The safe and reliable operation of high-voltage lithium metal batteries (LMBs) at elevated temperatures is currently hindered by the lack of electrolyte designs that exhibit a high thermal safety and oxidation resistance. Here, an in situ gelation strategy, combining a thermally stable sulfone-based electrolyte with N,N-dimethylacrylamide monomer, is proposed to fabricate a wide-temperature gel electrolyte that is thermally stable up to 235 °C and maintains high-voltage stability above 4.3 V at 90 °C. An oxidation-resistant and thermally stable gel protective layer enables the conformal coating of LiNi_0.6Co_0.2Mn_0.2O₂ particles in the cathode, effectively preventing electrolyte decomposition during high-voltage operation at elevated temperatures. As a result, the Li/LiNi_0.6Co_0.2Mn_0.2O₂ batteries with the resulting in situ gel electrolyte demonstrate exceptional cycle life and safety at 90 °C, even under abusive conditions. This study paves a new pathway to the development of high-energy LMBs operating under extremely high-temperature conditions.

中文翻译：

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酰胺调制的凝胶电解质使富镍阴极在 90 °C 时具有增强的相间稳定性

目前，由于缺乏具有高热安全性和抗氧化性的电解质设计，高压锂金属电池（LMB）在高温下安全可靠的运行受到阻碍。在这里，提出了一种原位凝胶策略，将热稳定的砜基电解质与N , N-二甲基丙烯酰胺单体相结合，以制造宽温凝胶电解质，该电解质在高达 235 °C 的温度下保持热稳定，并保持高于 235 °C 的高电压稳定性。 90°C 时为 4.3V。抗氧化且热稳定的凝胶保护层能够在正极中保形涂覆LiNi _0.6 Co _0.2 Mn _0.2 O ₂颗粒，有效防止高温高压运行期间电解液分解。因此，采用所得原位凝胶电解质的Li/LiNi _0.6 Co _0.2 Mn _0.2 O ₂电池即使在滥用条件下，也能在90 °C 下表现出出色的循环寿命和安全性。这项研究为开发在极高温条件下运行的高能LMB开辟了一条新途径。