All solid‐state batteries holds great promise for superiorly safe and high energy electrochemical energy storage. The ionic conductivity of electrolytes and its interfacial compatibility with the electrode are two critical factors in determining the electrochemical performance of all solid‐state batteries. It is a great challenge to simultaneously demonstrate fantastic ionic conductivity and compatible electrolyte/electrode interface to acquire a well‐performed all solid‐state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within a self‐supported 3D porous Li‐argyrodite (Li6PS5Cl) skeleton, the two bottlenecks are tackled successfully at once. As a result, all solid‐state lithium metal batteries with a 4.5 V LiNi0.8Mn0.1Co0.1O2 cathode designed by this integrated strategy demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid‐state nuclear magnetic resonance data suggest that Li+ mainly migrates along the continuous Li6PS5Cl phase to result in a room temperature conductivity of 4.6 × 10−4 S cm−1, which is 128 times higher than that of the corresponding polymer. Meanwhile, the inferior solid–solid electrolyte/electrode interface is integrated via in situ polymerization to lessen the interfacial resistance significantly. This study thereby provides a very promising strategy of solid electrolyte design to simultaneously meet both high ionic conductivity and good interfacial compatibility towards practical high‐energy‐density all solid‐state lithium batteries.
Solid‐state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid‐state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self‐supported three‐dimensional porous Li1.3Al0.3Ti1.7(PO4)3 framework, the as‐assembled solid‐state battery employing 4.5 V LiNi0.8Mn0.1Co0.1O2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid‐state nuclear magnetic resonance results reveal that Li+ migrates fast along the continuous Li1.3Al0.3Ti1.7(PO4)3 phase and Li1.3Al0.3Ti1.7(PO4)3/polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10−4 S cm−1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li1.3Al0.3Ti1.7(PO4)3 from being reduced by lithium metal. As a consequence of the compatible solid‐solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid‐state lithium metal battery.
Solid-state lithium batteries have drawn wide attention to address the safety issues of power batteries. However, the development of solid-state lithium batteries is substantially limited by the poor electrochemical performances originating from the rigid interface between solid electrodes and solid-state electrolytes. In this work, a composite of poly(vinyl carbonate) and LiSnPS solid-state electrolyte is fabricated successfully via in situ polymerization to improve the rigid interface issues. The composite electrolyte presents a considerable room temperature conductivity of 0.2 mS cm, an electrochemical window exceeding 4.5 V, and a Li transport number of 0.6. It is demonstrated that solid-state lithium metal battery of LiFeMnPO (LFMP)/composite electrolyte/Li can deliver a high capacity of 130 mA h g with considerable capacity retention of 88% and Coulombic efficiency of exceeding 99% after 140 cycles at the rate of 0.5 C at room temperature. The superior electrochemical performance can be ascribed to the good compatibility of the composite electrolyte with Li metal and the integrated compatible interface between solid electrodes and the composite electrolyte engineered by in situ polymerization, which leads to a significant interfacial impedance decrease from 1292 to 213 Ω cm in solid-state Li-Li symmetrical cells. This work provides vital reference for improving the interface compatibility for room temperature solid-state lithium batteries.
A highly selective ligand exchange reaction is realized in the self-assembled monolayer (SAM) of a triruthenium cluster on a gold electrode surface under precise electrochemical potential control. CO as well as NO molecules, which are known to play key roles in many chemical, biological, and environmental systems, can be efficiently introduced into the SAM by electrochemically tuning the electronic state of the Ru site. These unique surface reactions are more convenient and efficient than conventional ligand exchange reactions in solution and could be used for the elucidation of the electron-transfer mechanism in a biological system as well as in the development of molecular sensors and devices.
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