Structural modification and performance optimization of red phosphorus nanomaterials as anodes for lithium/sodium-ion batteries
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摘要: 開發高性能二次電池材料是緩解能源與環境危機的有效途徑。商業鋰離子電池石墨負極由于理論容量較低且在鈉離子電池中幾乎不顯示容量，無法滿足人類日益增長的能量需求。紅磷由于理論容量高（2596 mA?h?g–1）、氧化/還原電位適宜、地球資源占比豐富以及價格低廉等優點成為堿金屬離子電池研究中的熱點，有望成為商業化大規模儲能系統中應用的負極材料。但是，紅磷在作為負極材料時具有導電性差、體積膨脹大等缺點，導致活性材料利用率低，電極粉化現象嚴重，電極循環穩定性差，嚴重限制了其在二次電池中的商業應用。最近研究表明，通過合理的結構設計可以有效地提高紅磷的電子導電率及結構穩定性，進而改善紅磷負極的循環穩定性和倍率性能，促進紅磷在商業鋰/鈉離子電池中的廣泛應用。本文綜述了近年來納米紅磷負極材料在可控合成方法、結構設計與改性以及性能優化機理上的研究進展。最后，總結了目前紅磷負極材料研究存在的問題，并提出可能的應對策略，對納米紅磷基負極材料未來在電池領域發展前景進行了展望，旨在促進其商業應用。Abstract: Developing electrode materials for high-performance secondary batteries is one of the most effective approaches to alleviate energy and environmental crises. Nowadays, graphite anodes, which are widely used in commercial lithium-ion batteries, cannot satisfy the ever-growing energy needs of humans owing to their relatively low theoretical capacities and nearly no capacity in sodium-ion batteries. Therefore, developing new anodes with high capacity and energy density is necessary for next-generation large-scale energy systems. Red phosphorus has become an interesting topic in alkali-ion battery research and is expected to be commercially used as anode material in the next generation of secondary batteries owing to their intrinsic properties, such as their high activity, high theoretical specific capacity (2596 mA?h?g?1), suitable oxidation–reduction potential, highly abundant earth resources, and low cost of lithium/sodium-ion batteries. However, red phosphorus exhibits poor electrical conductivity and large volume expansion when used as electrode material, resulting in low utilization of active material, serious electrode pulverization, and poor electrode cycling stability, which seriously hindered their commercial application in next-generation rechargeable batteries. Recent studies have shown that the cycle stability and electronic conductivity of red phosphorus can be improved by rational structural design, which promotes the electrochemical performance of red phosphorus anodes. For example, reducing the material size to the nanoscale can effectively shorten the diffusion path, enhancing the ion diffusion rate while alleviating the volume expansion and pulverization of the active substance. Additionally, the size reduction changes the band energy of the red phosphorus, which can transform indirect into direct bandgap semiconductors. Besides, the external characteristics of the active materials affect the performance by reducing the internal stress generated by the phase transformation in charging and discharging cycles. By modifying the morphology and structure of red phosphorus to form porous, layer, hollow, or composite structures, the cyclability and chargeability of batteries could be optimized because the internal stress generated by the volume change of the active material can be effectively released, and the generation probability of cracks or fractures in the electrode is drastically reduced. Therefore, these strategies help alleviate electrode pulverization and promote the commercial application of red phosphorus in lithium/sodium-ion batteries. Herein, we review the recent research progress in controllable synthesis, structural design, and performance optimization mechanisms of red phosphorus-based nanocomposites. Finally, we summarize the challenges in current research on red phosphorus anode materials, propose potential solutions, and provide an outlook on the future development of red phosphorus-based anode materials in the energy storage system.
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Key words:
- red phosphorus /
- rechargeable battery /
- structure design /
- performance optimization /
- preparation
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圖 2 納米紅磷基負極的可控制備方法、多重納米結構和性能優化機理
Figure 2. Overview of the synthesis techniques, various structures, and performance optimization mechanisms of red phosphorus-based nanocomposites
圖 4 (a)HRPN形成機制示意圖[57]；(b)具有多孔殼的空心納米球在鋰化/鈉化和體積變化過程中的示意圖[58]；(c)碘摻雜HNPRP合成示意圖[59]；(d)多通道中空納米紅磷球[60]
Figure 4. (a) Schematic of the proposed formation mechanism of the HRPNs[57]; (b) schematic of hollow nanospheres with porous shells during lithiation/sodiation and volume variation[58]; (c) schematic of the iodine-doped HNPRP synthesis[59]; (d) multichannel hollow nano-red phosphorus ball[60]
圖 5 (a) HHPCNSs/P復合材料合成過程的示意圖[67]；(b) HPCNS/RP的V–C過程示意圖[68]；(c) P@PMCNFs的制作工藝示意圖[73]；(d) RPNP/MWNT復合材料合成的示意圖[75]
Figure 5. (a) Schematic of the synthesis process for the HHPCNSs/P composite[67]; (b) schematic of the V–C process[68]; (c) schematic of the fabrication process for P@PMCNFs[73]; (d) schematic of synthesis of RPNPs/MWNT composite[75]
圖 7 (a) P–SCNT復合材料的合成路線示意圖[85]；(b) SIB系統中C@P/GA電極示意圖[86]；(c)三維碳骨架(P/C復合材料)中超細紅磷顆粒合成過程的示意圖[87]
Figure 7. (a) Schematic and digital photographs of the synthetic route for P–SCNT composite[85]; (b) schematic of preparation of P@GS composite[86]; (c) schematic and digital photographs of the synthesis procedure for the ultrafine red phosphorus particles embedded in a 3D carbon framework (P/C composite)[87]
表 1 紅磷納米材料的電化學性能對比
Table 1. Comparison of the electrochemical properties of red phosphorus nanomaterials
Sample Preparation method Battery type Current density Cycle number Capacity/(mA?h?g?1) Honeycomb-like red phosphorus[47] Template-less hydrothermal Li 0.5 A?g?1 500 1201 Phosphorus composite nanosheets[52] Sublimation-induced Li 0.2 A?g?1 100 1683 Iodine-doped red phosphorus nanoparticles[6] Solution synthesis Li 0.4 A?g?1 150 1562 0.2C 100 1700 1C 500 900 Red phosphorus nanoparticles[53] Solution synthesis Li 0.1 A?g?1 100 1380 Hollow red phosphorus nanospheres[57] Molten-salt method Na 0.5C 50 1500 1C 600 737 Hollow red-phosphorus nanospheres[58] Wet-chemical synthesis Li 1C 600 1048 Na 1C 600 970 Hollow nanoporous red phosphorus[59] Solution synthesis Na 0.26 A?g?1 100 1658 2.6 A?g?1 1000 857 Multichannel nanoporous red phosphorus[60] Solvothermal synthesis Na 200 mA?g?1 100 1814 3200 mA?g?1 400 735 
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表 2 紅磷/碳復合材料電化學性能對比
Table 2. Comparison of the electrochemical properties of red phosphorus/carbon composites
Sample Preparation method Battery type Current density Cycle number Capacity/(mA?h?g?1) Red phosphorus/carbon nanocages[83] Evacuation-filling Na 100 mA?g?1 150 1363cp 5000 mA?g?1 1300 610cp Hollow porous carbon nanospheres/phosphorous[70] Vaporization/condensation Na 1 A?g?1 1000 548 Hollow carbon nanospheres to host phosphorus[71] Vaporization/condensation (secondary annealing) Na 4 A?g?1 2000 1027 8 A?g?1 2000 837 Crystalline red phosphorus/porous carbon nanofibers[72] Vaporization/adsorption Li 0.1C 100 2030 1C 100 1042 Red phosphorus/porous multichannel carbon nanofibers[73] Vaporization/condensation Na 500 mA?g?1 400 1123cp 1000 mA?g?1 400 918cp Phosphorus/N-doped carbon nanofiber composite[18] Vaporization/condensation Na 100 mA?g?1 55 731cp red Phosphorus/nanotube-backboned mesoporous carbon[74] Vaporization/condensation Na 0.25 A?g?1 150 756.8cp Red phosphorus nanoparticles/multi-walled carbon nanotube[75] In-situ deposition Li 200 mA?g?1 100 — Red phosphorus/Ti3C2Tx[80] Ball-milling Li 200 mA?g?1 200 818.2cp Ti3C2Tx MXene/carbon nanotubes@red phosphorus[81] Ball-milling Li 0.05C 500 2078 Red phosphorus/hierarchical micro–mesoporous carbon nanospheres[67] Vaporization/condensation Li 2 A?g?1 1000 1201.6 Red phosphorus/reduced graphene Oxide[77] Solution synthesis Na 173.26 mA?g?1 150 1249cp 5.12 A?g?1 1500 775 Sandwich-like phosphorus/reduced graphene oxide composites[78] Spraying strategy Li 100 mA?g?1 50 990 Red phosphorus/TiN/graphene[14] Ball-milling Na 0.2C 300 — Red phosphorus nanodots/reduced graphene oxide[79] physical vapor deposition Na 1594 mA?g?1 300 914cp 3D red phosphorus/sheared CNT sponge[85] Vaporization/condensation Li 2 A?g?1 2000 807cp 3D hierarchical integrated carbon/red phosphorus/graphene aerogel composite[86] Vaporization/condensation Na 1C 200 1095 0.1C 100 1867 Red phosphorus-filled 3D carbon material[87] Carbothermic reduction synthesis Na 0.2C 160 920cp Note: cp denotes specific capacity calculated as the mass of the composite.
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