A pyrene–poly(acrylic acid)–polyrotaxane supramolecular binder network for high-performance silicon negative electrodes
Cho, YunshikSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
Kim, JaeminSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
Elabd, AhmedDepartment of ChemistryUniversity of Fribourg Chemin de Musee 9 Fribourg 1700 Switzerland
Choi, SunghunSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
Park, KihoSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
Kwon, Tae‐wooGraduate School of Energy, Environment, Waterm, and Sustainability (EEWS)Korea Advanced Institute of Science and Technology (KAIST) 291 Daehak‐ro, Yuseong‐gu Daejeon 34141 Republic of Korea
Lee, JungminSamsung SDI R&D Center 130 Samsung‐ro, Yeongtong‐gu Suwon Gyeonggi‐do 16678 Republic of Korea
Char, KookheonSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
Coskun, AliDepartment of Chemistry, University of Fribourg, Switzerland
Choi, Jang WookSchool of Chemical and Biological Engineering and Institute of Chemical ProcessesSeoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
English
Although being incorporated in commercial lithium‐ion batteries for a while, the weight portion of silicon monoxide (SiOx, x ≈ 1) is only less than 10 wt% due to the insufficient cycle life. Along this line, polymeric binders that can assist in maintaining the mechanical integrity and interfacial stability of SiOx electrodes are desired to realize higher contents of SiOx. Herein, a pyrene–poly(acrylic acid) (PAA)– polyrotaxane (PR) supramolecular network is reported as a polymeric binder for SiOx with 100 wt%. The noncovalent functionalization of a carbon coating layer on the SiOx is achieved by using a hydroxylated pyrene derivative via the π–π stacking interaction, which simultaneously enables hydrogen bonding interactions with the PR– PAA network through its hydroxyl moiety. Moreover, the PR's ring sliding while being crosslinked to PAA endows a high elasticity to the entire polymer network, effectively buffering the volume expansion of SiOx and largely mitigating the electrode swelling. Based on these extraordinary physicochemical properties of the pyrene–PAA–PR supramolecular binder, the robust cycling of SiOx electrodes is demonstrated at commercial levels of areal loading in both half‐cell and full‐cell configurations.