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Organic electrodes with multi-role natural amino acid groups for sodium-ion batteries with high-capacity and long-life

通过引入天然氨基酸基团来设计高容量、 长寿命钠离子电池用有机分子电极

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Abstract

Organic electrodes possess numerous advantages of structure designability, high capacity, and accommodating large cations. However, the capacity of organic electrode materials in sodium-ion batteries remains low, and their solubility in organic electrolytes leads to a shortened lifespan. Researchers are thus concerned about enhancing their performance through compound design. In this study, we successfully improved both the capacity and cycling stability by simply grafting amino acids onto organic compounds (PMCDI). Firstly, the introduction of amino acids facilitated the formation of a more stable layered structure of PMCDI through hydrogen bonding. Additionally, the amino acid groups promoted intermolecular interactions between the organic electrode material and the carboxymethyl cellulose binder, thereby reducing interfacial resistance and significantly enhancing the cycling stability for over 2000 cycles. Secondly, both experimental and computational results revealed that the non-conjugated carboxylic acid group provided Na+ transport pathways and an additional reversible storage site, leading to an improvement in specific capacity (~300 mA h g−1). The strategy employed in this work sheds light on the design of organic molecules for future sodium-ion batteries.

摘要

有机电极具有结构可设计性强、 容量大、 可容纳大离子等优点. 然而, 在钠离子电池中, 有机电极材料的容量仍然很低, 且其在有机电解质中的高溶解度导致其寿命较短. 如何通过化合物设计来提高其性能一直是研究人员关注的问题. 本研究通过简单方法将氨基酸接枝到有机化合物上, 提高了其容量和循环稳定性. 首先, 氨基酸之间的氢键使其形成更稳定的层状结构; 氨基酸基团在有机电极材料和羧甲基纤维素粘合剂之间形成分子间相互作用, 降低界面阻力, 显著提高循环稳定性, 使得钠离子电池循环次数超过2000次. 其次, 实验和计算结果表明, 氨基酸基团提供了Na+转运途径和额外的可逆存储位点, 从而提高了比容量(~300 mA h g−1). 本策略可以启发未来钠离子电池的有机分子设计.

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (2019YFA0210600) and the National Natural Science Foundation of China (51922103 and BC0500463).

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China

    Shicong Zhang  (张世从), Tao Li  (李涛) & Tianquan Lin  (林天全)

  2. State Key Laboratory of High-performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics Chinese Academy of Sciences, Shanghai, 200050, China

    Xiaolin Zhao  (赵晓琳), Jianjun Liu  (刘建军) & Fuqiang Huang  (黄富强)

  3. State Key Laboratory of Rare Earth Materials Chemistry and Applications, Peking University, Beijing, 100871, China

    Fuqiang Huang  (黄富强)

  4. Zhangjiang Institute for Advanced Study (ZIAS), Shanghai Jiao Tong University, Shanghai, 201210, China

    Shicong Zhang  (张世从), Tao Li  (李涛) & Tianquan Lin  (林天全)

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  1. Shicong Zhang  (张世从)
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  2. Xiaolin Zhao  (赵晓琳)
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  3. Tao Li  (李涛)
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  6. Tianquan Lin  (林天全)
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Contributions

Author contributions Zhang S designed and engineered the samples; Zhang S, Zhao X and Li T performed the experiments; Zhang S wrote the paper with support from Liu J, Huang F and Lin T. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Jianjun Liu  (刘建军), Fuqiang Huang  (黄富强) or Tianquan Lin  (林天全).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Shicong Zhang received her PhD degree from the East China University of Science and Technology (2020). Currently, she is a post-doctor at Shanghai Jiao Tong University (SJTU). Her research interest focuses on the synthesis of novel organic electrode materials.

Xiaolin Zhao received her Bachelor degree from Taiyuan University of Technology in 2018 and PhD degree from Shanghai Institute of Ceramics, Chinese Academy of Sciences (SICCAS) in 2022. Currently, she is a post-doctor at SICCAS. Her research interest focuses on computational electrochemical study of organic/metal-organic electrode materials.

Tao Li received his Master’s degree from SICCAS (2020). And now he is a PhD student at SJTU. His research interests include zinc-ion batteries and novel electrolytes.

Jianjun Liu works as a professor at SICCAS. He received his PhD degree from Jilin University (2002). He did postdoctoral research at Emory University from 2003 to 2005, and worked as an assistant scientist at the Southern Illinois University from 2005 to 2011. His research interests include advanced computational electrochemical methods and electrode materials for sodium-ion batteries.

Fuqiang Huang is a professor at Peking University and SICCAS. He received his Bachelor degree from Jilin University (1993) and PhD degree from Beijing Normal University (1996). From 1996 to 2003, he was engaged in scientific research at the University of Michigan, Northwestern University, Siemens Corporation and University of Pennsylvania, respectively. His research interests include advanced energy storage materials, novel compound design and solid chemistry.

Tianquan Lin is a professor at SJTU. He received his Bachelor degree from the Central South University (2008) and PhD degree from SICCAS (2013). From 2013 to 2020, he worked as a researcher at Massachusetts Institute of Technology (MIT) and SICCAS. His research interests include novel materials and devices for (photo)electro-chemical energy storage.

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Zhang, S., Zhao, X., Li, T. et al. Organic electrodes with multi-role natural amino acid groups for sodium-ion batteries with high-capacity and long-life. Sci. China Mater. 66, 3817–3826 (2023). https://doi.org/10.1007/s40843-023-2545-y

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