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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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Mohamed, Tarek |
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Ertürk, Emre |
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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Weatherup, Rs
University of Oxford
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (28/28 displayed)
- 2024The Role of Salt Concentration in Stabilizing Charged Ni-Rich Cathode Interfaces in Li-ion Batteries
- 2024Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditionscitations
- 2023Effect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interfacecitations
- 2022Gently does it!: in situ preparation of alkali metal–solid electrolyte interfaces for photoelectron spectroscopycitations
- 2022Effect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interfacecitations
- 2022In situ and operando characterisation of Li metal – Solid electrolyte interfacescitations
- 2022Electrolyte reactivity at the charged Ni-rich cathode interface and degradation in Li-ion batteriescitations
- 2022Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries.
- 2022Electronic interactions and stability issues at the copper-graphene interface in air and in alkaline solution under electrochemical controlcitations
- 2020Understanding metal organic chemical vapour deposition of monolayer WS2: the enhancing role of au substrate for simple organosulfur precursorscitations
- 2020The origin of chemical inhomogeneity in garnet electrolytes and its impact on the electrochemical performancecitations
- 2020Graphene-passivated nickel as an efficient hole-injecting electrode for large area organic semiconductor devicescitations
- 2020Understanding metal organic chemical vapour deposition of monolayer WS<sub>2</sub>: the enhancing role of Au substrate for simple organosulfur precursors.
- 2019Reactive intercalation and oxidation at the buried graphene-germanium interface
- 2018Compressive Behavior and Failure Mechanisms of Freestanding and Composite 3D Graphitic Foamscitations
- 2018Insulator-to-Metallic Spin-Filtering in 2D-Magnetic Tunnel Junctions Based on Hexagonal Boron Nitridecitations
- 2017Chemical vapour deposition of freestanding sub-60 nm graphene gyroidscitations
- 2017Low temperature growth of fully covered single-layer graphene using a CoCu catalystcitations
- 2016In Situ Observations of Phase Transitions in Metastable Nickel (Carbide)/Carbon Nanocompositescitations
- 2016In Situ Graphene Growth Dynamics on Polycrystalline Catalyst Foilscitations
- 2016Time Evolution of the Wettability of Supported Graphene under Ambient Air Exposurecitations
- 2015Protecting nickel with graphene spin-filtering membranescitations
- 2015Spatial variability in large area single and few-layer CVD graphene
- 2014The role of the sp2:sp3 substrate content in carbon supported nanotube growthcitations
- 2014The influence of intercalated oxygen on the properties of graphene on polycrystalline Cu under various environmental conditionscitations
- 2014Low temperature growth of carbon nanotubes on tetrahedral amorphous carbon using Fe-Cu catalystcitations
- 2014Nitrogen controlled iron catalyst phase during carbon nanotube growthcitations
- 2012The phase of iron catalyst nanoparticles during carbon nanotube growthcitations
Places of action
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article
Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries.
Abstract
The chemical and electrochemical reactions at the positive electrode-electrolyte interface in Li-ion batteries are hugely influential on cycle life and safety. Ni-rich layered transition metal oxides exhibit higher interfacial reactivity than their lower Ni-content analogues, reacting via mechanisms that are poorly understood. Here, we study the pivotal role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells. While NMC111 exhibits similar parasitic currents with EC-containing and EC-free electrolytes during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, this is not the case for NMC811. Online gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte decomposition, which is higher for EC-containing than EC-free electrolytes. Combined findings from electrochemical impedance spectroscopy (EIS), TEM, solution NMR, ICP, and XPS reveal that the electrolyte solvent has a profound impact on the degradation of the Ni-rich cathode and the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher cathode interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstruction layer, more electrolyte solvent and salt breakdown, and higher amounts of transition metal dissolution. These processes are suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. Finally, new mechanistic insights into the chemical oxidation pathways of electrolyte solvents and, critically, the knock-on chemical and electrochemical reactions that further degrade the electrolyte and electrodes curtailing battery lifetime are provided.