Ending the Chase for a Perfect Binder: Role of Surface Chemistry Variation and its Influence on Silicon Anodes

Hays, Kevin A.; Armstrong, Beth L.; Veith, Gabriel M.

doi:10.1002/celc.202001066

Cited by 10 publications

(5 citation statements)

References 81 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…34 Hays et al also reported a much higher adhesion for PAAHbased Si/Gr electrodes compared to PAALi-based ones. 31 Contradictions between different studies may result from differences in the electrode manufacturing process (mixing and drying conditions), 42 the characteristics of the active material (particle size, silicon surface chemistry, and silicon/graphite ratio), 33,43 or the molar mass of the binder, 44 as well as the cycling conditions and, in particular, the choice of the electrolyte. This great diversity makes the rationalization difficult and highlights the need to understand and rationalize the underlying phenomena.…”

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

View full text Add to dashboard Cite

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.

show abstract

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

View full text Add to dashboard Cite

show abstract

“…In a study by Hays et al, it was found that at higher pH values, the zeta potential of nano-Si particles increases in magnitude, leading to a stronger particle-particle repulsion that can overcome the weak van der Waals attractions in the electrode slurry. 19 As a result, the Si particles tend to disperse better, which is beneficial for eventual electrode performance. We did not do any particle dispersion tests with our 5.…”

Section: δ =mentioning

confidence: 99%

The Effects of Lithium Ions and pH on the Function of Polyacrylic Acid Binder for Silicon Anodes

Sun

Wheeler

2023

J. Electrochem. Soc.

View full text Add to dashboard Cite

Binder plays a critical role in the performance of silicon anodes for lithium-ion batteries, specifically by connecting particles of active material and promoting adhesion to the current collector. Recent studies have differed on the relative cycle life of silicon anodes made from water-based polyacrylic acid (PAA) vs. LiOH-PAA binders. Differences between the two may be due to the pH value or the extra Li+ in the binder, both of which change when LiOH is added to PAA. Here we investigate the impact of these two variables on the performance of silicon anodes. Regarding the effect of Li+, cyclic voltammetry and electrochemical impedance spectroscopy results confirm our hypothesis that the extra Li+ facilitates ion transport. Regarding pH, we find that high pH in binders is detrimental to the electrode mechanical integrity, as observed in peeling tests and cross-sectional imaging. However, viscosity tests reveal that increased pH benefits the coating and mixing process. Our cycling results show that LiOH-PAA binder maintains greater cell capacity than does PAA, and further that LiOH-PAA at pH 4.5 leads to a cell with the highest capacity. Therefore, an intermediate pH is an optimal compromise between benefits observed for the low and high pH experiments.

show abstract

“…Traditionally, Sb thin films have been fabricated through slurry casting that consists of ball milling Sb powder, a conductive carbon additive, and a polymeric binder. Through this technique, various factors can be controlled, such as the strength of the polymeric binder, that helps maintain the mechanical integrity of the film, and the conductive additive that can improve electronic conductivity. − Other fabrication techniques used to study the properties and performance of Sb involve sputtering of Sb , and solvothermal methods, , but these techniques fall short due to cost and poor scalability.…”

Section: Introductionmentioning

confidence: 99%

Structural Control of Electrodeposited Sb Anodes through Solution Additives and Their Influence on Electrochemical Performance in Na-Ion Batteries

Nieto,

Windsor,

Kale

et al. 2023

J. Phys. Chem. C

View full text Add to dashboard Cite

Alloy-based materials such as antimony (Sb) are of interest for both Li/Na-ion batteries due to their high theoretical capacity and electronic conductivity. Of the various ways to fabricate Sb films (slurry casting, sputtering, etc.) one promising route is through electrodeposition. Electrodeposition is an industrially relevant synthetic technique that allows for the use of solution additives to control different characteristics such as film uniformity, morphology, and electrical conductivity. Solution additives such as cetyltrimethylammonium bromide (CTAB) and bis(3-sulfopropyl) disulfide (SPS) have been used to control different characteristics such as particle morphology and electrical conductivity in various electrodeposits but have not been applied to the electrodeposition of Sb for battery applications. In this study, Sb films were electrodeposited with varied concentrations of CTAB and SPS and the structure, morphology, composition, and electrochemical performance in Na-ion batteries were compared. We report that CTAB and SPS additives can significantly influence electrodeposited Sb films by altering the morphology and reduce the crystallinity, affecting the electrochemical performance. These studies provide valuable insight into the tunability of alloy-based films through electrodeposition and solution additives for battery applications.

show abstract

Ending the Chase for a Perfect Binder: Role of Surface Chemistry Variation and its Influence on Silicon Anodes

Cited by 10 publications

References 81 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 Effects of Lithium Ions and pH on the Function of Polyacrylic Acid Binder for Silicon Anodes

Structural Control of Electrodeposited Sb Anodes through Solution Additives and Their Influence on Electrochemical Performance in Na-Ion Batteries

Contact Info

Product

Resources

About