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A PF6−-Permselective Polymer Electrolyte with Anion Solvation Regulation Enabling Long-Cycle Dual-Ion Battery
Advanced Materials ( IF 27.4 ) Pub Date : 2021-12-24 , DOI: 10.1002/adma.202108665 Hongzhu Jiang 1, 2 , Xiaoqi Han 3 , Xiaofan Du 1 , Zheng Chen 1 , Chenglong Lu 1 , Xintong Li 1 , Huanrui Zhang 1 , Jingwen Zhao 1 , Pengxian Han 1 , Guanglei Cui 1, 4
Advanced Materials ( IF 27.4 ) Pub Date : 2021-12-24 , DOI: 10.1002/adma.202108665 Hongzhu Jiang 1, 2 , Xiaoqi Han 3 , Xiaofan Du 1 , Zheng Chen 1 , Chenglong Lu 1 , Xintong Li 1 , Huanrui Zhang 1 , Jingwen Zhao 1 , Pengxian Han 1 , Guanglei Cui 1, 4
Affiliation
Graphitic carbon that allows reversible anion (de)intercalation is a promising cathode material for cost-efficient and high-voltage dual-ion batteries (DIBs). However, one notorious but overlooked issue is the incomplete interfacial anion desolvation, which not only reduces the oxidative stability of electrolytes, but also results in solvent co-intercalation into graphite layers. Here, an “anion-permselective” polymer electrolyte with abundant cationic quaternary ammonium motif is developed to weaken the PF6−–solvent interaction and thus facilitates PF6− desolvation. This strategy significantly inhibits solvent co-intercalation as well as enhances the oxidation resistance of electrolyte, ensuring the structural integrity of graphite. As a result, the as-assembled graphite||Li cell achieves a superior cyclability with an average Coulombic efficiency of 99.0% (vs 95.7% for baseline electrolyte) and 87.1% capacity retention after 2000 cycles even at a high cutoff potential of 5.4 V versus Li+/Li. Besides, this polymer also forms a robust cathode electrolyte interface, working together to enable a long-life DIB. This strategy of tuning anion coordination environment provides a promising solution to regulate solvent co-intercalation chemistry for DIBs.
中文翻译:
一种具有阴离子溶剂化调节的 PF6−- 选择性渗透聚合物电解质,可实现长循环双离子电池
允许可逆阴离子(脱)嵌入的石墨碳是一种很有前途的阴极材料,可用于具有成本效益的高压双离子电池(DIB)。然而,一个臭名昭著但被忽视的问题是不完全的界面阴离子去溶剂化,这不仅降低了电解质的氧化稳定性,而且导致溶剂共嵌入石墨层。在这里,开发了一种具有丰富阳离子季铵基序的“阴离子选择性渗透”聚合物电解质,以削弱 PF 6 -溶剂相互作用,从而促进 PF 6 -去溶剂化。该策略显着抑制了溶剂共嵌入,并增强了电解质的抗氧化性,确保了石墨的结构完整性。因此,组装后的石墨||Li 电池具有出色的循环性能,平均库仑效率为 99.0%(基线电解质为 95.7%),即使在 5.4 V 的高截止电位下,2000 次循环后容量保持率也为 87.1%相对于 Li + /Li。此外,这种聚合物还形成了坚固的阴极电解质界面,共同作用以实现长寿命的 DIB。这种调节阴离子配位环境的策略为调节 DIB 的溶剂共插层化学提供了一种有前景的解决方案。
更新日期:2021-12-24
中文翻译:
一种具有阴离子溶剂化调节的 PF6−- 选择性渗透聚合物电解质,可实现长循环双离子电池
允许可逆阴离子(脱)嵌入的石墨碳是一种很有前途的阴极材料,可用于具有成本效益的高压双离子电池(DIB)。然而,一个臭名昭著但被忽视的问题是不完全的界面阴离子去溶剂化,这不仅降低了电解质的氧化稳定性,而且导致溶剂共嵌入石墨层。在这里,开发了一种具有丰富阳离子季铵基序的“阴离子选择性渗透”聚合物电解质,以削弱 PF 6 -溶剂相互作用,从而促进 PF 6 -去溶剂化。该策略显着抑制了溶剂共嵌入,并增强了电解质的抗氧化性,确保了石墨的结构完整性。因此,组装后的石墨||Li 电池具有出色的循环性能,平均库仑效率为 99.0%(基线电解质为 95.7%),即使在 5.4 V 的高截止电位下,2000 次循环后容量保持率也为 87.1%相对于 Li + /Li。此外,这种聚合物还形成了坚固的阴极电解质界面,共同作用以实现长寿命的 DIB。这种调节阴离子配位环境的策略为调节 DIB 的溶剂共插层化学提供了一种有前景的解决方案。