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Title: | Solution-gel-based surface modification of LiNi0.5Mn1.5O4−δ with amorphous Li–Ti–O coating | Authors: | ULU, Fulya Batuk, Maria Hadermann, Joke SAFARI, Momo DE SLOOVERE, Dries MYLAVARAPU, Satish Kumar D'HAEN, Jan JOOS, Bjorn VAN BAEL, Marlies HARDY, An |
Issue Date: | 2023 | Publisher: | ROYAL SOC CHEMISTRY | Source: | RSC Advances, 13 (47) , p. 33146 -33158 | Abstract: | LNMO (LiNi0.5Mn1.5O4-delta) is a high-energy density positive electrode material for lithium ion batteries. Unfortunately, it suffers from capacity loss and impedance rise during cycling due to electrolyte oxidation and electrode/electrolyte interface instabilities at high operating voltages. Here, a solution-gel synthesis route was used to coat 0.5-2.5 mu m LNMO particles with amorphous Li-Ti-O (LTO) for improved Li conduction, surface structural stability and cyclability. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) analysis coupled with energy dispersive X-ray (EDX) showed Ti-rich amorphous coatings/islands or Ti-rich spinel layers on many of the LTO-modified LNMO facets, with a thickness varying from about 1 to 10 nm. The surface modification in the form of amorphous islands was mostly possible on high-energy crystal facets. Physicochemical observations were used to propose a molecular mechanism for the surface modification, combining insights from metalorganic chemistry with the crystallographic properties of LNMO. The improvements in functional properties were investigated in half cells. The cell impedance increased faster for the bare LNMO compared to amorphous LTO modified LNMO, resulting in R-ct values as high as 1247 Omega (after 1000 cycles) for bare LNMO, against 216 Omega for the modified material. At 10C, the modified material boosted a 15% increase in average discharge capacity. The improvements in electrochemical performance were attributed to the increase in electrochemically active surface area, as well as to improved HF-scavenging, resulting in the formation of protective byproducts, generating a more stable interface during prolonged cycling. | Notes: | Okudur, FU (corresponding author), Hasselt Univ, Inst Mat Res Imo Imomec, EnergyVille 2,Thor Pk 8320,3590 Diepenbeek, B-3600 Diepenbeek, Belgium.; Okudur, FU (corresponding author), Imec Div Imomec, Design & Synth Inorgan Mat, Agoralaan,EnergyVille 2,Thor Pk 8320,3590 Diepenbe, B-3600 Diepenbeek, Belgium. fulya.uluokudur@imec.be; maria.batuk@uantwerpen.be; joke.hadermann@uantwerpen.be; momo.safari@uhasselt.be; dries.desloovere@uhasselt.be; bjorn.joos@uhasselt.be; jan.dhaen@uhasselt.be; an.hardy@uhasselt.be |
Document URI: | http://hdl.handle.net/1942/41930 | ISSN: | 2046-2069 | e-ISSN: | 2046-2069 | DOI: | 10.1039/d3ra05599j | ISI #: | 001102666700001 | Rights: | Open Access Article. Published on 09 November 2023. Downloaded on 12/11/2023 10:27:07 AM. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. | Category: | A1 | Type: | Journal Contribution |
Appears in Collections: | Research publications |
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Solution-gel-based surface modification of LiNi0.5Mn1.5O4−δ with amorphous Li–Ti–O coating.pdf | Published version | 4.29 MB | Adobe PDF | View/Open |
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