A Pyrene–Poly(acrylic acid)–Polyrotaxane Supramolecular Binder Network for High‐Performance Silicon Negative Electrodes

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.

[1]  Seong‐Hyeon Hong,et al.  Stable Silicon Anode for Lithium Ion Battery through Covalent Bond Formation with Binder via Esterification. , 2019, ACS applied materials & interfaces.

[2]  J. Choi,et al.  Mussel-Inspired Self-Healing Metallopolymers for Silicon Nanoparticle Anodes. , 2019, ACS nano.

[3]  A. Rogach,et al.  Electrochemical Techniques in Battery Research: A Tutorial for Nonelectrochemists , 2019, Advanced Energy Materials.

[4]  David G. Mackanic,et al.  Designing polymers for advanced battery chemistries , 2019, Nature Reviews Materials.

[5]  Jang Wook Choi,et al.  Prospect for Supramolecular Chemistry in High-Energy-Density Rechargeable Batteries , 2019, Joule.

[6]  Yunlong Zhao,et al.  Silicon oxides: a promising family of anode materials for lithium-ion batteries. , 2019, Chemical Society reviews.

[7]  Gao Liu,et al.  A Quadruple-Hydrogen-Bonded Supramolecular Binder for High-Performance Silicon Anodes in Lithium-Ion Batteries. , 2018, Small.

[8]  E. Reichmanis,et al.  SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes , 2018, ACS Applied Energy Materials.

[9]  Haeshin Lee,et al.  A “Sticky” Mucin‐Inspired DNA‐Polysaccharide Binder for Silicon and Silicon–Graphite Blended Anodes in Lithium‐Ion Batteries , 2018, Advanced materials.

[10]  Jiulin Wang,et al.  Silicon Microparticle Anodes with Self-Healing Multiple Network Binder , 2018 .

[11]  J. Choi,et al.  The emerging era of supramolecular polymeric binders in silicon anodes. , 2018, Chemical Society reviews.

[12]  Tao Gao,et al.  Self-Healing Chemistry between Organic Material and Binder for Stable Sodium-Ion Batteries , 2017 .

[13]  Xingyi Zhou,et al.  Material and Structural Design of Novel Binder Systems for High-Energy, High-Power Lithium-Ion Batteries. , 2017, Accounts of chemical research.

[14]  Jaephil Cho,et al.  Confronting Issues of the Practical Implementation of Si Anode in High-Energy Lithium-Ion Batteries , 2017 .

[15]  J. Choi,et al.  Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries , 2017, Science.

[16]  Jitong Wang,et al.  Kinetically-enhanced polysulfide redox reactions by Nb2O5 nanocrystals for high-rate lithium–sulfur battery , 2016 .

[17]  J. Choi,et al.  Mussel-Inspired Polydopamine Coating for Enhanced Thermal Stability and Rate Performance of Graphite Anodes in Li-Ion Batteries. , 2016, ACS applied materials & interfaces.

[18]  Doron Aurbach,et al.  Promise and reality of post-lithium-ion batteries with high energy densities , 2016 .

[19]  Myung Won Seo,et al.  Controlled Prelithiation of Silicon Monoxide for High Performance Lithium-Ion Rechargeable Full Cells. , 2016, Nano letters.

[20]  Erhan Deniz,et al.  Dynamic Cross-Linking of Polymeric Binders Based on Host-Guest Interactions for Silicon Anodes in Lithium Ion Batteries. , 2015, ACS nano.

[21]  Taek-Soo Kim,et al.  Millipede-inspired structural design principle for high performance polysaccharide binders in silicon anodes , 2015 .

[22]  Taek-Soo Kim,et al.  Systematic Molecular‐Level Design of Binders Incorporating Meldrum's Acid for Silicon Anodes in Lithium Rechargeable Batteries , 2014, Advanced materials.

[23]  Donghai Wang,et al.  Interpenetrated Gel Polymer Binder for High‐Performance Silicon Anodes in Lithium‐ion Batteries , 2014 .

[24]  Taek-Soo Kim,et al.  Hyperbranched β-cyclodextrin polymer as an effective multidimensional binder for silicon anodes in lithium rechargeable batteries. , 2014, Nano letters.

[25]  Zhenan Bao,et al.  Self-healing chemistry enables the stable operation of silicon microparticle anodes for high-energy lithium-ion batteries. , 2013, Nature chemistry.

[26]  Guihua Yu,et al.  Three-dimensional hierarchical ternary nanostructures for high-performance Li-ion battery anodes. , 2013, Nano letters.

[27]  Zhenan Bao,et al.  Stable Li-ion battery anodes by in-situ polymerization of conducting hydrogel to conformally coat silicon nanoparticles , 2013, Nature Communications.

[28]  Shuru Chen,et al.  Enhanced performance of SiO/Fe2O3 composite as an anode for rechargeable Li-ion batteries , 2013 .

[29]  Jang Wook Choi,et al.  A bifunctional approach for the preparation of graphene and ionic liquid-based hybrid gels , 2013 .

[30]  Shuru Chen,et al.  Silicon core-hollow carbon shell nanocomposites with tunable buffer voids for high capacity anodes of lithium-ion batteries. , 2012, Physical chemistry chemical physics : PCCP.

[31]  Jaephil Cho,et al.  A highly cross-linked polymeric binder for high-performance silicon negative electrodes in lithium ion batteries. , 2012, Angewandte Chemie.

[32]  Jaephil Cho,et al.  Chemical-assisted thermal disproportionation of porous silicon monoxide into silicon-based multicomponent systems. , 2012, Angewandte Chemie.

[33]  Jian Yu Huang,et al.  Size-dependent fracture of silicon nanoparticles during lithiation. , 2011, ACS nano.

[34]  G. Yushin,et al.  A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries , 2011, Science.

[35]  Igor Luzinov,et al.  Toward efficient binders for Li-ion battery Si-based anodes: polyacrylic acid. , 2010, ACS applied materials & interfaces.

[36]  G. Yushin,et al.  High-performance lithium-ion anodes using a hierarchical bottom-up approach. , 2010, Nature materials.

[37]  Chunsheng Wang,et al.  A polymer scaffold binder structure for high capacity silicon anode of lithium-ion battery. , 2010, Chemical communications.

[38]  Martin Winter,et al.  Silicon/Graphite Composite Electrodes for High-Capacity Anodes: Influence of Binder Chemistry on Cycling Stability , 2008 .

[39]  Candace K. Chan,et al.  High-performance lithium battery anodes using silicon nanowires. , 2008, Nature nanotechnology.

[40]  M. Miyachi,et al.  Electrochemical Properties and Chemical Structures of Metal-Doped SiO Anodes for Li-Ion Rechargeable Batteries , 2007 .