Glyoxalated polyacrylamide as a covalently attachable and rapidly cross-linkable binder for Si electrode in lithium ion batteries

Yoo, Jung-Keun; Jeon, Jaebeom; Kang, Kisuk; Jung, Yeon Sik

doi:10.1007/s13391-017-6288-1

Cited by 10 publications

(7 citation statements)

References 23 publications

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“…From the first charge‐discharge profiles (Figure 4(b)), the plateaus of typical Si‐MP electrodes are observed in all the electrodes at 0.43 and 0.07 V (vs. Li/Li + ), corresponding to the two‐phase reaction between crystalline Si and amorphous lithiated Si ( a‐ Li x Si) [2,3] . The initial Coulombic efficiency (ICE) of electrodes with the PANa 0.8 Fe y binder is the highest (92.3 %) at 1 mol % Fe, and less surface area of Si‐MP than Si‐NP gives rise to more than 90 % of ICE [26–36] . The cyclic voltammograms of PAA/CB and PANa 0.8 Fe y /CB composites show little sign of side reactions (Figure S8).…”

Section: Resultsmentioning

confidence: 99%

“…[2,3] The initial Coulombic efficiency (ICE) of electrodes with the PANa 0.8 Fe y binder is the highest (92.3 %) at 1 mol % Fe, and less surface area of Si-MP than Si-NP gives rise to more than 90 % of ICE. [26][27][28][29][30][31][32][33][34][35][36] The cyclic voltammograms of PAA/CB and PANa 0.8 Fe y / CB composites show little sign of side reactions ( Figure S8). Regardless of the Fe 3 + compositions, similar shapes are shown with a reduction of fluoroethylene carbonate (FEC) at 1.5 V (vs. Li/Li + ) during the first scan.…”

Section: Electrochemical Properties Of Si-mp Electrodementioning

confidence: 99%

“…In the early stage of binder research, Si-nanoparticle (Si-NP) electrode has achieved great enhancement by using polymers with abundant polar functional groups, such as carboxymethyl cellulose (CMC), [24] alginate (Alg), [25] and polyacrylic acid (PAA). [26] The polymer architectures were also modified to improve the adhesion of electrode by branching [27][28][29] or cross-linking via covalent bonds [30][31][32][33] and non-covalent interactions. [34][35][36][37][38] In addition, chemical structure of the polymer has been varied to make a multi-functional binder with acceptable flexibility and electronic conductivity.…”

Section: Introductionmentioning

confidence: 99%

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Metal‐Coordination Mediated Polyacrylate for High Performance Silicon Microparticle Anode

Woo

Gil

Kim

et al. 2020

Batteries & Supercaps

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As opposed to nano-Si anodes, Si-microparticle (Si-MP)-based negative electrode is still in an immature stage due to the fragility of particles of which dimension is farther from the critical size of Si. In terms of binder chemistry, the established strategies for nano-Si anode can be moderately transferred to designing functional binders for commercially available Si-MP. However, only a few studies have reported acceptable electrochemical properties of Si-MP in the level of designing novelbinder systems. Herein, the ionically crosslinked polyacrylate (PANa 0.8 Fe y) inspired by metallo-supramolecular polymers is introduced as a binder for Si-MP anode. Although cracking of Si-MP is inevitable during cycles, the electrode components can effectively be confined within the supramolecular network, which reversibly adjusts its architecture via iron (Fe 3 +)-carboxylate coordination. With appropriate compositions, the incorporation of ferric ion to sodium polyacrylate allows the Si-MP to exhibit an excellent round-trip capacity of~1400 mAh g À 1 after 400 cycles. The resulting electrochemical performance is demonstrated by several correlated factors: (i) type of supramolecular interactions, (ii) effect of cations (Na + /Fe 3 +) on the conformation of polymer, and (iii) mechanical properties of the electrode.

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Section: Resultsmentioning

confidence: 99%

Section: Electrochemical Properties Of Si-mp Electrodementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Metal‐Coordination Mediated Polyacrylate for High Performance Silicon Microparticle Anode

Woo

Gil

Kim

et al. 2020

Batteries & Supercaps

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“…It has also been suggested that the structural modification of multifunctional binders could enhance the interactions of polymer–polymer as an effective method for dissipating the mechanical stresses and confining the active materials in their carbon‐chain network . For example, the hyperbranched‐type binder (β‐cyclodextrin), which can form multidimensional hydrogen bonding with Si particles, exhibited a remarkable improvement on cycling .…”

Section: Introductionmentioning

confidence: 99%

3D Meshlike Polyacrylamide Hydrogel as a Novel Binder System via in situ Polymerization for High‐Performance Si‐Based Electrode

Woo

Park

Kim

et al. 2019

Adv Materials Inter

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Silicon has been considered as a promising anode material due to its high theoretical capacity (3579 mAh g−1), however, it suffers from capacity degradation owing to the series of multiscale fractures in the electrode caused by the volume variation (≈300%) during phase transitions. The molecular/structural design of polymeric binders has been pivotal in overcoming the challenges to improve the integrity of Si anode via strong interactions between active materials and binders. In this respect, the covalently crosslinked polyacrylamide (PAM) network, which effectively maintains its mechanical strength and shape, is introduced as a novel binder system for Si active materials. Unlike the thermal crosslinking, the abundant polar‐functional groups, related to the strong interactions between Si and polymer, are not sacrificed in their network by virtue of the in situ polymerization. Through the PAM gel, the Si‐based electrode exhibits a superior capacity of ≈1526 mAh g−1 at an optimized crosslinker concentration after 500 cycles. In addition, the effect of the chemical/mechanical properties of PAM gel on the electrochemical properties of Si is adequately elucidated. The results will provide meaningful insight regarding the design of novel binders, especially in the application of the covalently crosslinked structure to Si‐based electrodes.

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“…13 Yoo et al also studied a cross-linked PAM network as a binder in Si anodes and found that systematic variations of the cross-link density had a significant impact on performance and stability. 14 While these studies indicate that PAM is a promising material for Si anodes, these studies did not conduct an analysis of various physicochemical properties relevant to battery performance, including adhesion strength, electrolyte uptake, and electrochemical stability. These studies also utilized in situ cross-linking and/or polymerization to produce the binder, which increases the complexity of the electrode fabrication process.…”

Section: Introductionmentioning

confidence: 99%

A Comprehensive Study of Hydrolyzed Polyacrylamide as a Binder for Silicon Anodes

Miranda

Haregewoin

et al. 2019

ACS Appl. Mater. Interfaces

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Silicon anodes have a high theoretical capacity for lithium storage, but current composite electrode formulations are not sufficiently stable under long-term electrochemical cycling. The choice of polymeric binder has been shown to impact stability and capacity of silicon anodes for electrochemical energy storage. While several promising polymeric binders have been identified, there is a knowledge gap in how various physicochemical propertiesincluding adhesion, mechanical integrity, and ion diffusionimpact electrochemical stability and performance. In this work, we comprehensively investigate the physical properties and performance of a molecular-weight series (3−20 × 10 6 g/ mol) of partially hydrolyzed polyacrylamide (HPAM) in silicon anodes. We quantify the mechanical strength, electrolyte uptake, adhesion to silicon, copper, and carbon, as well as electrochemical performance and stability and find that HPAM satisfies many of the properties generally believed to be favorable, including good adhesion, high strength, and electrochemical stability. HPAM does not show any electrolyte uptake regardless of any molecular weight studied, and thin films of mid-and high-molecular-weight HPAM on silicon surfaces suppress lithiation of silicon. The resulting composite electrodes exhibit an electrochemical storage capacity greater than 3000 mAh/g initially and 1639 mAh/g after 100 cycles. We attribute capacity fade to failure of mechanical properties of the binder or an excess of the solid electrolyte interphase layer being formed at the Si surface. While the highest-molecular-weight sample was expected to perform the best given its stronger adhesion and bulk mechanical properties, we found that HPAM of moderate molecular weight performed the best. We attribute this to a trade-off in mechanical strength and uniformity of the resulting electrode. This work demonstrates promising performance of a low-cost polymer as a binder for Si anodes and provides insight into the physical and chemical properties that influence binder performance.

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Glyoxalated polyacrylamide as a covalently attachable and rapidly cross-linkable binder for Si electrode in lithium ion batteries

Cited by 10 publications

References 23 publications

Metal‐Coordination Mediated Polyacrylate for High Performance Silicon Microparticle Anode

Metal‐Coordination Mediated Polyacrylate for High Performance Silicon Microparticle Anode

3D Meshlike Polyacrylamide Hydrogel as a Novel Binder System via in situ Polymerization for High‐Performance Si‐Based Electrode

A Comprehensive Study of Hydrolyzed Polyacrylamide as a Binder for Silicon Anodes

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