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铝离子电池正极材料研究进展

程成 雷鑫 孙涛 范红玉 申薛靖 武湛君

程成, 雷鑫, 孙涛, 等. 铝离子电池正极材料研究进展[J]. 复合材料学报, 2024, 42(0): 1-27.
引用本文: 程成, 雷鑫, 孙涛, 等. 铝离子电池正极材料研究进展[J]. 复合材料学报, 2024, 42(0): 1-27.
CHENG Cheng, LEI Xin, SUN Tao, et al. Research progress of cathode materials for aluminum-ion batteries[J]. Acta Materiae Compositae Sinica.
Citation: CHENG Cheng, LEI Xin, SUN Tao, et al. Research progress of cathode materials for aluminum-ion batteries[J]. Acta Materiae Compositae Sinica.

铝离子电池正极材料研究进展

基金项目: 青年人才托举工程(YESS20200084); 国家自然科学基金(No.12302218); 中国博士后科学基金(2022M721851)
详细信息
    通讯作者:

    孙涛,博士,教授,硕士生导师,研究方向为纳米功能材料可控制备、耐极端环境复合材料设计和制备、高性能铝离子电池和关键材料设计用开发 E-mail: suntao@jiangnan.edu.cn

    范红玉,博士,副教授,硕士生导师,研究方向为纳米功能材料 E-mail:fanhy@jiangnan.edu.cn

    武湛君,博士,教授,博士生导师,研究方向为先进复合材料与结构、结构健康监测、智能/纳米材料与结构、铝离子电池与储能结构E-mail: wuzhj@jiangnan.edu.cn

  • 中图分类号: TM911;TB333

Research progress of cathode materials for aluminum-ion batteries

Funds: Young Elite Scientists Sponsorship Program by CAST (YESS20200084); National Natural Science Foundation of China (No.12302218); China Postdoctoral Science Foundation (2022M721851)
  • 摘要: 铝离子电池具有高理论比容量、安全性高、低成本、原料来源充足等优势,被认为是锂离子电池的潜在替代品。但正极材料固有特性的不足极大地限制了铝离子电池的进一步发展。本文总结了正极材料在铝离子电池应用领域所发挥的重要作用,综述了铝离子电池正极材料的作用机制和研究进展,概述了碳基、过渡金属氧化物、硫化物、有机材料、金属有机骨架化合物等正极材料对铝离子电池电化学性能的影响。最后,对正极材料在铝离子电池领域亟需解决的问题进行了探讨,对未来铝离子电池正极材料的发展方向提出了展望。

     

  • 图  1  电化学中常见金属元素比容量、标准反应电位(相对于标准氢电极)、地壳中元素储量和阳离子半径[21]

    Figure  1.  Specific capacities, standard reaction potentials (vs standard hydrogen electrode), abundances of elements in the Earth’s crust, and cation radii for common metal elements in electrochemistry[21]

    图  2  (a) Al/石墨(PG)电池放电过程示意图;(b) Al/PG电池的恒流充放电曲线;(c) Al/PG电池的循环性能[28]

    Figure  2.  (a) Schematic drawing of the Al/graphite(PG) cell during discharge; (b) The charge and discharge curves of an Al/PG cell; (c) The cycling performance of an Al/PG cell [28]

    图  3  (a) 小石墨纳米片(SGN)制备工艺示意图;(b) 天然石墨(NG)的SEM图像;(c) SGN的SEM图像[31]

    Figure  3.  (a) Schematic illustration of the preparation process of small graphite nanosheets (SGN); (b) SEM image of natural graphite(NG) and (c) SEM image of SGN[31]

    图  4  SGN的电化学性能。(a) NG和SGN在不同电流密度下的循环充放电曲线;(b) 不同电流密度下的速率性能;(c) SGN的循环性能[31]

    Figure  4.  The electrochemical performance of the SGN. (a) the charge and discharge curves of the cycle of NG and SGN at different current densities;(b) The rate performance test at different current densities; (c) The cycling performance of SGN [31]

    图  5  (a) 原始EG3 K独立膜的SEM图像;(b), (c) 独立EG3 K阴极膜在充满电状态时的表面和截面SEM图像;(d), (e) EG3 K正极材料在充满电状态时的TEM图像[14]

    Figure  5.  (a) SEM image of the original EG3 K free-standing film; (b), (c) surface and cross-section SEM images of the free-standing EG3 K cathode film at the fully charged state; (d), (e) TEM images of the EG3 K cathode material at the fully charged state [14]

    图  6  (a) 不同电流密度下具有独立正极膜的EG3 K AIB的循环性能;(b), (c) EG3 K涂层AIB在不同电流密度下的循环性能[15]

    Figure  6.  (a) Cycling performance at different current densities of the EG3 K AIB system with the free-standing cathode film; (b), (c) cycling performance at different current densities of the EG3 K- coating AIB system[15]

    图  7  (a) 柔性BDC-1800的照片;(b) 八种原始集电器的密度[35]

    Figure  7.  (a) Photos of the flexible BDC-1800; (b) The density of the eight types of pristine current collectors [35]

    图  8  石墨烯气凝胶(GA)薄膜正极的制造工艺示意图[40]

    Figure  8.  Illustration of the fabrication process of graphene aerogel (GA) film cathode [40]

    图  9  GA薄膜的形貌和结构表征。(a) 低倍率SEM图像;(b) 高倍率SEM图像;(c) GA TEM图像;(d), (e)低倍率和高倍率GA薄膜截面SEM图像;(f) GA薄膜俯视图SEM图像 [40]

    Figure  9.  Morphological and structural characterizations of GA films.(a) Low- magnification SEM images; (b) High-magnification SEM images; (c) TEM image of GA; (d), (e) Low and high magnification cross-section SEM images of GA films; (f) Top-view SEM images of GA films[40]

    图  10  Al/GA的电化学性能。(a) 充放电曲线;(b) 速率性能;(c) 不同电流密度下Al/ GA的长循环稳定性 [40]

    Figure  10.  Electrochemical characterization of Al/GA. (a) the charge–discharge curves; (b) rate capability; (c) long-term cycling stability at different current densities[40]

    图  11  (a) 少层石墨烯纳米片(FLG)正极制备过程示意图;(b) FLG的平坦表面和高结晶度(插入衍射点)的TEM图像;(c) 单层(左)、双层(中)和五层(右)FLG纳米片的HRTEM图像;(d) FLG薄膜的横切面;(e) FLG膜的俯视SEM图像[27]

    Figure  11.  (a) Scheme describing Low-layer graphene nanosheets (FLG) cathode formation; (b) TEM image showing the flat surface, and high crystallinity (inset diffraction spots) of FLG; (c) HRTEM images of single-layer (left), double-layer (middle), and five-layer (right) FLG nanosheets; (d) Cross-section of FLG ; (e) top-view SEM images of FLG film[27]

    图  12  FLG AIBs的电化学性能。(a) 倍率性能;(b) 不同循环下的充放电曲线;(c) 10 A/g电流密度下的循环性能[27]

    Figure  12.  Electrochemical characterization of FLG-AIBs. (a) The rate capability of FLG-AIBs obtained at different current densities; (b) The charge–discharge curves of Al/GA at different cycle; (c) The cycling stability tested at 10 A/g [27]

    图  13  (a) 多壁碳纳米管(MWCNTs)不能储存AlCl4示意图;(b) 柔性多壁碳纳米管(UCNTs)储存AlCl4示意图;(c) UCNTs制备的可弯曲柔性电极;(d), (e) 优化后UCNTs的SEM图和TEM图;(f) 优化后UCNTs外缘的HR-TEM图像[45]

    Figure  13.  (a) Multi-walled carbon nanotubes (MWCNTs) which cannot store AlCl4; (b) The unzipped multiwalled carbon nanotubes (UCNTs) to store chloroaluminate anions; (c) The digital photograph of a bendable flexible electrode prepared using the optimized unzipped carbon nanotubes; (d), (e) SEM image and TEM image of the optimized unzipped carbon nanotubes; (f) HR-TEM image for the external edge of the optimized unzipped carbon nanotubes[45]

    图  14  (a) UCNT电极的充放电曲线;(b) UCNT-Al电池的循环性能[45]

    Figure  14.  (a) The charge-discharge curves of the UCNT electrode; (b) Cycle performance of a UCNT-Al pouch cell [45]

    图  15  (a) 碳纳米卷的合成步骤示意图;(b) 高温裂解温度达到1000℃时,中间产物的SEM图像;(c), (d)碳纳米卷的SEM图像;(e) 样品的TEM图像;(f) 高倍率TEM,插图中IFFT图像显示了单个石墨烯层[46]

    Figure  15.  (a) Schematic illustration of the fabrication steps for the synthesis of carbon nanoscrolls; (b) SEM image of the intermediate state product when the annealing temperature reaches 1000℃; (c), (d) SEM images of the as-prepared carbon nanoscrolls; (e) Typical TEM image of the sample; (f) High-resolution TEM. The IFFT image in the illustration exhibits a single graphene layer. [46]

    图  16  合成碳纳米卷的循环性能。(a) 充放电曲线;(b) 长期循环性能[46]

    Figure  16.  Cycle performance of as-synthesized carbon nanoscrolls. (a) Selected galvanostatic charge−discharge curves; (b) Long-term cycle performance of carbon nanoscrolls [46]

    图  17  (a) LiV3O8 (LVO)的SEM图;(b) LVO的低倍率TEM图;(c) 高倍率TEM图[48]

    Figure  17.  (a) SEM image of LiV3O8 (LVO); (b), (c)low-magnification and high-magnification TEM image of LVO [48]

    图  18  (a) 不同电流密度下的倍率性能;(b) 0.59 C电流密度下的循环性能[48]

    Figure  18.  (a) The rate performances at different current densities; (b) cycle life curve at 0.59 C[48]

    图  19  (a) Co3S4微球的XRD图谱;(b) SEM图像;(c), (d) TEM图像。其中(b)中的插图是Co3S4微球的EDS光谱。(d)中的插图是Co3S4微球的HRTEM图像[50]

    Figure  19.  (a) XRD pattern; (b) SEM image; (c), (d) TEM image of the Co3S4 microspheres. Inset in (b) is an EDS spectrum of the Co3S4 microspheres. Inset in (d) is an HRTEM image of the Co3S4 microspheres[50]

    图  20  (a) Co3S4正极的初始充放电曲线;(b) 循环性能;(c) Co3S4正极用于AIBs与其他代表性金属氧化物/硫化物的循环性能的比较;(d) 不同电流密度下的倍率性能[50]

    Figure  20.  (a) Initial discharge/charge curves of a Co3S4 cathode; (b) Cycling performance of a Co3S4 cathode; (c) Comparison of the cycling performance of Co3S4 cathodes with other representative metal oxides/sulfides for AIBs; (d) Rate performance of a Co3S4 cathode at different current densities[50]

    图  21  MoSe2 HNRA正极应用于AIBs的示意图。(a) 通过掠角沉积系统生长Mo HNRA;(b) 等离子体辅助硒化过程;(c)基于MoSe2 HNRA的AIB的工作机制[52]

    Figure  21.  Schematic illustration of the MoSe2 HNRA toward AIBs.(a) Growth of Mo HNRAs by the glancing angle depositing system;(b) The plasma-assisted selenization process; (c) Working mechanism of the MoSe2 HNRA-based AIBs[52]

    图  22  MoSe2 HNRA正极的电化学性能。(a) 充放电曲线;(b), (c) 不同电流密度的循环性能[52]

    Figure  22.  Electrochemical performance of MoSe2 HNRA. (a) Comparison of charge/discharge curves; (b), (c) Cycling performance of MoSe2 HNRA-based AIBs at different current densities [52]

    图  23  铝离子电池中n型、p型和双极型有机正极的反应化学[55, 56]

    Figure  23.  The reaction chemistries of n-types, p-type and bipolar organic positive electrodes in Al-ion batteries[55, 56]

    图  24  羰基化合物的分子结构[56]

    Figure  24.  Molecular structures of carbonyl compounds[56]

    图  25  (a) 三种PQ化合物的结构式—PQ单体(PQ-Ref)、线性PQ三聚体(PQ-Lin)和PQ三角形(PQ-Δ); (b) PQ-Δ(蓝色)的电化学氧化还原化学及其示意图; (c) PQ-Δ及PQ衍生物的循环性能; (d)PQ-Δ倍率性能; (e) 2 A/g的电流密度下PQ-Δ的循环性能; (f) 0.2 A/g电流密度下PQ-Δ-HY的循环性能;(g) PQ-Δ-HY的倍率性能[63]

    Figure  25.  (a) Structural formulae of three PQ compounds—the PQ monomer (PQ-Ref), the linear PQ trimer (PQ-Lin) and the PQ triangle (PQ-Δ); (b) Electrochemical redox chemistry of PQ-Δ (blue) and its schematic representation; (c) Cycling performances of PQ derivatives; (d) Rate capability measurement of PQ-Δ; (e) Extended cycling test of PQ-Δ; (f) Cycling performance of PQ-Δ-HY at the current rate of 0.2 A/g (2C); (g) Rate capability measurement of PQ-Δ-HY[63]

    图  26  (a) PTCDA聚合反应机制; (b) PTCDA正极在充放电过程中的电化学氧化还原反应; (c) 倍率能力; (d) 循环稳定性; (e) 软包电池原理图; (f) AIBs中不同有机正极材料的比较[64]

    Figure  26.  (a) The polymerization reaction mechanism of PTCDA; (b) The electrochemical redox reaction of PTCDA in the process of charge and discharge; (c) The rate capability; (d) Cycling stability; (e) Schematic diagram of soft pack battery; (f) Comparison of different organic positive electrode materials in AlBs[64]

    图  27  (a), (b) H2TPP和H2TCPP的分子结构; (c) H2TPP-xAlCl2模型正的DFT计算得出的反应过程的吉布斯自由能; (d)采用分子静电电位法对H2TPP电极进行两步氧化还原; (e) H2TPP和H2TCPP的循环性能[65]

    Figure  27.  (a), (b) Molecular structure of H2TPP and H2TCPP; (c) The Gibbs free energy of the reaction process from DFT calculations for H2TPP-xAlCl2 model positive; (d) Two-step redox process of H2TPP electrode obtained by molecular electrostatic potential (MESP) method; (e) Cycling stability of H2TPP and H2TCPP[65]

    图  28  (a) 四氰基乙烯(TCNE)、四氰基醌二甲烷(TCNQ)和四(4-氰基苯基)甲烷(TCPM)的化学结构; (b) ,(c) 利用密度泛函理论(DFT)计算的TCNE、TCNQ和TCPM的分子静电势(MESP)图、最低未占据分子轨道(LUMO)和最高占据分子轨道(HOMO); (d) TCNQ的充放电机制; (e) 带乙炔黑改性隔膜和未带的Al-TCNQ 电池中的循环性能[60]

    Figure  28.  (a) Chemical structures of tetracyanoethylene (TCNE), tetracyanoquinodimethane (TCNQ), and tetrakis(4-cyanophenyl)methane (TCPM);(b, c) The molecular electrostatic potential (MESP) map, the lowest unoccupied molecular orbital (LUMO) and the highest occupied molecular orbital (HOMO) of TCNE, TCNQ, and TCPM calculated using density functional theory (DFT); (d) The electrochemical redox reactions based on two-electron reaction; (e) Cycling performance of TCNQ in the Al batteries with and without acetylene black modified separator[60]

    图  29  CuTe@C复合材料的制备[73]

    Figure  29.  The preparation process of CuTe@C composite material[73]

    图  30  CuTe@C的电化学性能。(a) 不同电流密度下的倍率性能;(b) CuTe@C正极与其他文献中的正极的比较;(c) 循环性能[73]

    Figure  30.  Electrochemical performances of CuTe@C. (a) The rate performance; (b) Comparison of CuTe@C electrode with other reported materials;(c) Cycling performance [73]

    图  31  NiTe2@Cu正极的电化学性能。(a) 充放电曲线;(b) 倍率性能;(c) 200 mA/g电流密度下的NiTe2@Cu与NiTe2的循环性能的比较[74]

    Figure  31.  Electrochemical properties of NiTe2@Cu. (a) Comparison of charge/discharge curves; (b) The rate performance; (c) Comparison of the cycle performance of NiTe2@Cu and NiTe2 at 200 mA/g[74]

    图  32  Ti3AlC2的扫描电镜图像。(a), (b) Ti3C2;(c), (d) Ti3C2@CTAB;(e), (f) Ti3C2@CTAB-Se;(g), (h) 不同放大倍率下的Ti3C2@CTAB-Se [76]

    Figure  32.  SEM images of Ti3AlC2. (a), (b) Ti3C2; (c), (d) Ti3C2@CTAB; (e), (f) Ti3C2@CTAB-Se; (g), (h) at different magnifications[76]

    图  33  (a) 不同电流密度下Ti3C2@CTAB-Se的充放电曲线;(b) 循环性能;(c) 本文与其他文献中铝电池正极材料在容量和电压中的比较[76]

    Figure  33.  (a) The charge–discharge curves of Ti3C2@CTAB-Se at different current densities; (b) The cycles performance; (c) A comparison of capacity and voltage of aluminum batteries cathode materials in this work and literature[76]

    图  34  (a) 铝硫电池放电过程示意图;(b), (c) Al-S电池的充放电曲线和循环稳定性[1, 78]

    Figure  34.  (a) Illustration of discharge process for Al-S batteries; (b), (c) Charge/discharge curves and Cycling stability of an Al-S battery [1, 78]

    图  35  (a) 中空纳米管碳包覆碲(Te@CT)的制备示意图;(b) Te@CW SEM图;(c) Te@CT SEM图;(d), (e) Te@CW TEM图;(f), (g) Te@CT TEM图[81]

    Figure  35.  (a) The preparation schematic diagram of hollow nanotube carbon-coated tellurium (Te@CT); (b) SEM diagram of Te@CW; (c) SEM diagram of Te@CT; (d), (e) TEM diagram of Te@CW; (f), (g) TEM diagram of Te@CT[81]

    图  36  Te@CT的电化学性能。(a) 倍率性能曲线;(b) 循环性能[81]

    Figure  36.  The electrochemical performance of Te@CT. (a) The rate performance; (b) cycle performance [81]

    图  37  N-PC-rGO-Te合成过程和形态表征。(a) N-PC-Te和N-PC-rGO-Te复合电极的合成过程示意图;(b-e) ZIF-67,N-PC-27,N-PC-Te和N-PC-rGO-Te的SEM图像,插图是相应的单个十二面体;(f-i) 相应的透射电镜图像[82]

    Figure  37.  Synthesis process and morphology characterizations. (a) Schematic illustration of the synthetic procedure of the N-PC-Te and N-PC-rGO-Te composite electrodes; (b-e) SEM images of ZIF-67, N-PC-27, N-PC-Te and N-PC-rGO-Te, and

    N-PC—N-doped porous carbon; rGO—reduced graphene oxide inset is the corresponding single dodecahedron; (f-i) The corresponding TEM images[82]

    图  38  N-PC-rGO-Te正极的电化学性能。(a), (b)不同电流密度下的速率性能及相应的充放电曲线;(c) 500 mA/g电流密度下循环性能[82]

    Figure  38.  The electrochemical performances of N-PC-rGO-Te positive electrode. (a), (b) The rate performance and corresponding charge/discharge curves at various current densities; (c) The cycling performance at a current density of 500 mA/g [82]

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  • 收稿日期:  2023-11-08
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