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High performance Li-, Na-, and K-ion storage in electrically conducting coordination polymers
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-08-08 , DOI: 10.1039/d2ee00566b
Jiande Wang 1 , Xiaolong Guo 1 , Petru Apostol 1 , Xuelian Liu 1 , Koen Robeyns 1 , Loïk Gence 2 , Cristian Morari 3 , Jean-François Gohy 1 , Alexandru Vlad 1
Affiliation  

Coordination polymers (CPs) made of redox-active organic moieties and metal ions emerge as an important class of electroactive materials for battery applications. However, the design and synthesis of high voltage alkali-cation reservoir anionic CPs remains challenging, hindering their practical applications. Herein, we report a family of electrically conducting alkali-cation reservoir CPs with the general formula of A2-TM-PTtSA (wherein A = Li+, Na+, or K+; TM = Fe2+, Co2+, or Mn2+; and PTtSA = benzene-1,2,4,5-tetra-methylsulfonamide). The incorporation of transition metal centers not only enables intrinsic high electrical conductivity, but also shows an impressive redox potential increase of as high as 1 V as compared to A4-PTtSA analogues, resulting in a class of organometallic cathode materials with a high average redox potential of 2.95–3.25 V for Li-, Na- and K-ion batteries. A detailed structure – composition – physicochemical properties – performance correlation study is provided relying on experimental and computational analysis. The best performing candidate shows excellent rate capability (86% of the nominal capacity retained at 10C rate), remarkable cycling stability (96.5% after 1000 cycles), outstanding tolerance to low carbon content (5 wt%), high mass loading (50 mg cm−2), and extreme utilisation conditions of low earth orbit space environment tests. The significance of the disclosed alkali-ion reservoir cathodes is further emphasized by utilizing conventional Li-host graphite anode for full cell assembly, attaining a record voltage of 3 V in an organic cathode Li-ion proof-of-concept cell.

中文翻译:

导电配位聚合物中的高性能锂、钠和钾离子存储

由氧化还原活性有机部分和金属离子制成的配位聚合物 (CP) 成为电池应用中一类重要的电活性材料。然而,高压碱阳离子储层阴离子CP的设计和合成仍然具有挑战性,阻碍了它们的实际应用。在此,我们报告了一系列具有通式 A 2 -TM-PTtSA(其中 A = Li +、Na +或 K +;TM = Fe 2+、Co 2+或锰2+; 和 PTtSA = 苯-1,2,4,5-四甲基磺酰胺)。过渡金属中心的加入不仅能够实现固有的高电导率,而且与 A 4 -PTtSA 类似物相比,还显示出高达 1 V 的令人印象深刻的氧化还原电位增加,从而产生了一类具有高平均氧化还原的有机金属正极材料锂离子、钠离子和钾离子电池的电位为 2.95–3.25 V。依靠实验和计算分析,提供了详细的结构-成分-物理化学性质-性能相关性研究。表现最佳的候选材料表现出优异的倍率性能(在 10C 倍率下保持 86% 的标称容量)、出色的循环稳定性(1000 次循环后为 96.5%)、出色的低碳含量耐受性(5 wt%)、高质量负载(50 mg厘米−2 ),以及低地球轨道空间环境试验的极端利用条件。通过使用常规的锂主体石墨阳极进行全电池组装,进一步强调了所公开的碱离子储层阴极的重要性,在有机阴极锂离子概念验证电池中获得了创纪录的 3 V 电压。
更新日期:2022-08-08
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