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Unraveling the Potassium Storage Mechanism in Graphite Foam

机译：阐明石墨泡沫中钾的储存机理

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摘要

Potassium-intercalated graphite intercalation compounds (K-GICs) are of particular physical and chemical interest due to their versatile structures and fascinating properties. Fundamental insights into the K+ storage mechanism, and the complex kinetics/thermodynamics that control the reactions and structural rearrangements allow manipulating K-GICs with desired functionalities. Here operando studies including in situ Raman mapping and in situ X-ray diffraction (XRD) characterizations, in combination with density-functional theory simulations are carried out to correlate the real-time electrochemical K+ intercalation/deintercalation process with structure/component evolution. The experimental results, together with theoretical calculations, reveal the reversible K-GICs staging transition: C - stage 5 (KC60) - stage 4 (KC48) - stage 3 (KC36) - stage 2 (KC24/KC16) - stage 1 (KC8). Moreover, the staging transition is clearly visualized and an intermediate phase of stage 2 with the stoichiometric formula of KC16 is identified. The staging transition mechanism involving both intrastage transition from KC24 (stage 2) to KC16 (stage 2) and interstage transition is proposed. The present study promotes better fundamental understanding of K+ storage behavior in graphite, develops a nondestructive technological basis for accurately capture nonuniformity in electrode phase evolution across the length scale of graphite domains, and offers guidance for efficient research in other GICs.
机译：钾插层石墨插层化合物（K-GIC）由于其通用的结构和引人入胜的性能而特别受物理和化学关注。对K +储存机理的基本见解以及控制反应和结构重排的复杂动力学/热力学，可以操纵具有所需功能的K-GIC。在这里，包括原位拉曼映射和原位X射线衍射（XRD）表征在内的操作研究与密度泛函理论仿真相结合，将实时电化学K +嵌入/脱嵌过程与结构/组分演化相关联。实验结果与理论计算一起揭示了可逆的K-GIC过渡阶段：C-阶段5（KC60）<->阶段4（KC48）<->阶段3（KC36）<->阶段2（KC24 / KC16）<->阶段1（KC8）。此外，可以清楚地看到阶段过渡，并确定具有化学计量公式为KC16的阶段2的中间阶段。提出了涉及从KC24（阶段2）到KC16（阶段2）的阶段内转换和阶段间转换的阶段转换机制。本研究促进了对石墨中K +储存行为的更好的基本理解，为准确捕获整个石墨域长度尺度上电极相演化的不均匀性提供了无损技术基础，并为其他GIC中的有效研究提供了指导。

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  • 来源
    《Advanced energy materials》 |2019年第22期|1900579.1-1900579.11|共11页
  • 作者

    Liu Jilei; Yin Tingting; Tian Bingbing; Zhang Bowei; Qian Cheng; Wang Zhiqiang; Zhang Lili; Liang Pei; Chen Zhen; Yan Jiaxu; Fan Xiaofeng; Lin Jianyi; Chen Xiaohua; Huang Yizhong; Loh Kian Ping; Shen Ze Xiang;

  • 作者单位

    Hunan Univ, Coll Mat Sci & Engn, Hunan Prov Key Lab Adv Carbon Mat & Appl Technol, Changsha 410082, Hunan, Peoples R China;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

    Shenzhen Univ, Coll Optoelect Engn, Minist Educ & Guangdong Prov, Key Lab Optoelect Devices & Syst,Int Collaborat L, Shenzhen 518060, Peoples R China;

    Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

    Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

    ASTAR, Inst Chem Engn & Sci, 1 Pesek Rd, Jurong Isl 627833, Singapore;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

    Nanjing Tech Univ Nanjing Tech, Jiangsu Natl Synergist Innovat Ctr Adv Mat SICAM, Key Lab Flexible Elect KLOFE, 30 South Puzhu Rd, Nanjing 211816, Jiangsu, Peoples R China|Nanjing Tech Univ Nanjing Tech, Jiangsu Natl Synergist Innovat Ctr Adv Mat SICAM, IAM, 30 South Puzhu Rd, Nanjing 211816, Jiangsu, Peoples R China;

    Jilin Univ, Coll Mat Sci & Engn, Changchun 130012, Jilin, Peoples R China;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

    Hunan Univ, Coll Mat Sci & Engn, Hunan Prov Key Lab Adv Carbon Mat & Appl Technol, Changsha 410082, Hunan, Peoples R China;

    Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

    Natl Univ Singapore, Dept Chem, Ctr Adv 2D Mat CA2DM, 3 Sci Dr 3, Singapore 117543, Singapore|Natl Univ Singapore, Graphene Res Ctr, 3 Sci Dr 3, Singapore 117543, Singapore;

    Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore;

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  • 正文语种 eng
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  • 关键词

    intrastage; K-GICs; mechanism; operando; stage transition;

    机译：九个人;K-GICS;机制;Operando;舞台过渡;

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