Interweaving Elastic and Hydrogen Bond‐Forming Polymers into Highly Tough and Stress‐Relaxable Binders for High‐Performance Silicon Anode in Lithium‐Ion Batteries

Author:

Jeong Daun1,Yook Jinsol2,Kwon Da‐Sol13,Shim Jimin1ORCID,Lee Jong‐Chan2ORCID

Affiliation:

1. Energy Storage Research Center Korea Institute of Science and Technology (KIST) 14 Gil 5 Hwarang‐ro, Seongbuk‐gu Seoul 02792 Republic of Korea

2. School of Chemical and Biological Engineering and Institute of Chemical Processes Seoul National University 1, Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea

3. Department of Chemical and Biological Engineering Korea University 145, Anam‐ro, Seongbuk‐gu Seoul 02841 Republic of Korea

Abstract

AbstractA central challenge in practically using high‐capacity silicon (Si) as anode materials for lithium‐ion batteries is alleviating significant volume change of Si during cycling. One key to resolving the failure issues of Si is exploiting carefully designed polymer binders exhibiting mechanical robustness to retain the structural integrity of Si electrodes, while concurrently displaying elasticity and toughness to effectively dissipate external stresses exerted by the volume changes of Si. Herein, a highly elastic and tough polymer binder is proposed by interweaving polyacrylic acid (PAA) with poly(urea‐urethane) (PUU) elastomer for Si anodes. By systematically tuning molecular parameters, including molecular weights of hard/soft segments and structures of hard segment components, it is demonstrated that the mechanical properties of polymer binders, such as elasticity, toughness, and stress relaxation ability, strongly affect the cycling performance of Si electrodes. This study provides new insight into the rational design of polymer binders capable of accommodating the volume changes of Si, primarily by judicious modulation of the mechanical properties of polymer binders.

Funder

National Research Foundation of Korea

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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