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

Miranda, Andrea; Li, Xiaoyi; Haregewoin, Atetegeb Meazah; Sarang, Kasturi; Lutkenhaus, Jodie; Kostecki, Robert; Verduzco, Rafael

doi:10.1021/acsami.9b13257

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

Journal Article · Thu Oct 24 00:00:00 EDT 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.9b13257· OSTI ID:1765552

Miranda, Andrea ^[1]; Li, Xiaoyi ^[1]; ^[2]; Sarang, Kasturi ^[3]; ^[3]; Kostecki, Robert ^[2]; ^[1]

Rice Univ., Houston, TX (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Texas A & M Univ., College Station, TX (United States)

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 × 10⁶ g/mol) of partially hydrolyzed polyacrylamide (HPAM) in silicon anodes. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; SC0014664; EE0006443

OSTI ID:: 1765552

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 47 Vol. 11; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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