In electrochemical devices, such as batteries, traditional electric double layer (EDL) theory holds that cations in the cathode/electrolyte interface will be repelled during charging, leaving a large amount of free solvents. This promotes the continuous anodic decomposition of the electrolyte, leading to a limited operation voltage and cycle life of the devices. In this work, we design a new EDL structure with adaptive and passivating properties. It is enabled by adding functional anionic additives in the electrolyte, which can selectively bind with cations and free solvents, forming unique cation-rich and branch-chain like supramolecular polymer structures with high electrochemical stability in the EDL inner layer. Due to this design, the anodic decomposition of ether-based electrolytes is significantly suppressed in the high voltage cathodes and the battery shows outstanding performances such as super-fast charging/discharging and ultra-low temperature applications, which is extremely hard in conventional electrolyte design principle. This unconventional EDL structure breaks the inherent perception of the classical EDL rearrangement mechanism and greatly improve electrochemical performances of the device.

Despite the fact that lithium–sulfur batteries are regarded as promising next-generation rechargeable battery systems owning to high theoretical specific capacity (1675 mA h g–1) and energy density (2600 W h kg–1), several issues such as poor electrical conductivity, sluggish redox kinetics, and severe “shuttle effect” in electrodes still hinder their practical application. MXenes, novel two-dimensional materials with high conductivity, regulable interlayer spacing, and abundant functional groups, are widely applied in energy storage and conversion fields. In this work, a Ti3C2/carbon hybrid with expanded interlayer spacing is synthesized by one-step heat treatment in molten potassium hydroxide. The subsequent experiments indicate that the as-prepared Ti3C2/carbon hybrid can effectively regulate polysulfide redox conversion and has strong chemisorption interaction to polysulfides. Consequently, the Ti3C2/carbon-based sulfur cathode boosts the performance in working lithium–sulfur batteries, in terms of an ultrahigh initial discharge capacity (1668 mA h g–1 at 0.1 C), an excellent rate performance (520 mA h g–1 at 5 C), and an outstanding capacity retention of 530 mA h g–1 after 500 cycles at 1 C with a low capacity fade rate of 0.05% per cycle and stable Coulombic efficiency (nearly 99%). The above results indicate that this composite with high catalytic activity is a potential host material for further high-performance lithium–sulfur batteries.

No abstract

A fluorinated amide molecule with two functional segments, namely, an amide group with a high donor number to bind lithium ions and a fluorine chain to expel carbonate solvents and mediate the formation of LiF, was designed to regulate the interfacial chemistry. As expected, the additive preferably appears in the first solvation sheath of lithium ions and is electrochemically reduced on the anode, and thus an inorganic-rich solid electrolyte interphase is generated. The morphology of deposited lithium metal evolves from brittle dendrites into a granular shape. Consequently, the Li||LiFePO 4 cell shows an excellent capacity retention of 92.7% at a high rate of 5 C after 800 cycles. Besides, the Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 cell succeeds to maintain 98.1% of the initial capacity after 100 cycles at 1 C. Our designing of N,Ndiethyl-2,3,3,3-tetrafluoropropionamide (denoted as DETFP) highlights the importance of a "high donor number" and may shed light on the design principles of electrolytes for high performance batteries.