吩嗪类衍生物用于快速充放电和长寿命的水系钾离子全电池负极

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中文摘要：有机电极材料因具有结构多样性和可持续性,在水系钾离子电池研究领域展示出广阔的前景,但它们大多数存在导电性差、易溶于电解液的问题,导致电极活性物质利用率低、循环稳定性差.本文通过含氮苯环的共轭延申、引入氰基活性中心,获得了3CN-HATN.与经典吩嗪负极相比,3CN-HATN的最低未占据分子轨道能级更低,更容易被还原,且其能带隙较窄,改善了导电性,其共轭结构可有效抑制循环过程中3CN-HATN的溶解.3CN-HATN负极在80 C(1 C=350 mA g-1)下比容量高达233.8 mAh g-1,将其与Ni(OH)2正极匹配,构建的水系钾离子全电池具备优异的循环稳定性和快充性能,30 C下循环10,000圈后容量保持率达81.5％.

外文标题：A phenazine-derived organic anode for ultrafast and long-life aqueous potassium-ion full cells

外文摘要：Organic electrode materials hold great promise for advancing the development of aqueous potassium-ion batteries(AKIBs)due to their structural diversity and sus-tainability.However,they still encounter challenges such as low electroactive mass contribution and undesirable cycling performance resulting from intrinsic poor electronic con-ductivity and severe solubility issues.Herein,tricyano-sub-stituted hexaazatrinnphthalene(3CN-HATN)was designed by enlarging the conjugated N-heteroaromatic structure and in-troducing cyano(C=N)moieties as additional redox centers.Compared with the typical phenazine anode,the decrease in the lowest unoccupied molecular orbital energy level endows 3CN-HATN with a preferable reduction reaction.The nar-rower band gap ensures higher utilization of 3CN-HATN,while the elongation of π-conjugated structure effectively in-hibits the dissolution in aqueous electrolytes.As a result,the 3CN-HATN anode achieves a remarkable capacity of 233.8 mA h g-1 at an ultrahigh rate of 80 C(1 C=350 mA g-1),retaining an impressive 87.5％of the capacity at 2 C.When coupled with commercial Ni(OH)2 cathode,the as-assembled full cells exhibit outstanding cycling stability,maintaining a capacity retention of 81.5％after 10,000 cycles at 30 C.This work underscores the significance of molecular engineering in the development of redox-active organic materials for con-structing high-performance AKIBs.

外文关键词：

aqueous rechargeable batteriesπ-conjugated struc-tureorganic electrodesK+storagephenazine derivatives

作者：

郑易帆、于丹丹、王健晨、杨杰、罗稳、戈天奇、秦来顺、黄岳翔、陈达

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作者单位：

College of Materials and Chemistry,China Jiliang University,Hangzhou 310018,China

Hydrogen Energy Research Center PetroChina Petrochemical Research Institute,Beijing 102200,China

关键词：

aqueous rechargeable batteries π-conjugated struc-ture organic electrodes K+storage phenazine derivatives

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational College Students Innovation and Entrepreneurship Training ProgramScience and Technology Innovation Activity Program for College Students in Zhejiang Province(New Seedling Talent Program)Pro

项目编号：

52002081519722942023103560332024R409055

出版年：

2024

DOI：

10.1007/s40843-023-2796-5

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(5)