Fangfang Chen, Xiaoen Wang, Michel Armand, Maria Forsyth
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引用次数: 41
Abstract
Polymer electrolytes provide a safe solution for future solid-state high-energy-density batteries. Materials that meet the simultaneous requirement of high ionic conductivity and high transference number remain a challenge, in particular for new battery chemistries beyond lithium such as Na, K and Mg. Herein, we demonstrate the versatility of a polymeric ionic liquid (PolyIL) as a polymer solvent to achieve this goal for both Na and K. Using molecular simulations, we predict and elucidate fast alkali metal ion transport in PolyILs through a structural diffusion mechanism in a polymer-in-salt environment, facilitating a high metal ion transference number simultaneously. Experimental validation of these computationally designed Na and K polymer electrolytes shows good ionic conductivities up to 1.0 × 10−3 S cm−1 at 80 °C and a Na+ transference number of ~0.57. An electrochemical cycling test on a Na∣2:1 NaFSI/PolyIL∣Na symmetric cell also demonstrates an overpotential of 100 mV at a current density of 0.5 mA cm−2 and stable long-term Na plating/stripping performance of more than 100 hours. PolyIL-based polymer-in-salt strategies for new solid-state electrolytes thus offer an alternative route to design high-performance next-generation sustainable battery chemistries. Polymer electrolytes provide a safe solution for future solid-state high-energy-density batteries, but combining high ionic conductivity and a high transference number is a challenge. A polymeric ionic liquid used as a polymer solvent is now shown to be promising for both sodium and potassium batteries.
聚合物电解质为未来的固态高能量密度电池提供了一种安全的解决方案。同时满足高离子电导率和高转移数量要求的材料仍然是一项挑战,尤其是对于锂以外的新型电池化学物质,如 Na、K 和 Mg。在此,我们展示了聚合物离子液体(PolyIL)作为聚合物溶剂的多功能性,以实现对 Na 和 K 的这一目标。通过分子模拟,我们预测并阐明了聚合物离子液体通过聚合物盐环境中的结构扩散机制实现碱金属离子的快速传输,从而同时促进高金属离子转移数量。对这些通过计算设计的 Na 和 K 聚合物电解质进行的实验验证表明,在 80 °C 时,其离子电导率高达 1.0 × 10-3 S cm-1,Na+离子转移数约为 0.57。在 Na∣2:1 NaFSI/PolyIL∣Na 对称电池上进行的电化学循环测试也表明,在 0.5 mA cm-2 的电流密度下,过电位为 100 mV,Na 的长期稳定电镀/剥离性能超过 100 小时。因此,基于 PolyIL 的盐中聚合物新固态电解质策略为设计高性能的下一代可持续电池化学材料提供了另一条途径。聚合物电解质为未来的固态高能量密度电池提供了一种安全的解决方案,但如何将高离子电导率和高转移数结合起来是一项挑战。目前,一种用作聚合物溶剂的聚合物离子液体已被证明有望用于钠电池和钾电池。
期刊介绍:
Nature Materials is a monthly multi-disciplinary journal aimed at bringing together cutting-edge research across the entire spectrum of materials science and engineering. It covers all applied and fundamental aspects of the synthesis/processing, structure/composition, properties, and performance of materials. The journal recognizes that materials research has an increasing impact on classical disciplines such as physics, chemistry, and biology.
Additionally, Nature Materials provides a forum for the development of a common identity among materials scientists and encourages interdisciplinary collaboration. It takes an integrated and balanced approach to all areas of materials research, fostering the exchange of ideas between scientists involved in different disciplines.
Nature Materials is an invaluable resource for scientists in academia and industry who are active in discovering and developing materials and materials-related concepts. It offers engaging and informative papers of exceptional significance and quality, with the aim of influencing the development of society in the future.