Electrolyte design is critical for enabling next-generation batteries with higher energy densities. Hydrofluoroether (HFE) solvents have drawn a lot of attention as the electrolytes based on HFEs showed great promise to deliver highly desired properties, including high oxidative stability, ionic conductivity, as well as enhanced lithium metal compatibility. However, the structure-dynamics-properties relationships and design principles for high-performance HFE solvents are still poorly understood. Herein, we proposed four novel asymmetric HFE designs by systematically varying polyether and fluorocarbon structural building blocks. By leveraging molecular dynamics (MD) modeling to analyze the solvation structures and predict the properties of the corresponding 1 M lithium bis(fluorosulfonyl)imide (LiTFSI) solutions, we downselected the most promising candidate based on high conductivity, solvation species distribution, and oxidative stability for extensive electrochemical characterizations. The formulated electrolyte demonstrated properties consistent with the predictions from the simulations and showed muchimproved capacity retention as well as Coulombic efficiency compared to the baseline electrolytes when cycled in lithium metal cells. This work exemplifies the construction of candidate electrolytes from building block functional moieties to engineer fundamental solvation structures for desired electrolyte properties and guide the discovery and rational design of new solvent materials.

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Challenge of developing new formulations of water-in-salt electrolytes are addressed via mixed cation strategy: cheaper (by at least an order of magnitude) and more soluble salts featuring alkali cations beyond lithium, such as potassium, are used to create the water-in-salt condition.

Human skin has different types of tactile receptors that can distinguish various mechanical stimuli from temperature. We present a deformable artificial multimodal ionic receptor that can differentiate thermal and mechanical information without signal interference. Two variables are derived from the analysis of the ion relaxation dynamics: the charge relaxation time as a strain-insensitive intrinsic variable to measure absolute temperature and the normalized capacitance as a temperature-insensitive extrinsic variable to measure strain. The artificial receptor with a simple electrode-electrolyte-electrode structure simultaneously detects temperature and strain by measuring the variables at only two measurement frequencies. The human skin–like multimodal receptor array, called multimodal ion-electronic skin (IEM-skin), provides real-time force directions and strain profiles in various tactile motions (shear, pinch, spread, torsion, and so on).

The emergence of wearable electronics puts batteries closer to the human skin, exacerbating the need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy to overcome the canonical tradeoff between mechanical robustness and ionic conductivity in polymer electrolytes. The supramolecular lithium ion conductor utilizes orthogonally functional H-bonding domains and ion-conducting domains to create a polymer electrolyte with unprecedented toughness (29.3 MJ m−3) and high ionic conductivity (1.2 × 10−4 S cm−1 at 25 °C). Implementation of the supramolecular ion conductor as a binder material allows for the creation of stretchable lithium-ion battery electrodes with strain capability of over 900% via a conventional slurry process. The supramolecular nature of these battery components enables intimate bonding at the electrode-electrolyte interface. Combination of these stretchable components leads to a stretchable battery with a capacity of 1.1 mAh cm−2 that functions even when stretched to 70% strain. The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications.

Solid polymer electrolytes (SPEs) promise to improve the safety and performance of lithium ion batteries (LIBs). However, the low ionic conductivity and transference number of conventional poly(ethylene oxide) (PEO) based SPEs preclude their widespread implementation.Herein, we introduce crosslinked poly(tetrahydrofuran) (xPTHF) as a promising polymer matrix for This article is protected by copyright. All rights reserved. 2"beyond PEO" SPEs. The crosslinking procedure creates thermally stable, mechanically robust membranes for use in LIBs. Molecular Dynamics and Density Functional Theory (DFT) simulations accompanied by 7 Li NMR measurements show that the lower spatial concentration of oxygen atoms in the xPTHF backbone leads to loosened O-Li + coordination. This weakened interaction enhances ion transport; xPTHF has a high lithium transference number of 0.53 and higher lithium conductivity than a xPEO SPE of the same length at room temperature. We demonstrate that organic additives further weaken the O-Li + interaction, enabling room temperature ionic conductivity of 1.2*10 -4 S cm -1 with 18 wt.% DMF in xPTHF. In a solid state LIB application, neat xPTHF SPEs cycle with near theoretical capacity for 100 cycles at 70 ºC, with rate capability up to 1C. The plasticized xPTHF SPEs operate at room temperature while maintaining respectable rate capability and capacity. The novel PTHF system demonstrated here represents an exciting platform for future studies involving SPEs.

Implementation of lithium (Li)-metal anodes requires developments to solve the heterogeneity and instability issues of naturally formed solid-electrolyte interphase (SEI). The artificial SEI, as an alternative, enables an ideal interface by regulating critical features such as fast ion transport, conformal protection, and parasitic reaction mitigation. Herein, for the first time, we integrate all of these desired properties into a single matrix, the dynamic single-ion-conductive network (DSN), as a multifunctional artificial SEI. The DSN incorporates the tetrahedral Al(OR) 4 À (R = soft fluorinated linker) centers as both dynamic bonding motifs and counter anions, endowing it with flowability and Li + single-ion conductivity. Simultaneously, the fluorinated linkers provide chain mobility and electrolyte-blocking capability. A solution-processed DSN coating was found to simultaneously hinder electrolyte penetration, mitigate side reactions between Li and electrolyte, maintain low interfacial impedance, and allow homogenous Li deposition. With this coating, long cycle life and high Coulombic efficiency are achieved for Li-metal battery in a commercial carbonate electrolyte.

Deformable energy storage devices are needed to power the next generation of wearable electronics. This review highlights the most recent advances in stretchable energy storage devices with a focus on batteries and supercapacitors.