Research progress of cathode materials for aluminum-ion batteries
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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。Abstract: With high theoretical specific capacity, high safety, low cost, and sufficient raw material sources, aluminum-ion batteries have been regarded as potential alternatives to lithium-ion batteries. However, the shortcomings of the inherent characteristics of the cathode material have greatly limited the further development of aluminum-ion batteries. In this paper, the important role of cathode materials in the application filed of aluminum ion battery was summarized, the mechanism of action and research progress of aluminum ion electrode materials were reviewed, and the effects of various cathode materials such as carbon-based, transition metal oxides and sulfides, organic materials and metal-organic skeletal compounds on the electrochemical performance of aluminum ion batteries were summarize. Finally, the problems that need to be solved urgently in the field of positive electrode materials for aluminum ion batteries are discussed, and the future development direction of positive electrode materials for aluminum ion batteries is proposed.
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Key words:
- Al ion batteries /
- cathode material /
- reaction mechanism /
- electrochemical performance /
- new energy
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图 5 (a) 原始膨胀石墨(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 expanded graphite (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 Al离子电池(AIBs)的循环性能；((b), (c)) EG3 K涂层AIBs在不同电流密度下的循环性能[15]
ET—Triethylamine hydrochloride
Figure 6. (a) Cycling performance at different current densities of the EG3 K Al ion battery (AIBs) system with the free-standing cathode film; ((b), (c)) Cycling performance at different current densities of the EG3 K-coating AIBs system[15]
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) 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 image; (b) High-magnification SEM image; (c) TEM image; ((d), (e)) Low and high magnification cross-section SEM images of GA films; (f) Top-view SEM image of GA films[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；FLG薄膜的横切面(d)及俯视(e)的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; Cross-section (d) and top-view (e) SEM images of FLG film[27]
图 13 (a) 多壁碳纳米管(MWCNTs)不能储存$\mathrm{AlCl}_4^{-} $示意图；(b) 柔性多壁碳纳米管(UCNTs)储存$\mathrm{AlCl}_4^{-} $示意图；(c) UCNTs制备的可弯曲柔性电极；((d), (e)) 优化后UCNTs的SEM图像和TEM图像；(f) 优化后UCNTs外缘的HRTEM图像[45]
Figure 13. (a) Multi-walled carbon nanotubes (MWCNTs) which cannot store $\mathrm{AlCl}_4^{-} $; (b) Unzipped multiwalled carbon nanotubes (UCNTs) to store $\mathrm{AlCl}_4^{-} $; (c) Digital photograph of a bendable flexible electrode prepared using the optimized UCNTs; ((d), (e)) SEM image and TEM image of the optimized UCNTs; (f) HRTEM image for the external edge of the optimized UCNTs[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 19 Co3S4微球的XRD图谱(a)、SEM图像(b)及其TEM图像((c), (d)) (Fig.19(b)中的插图是Co3S4微球的EDS光谱；Fig.19(d)中的插图是Co3S4微球的HRTEM图像[50])
Figure 19. XRD pattern (a), SEM image (b) and TEM images ((c), (d)) of the Co3S4 microspheres (Inset in Fig.19(b) is an EDS spectrum of the Co3S4 microspheres; Inset in Fig.19(d) is an HRTEM image of the Co3S4 microspheres[50])
图 20 Co3S4正极的初始充放电曲线(a)和循环性能(b)；(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Co3S4正极倍率性能[50]
Figure 20. Initial discharge/charge curves (a) and cycling performance (b) of Co3S4 cathode; (c) Comparison of the cycling performance of Co3S4 cathodes with other representative metal oxides/sulfides for AIBs; (d) Rate performance of Co3S4 cathode at different current densities[50]
图 21 MoSe2 螺旋纳米棒阵列(HNRA)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AIBs的工作机制[52]
GLAD—Glancing angle deposition; ICP—Low temperature plasma assisted
Figure 21. Schematic illustration of the MoSe2 helical nanorod arrays(HNRA) toward AIBs: (a) Growth of Mo HNRAs by the glancing angle depositing system; (b) Plasma-assisted selenization process; (c) Working mechanism of the MoSe2 HNRA-based AIBs[52]
图 25 (a) 菲醌(PQ)单体(PQ-Ref)、线性PQ三聚体(PQ-Lin)和PQ三角形(PQ-Δ)的结构式；(b) PQ-Δ的电化学氧化还原反应及其示意图；(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电流密度下三角形大环共混化合物(PQ-Δ-HY)的循环性能；(g) PQ-Δ-HY的倍率性能[63]
Figure 25. (a) Structural formulae of phenquinone (PQ) monomer (PQ-Ref), linear PQ trimer (PQ-Lin) and PQ triangle (PQ-Δ); (b) Electrochemical redox chemistry of PQ-Δ and its schematic representation; (c) Cycling performances of PQ-Δ and PQ derivatives; (d) Rate capability measurement of PQ-Δ; (e) Extended cycling test of PQ-Δ at 2 A/g; (f) Cycling performance of PQ-Δ-HY at the current rate of 0.2 A/g; (g) Rate capability measurement of PQ-Δ-HY[63]
图 26 (a) 苝-3, 4, 9, 10-四羧酸二酐(PTCDA)的聚合反应机制；PTCDA正极在充放电过程中的电化学氧化还原反应(b)、倍率性能和循环稳定性((c), (d))；(e) 软包电池原理图；(f) AIBs中不同有机正极材料的比较[64]
PI—Polyimide
Figure 26. (a) Polymerization reaction mechanism of perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA); Electrochemical redox reaction (b), rate capability and cycling stability ((c), (d)) of PTCDA in the process of charge and discharge; (e) Schematic diagram of soft pack battery; (f) Comparison of different organic positive electrode materials in AIBs[64]
图 27 ((a), (b)) 5, 10, 15, 20-四苯基卟啉(H2TPP)和5, 10, 15, 20-四(4-羧基苯基)卟啉(H2TCPP)的分子结构；(c) H2TPP-xAlCl2模型修正的密度泛函理论(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(MESP)对H2TPP电极进行两步氧化还原；(e) H2TPP和H2TCPP循环性能[65]
ΔG—Gibbs free energy
Figure 27. ((a), (b)) Molecular structure of 5, 10, 15, 20-tetraphenyl porphyrin (H2TPP) and 5, 10, 15, 20-tetraphenyl (4-carboxyphenyl) porphyrin (H2TCPP); (c) Gibbs free energy of the reaction process fromdensity functional theory (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) 基于双电子反应的电化学氧化还原反应；(e) 带乙炔黑改性隔膜和未带的Al-TCNQ 电池中的循环性能[60]
ABMS—Acetylene black modified separator; Eg—Energy gap
Figure 28. (a) Chemical structures of tetracyanoethylene (TCNE), tetracyanoquinodimethane (TCNQ), and tetrakis(4-cyanophenyl)methane (TCPM);((b), (c)) 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) 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 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) Charge-discharge curves of Ti3C2@CTAB-Se at different current densities; (b) Cycles performance; (c) Comparison of capacity and voltage of aluminum batteries cathode materials in this work and literature[76]
图 37 (a) N-PC-Te和N-PC-rGO-Te复合电极的合成过程示意图；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)((b)~(e))及相应的透射电镜图像((f)~(i))[82]
Figure 37. (a) Schematic illustration of the synthetic procedure of the N-PC-Te and N-PC-rGO-Te composite electrodes; SEM images ((b)-(e)) and corresponding TEM images ((f)-(i)) of ZIF-67, N-PC-27, N-PC-Te and N-PC-rGO-Te[82]
N-PC—N-doped porous carbon; rGO—Reduced graphene oxide inset is the corresponding single dodecahedron; PDDA—Polydiallyl dimethyl ammonium chloride
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. Electrochemical performances of N-PC-rGO-Te positive electrode: ((a), (b)) Rate performance and corresponding charge/discharge curves at various current densities; (c) Cycling performance at a current density of 500 mA/g[82]
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