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Activating Interfacial Ion Exchange in Composite Electrolytes to Realize High‐Rate and Long‐Cycling Solid‐State Lithium Batteries
AbstractComposite solid electrolytes (CSEs) are promising candidates for solid‐state lithium metal batteries. However, the poor cross‐phase Li+ transport restricts the rate performance and cycle life of the batteries. Herein, we revealed the Li+ percolation behavior in poly(vinylidene fluoride) (PVDF)‐based CSEs with Li6.4La3Zr1.4Ta0.6O12 filler. The de‐coordination barrier from Li+ clusters determines interfacial Li+ transport capability. We then employed a designed N‐methyl‐2,2,2‐trifluoroacetamide (NMTFA) ligand to lower the de‐coordination energy and activate interfacial Li+ exchange. The ionic conductivity is therefore increased from 3.32 × 10−4 to 7.30 × 10−4 S cm−1. By tracking the 6Li and 7Li substitution process, it was identified that the proportion of interfacial Li+ transport increases from 11% to 26%. The NMTFA also contributes to the formation of inorganic‐rich interphases with electrodes. As a result, the Li||LiNi0.8Co0.1Mn0.1O2 solid‐state batteries exhibit ultra‐long lifespans of 2400, 3000, and 10 000 times at 2, 5, and 10C, respectively, as well as achieve 1000 cycles at 50 °C and 300 cycles at −30 °C. This work highlights the critical role of interfacial Li+ transport for the CSEs with “polymer‐Li+ clusters‐filler” configuration to realize high‐rate and long‐cycling solid‐state lithium batteries.
Bio‐Inspired Self‐Activating Polydimethylsiloxane‐Modified CrO<sub><i>x</i></sub>/Al<sub>2</sub>O<sub>3</sub> Catalyst for Acetylene Semihydrogenation
AbstractBiomimetic approach is a nature‐driven strategy for designing functional materials to meet the industrial challenges. Here we demonstrate the bio‐inspired discovery of a self‐activating catalyst, with polydimethylsiloxane anchored over the surface of CrOx/Al2O3, exhibiting comparable performance with noble metallic catalysts for acetylene semihydrogenation. In addition, the dynamic movement of polymer chains with high flexibility renders the catalyst to impose proactive perturbation to the undesired coke precursors generated in reaction, analogous to the function of hair‐like cilia on the surface of respiratory epithelial cells, thus avoiding the site‐blocking induced by carbonaceous deposits and sustaining the catalyst stable for 1000 h without any deactivation. This study paves the way to develop other heterogeneous catalysts with high efficiency and durability via mimicking the innate defense mechanism of natural organisms.