Role of binders in solid electrolyte interphase formation in lithium ion batteries studied with hard X-ray photoelectron spectroscopy

Young, Benjamin; Nguyen, Cao Cuong; Lobach, Anton; Heskett, David R.; Woicik, J. C.; Lucht, Brett L.

doi:10.1557/jmr.2018.363

Cited by 19 publications

(20 citation statements)

References 27 publications

(29 reference statements)

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“…11,14,[17][18][19] This one appears not only essential to constrain the volume expansion of the electrode or maintain contact with the current collector, but also to minimize the degradation of the liquid electrolyte by pre-forming an "artificial" protective SEI layer. 11,14,20,21 The preparation and processing of the electrode slurry (e.g. type of grinding, casting speed, drying temperature) and electrode parameters (porosity [22][23][24] and thickness 25 ) are also critical to the electrochemical behavior of the electrode.…”

Section: Introductionmentioning

confidence: 99%

Influence of the Polyacrylic Acid Binder Neutralization Degree on the Initial Electrochemical Behavior of a Silicon/Graphite Electrode

Xiong

Dupré

Mazouzi

et al. 2021

ACS Appl. Mater. Interfaces

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The role of the physico-chemical properties of the water soluble PAA binder on the lithium electrochemical performance of highly loaded silicon/graphite 50/50 wt% negative electrodes has been examined as a function of the neutralization degree x in PAAH1-xLix at initial cycle in an electrolyte not-containing ethylene carbonate. Electrode processing in acidic PAAH binder at pH 2.5 leads to a deep copper corrosion resulting in a significant electrode cohesion and adhesion to the current collector surface, but the strong binder rigidity may explain the big cracks occurring at the electrode surface at first cycle. The non-uniform binder coating on the materials surface leads to an important degradation of the electrolyte explaining the lowest initial coulombic efficiency and the lowest reversible capacity among the studied electrodes. When processed in neutral pH, the PAAH0.22Li0.78 binder forms a conformal artificial SEI layer on the materials surface, which minimizes the electrolyte reduction at first cycle and then maximizes the initial coulombic efficiency. However, the low mechanical resistance of the electrode and its strong cracking explain its low reversible capacity. Electrodes prepared at intermediate pH 4 combine the positive assets of electrodes prepared at acidic and neutral pH. They lead to the best initial performance with a notable areal capacity of 7.2 mAh cm -2 and the highest initial coulombic efficiency at around 90%, a value much larger than the usual range reported for silicon/graphite anodes. All data obtained with complementary characterization techniques were discussed as a function of the PAA polymeric chain molecular conformation, microstructure, and surface 3 adsorption or grafting, emphasizing the tremendous role of the binder on the electrode initial performance.

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Section: Introductionmentioning

confidence: 99%

Influence of the Polyacrylic Acid Binder Neutralization Degree on the Initial Electrochemical Behavior of a Silicon/Graphite Electrode

Xiong

Dupré

Mazouzi

et al. 2021

ACS Appl. Mater. Interfaces

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“…This leads to the question of how the addition of an insulating polymeric binder, added to mitigate the effect of Si expansion in composite slurries, affects the SEI formation. We know that the binder has a role in electrochemistry regardless of the anode. , For example, the commonly used binder PVDF does not work in silicon-based chemistries, but the use of poly(acrylic acid) (PAA) does. − In addition, the components of composite-based electrodes can change the SEI. Indeed, one study looking at different surface area carbons, the choice of PAA, and CMC binders led to an “artificial SEI” that enhanced the cyclability .…”

Section: Introductionmentioning

confidence: 99%

The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes

Browning

Sacci

Doucet

et al. 2020

ACS Appl. Mater. Interfaces

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We use neutron reflectometry to study how the polymeric binder, poly(acrylic acid) (PAA), affects the in situ formation and chemical composition of the solid−electrolyte interphase (SEI) formation on a silicon anode at various states of charge. The reflectivity is correlated with electrochemical quartz crystal microbalance to better understand the viscoelastic effects of the polymer during cycling. The use of model thin films allows for a well-controlled interface between the amorphous Si surface and the PAA layer. If the PAA perfectly coats the Si surface and standard processing conditions are used, the binder will prevent the lithiation of the anode. The PAA suppresses the growth of a new layer formed at early states of discharge (open circuit voltage to 0.8 V vs Li/Li + ), protecting the surface of the anode. At 0.15 V, the SEI layer underneath the PAA changes in chemical composition as indicated by an increase in the scattering length density and thickness as the layer incorporates components from the electrolyte, most likely the salt. At lithiated and delithiated states, the SEI layer changes in chemical composition and grows in thickness with delithiation and shrinks during lithiation.

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“…Preferential solvent reduction on the basal plane at lower potential vs. Li + /Li determines larger organic content in the SEI 1 . Besides, the SEI growth and structure depend on binder material 23,24 . To the best of our knowledge, only two in situ AFM measurement of SEI formation were reported on a composite electrode comprised of graphite powder mixed with polyvinylidene difluoride (PVDF) binder and a conductive additive: (1) in 1997 25 authors reported difficulties of such measurements, and (2) in 2017 26 the imaging quality was not enough to observe SEI formation due to rough surface and AFM tip contamination.…”

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confidence: 99%

Solid-electrolyte interphase nucleation and growth on carbonaceous negative electrodes for Li-ion batteries visualized with in situ atomic force microscopy

Luchkin

Lipovskikh

Katorova

et al. 2020

Sci Rep

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Li-ion battery performance and life cycle strongly depend on a passivation layer called solid-electrolyte interphase (SEI). Its structure and composition are studied in great details, while its formation process remains elusive due to difficulty of in situ measurements of battery electrodes. Here we provide a facile methodology for in situ atomic force microscopy (AFM) measurements of SEI formation on cross-sectioned composite battery electrodes allowing for direct observations of SEI formation on various types of carbonaceous negative electrode materials for Li-ion batteries. Using this approach, we observed SEI nucleation and growth on highly oriented pyrolytic graphite (HOPG), MesoCarbon MicroBeads (MCMB) graphite, and non-graphitizable amorphous carbon (hard carbon). Besides the details of the formation mechanism, the electrical and mechanical properties of the SEI layers were assessed. The comparative observations revealed that the electrode potentials for SEI formation differ depending on the nature of the electrode material, whereas the adhesion of SEI to the electrode surface clearly correlates with the surface roughness of the electrode. Finally, the same approach applied to a positive LiNi1/3Mn1/3Co1/3O2 electrode did not reveal any signature of cathodic SEI thus demonstrating fundamental differences in the stabilization mechanisms of the negative and positive electrodes in Li-ion batteries.

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Role of binders in solid electrolyte interphase formation in lithium ion batteries studied with hard X-ray photoelectron spectroscopy

Abstract: Abstract

Cited by 19 publications

References 27 publications

Influence of the Polyacrylic Acid Binder Neutralization Degree on the Initial Electrochemical Behavior of a Silicon/Graphite Electrode

Influence of the Polyacrylic Acid Binder Neutralization Degree on the Initial Electrochemical Behavior of a Silicon/Graphite Electrode

The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes

Solid-electrolyte interphase nucleation and growth on carbonaceous negative electrodes for Li-ion batteries visualized with in situ atomic force microscopy

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