexes of dimethyltriazacyclophane

Acta Crystallographica Section C Structural Chemistry ◽

10.1107/s2053229618015255 ◽

2018 ◽

Vol 74 (12) ◽

pp. 1641-1649

Author(s):

Wei-Tsung Lee ◽

Matthias Zeller ◽

David Upp ◽

Yuliya Politanska ◽

Doug Steinman ◽

...

Keyword(s):

Density Functional Theory ◽

Solid State ◽

Dft Calculations ◽

Density Functional Calculations ◽

Density Functional ◽

Coordination Mode ◽

Functional Theory ◽

Metal Centers ◽

Bonding Interaction

Treatment of the ortho-triazacyclophane 1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-triene [(C6H5)3(NH)(NCH3)2, L1] with Fe[N(SiMe3)2]2 yields the dimeric iron(II) complex bis(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido)bis[(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido)iron(II)], [Fe(C20H18N3)4] or Fe2(L1)4 (9). Dissolution of 9 in tetrahydrofuran (THF) results in solvation by two THF ligands and the formation of a simpler monoiron complex, namely bis(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido-κN 7)bis(tetrahydrofuran-κO)iron(II), [Fe(C20H18N3)2(C4H8O)2] or (L1)2Fe(THF)2 (10). The reaction is reversible and 10 reverts in vacuo to diiron complex 9. In the structures of both 9 and 10, the monoanionic triazacyclophane ligand L1− is observed in only the less-symmetric saddle conformation. No bowl-shaped crown conformers are observed in the solid state, thus preventing chelating κ3-coordination to the metal as had been proposed earlier based on density functional theory (DFT) calculations. Instead, the L1− ligands are bound in either a η2-chelating fashion through the amide and one amine donor (for one of the four ligands of 9), or solely through their amide N atoms in an even simpler monodentate η1-coordination mode. Density functional calculations on dimer 9 revealed nearly full cationic charges on each Fe atom and no bonding interaction between the two metal centers, consistent with the relatively long Fe...Fe distance of 2.912 (1) Å observed in the solid state.

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Na-ion diffusion in a NASICON-type solid electrolyte: a density functional study

Physical Chemistry Chemical Physics ◽

10.1039/c6cp05164b ◽

2016 ◽

Vol 18 (39) ◽

pp. 27226-27231 ◽

Cited By ~ 13

Author(s):

Kieu My Bui ◽

Van An Dinh ◽

Susumu Okada ◽

Takahisa Ohno

Keyword(s):

Density Functional Theory ◽

Solid Electrolyte ◽

Electronic Structures ◽

Density Functional ◽

Diffusion Mechanism ◽

Functional Study ◽

Ion Diffusion ◽

Functional Theory ◽

Density Functional Study ◽

Nasicon Type

Based on density functional theory, we have systematically studied the crystal and electronic structures, and the diffusion mechanism of the NASICON-type solid electrolyte Na3Zr2Si2PO12.

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CO2 activation through silylimido and silylamido zirconium hydrides supported on N-donor chelating SBA15 surface ligands

Chemical Communications ◽

10.1039/c5cc08821f ◽

2016 ◽

Vol 52 (12) ◽

pp. 2577-2580 ◽

Cited By ~ 8

Author(s):

Farhan Ahmad Pasha ◽

Anissa Bendjeriou-Sedjerari ◽

Edy Abou-Hamad ◽

Kuo-Wei Huang ◽

Jean-Marie Basset

Keyword(s):

Density Functional Theory ◽

Solid State ◽

Solid State Nmr ◽

Density Functional ◽

Density Functional Theory Calculations ◽

Co2 Activation ◽

Functional Theory ◽

Surface Ligands ◽

Different Types ◽

Zirconium Hydrides

Density functional theory calculations and 2D 1H–13C HETCOR solid state NMR spectroscopy prove that CO2 can be used to probe, by its own reactivity, different types of N-donor surface ligands on SBA15-supported ZrIV hydrides: [(Si–O–)(Si–N)[Zr]H] and [(Si–NH–)(Si–X–)[Zr]H2] (XO or NH).

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