Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion Batteries

Shi, Zhangxing; Jiang, Sisi; Robertson, Lily A.; Zhao, Yuyue; Sarnello, Erik; Li, Tao; Chen, Wei; Zhang, Zhengcheng; Zhang, Lu

doi:10.1021/acsami.0c18559

Title: Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion Batteries

Journal Article · Wed Dec 16 00:00:00 EST 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c18559· OSTI ID:1777918

^[1]; Jiang, Sisi ^[1];

^[2]; Zhao, Yuyue ^[2]; Sarnello, Erik ^[3];

^[4];

^[5];

^[2];

^[2]

Argonne National Lab. (ANL), Lemont, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States). Joint Center for Energy Storage Research (JCESR)
Northern Illinois Univ., DeKalb, IL (United States)
Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
Argonne National Lab. (ANL), Lemont, IL (United States). Inst. for Molecular Engineering; Univ. of Chicago, IL (United States). Inst. for Molecular Engineering

Neutralization of poly(acrylic acid) (PAA)-based binders using lithium hydroxide is a common strategy for fabricating silicon anode laminates, which improves rheological properties of slurries toward high-quality electrode laminates. However, the significantly increased basicity causes degradation of Si particles while the irreversible conversion of carboxylic acid groups to lithium carboxylates undermines the binding strength, collectively leading to adverse cycling performance of the fabricated Si anodes. Herein, a novel neutralization process for PAA binders is developed. A weak base, ammonia (NH₃), was discovered as a neutralizing agent that still promotes rheological response of binder solutions but results in a reduced pH increase. Interestingly, the resulting ammonium carboxylate groups may cleave during the drying process to restore the neutralized PAA (PAA-NH₃) binders to their pristine states. The best-performing composition of 50% neutralization (PAA-50%NH₃) provides comparable rheological response as a PAA-Li binder as well as much improved cycling performance. Additionally, the half-cells using the PAA-50%NH₃ binder can deliver 60% capacity retention over 100 cycles at C/3 rate, affording a 23.8% increase compared to PAA-Li half-cells. This restorable neutralization process of PAA binders represents an innovative strategy of mitigating issues from slurry processing of Si particles to achieve concurrent improvements in high-quality lamination and cycling performance.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1777918

Journal Information:: ACS Applied Materials and Interfaces, Vol. 12, Issue 52; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (40)

Reversible Cycling of Crystalline Silicon Powder Obrovac, M. N.; Krause, L. J. Journal of The Electrochemical Society, Vol. 154, Issue 2 https://doi.org/10.1149/1.2402112	journal	January 2007
Understanding Polyacrylic Acid and Lithium Polyacrylate Binder Behavior in Silicon Based Electrodes for Li-Ion Batteries Porcher, W.; Chazelle, S.; Boulineau, A. Journal of The Electrochemical Society, Vol. 164, Issue 14 https://doi.org/10.1149/2.0821714jes	journal	January 2017
Electrostatic and Hydrophobic Interactions in NaCMC Aqueous Solutions: Effect of Degree of Substitution Lopez, Carlos G.; Colby, Ralph H.; Cabral, João T. Macromolecules, Vol. 51, Issue 8 https://doi.org/10.1021/acs.macromol.8b00178	journal	April 2018
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Poly(4-vinylbenzoic acid): A Re-Engineered Binder for Improved Performance from Water-Free Slurry Processing for Silicon Graphite Composite Electrodes Hu, Bin; Jiang, Sisi; Shkrob, Ilya A. ACS Applied Energy Materials, Vol. 2, Issue 9 https://doi.org/10.1021/acsaem.9b00987	journal	August 2019
Silicon-Based Anodes for Lithium-Ion Batteries: From Fundamentals to Practical Applications Feng, Kun; Li, Matthew; Liu, Wenwen Small, Vol. 14, Issue 8 https://doi.org/10.1002/smll.201702737	journal	January 2018
Sodium Carboxymethyl Cellulose Li, Jing; Lewis, R. B.; Dahn, J. R. Electrochemical and Solid-State Letters, Vol. 10, Issue 2 https://doi.org/10.1149/1.2398725	journal	January 2007
Adhesive Polymers as Efficient Binders for High-Capacity Silicon Electrodes Pan, Yiyang; Ge, Sirui; Rashid, Zahid ACS Applied Energy Materials, Vol. 3, Issue 4 https://doi.org/10.1021/acsaem.9b02420	journal	March 2020
Colossal Reversible Volume Changes in Lithium Alloys Beaulieu, L. Y.; Eberman, K. W.; Turner, R. L. Electrochemical and Solid-State Letters, Vol. 4, Issue 9 https://doi.org/10.1149/1.1388178	journal	January 2001
Viscosity, shear strength, and peel strength on poly(ethylene terephthalate) of (natural rubber)-based adhesives containing hybrid tackifiers Poh, B. T.; Syed Putra, S. Z. Firdaus Journal of Vinyl and Additive Technology, Vol. 17, Issue 3 https://doi.org/10.1002/vnl.20273	journal	July 2011
Acrylic random copolymer and network binders for silicon anodes in lithium-ion batteries Son, Jinha; Vo, Thuan Ngoc; Cho, Seungwan Journal of Power Sources, Vol. 458 https://doi.org/10.1016/j.jpowsour.2020.228054	journal	May 2020
Dynamics of a High Molecular Weight Polyelectrolyte Pabon, Martial; Selb, Joseph; Candau, Françoise Langmuir, Vol. 14, Issue 4 https://doi.org/10.1021/la971021i	journal	February 1998
Quantifying gas generation from slurries used in fabrication of Si-containing electrodes for lithium-ion cells Rodrigues, Marco-Tulio F.; Trask, Stephen E.; Shkrob, Ilya A. Journal of Power Sources, Vol. 395 https://doi.org/10.1016/j.jpowsour.2018.05.071	journal	August 2018
Challenges in Lithium‐Ion‐Battery Slurry Preparation and Potential of Modifying Electrode Structures by Different Mixing Processes Wenzel, Valentin; Nirschl, Hermann; Nötzel, Dorit Energy Technology, Vol. 3, Issue 7 https://doi.org/10.1002/ente.201402218	journal	May 2015
Re‐Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium‐Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders Jiang, Sisi; Hu, Bin; Shi, Zhangxing Advanced Functional Materials, Vol. 30, Issue 10 https://doi.org/10.1002/adfm.201908558	journal	December 2019
The existence of optimal molecular weight for poly(acrylic acid) binders in silicon/graphite composite anode for lithium-ion batteries Hu, Bin; Shkrob, Ilya A.; Zhang, Shuo Journal of Power Sources, Vol. 378 https://doi.org/10.1016/j.jpowsour.2017.12.068	journal	February 2018
Effect of Binder Architecture on the Performance of Silicon/Graphite Composite Anodes for Lithium Ion Batteries Cao, Peng-Fei; Naguib, Michael; Du, Zhijia ACS Applied Materials & Interfaces, Vol. 10, Issue 4 https://doi.org/10.1021/acsami.7b13205	journal	January 2018
Toward Efficient Binders for Li-Ion Battery Si-Based Anodes: Polyacrylic Acid Magasinski, Alexandre; Zdyrko, Bogdan; Kovalenko, Igor ACS Applied Materials & Interfaces, Vol. 2, Issue 11 https://doi.org/10.1021/am100871y	journal	October 2010
Studies of the viscosity and sedimentation of suspensions Part 1. - The viscosity of suspension of spherical particles Ward, S. G.; Whitmore, R. L. British Journal of Applied Physics, Vol. 1, Issue 11 https://doi.org/10.1088/0508-3443/1/11/303	journal	November 1950
Biomolecular Assembly of Thermoresponsive Superlattices of the Tobacco Mosaic Virus with Large Tunable Interparticle Distances Li, Tao; Zan, Xingjie; Winans, Randall E. Angewandte Chemie International Edition, Vol. 52, Issue 26 https://doi.org/10.1002/anie.201209299	journal	May 2013
Effect of binder and composition ratio on electrochemical performance of silicon/graphite composite battery electrode Farooq, Umer; Choi, Jeong-Hee; Atif Pervez, Syed Materials Letters, Vol. 136 https://doi.org/10.1016/j.matlet.2014.08.059	journal	December 2014
Small Angle X-ray Scattering for Nanoparticle Research Li, Tao; Senesi, Andrew J.; Lee, Byeongdu Chemical Reviews, Vol. 116, Issue 18 https://doi.org/10.1021/acs.chemrev.5b00690	journal	April 2016
Designing nanostructured Si anodes for high energy lithium ion batteries Wu, Hui; Cui, Yi Nano Today, Vol. 7, Issue 5 https://doi.org/10.1016/j.nantod.2012.08.004	journal	October 2012
The emerging era of supramolecular polymeric binders in silicon anodes Kwon, Tae-woo; Choi, Jang Wook; Coskun, Ali Chemical Society Reviews, Vol. 47, Issue 6 https://doi.org/10.1039/C7CS00858A	journal	January 2018
In Situ Observation and Long-Term Reactivity of Si/C/CMC Composites Electrodes for Li-Ion Batteries Bridel, J-S.; Azaïs, T.; Morcrette, M. Journal of The Electrochemical Society, Vol. 158, Issue 6 https://doi.org/10.1149/1.3581024	journal	January 2011
A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries Kovalenko, I.; Zdyrko, B.; Magasinski, A. Science, Vol. 334, Issue 6052 https://doi.org/10.1126/science.1209150	journal	September 2011
Measurement and Analysis of Adhesion Property of Lithium-Ion Battery Electrodes with SAICAS Son, Bongki; Ryou, Myung-Hyun; Choi, Jaecheol ACS Applied Materials & Interfaces, Vol. 6, Issue 1 https://doi.org/10.1021/am404580f	journal	December 2013
Effect of high adhesive polyvinyl alcohol binder on the anodes of lithium ion batteries Park, Hye-Kyoung; Kong, Byung-Seon; Oh, Eun-Suok Electrochemistry Communications, Vol. 13, Issue 10 https://doi.org/10.1016/j.elecom.2011.06.034	journal	October 2011
Li-alloy based anode materials for Li secondary batteries Park, Cheol-Min; Kim, Jae-Hun; Kim, Hansu Chemical Society Reviews, Vol. 39, Issue 8, p. 3115-3141 https://doi.org/10.1039/b919877f	journal	January 2010
Confronting Issues of the Practical Implementation of Si Anode in High-Energy Lithium-Ion Batteries Chae, Sujong; Ko, Minseong; Kim, Kyungho Joule, Vol. 1, Issue 1 https://doi.org/10.1016/j.joule.2017.07.006	journal	September 2017
Exploring Chemical, Mechanical, and Electrical Functionalities of Binders for Advanced Energy-Storage Devices Chen, Hao; Ling, Min; Hencz, Luke Chemical Reviews, Vol. 118, Issue 18 https://doi.org/10.1021/acs.chemrev.8b00241	journal	August 2018
Standardization of peeling tests for assessing the cohesion and consolidation characteristics of historic stone surfaces Drdácký, Miloš; Lesák, Jaroslav; Rescic, Silvia Materials and Structures, Vol. 45, Issue 4 https://doi.org/10.1617/s11527-011-9778-x	journal	September 2011
Understanding of pre-lithiation of poly(acrylic acid) binder: Striking the balances between the cycling performance and slurry stability for silicon-graphite composite electrodes in Li-ion batteries Hu, Bin; Jiang, Sisi; Shkrob, Ilya A. Journal of Power Sources, Vol. 416 https://doi.org/10.1016/j.jpowsour.2019.01.068	journal	March 2019
Millipede-inspired structural design principle for high performance polysaccharide binders in silicon anodes Jeong, You Kyeong; Kwon, Tae-woo; Lee, Inhwa Energy & Environmental Science, Vol. 8, Issue 4 https://doi.org/10.1039/C5EE00239G	journal	January 2015
Systematic Investigation of Binders for Silicon Anodes: Interactions of Binder with Silicon Particles and Electrolytes and Effects of Binders on Solid Electrolyte Interphase Formation Nguyen, Cao Cuong; Yoon, Taeho; Seo, Daniel M. ACS Applied Materials & Interfaces, Vol. 8, Issue 19 https://doi.org/10.1021/acsami.6b03357	journal	May 2016
Hydrogen generation by reaction of Si nanopowder with neutral water Kobayashi, Yuki; Matsuda, Shinsuke; Imamura, Kentaro Journal of Nanoparticle Research, Vol. 19, Issue 5 https://doi.org/10.1007/s11051-017-3873-z	journal	May 2017
Lithium-Ion Batteries Writer, Beta https://doi.org/10.1007/978-3-030-16800-1	book	January 2019
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction Obrovac, M. N.; Christensen, Leif Electrochemical and Solid-State Letters, Vol. 7, Issue 5 https://doi.org/10.1149/1.1652421	journal	January 2004
Si Oxidation and H ₂ Gassing During Aqueous Slurry Preparation for Li-Ion Battery Anodes Hays, Kevin A.; Key, Baris; Li, Jianlin The Journal of Physical Chemistry C, Vol. 122, Issue 18 https://doi.org/10.1021/acs.jpcc.8b01062	journal	April 2018
Charge density effects on polyelectrolyte dynamic rheology Harrington, John C. Journal of Applied Polymer Science, Vol. 107, Issue 5 https://doi.org/10.1002/app.27405	journal	January 2007

Similar Records

A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes

Journal Article · Mon Dec 06 00:00:00 EST 2021 · Journal of Materials Chemistry. A · OSTI ID:1777918

Shi, Zhangxing; Liu, Qian; Yang, Zhenzhen; +5 more

Understanding of pre-lithiation of poly(acrylic acid) binder: Striking the balances between the cycling performance and slurry stability for silicon-graphite composite electrodes in Li-ion batteries

Journal Article · Wed Feb 06 00:00:00 EST 2019 · Journal of Power Sources · OSTI ID:1777918

Hu, Bin; Jiang, Sisi; Shkrob, Ilya A.; +8 more

Re-Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium-Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders

Journal Article · Fri Dec 27 00:00:00 EST 2019 · Advanced Functional Materials · OSTI ID:1777918

Jiang, Sisi; Hu, Bin; Shi, Zhangxing; +3 more

Related Subjects

25 ENERGY STORAGE
poly(acrylic acid) binder
neutralization
lamination
silicon anodes
lithium-ion batteries
x-ray scattering
electrodes
electrochemical cells
viscosity
silicon

Title: Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion Batteries

Citation Formats

References (40)

Similar Records

Related Subjects