The normal operation of lithium‐ion batteries (LIBs) at ultralow temperature (<−40 °C) is significant for cold‐climate applications; however, their operation is plagued by the low capacity of the conventional intercalation cathodes due to their sluggish kinetics and the slow solid diffusion of Li+ in their frameworks. Here, it is demonstrated that amorphization is an effective strategy to promote the low‐temperature dynamics of cathodes by relieving the blocking effect of a dense lattice structure on ion transport under cryogenic conditions. As a result, due to the decreased charge transport impedance and enhanced Li+ diffusion rate, the obtained covalent amorphous polymer (CAP) with an abundance of pyrazine and carbonyl active sites displays a remarkably outstanding specific capacity of 141 mAh g−1 at −80 °C, which is superior to its structural analog, a covalent crystalline polymer (43.8 mAh g−1). Furthermore, 84.7% of the initial capacity of the CAP can be retained after 500 cycles of charge and discharge at −60 °C. Molecular dynamic simulations show that the channel‐rich amorphous structure is highly conducive for lithium ions to diffuse quickly in the interstitial space of organic solids. This work provides an effective strategy regarding the amorphization of crystalline cathodes to develop low‐temperature (Low‐T) batteries.

The extremely low nitrogen (N 2 ) solubility in aqueous solution greatly limits the gas reactant supply to catalysts resulting in a bottleneck in establishing efficient electrocatalytic N 2 reduction reaction (NRR). Here, aiming at fairly few N 2 dissolving in aqueous electrolyte, an N 2 -microextractor (NME) that can extract the N 2 from water, then feed it to catalysts on electrodes, is reported. The NME consists of polymer framework and extractant that possess high solubility for N 2 , which serves as an ultra-thin interfacial system wrapping around electrodes. As expected, the enhancement of N 2 supply in NRR leads to a record-high Faradaic efficiency (80.1%) with an ammonia yield rate of 58.3 µg h −1 mg −1 under ambient conditions. This is of great significance to a sustainable "Ammonia Economy.

The practical application of aqueous high-rate Zn metal battery (ZMB) is limited due to accelerated dendrite formation at high current densities. It is urgent to find an electrolyte, which could not only be mechanically stiff to clamp down dendrites but also not sacrifice ionic conductivity and interfacial compatibility. Herein, a new type of dynamically “solid–liquid” interconvertible electrolyte based on non-Newtonian fluid (NNFE) is proposed. Liquidity characteristic of NNFE is favorable for electrochemical kinetics and interfacial compatibility. Furthermore, in an area with high current rate NNFE would respond and mechanically stiffen to dissuade localized increase in Zn dendrite growth. Even at a current density of 50 mA cm–2, NNFE enables reversible and stable operation of a Zn symmetrical cell over 20 000 cycles. For Zn//Na5V12O32 (NVO) full cell, the NNFE also realizes lengthy cycling for 5000 periods at 5 A g–1. This research opens up new inspirations to high-rate Zn metal even other metal batteries.

No abstract

The humidity-sensitive electrolytes necessitate the stringent conditions of lithium battery manufacturing and, thus, increase the fabrication complexity and cost. We herein report a water-tolerant solid polymer electrolyte (WT-SPE) with high Li+ conductivity (2.08 × 10−4 S cm−1 at room temperature) and electrochemically stable window (up to 4.7 V vs Li/Li+), which utilizes moisture to initiate rapid polymerization and form dense structures to achieve a facile battery manufacturing in humid air without the need of a glovebox. Molecular dynamics simulations attribute this hydrophobic behavior to the hindered transfer of a water molecule in dense WT-SPE. A stable SEI layer composed of a polymeric framework and other organic/inorganic small molecular compounds contributes to the sustainable operation of batteries. As a result, the Li|WT-SPE|LiCoO2 cells manufactured in the air exhibit a high initial capacity of 192 mA h g−1 at 0.1C and an excellent capacity retention for 300 cycles at 1C. The great advantage significantly simplifies the battery assembly process in air environment and can also maintain good interfacial contact between an electrolyte and electrodes thanks to in situ initiated polymerization, which shows great superiority and promise in the alternatives of traditional liquid and polymer electrolytes for low-cost and facile fabrication of batteries in ambient atmosphere.