Copolymer Solid-State Electrolytes for 3D Microbatteries via Initiated Chemical Vapor Deposition.

Reliable integration of thin film solid-state polymer electrolytes (SPEs) with 3D electrodes is one major challenge in microbattery fabrication. We used initiated chemical vapor deposition (iCVD) to produce a series of nanoscale copolymer films comprising hydroxyethyl methacrylate and ethylene glycol diacrylate. Conformal copolymer coatings were applied to a variety of patterned 3D electrodes and subsequently converted into ionic conductors by lithium salt doping. Broad tunability in ionic conductivity was achieved by optimizing the copolymer cross-linking density and matrix polarity, resulting in a room-temperature conductivity of (6.1 ± 2.7) × 10-6 S cm-1, the highest value reported for conformal, nanoscale SPEs.

[1]  T. Christiansen,et al.  High-power lithium-ion microbatteries from imprinted 3D electrodes of sub-10 nm LiMn2O4/Li4Ti5O12 nanocrystals and a copolymer gel electrolyte , 2018, Nano Energy.

[2]  T. Gustafsson,et al.  Self-supported three-dimensional nanoelectrodes for microbattery applications. , 2009, Nano letters.

[3]  V. Ganesan,et al.  Effect of Polymer Polarity on Ion Transport: A Competition between Ion Aggregation and Polymer Segmental Dynamics. , 2018, ACS macro letters.

[4]  Bing Sun,et al.  Toward Solid-State 3D-Microbatteries Using Functionalized Polycarbonate-Based Polymer Electrolytes. , 2018, ACS applied materials & interfaces.

[5]  Ya‐Xia Yin,et al.  In-situ plasticized polymer electrolyte with double-network for flexible solid-state lithium-metal batteries , 2018 .

[6]  K. Gleason,et al.  Initiated Chemical Vapor Deposition (iCVD) of Poly(alkyl acrylates): An Experimental Study , 2006 .

[7]  B. Dunn,et al.  Synthesis and Properties of a Photopatternable Lithium‐Ion Conducting Solid Electrolyte , 2018, Advanced materials.

[8]  P. Ajayan,et al.  Conformal coating of thin polymer electrolyte layer on nanostructured electrode materials for three-dimensional battery applications. , 2011, Nano letters.

[9]  Christopher P. Rhodes,et al.  Nanoscale Polymer Electrolytes: Ultrathin Electrodeposited Poly(Phenylene Oxide) with Solid-State Ionic Conductivity , 2004 .

[10]  Yi-Ming Sun,et al.  Sorption/desorption properties of water vapour in poly(2-hydroxyethyl methacrylate): 1. Experimental and preliminary analysis , 1996 .

[11]  Yang Liu,et al.  Electrolyte stability determines scaling limits for solid-state 3D Li ion batteries. , 2011, Nano letters.

[12]  S. Seki,et al.  Distinct difference in ionic transport behavior in polymer electrolytes depending on the matrix polymers and incorporated salts. , 2005, The journal of physical chemistry. B.

[13]  Hyo-Jeong Ha,et al.  A facile approach to fabricate self-standing gel-polymer electrolytes for flexible lithium-ion batteries by exploitation of UV-cured trivalent/monovalent acrylate polymer matrices , 2011 .

[14]  R. J. Sengwa,et al.  Role of preparation methods on the structural and dielectric properties of plasticized polymer blend electrolytes: Correlation between ionic conductivity and dielectric parameters , 2014 .

[15]  B. Reeja‐Jayan,et al.  A Group of Cyclic Siloxane and Silazane Polymer Films as Nanoscale Electrolytes for Microbattery Architectures , 2015 .

[16]  Bruno Scrosati,et al.  Polymer electrolytes: Present, past and future , 2011 .

[17]  Bruce Dunn,et al.  Three-dimensional battery architectures. , 2004, Chemical reviews.

[18]  R. J. Sengwa,et al.  Effects of plasticizer and nanofiller on the dielectric dispersion and relaxation behaviour of polymer blend based solid polymer electrolytes , 2015 .

[19]  K. Gleason,et al.  Initiated chemical vapor deposition of linear and cross-linked poly(2-hydroxyethyl methacrylate) for use as thin-film hydrogels. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[20]  Justin C. Lytle,et al.  Photonic Crystal Structures as a Basis for a Three‐Dimensionally Interpenetrating Electrochemical‐Cell System , 2006 .

[21]  K. Carter,et al.  Direct Imprinting of Scalable, High-Performance Woodpile Electrodes for Three-Dimensional Lithium-Ion Nanobatteries. , 2018, ACS applied materials & interfaces.

[22]  J. Yagüe,et al.  25th Anniversary Article: CVD Polymers: A New Paradigm for Surface Modifi cation and Device Fabrication , 2013, Advanced materials.

[23]  R. Faccio,et al.  Experimental and Theoretical Study of Ionic Pair Dissociation in a Lithium Ion-Linear Polyethylenimine-Polyacrylonitrile Blend for Solid Polymer Electrolytes. , 2017, The journal of physical chemistry. B.

[24]  Bruce Dunn,et al.  High Areal Energy Density 3D Lithium-Ion Microbatteries , 2018 .

[25]  C. Angell Mobile Ions in Amorphous Solids , 1992 .

[26]  A. Pearse,et al.  Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte , 2017, 1702.04009.

[27]  Laura C. Bradley,et al.  Microstructured Films Formed on Liquid Substrates via Initiated Chemical Vapor Deposition of Cross-Linked Polymers. , 2015, Langmuir : the ACS journal of surfaces and colloids.

[28]  N. Hendricks,et al.  Direct Patterning of Robust One-Dimensional, Two-Dimensional, and Three-Dimensional Crystalline Metal Oxide Nanostructures Using Imprint Lithography and Nanoparticle Dispersion Inks , 2017 .