鈉離子電池P2相鎳錳基層狀氧化物正極材料的研究進展

姜娜; 孫珞然; 王慧麗; 伍忠漢; 焦培鑫; 張凱

doi:10.13374/j.issn2095-9389.2022.08.22.003

鈉離子電池P2相鎳錳基層狀氧化物正極材料的研究進展

doi: 10.13374/j.issn2095-9389.2022.08.22.003

姜娜^{1, 2},
孫珞然^{1, 2},
王慧麗^{1, 2},
伍忠漢^{1, 2},
焦培鑫^{1, 2},
張凱^{1, 2, ,}

1.
南開大學化學學院先進能源材料化學教育部重點實驗室，天津 300071
2.
物質綠色創造與制造海河實驗室，天津 300192

基金項目: 國家自然科學基金資助項目（22005155，52072186）；中國科協青年人才托舉工程資助項目（2019QNRC001）；南開大學中央高校基本科研業務費資助專項（63223015）；天津市物質綠色創造與制造海河實驗室資助項目（ZYTS202104）

詳細信息

通訊作者:
E-mail: zhangkai_nk@nankai.edu.cn

中圖分類號: TG142.71
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- 被引次數: 0
出版歷程
- 收稿日期: 2022-08-22
- 網絡出版日期: 2022-09-26
- 刊出日期: 2023-07-25

Recent advances in P2-type Ni–Mn-based layered oxide cathodes for sodium-ion batteries

JIANG Na^{1, 2},
SUN Luo-ran^{1, 2},
WANG Hui-li^{1, 2},
WU Zhong-han^{1, 2},
JIAO Pei-xin^{1, 2},
ZHANG Kai^{1, 2
, ,}

1.
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
2.
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China

More Information

Corresponding author: E-mail: zhangkai_nk@nankai.edu.cn

摘要

摘要: P2型Na_0.67[Ni, Mn]O₂材料由于較高的比容量、工作電壓以及較好的空氣穩定性成為最具前景的鈉離子電池正極材料之一。然而，高壓相變、Na⁺/空位有序排布以及由Mn³⁺引起的Jahn–Teller扭曲導致該類材料充放電過程中面臨結構失穩以及性能衰減的挑戰。本綜述從P2型Na_0.67[Ni, Mn]O₂材料的失效機制出發，系統闡述了該類材料的最新進展。最后，對其未來的發展方向進行了展望。本文將為P2-type Na_0.67[Ni, Mn]O₂材料的研發與商業化提供借鑒。
- 鈉離子電池 /
- 正極材料 /
- 鎳錳基層狀氧化物 /
- 性能衰退機制 /
- 離子摻雜 /
- 表面修飾 /
- P2/O3雙相結構
Abstract: As concerns over environmental contamination and rapid consumption of fossil fuels continue to grow, it is important for energy storage technology to reduce the intermittency of clean and renewable energy sources. So far, lithium-ion batteries (LIBs), commercialized by SONY corporation in 1991, have been the most widely used rechargeable batteries for various energy storage devices. Due to the ever-increasing demand for lithium employment in mobile electronic devices and electric vehicles (EVs), the price of Li resources is rising year by year. It is well known that worthwhile lithium resources are only found in a few countries (mainly in South America). Recently, sodium-ion batteries (SIBs) have been regarded as promising alternatives to LIBs for future large-scale energy storage systems (ESSs) owing to their low cost, abundant reservoirs of Na resources and similar characteristics to LIBs. Developing high-performance cathode materials is crucial to realize the commercialization of the SIB technology. Sodium transition metal oxides (Na_xTMO₂), especially for Ni–Mn-based compounds, have received significant attention thanks to their high specific capacity and operating voltage. Normally, layered Na_xTMO₂ materials have two types of crystal structures: P2 and O3, according to the surrounding Na environment and the number of unique oxygen layers occupied within the lattice. Compared with the O3 phase, the P2-type structure has open diffusion channels for the transport of Na⁺ and relatively rare phase transitions, which make P2-type Na_0.67[Ni, Mn]O₂ (NNMO) one of the most promising cathodes for SIBs. However, NNMO materials generally suffer from irreversible P2–O2 phase transformations, Na⁺/vacancy ordering transitions and Jahn–Teller distortion of Mn^(III)O₆ octahedra, leading to structural deterioration and performance degradation during the charge and discharge processes. In detail, the P2–O2 phase transition inevitably causes significant lattice volume change (~20%) and even the formation of cracks, resulting in the stripping of active substances from the collector and serious capacity decay during cycling. The Na⁺/vacancy ordering in NNMO causes the multi-step two-phase reactions, which may increase the activation energy barrier for Na⁺ hops between adjacent prismatic sites, consequently hindering Na⁺ diffusion. Additionally, the lattice distortion and P2-P’2 phase transition induced by the Jahn–Teller effect also impede Na⁺ migration, leading to the sluggish kinetics of Na⁺ (de)intercalation. In this review, the recent progress on NNMO cathodes is summarized, including ion-doping, surface modification and composite structure. The comprehensive and integrated explanation of the structure–function–performance relationship of these optimized cathodes is further presented. Moreover, the existing challenges of NNMO and possible remedies are also discussed. It is expected that this review can provide new insights into the commercialization of NNMO for SIBs.
- sodium-ion batteries /
- cathode materials /
- Ni–Mn based layered oxides /
- performance degradation mechanism /
- ion-doping /
- surface modification /
- P2/O3 mixture

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圖 1 (a) P2相晶體結構示意圖; (b) O3相晶體結構示意圖 (c) P2-Na_2/3Mn_2/3Ni_1/3O₂材料首周充放電曲線^[9]

Figure 1. (a) Schematic of P2 phase crystal structure; (b) schematic of O3 phase crystal structure; (c) initial charge/discharge curve of P2-Na_2/3Mn_2/3Ni_1/3O₂^[9]

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圖 2 (a) 總熒光產額(TFY)模式下Ni-L3邊以及擬合曲線^[17]; (b) P2-Na_2/3Mn_2/3Ni_1/3O₂材料的非彈性散射共振光譜(mRIXS)圖像(關鍵的氧的氧化還原特征由紅色箭頭指出)^[17]; (c)通過對(b)中的兩條虛線之間的區域進行積分提取出的非彈性散射共振光譜-超特定熒光產率(mRIXS-sPFY)光譜^[17]; (d) mRIXS-sPFY光譜531 eV處峰面積^[17]; (e) 通過對Ni、O氧化還原以及不可逆反應獨立量化來解析總電化學容量^[17]; (f) P2-Na_2/3Mn_2/3Ni_1/3O₂電極的PDOS圖^[9]

Figure 2. (a) Ni-L3 edge TFY (solid) and fitted curves^[17]; (b) corresponding mRIXS images of Na_2/3Ni_1/3Mn_2/3O₂ electrode, the key oxygen redox features are indicated by the red arrows^[17]; (c) mRIXS-sPEY spectra extracted from mRIXS by integrating the characteristic 523.7 eV emission energy range, as indicated by the two horizontal dashed lines in Fig.2 (b)^[17]; (d) mRIXS-sPFY 531 eV peak areas^[17]; (e) decipher the total electrochemical capacity by independent quantifications of Ni, Mn and O redox^[17]; (f) PDOS of Na_2/3Ni_1/3Mn_2/3O₂ electrode^[9]

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圖 3 (a) P2相高壓相變示意圖^[18]; (b)Na_2/3Mn_2/3Ni_1/3O₂材料首圈充放電過程中的晶體結構演變^[19]; (c) Na_2/3Mn_2/3Ni_1/3O₂材料不同電壓區間內循環50周后SEM圖（從左至右依次為原始樣品、2～3.8 V、2.0～4.1 V、2.0～4.25 V、2.0～4.5 V）^[20]

Figure 3. (a) Schematic of P2 phase in the high voltage region;^[18] (b) Na_2/3Mn_2/3Ni_1/3O₂ phase transition in the initial charge/discharge process^[19]; (c) SEM images of Na_2/3Mn_2/3Ni_1/3O₂ electrode after 50 cycles in different voltage ranges (From the left to right: pristine sample, 2.0–3.8 V, 2.0–4.1 V, 2.0–4.25 V, 2.0–4.5 V)^[20]

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圖 4 Na_x[Mn_2/3Ni_1/3]O₂材料的面內Na⁺有序排布示意圖. (a) x=2/3; (b) x=1/2; (c) x=1/3 (綠色球為Na_e位點;粉色球為Na_f位點)^[21]

Figure 4. In-plane Na-ions orderings of Na_x[Mn_2/3 Ni_1/3]O₂: (a) x=2/3; (b) x=1/2; (c) x=1/3 (green balls: Na-ions on Na_e sites; pink balls: Na-ions on Na_f sites)^[21]

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圖 5 (a) Mn³⁺的八面體構型示意圖; (b) Mn³⁺的Jahn–Teller扭曲示意圖^[23]; (c) Na_0.62Ni_1/4Mn_3/4O₂材料在1.5~4.5 V電壓區間內的原位XRD圖譜^[24]

Figure 5. (a) Schematic of Mn³⁺ octahedral configuration; (b) schematic of Jahn–Teller distortion for Mn^3+[23]; (c) in-situ XRD patterns of Na_0.62Ni_1/4Mn_3/4O₂ electrode during the charge/discharge processes in the voltage range of 1.5–4.5 V^[24]

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圖 6 (a) Mg²⁺進入Na_0.70Ni_0.40Mn_0.60O₂材料AM層起到支柱作用示意圖^[29]; (b) P2-Na_2/3Ni_1/3Mn_2/3O₂和P2-Na_2/3Ni_1/3Mn_1/3Ti_1/3O₂材料中Na_e和Na_f的能量差計算結果^[22]; (c) P2相結構中Li⁺可以在TM層與AM層之間可逆遷移示意圖; (d) Na_0.66I_yNi_zMn_1–y–zO₂ (0.60 ≤ x ≤ 0.80, 0 ≤ y ≤ 0.17, 0.20 ≤ z ≤0.33)材料的比容量與循環穩定性性能對比^[32]

Figure 6. (a) Schematic diagram of the pillar effect of Mg²⁺ for Na_0.70Ni_0.4Mn_0.60O₂ electrode^[29]; (b) calculated energy difference between the Na_e and Na_f sites for P2-Na_2/3Ni_1/3Mn_2/3O₂ and P2-Na_2/3Ni_1/3Mn_1/3Ti_1/3O₂ eletrodes^[22]; (c) reversible migration of Li⁺ between the TM and AM layers in P2 phase; (d) comparison of capacity and cycle stability of Na_0.66I_yNi_zMn_1–y–zO₂ (0.60 ≤ x ≤ 0.80, 0 ≤ y ≤ 0.17, 0.20 ≤ z ≤0.33) substituted with different inert cations^[32]

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圖 7 (a) Cu²⁺摻雜作用機制^[37]; (b) Co³⁺離子摻雜作用機制^[39]; (c) Na⁺在Na_2/3Ni_1/3Mn_2/3O₂、Na_2/3Mn_1/3Co_2/3O₂以及Na_2/3Mn_1/2Ni_1/6Co_1/3O₂材料內的分布狀態^[40]

Figure 7. (a) Mechanisms of Cu-doping^[37]; (b) mechanisms of Co-doping^[39]; (c) distribution of Na⁺ in Na_2/3Ni_1/3Mn_2/3O₂, Na_2/3Mn_1/3Co_2/3O₂, and Na_2/3Mn_1/2Ni_1/6Co_1/3O₂ electrodes^[40]

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圖 8 (a) Na_2/3Ni_1/6Mn_2/3Cu_1/9Mg_1/18O₂在5C電流密度下的長循環穩定性^[41]; (b) [Na_0.67Zn_0.05]Ni_0.18Cu_0.1Mn_0.67O₂材料的在[–220]方向的ABF-STEM圖; (c) [Na_0.67Zn_0.05]Ni_0.18Cu_0.1Mn_0.67O₂材料在10 C的電流密度下的長循環穩定性^[42]; (d) P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂材料在2.0～4.3 V的電壓區間內不同循環圈數的放電dQ/dV曲線; (e) P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂材料在2.0～4.0 V的電壓區間內不同循環圈數的放電dQ/dV曲線; (f) P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂材料在2.0～4.3 V的電壓區間內循環1周、10周、20周、30周以及50周后Mn的K邊吸收光譜^[43]

Figure 8. (a) Long-term cycling stability of Na_2/3Ni_1/6Mn_2/3Cu_1/9Mg_1/18O₂ electrode at 5C^[41]; (b) ABF-STEM image of [Na_0.67Zn_0.05]Ni_0.18Cu_0.1Mn_0.67O₂ electrode viewed from [–220] axis; (c) long-term cycling stability of [Na_0.67Zn_0.05]Ni_0.18Cu_0.1Mn_0.67O₂ electrode at 10C^[42]; (d) discharge dQ/dV curves within 2.0–4.3 V for P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂ electrode; (e) discharge dQ/dV curves within 2.0–4.0 V for P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂ electrode; (f) Mn K-edge XAS results collected at the 2 V discharged state after the 1st, 10th, 20th, 30th, and 50th cycles within 2.0–4.3 V for P2-Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂ electrode^[43]

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圖 9 (a)多組分摻雜電極作用機制;(b)CuMgTi-571在10C的電流密度下的長循環穩定性^[44]

Figure 9. (a) Functional mechanism of multicomponent-doped electrode; (b) long-term cycling stability of CuMgTi-571 at 10C^[44]

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圖 10 (a) Ca²⁺和空位摻雜的Na_0.66Ni_0.33Mn_0.67O₂電極晶體結構示意圖; (b) P2-Na_0.76Ca_0.05[Ni_0.23□_0.08Mn_0.69]O₂正極在不同電流密度下的循環穩定性^[46]

Figure 10. (a) Schematic of the crystal structure of Ca²⁺ and vacancy co-doped Na_0.66Ni_0.33Mn_0.67O₂ electrode; (b) cycling stability of P2-Na_0.76Ca_0.05[Ni_0.23□_0.08Mn_0.69]O₂ cathode at different current densities^[46]

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圖 11 (a)采用熔體–浸漬工藝在Na_2/3[Ni_1/3Mn_2/3]O₂材料表面構筑NaPO₃包覆層示意圖^[49]; (b) Na_0.66Ni_0.26Zn_0.07Mn_0.67O₂(NNZM)和Na_0.66Ni_0.26Zn_0.07Mn_0.67O₂/0.06ZnO (NNZM/0.06ZnO)電極表面CEI膜對比示意圖;(c)NNZM和NNZM/0.06ZnO在100 mA·g^–1的電流密度下的循環性能^[52]

Figure 11. (a) Schematic of melt–impregnation of NaPO₃ coating on Na_2/3[Ni_1/3Mn_2/3]O₂^[49]; (b) schematic of the CEI films formed on the Na_0.66Ni_0.26Zn_0.07Mn_0.67O₂(NNZM) and Na_0.66Ni_0.26Zn_0.07Mn_0.67O₂/0.06ZnO (NNZM/0.06ZnO) particles; (c) cycling performance of NNZM and NNZM/0.06ZnO at 100 mA·g^–1[52]

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圖 12 (a) P2-Na_2/3Ni_1/3Mn_0.57Ti_0.1O₂、(b) O3-NaNi_1/3Fe_1/3Mn_1/3O₂以及(c) P2/O3-Na_0.754Ni_0.326Mn_0.501Fe_0.098Ti_0.07O₂材料在鈉離子脫嵌過程中的晶體結構變化示意圖^[53]; (d) P2-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ,O3-Na_0.8Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ以及P2/O3-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ電極在2.0～4.05 V電壓區間內的倍率性能; (e) P2-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ,O3-Na_0.8Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ以及P2/O3-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ電極在2.0～4.05 V電壓區間內及240 mA·g^–1下的循環穩定性^[54]

Figure 12. Schematic of structural changes of (a) P2-Na_2/3Ni_1/3Mn_0.57Ti_0.1O₂, (b) O3-NaNi_1/3Fe_1/3Mn_1/3O₂ and (c) P2/O3-Na_0.754Ni_0.326Mn_0.501Fe_0.098Ti_0.07O₂ during Na (de)sodiation^[53]; (d) rate capabilities of P2-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ, O3-Na_0.8Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ and P2/O3-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ electrode tested within 2.0–4.05 V, (e) cycling performances of P2-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ, O3-Na_0.8Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ and P2/O3-Na_0.7Ni_0.2Cu_0.1Fe_0.2Mn_0.5O_2–δ electrode tested at a rate of 240 mA·g^–1 within 2.0–4.05 V^[54]

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表 1 不同元素摻雜對P2-Na_0.67[Ni, Mn]O₂材料性能提升對比

Table 1. Comparison of performance of P2-Na_0.67[Ni, Mn]O₂ materials improved by doping different elements

Materials	Initial capacity/(mA·h·g^–1)	Rate performance/ (mA·h·g^–1)	Cycle performance/(mA·h·g^–1)	References
Na_2/3Ni_1/3Mn_2/3O₂	167 (12 mA·g^–1) (2.0–4.4 V)	30 (2C)	167 (12 mA·g^–1) 30% (100 cycles)	[7]
Na_0.62Ni_1/4Mn_3/4O₂	185 (15 mA·g^–1) (1.5–4.3 V)	120(500 mA·g^–1)	185 (15 mA·g^–1) 84% (50 cycles)	[24]
Na_0.67Mn_0.67Ni_0.28Mg_0.05O₂	123 (0.1C) (2.5–4.35 V)	—	123 (0.1C) 85% (50 cycles)	[27]
Na_0.67Mg_0.05[Mn_0.60Ni_0.20Mg_0.15]O₂	130 (0.2C) (1.5–4.2 V)78 (1C) (2.5–4.2 V)	57 (25C)	78 (1C) 79% (1000 cycles)130 (0.2C) 73% (180 cycles)	[29]
Na_0.67Ni_0.23Mn_0.67Mg_0.1O₂	117 (0.1C) (2.5–4.4 V)	60 (5C)	117 (0.1C) 95.3%(50 cycles)70 (5C) 90.9% (1000 cycles)	[30]
Na_2/3Ni_1/3Mn_1/2Ti_1/6O₂	127 (12.1 mA·g^–1) (2.5–4.5 V)	90 (2C)	127 (12.1 mA·g^–1 ) 90.5% (20 cycles)	[31]
Na_2/3Ni_1/3Mn_1/3Ti_1/3O₂	90 (0.1C) (2.5–4.15 V)	70 (20C)	87 (1 C) 83.9% (500 cycles)	[22]
Na_0.80Li_0.12Ni_0.22Mn_0.66O₂	118 (0.1C) (2.0–4.4 V)	70.8 (5C)	118 (0.1C) 91% (50 cycles)	[33]
Na_0.67Mn_0.6Ni_0.2Li_0.2O₂	100 (0.1C) (2.0–4.6 V)	70 (2C)	110 (0.1C) 102% (100 cycles)	[34]
Na_0.66Ni_0.26Mn_0.67Zn_0.07O2	127 (12 mA·g^–1) (2.2–4.3 V)	—	127 (12 mA·g^–1) 93.1% (10 cycles)	[13]
Na_0.6Ni_0.22Al_0.11Mn_0.66O₂	252 (20 mA·g^–1)(1.5–4.6 V)	140 (5 C)	252 (20 mA·g^–1) 80% (50 cycles)	[32]
Na_0.67Ni_0.1Cu_0.2Mn_0.7O₂	120 (0.1C) (2.0–4.5 V)	55 (20C)	120 (0.1C) 67% (100 cycles)	[37]
Na_0.7Mn_0.7Ni_0.2Co_0.1O₂	160 (50 mA·g^–1) (1.5–4.0 V)	75 (500 mA·g^–1)	100 (1 A·g^–1) 87% (300 cycles)	[39]
Na_2/3Ni_1/6Mn_2/3Cu_1/9Mg_1/18O₂	87.9 (0.5C) (2.5–4.15 V)	60 (30C)	80 (5C) 81.4% (500 cycles)	[41]
[Na_0.67Zn_0.05]Ni_0.18Cu_0.1Mn_0.67O₂	100 (0.1C) (2.5–4.4 V)	60 (10C)	60 (10C) 80.6% (2000 cycles)	[42]
Na_0.75Ca_0.04[Li_0.1Ni_0.2Mn_0.67]O₂	130 (0.1 V) (2.0–4.3 V)	68.8 (20C)	80 (10C) 87.7% (500 cycles)	[43]
Na_0.62Mn_0.67Ni_0.23Cu_0.05Mg_0.03Ti_0.06O₂	148.2 (0.1C) (2.0–4.3 V)	80 (10C)	120 (1C) 87% (500 cycles)78.6 (10C) 75% (2000 cycles)	[44]
Na_0.7Li_0.03Mg_0.03Ni_0.27Mn_0.6Ti_0.07O₂	135 (0.1C) (2.2–4.4 V)	110 (4C)	116.8 (2C) 82% (200 cycles)	[45]
Na_0.76Ca_0.05[Ni_0.23□_0.08Mn_0.69]O₂	153.9 (0.1C) (2.0–4.3 V)	74.6 (20C)	95 (5C) 75.3% (200 cycles)	[46]

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