| People | Locations | Statistics |
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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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Grey, Cp
The Faraday Institution
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Topics
Publications (23/23 displayed)
- 2024The effect of interface heterogeneity on zinc metal anode cyclability.
- 20233D Nanocomposite Thin Film Cathodes for Micro-Batteries with Enhanced High-Rate Electrochemical Performance over Planar Films
- 2022Effect of Lithiation upon the Shear Strength of NMC811 Single Crystals
- 2022Importance of Superstructure in Stabilizing Oxygen Redox in P3-Na 0.67 Li 0.2 Mn 0.8 O 2
- 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.
- 2022Forced Disorder in the Solid Solution Li3P-Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes.
- 2021Endogenous 17 O Dynamic Nuclear Polarization of Gd-Doped CeO 2 from 100 to 370 K
- 2021Stabilized tilted-octahedra halide perovskites inhibit local formation of performance-limiting phasescitations
- 2020Revealing the Structure and Oxygen Transport at Interfaces in Complex Oxide Heterostructures via ¹⁷O NMR Spectroscopy
- 2020Investigating the effect of a fluoroethylene carbonate additive on lithium deposition and the solid electrolyte interphase in lithium metal batteries using: In situ NMR spectroscopy
- 2020Establishing Ultralow Activation Energies for Lithium Transport in Garnet Electrolytes.
- 2020Establishing ultra-low activation energies for lithium transport in garnet electrolytes.citations
- 2018The use of strontium ferrite in chemical looping systemscitations
- 2018Interface Instability in LiFePO4–Li3+xP1–xSixO4 All-Solid-State Batteries
- 2018Crystal Structures, Local Atomic Environments, and Ion Diffusion Mechanisms of Scandium-Substituted Sodium Superionic Conductor (NASICON) Solid Electrolytescitations
- 2017Metal-Organic Nanosheets Formed via Defect-Mediated Transformation of a Hafnium Metal-Organic Frameworkcitations
- 2017How Strong Is the Hydrogen Bond in Hybrid Perovskites?citations
- 2017Structural Simplicity as a Restraint on the Structure of Amorphous Silicon
- 2017Investigating Sodium Storage Mechanisms in Tin Anodes: A Combined Pair Distribution Function Analysis, Density Functional Theory and Solid-State NMR Approach
- 2017Mg x Mn 2-x B 2 O 5 Pyroborates (2/3 ≤ x ≤ 4/3): High Capacity and High Rate Cathodes for Li-Ion Batteries
- 2014Three-dimensional characterization of electrodeposited lithium microstructures using synchrotron X-ray phase contrast imagingcitations
- 2013Lithiation of silicon via lithium Zintl-defect complexes from first principles
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.