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Aging of electrode/electrolyte interfaces in LiFePO4/graphite cells cycled with and without PMS additive
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
Helmholtz Zentrum Berlin Germany.
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2014 (Engelska)Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 118, nr 24, s. 12649-12660Artikel i tidskrift (Refereegranskat) Published
Ort, förlag, år, upplaga, sidor
2014. Vol. 118, nr 24, s. 12649-12660
Nationell ämneskategori
Oorganisk kemi
Identifikatorer
URN: urn:nbn:se:uu:diva-219334DOI: 10.1021/jp502732jISI: 000337783900009OAI: oai:DiVA.org:uu-219334DiVA, id: diva2:699234
Forskningsfinansiär
StandUpTillgänglig från: 2014-02-26 Skapad: 2014-02-26 Senast uppdaterad: 2017-12-30
Ingår i avhandling
1. The Complex Nature of the Electrode/Electrolyte Interfaces in Li-ion Batteries: Towards Understanding the Role of Electrolytes and Additives Using Photoelectron Spectroscopy
Öppna denna publikation i ny flik eller fönster >>The Complex Nature of the Electrode/Electrolyte Interfaces in Li-ion Batteries: Towards Understanding the Role of Electrolytes and Additives Using Photoelectron Spectroscopy
2014 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

The stability of electrode/electrolyte interfaces in Li-ion batteries is crucial to the performance, lifetime and safety of the entire battery system. In this work, interface processes have been studied in LiFePO4/graphite Li-ion battery cells. 

The first part has focused on improving photoelectron spectroscopy (PES) methodology for making post-mortem battery analyses. Exposure of cycled electrodes to air was shown to influence the surface chemistry of the graphite. A combination of synchrotron and in-house PES has facilitated non-destructive interface depth profiling from the outermost surfaces into the electrode bulk. A better understanding of the chemistry taking place at the anode and cathode interfaces has been achieved. The solid electrolyte interphase (SEI) on a graphite anode was found to be thicker and more inhomogeneous than films formed on cathodes. Dynamic changes in the SEI on cycling and accumulation of lithium close to the carbon surface have been observed.   

Two electrolyte additives have also been studied: a film-forming additive propargyl methanesulfonate (PMS) and a flame retardant triphenyl phosphate (TPP). A detailed study was made at ambient and elevated temperature (21 and 60 °C) of interface aging for anodes and cathodes cycled with and without the PMS additive. PMS improved cell capacity retention at both temperatures. Higher SEI stability, relatively constant thickness and lower loss of cyclable lithium are suggested as the main reasons for better cell performance. PMS was also shown to influence the chemical composition on the cathode surface.

The TPP flame retardant was shown to be unsuitable for high power applications. Low TPP concentrations had only a minor impact on electrolyte flammability, while larger amounts led to a significant increase in cell polarization. TPP was also shown to influence the interface chemistry at both electrodes.

Although the additives studied here may not be the final solution for improved lifetime and safety of commercial batteries, increased understanding has been achieved of the degradation mechanisms in Li-ion cells. A better understanding of interface processes is of vital importance for the future development of safer and more reliable Li-ion batteries.

Ort, förlag, år, upplaga, sidor
Uppsala: Acta Universitatis Upsaliensis, 2014. s. 74
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1129
Nyckelord
Li-ion battery, LiFePO4/graphite cell, interface, electrolyte additives, solid electrolyte interphase (SEI), photoelectron spectroscopy (PES), synchrotron
Nationell ämneskategori
Oorganisk kemi
Forskningsämne
Kemi med inriktning mot oorganisk kemi
Identifikatorer
urn:nbn:se:uu:diva-219336 (URN)978-91-554-8890-1 (ISBN)
Disputation
2014-04-11, Häggsalen, Ångström Laboratory, Lägerhyddsvägen 1, Uppsala, 10:15 (Engelska)
Opponent
Handledare
Tillgänglig från: 2014-03-20 Skapad: 2014-02-26 Senast uppdaterad: 2014-04-29

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Ciosek Högström, KatarzynaHahlin, MariaRensmo, HåkanEdström, Kristina

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