ABSTRACT
Despite the enormous interest in inorganic/polymer composite solid-state electrolytes (CSEs) for solid-state batteries (SSBs), the underlying ion transport phenomena in CSEs have not yet been elucidated. Here, we address this issue by formulating a mechanistic understanding of bi-percolating ion channels formation and ion conduction across inorganic-polymer electrolyte interfaces in CSEs. A model CSE is composed of argyrodite-type Li6PS5Cl (LPSCl) and gel polymer electrolyte (GPE, including Li+-glyme complex as an ion-conducting medium). The percolation threshold of the LPSCl phase in the CSE strongly depends on the elasticity of the GPE phase. Additionally, manipulating the solvation/desolvation behavior of the Li+-glyme complex in the GPE facilitates ion conduction across the LPSCl-GPE interface. The resulting scalable CSE (area = 8 × 6 (cm × cm), thickness ~ 40 µm) can be assembled with a high-mass-loading LiNi0.7Co0.15Mn0.15O2 cathode (areal-mass-loading = 39 mg cm-2) and a graphite anode (negative (N)/positive (P) capacity ratio = 1.1) in order to fabricate an SSB full cell with bi-cell configuration. Under this constrained cell condition, the SSB full cell exhibits high volumetric energy density (480 Wh Lcell-1) and stable cyclability at 25 °C, far exceeding the values reported by previous CSE-based SSBs.
ABSTRACT
Despite the ever-increasing demand for transparent power sources in wireless optoelectronics, most of them have still relied on synthetic chemicals, thus limiting their versatile applications. Here, a class of transparent nanocellulose paper microsupercapacitors (TNP-MSCs) as a beyond-synthetic-material strategy is demonstrated. Onto semi-interpenetrating polymer network-structured, thiol-modified transparent nanocellulose paper, a thin layer of silver nanowire and a conducting polymer (chosen as a pseudocapacitive electrode material) are consecutively introduced through microscale-patterned masks (which are fabricated by electrohydrodynamic jet printing) to produce a transparent conductive electrode (TNP-TCE) with planar interdigitated structure. This TNP-TCE, in combination with solid-state gel electrolytes, enables on-demand (in-series/in-parallel) cell configurations in a single body of TNP-MSC. Driven by this structural uniqueness and scalable microfabrication, the TNP-MSC exhibits improvements in optical transparency (T = 85%), areal capacitance (0.24 mF cm-2 ), controllable voltage (7.2 V per cell), and mechanical flexibility (origami airplane), which exceed those of previously reported transparent MSCs based on synthetic chemicals.
Subject(s)
Nanowires , Silver , Electric Capacitance , Electric Conductivity , PolymersABSTRACT
Recent findings demonstrate that cellulose, a highly abundant, versatile, sustainable, and inexpensive material, can be used in the preparation of very stable and flexible electrochemical energy storage devices with high energy and power densities by using electrodes with high mass loadings, composed of conducting composites with high surface areas and thin layers of electroactive material, as well as cellulose-based current collectors and functional separators. Close attention should, however, be paid to the properties of the cellulose (e.g., porosity, pore distribution, pore-size distribution, and crystallinity). The manufacturing of cellulose-based electrodes and all-cellulose devices is also well-suited for large-scale production since it can be made using straightforward filtration-based techniques or paper-making approaches, as well as utilizing various printing techniques. Herein, the recent development and possibilities associated with the use of cellulose are discussed, regarding the manufacturing of electrochemical energy storage devices comprising electrodes with high energy and power densities and lightweight current collectors and functional separators.
ABSTRACT
Porous crystalline materials such as covalent organic frameworks and metal-organic frameworks have garnered considerable attention as promising ion conducting media. However, most of them additionally incorporate lithium salts and/or solvents inside the pores of frameworks, thus failing to realize solid-state single lithium-ion conduction behavior. Herein, we demonstrate a lithium sulfonated covalent organic framework (denoted as TpPa-SO3Li) as a new class of solvent-free, single lithium-ion conductors. Benefiting from well-designed directional ion channels, a high number density of lithium-ions, and covalently tethered anion groups, TpPa-SO3Li exhibits an ionic conductivity of 2.7 × 10-5 S cm-1 with a lithium-ion transference number of 0.9 at room temperature and an activation energy of 0.18 eV without additionally incorporating lithium salts and organic solvents. Such unusual ion transport phenomena of TpPa-SO3Li allow reversible and stable lithium plating/stripping on lithium metal electrodes, demonstrating its potential use for lithium metal electrodes.
ABSTRACT
The ongoing surge in demand for high-performance energy storage systems inspires the relentless pursuit of advanced materials and structures. Components of energy storage systems are generally based on inorganic/metal compounds, carbonaceous substances, and petroleum-derived hydrocarbon chemicals. These traditional materials, however, may have difficulties fulfilling the ever-increasing requirements of energy storage systems. Recently, nanocellulose has garnered considerable attention as an exceptional 1D element due to its natural abundance, environmental friendliness, recyclability, structural uniqueness, facile modification, and dimensional stability. Recent advances and future outlooks of nanocellulose as a green material for energy storage systems are described, with a focus on its application in supercapacitors, lithium-ion batteries (LIBs), and post-LIBs. Nanocellulose is typically classified as cellulose nanofibril (CNF), cellulose nanocrystal (CNC), and bacterial cellulose (BC). The unusual 1D structure and chemical functionalities of nanocellulose bring unprecedented benefits to the fabrication and performance of energy storage materials and systems, which lie far beyond those achievable with conventional synthetic materials. It is believed that this progress report can stimulate research interests in nanocellulose as a promising material, eventually widening material horizons for the development of next-generation energy storage systems, that will lead us closer to so-called Battery-of-Things (BoT) era.
ABSTRACT
Facile/sustainable utilization of sulfur active materials is an ultimate challenge in high-performance lithium-sulfur (Li-S) batteries. Here, as a membrane-driven approach to address this issue, we demonstrate a new class of polysulfide-breathing (capable of reversibly adsorbing and desorbing polysulfides)/dual (electron and ion) conductive, heterolayered battery separator membranes (denoted as "MEC-AA separators") based on 0D (nanoparticles)/1D (nanofibers) composite mats. The MEC-AA separator is fabricated through an in-series, concurrent electrospraying/electrospinning process. The top layer of the MEC-AA separator comprises close-packed mesoporous MCM-41 nanoparticles spatially besieged by multiwalled carbon nanotubes (MWNT) wrapped poly(ether imide) (PEI) nanofibers. The MCM-41 in the top layer shows reversible adsorption/desorption of polysulfides, and the MWNT-wrapped PEI nanofibers act as a dual-conductive upper current collector. Preferential deposition of the MWNTs along the PEI nanofibers and dispersion state of the separator components are elucidated theoretically using computational methods. The support layer, which consists of densely packed Al2O3 nanoparticles and polyacrylonitrile nanofibers, serves as a mechanically/thermally stable and polysulfide-capturing porous membrane. The unique structure and multifunctionality of the MEC-AA separator allow for substantial improvements in redox reaction kinetics and cycling performance of Li-S cells far beyond those achievable with conventional polyolefin separators. The heterolayered nanomat-based membrane strategy opens a new route toward electrochemically active/permselective advanced battery separators.
