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Capturing dynamic l...
Capturing dynamic ligand-to-metal charge transfer with a long-lived cationic intermediate for anionic redox
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Li, Biao (författare)
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Kumar, Khagesh (författare)
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Roy, Indrani (författare)
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Morozov, Anatolii V. (författare)
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Emelyanova, Olga V. (författare)
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- Zhang, Leiting (författare)
- Battery Electrodes and Cells, Electrochemistry Laboratory, Paul Scherrer Institute, Villigen-PSI, Switzerland
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Koç, Tuncay (författare)
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Belin, Stéphanie (författare)
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Cabana, Jordi (författare)
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Dedryvère, Rémi (författare)
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Abakumov, Artem M. (författare)
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Tarascon, Jean-Marie (författare)
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(creator_code:org_t)
- 2022-06-20
- 2022
- Engelska.
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Ingår i: Nature Materials. - : Springer Nature. - 1476-1122 .- 1476-4660. ; 21:10, s. 1165-1174
- Relaterad länk:
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Reversible anionic redox reactions represent a transformational change for creating advanced high-energy-density positive-electrode materials for lithium-ion batteries. The activation mechanism of these reactions is frequently linked to ligand-to-metal charge transfer (LMCT) processes, which have not been fully validated experimentally due to the lack of suitable model materials. Here we show that the activation of anionic redox in cation-disordered rock-salt Li1.17Ti0.58Ni0.25O2 involves a long-lived intermediate Ni3+/4+ species, which can fully evolve to Ni2+ during relaxation. Combining electrochemical analysis and spectroscopic techniques, we quantitatively identified that the reduction of this Ni3+/4+ species goes through a dynamic LMCT process (Ni3+/4+–O2− → Ni2+–On−). Our findings provide experimental validation of previous theoretical hypotheses and help to rationalize several peculiarities associated with anionic redox, such as cationic–anionic redox inversion and voltage hysteresis. This work also provides additional guidance for designing high-capacity electrodes by screening appropriate cationic species for mediating LMCT.
Ämnesord
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
Nyckelord
- Kemi med inriktning mot materialkemi
- Chemistry with specialization in Materials Chemistry
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- ref (ämneskategori)
- art (ämneskategori)
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Till lärosätets databas
- Av författaren/redakt...
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Li, Biao
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Kumar, Khagesh
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Roy, Indrani
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Morozov, Anatoli ...
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Emelyanova, Olga ...
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Zhang, Leiting
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visa fler...
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Koç, Tuncay
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Belin, Stéphanie
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Cabana, Jordi
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Dedryvère, Rémi
-
Abakumov, Artem ...
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Tarascon, Jean-M ...
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visa färre...
- Om ämnet
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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Nature Materials
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Uppsala universitet