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Title: | Remarkable lowering in the synthesis temperature of LiMn2O4 via citrate solution-gel synthesis facilitated by ethanol | Authors: | MAINO, Giulia CARLEER, Robert MARCHAL, Wouter BONNEUX, Gilles HARDY, An VAN BAEL, Marlies |
Issue Date: | 2017 | Publisher: | ROYAL SOC CHEMISTRY | Source: | DALTON TRANSACTIONS, 46(43), p. 14934-14946 | Abstract: | LiMn2O4 (LMO) is interesting from the viewpoint of its energy storage applications as it is a cathode in lithium ion batteries (LIB), which contains no rare, toxic or expansive elements, while it provides a high theoretical capacity (148 mA h g(-1)) at a reasonable voltage (4 V region) and a higher thermal stability compared to cobalt based cathodes and has a good rechargeability and cycling stability due to its spinel structure. Low temperature synthesis routes for cathode materials are currently gaining attention, in order to decrease the ecological footprint of the final LIB. Here, the crystallization temperature of LMO by a citrate based solution-gel synthesis was significantly lowered, to as low as 250 degrees C by the addition of ethanol to the precursor. The role of ethanol in this synthesis process was explored. It was found to lead to a considerable increase in the oxidation rate of the redox couple Mn2+/Mn3+, a lowering of the precursor decomposition temperature by 200 degrees C, besides a drastic decrease in the crystallization temperature (reaching 250 degrees C). Moreover, the main cause was identified to be an esterification reaction of ethanol with the carboxylic acid in the precursor complexes, taking place before the oxide formation. The insights obtained strengthen the knowledge regarding citrato-Mn2+/Mn3+ complexes present in aqueous solution-gel synthesis routes and are relevant for the preparation of various manganese containing oxides. Moreover, the precursor developed opens up a new possibility for the low temperature synthesis of LMO powders and thin films for application in LIB. In the case of thin film batteries, the low temperature processing provides compatibility with other materials in the thin film battery stack, avoiding undesired oxidations or interfacial reactions. | Notes: | [Maino, G.; Marchal, W.; Bonneux, G.; Hardy, A.; Van Bael, M. K.] UHasselt Hasselt Univ, Inst Mat Res IMO IMOMEC, Inorgan & Phys Chem, Agoralaan, B-3590 Diepenbeek, Belgium. [Carleer, R.] Hasselt Univ, Inst Mat Res, Appl & Analyt Chem, Agoralaan, B-3590 Diepenbeek, Belgium. [Hardy, A.; Van Bael, M. K.] IMEC, Div IMOMEC, B-3590 Diepenbeek, Belgium. | Document URI: | http://hdl.handle.net/1942/25702 | ISSN: | 1477-9226 | e-ISSN: | 1477-9234 | DOI: | 10.1039/c7dt03100a | ISI #: | 000414775000029 | Rights: | This journal is © The Royal Society of Chemistry 2017 | Category: | A1 | Type: | Journal Contribution | Validations: | ecoom 2018 |
Appears in Collections: | Research publications |
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c7dt03100a.pdf Restricted Access | Published version | 4.1 MB | Adobe PDF | View/Open Request a copy |
draft.pdf Restricted Access | Peer-reviewed author version | 2.4 MB | Adobe PDF | View/Open Request a copy |
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