Mg掺杂提升钠离子电池正极材料高电压循环性能

许伟良; 党荣彬; 杨佯; 郭秋卜; 丁飞翔; 韩帅; 唐小涵; 刘渊; 左战春; 王晓琦; 杨瑞; 金旭; 容晓晖; 洪捐; 许宁; 胡勇胜

doi:10.7498/aps.72.20222098

摘要

钠离子电池层状氧化物正极材料具有高容量、易合成等优势, 表现出巨大的应用潜力. 为了开发出高容量、长循环的正极材料, 本文提出对NaNi_0.4Cu_0.1Mn_0.4Ti_0.1O₂ (NCMT)用Mg²⁺部分取代Ni²⁺的改性策略, 设计并合成了高容量、长循环的NaNi_0.35Mg_0.05Cu_0.1Mn_0.4Ti_0.1O₂ (NCMT-Mg)正极材料. 该材料在2.4—4.3 V电压范围内, 显示165 mAh·g^–1的高可逆比容量. 在0.1 C的倍率下循环350周后, 仍有111 mAh·g^–1的可逆比容量, 容量保持率为67.3%, 相较于未掺杂的原始样品提升了约13%. 本文对其进行了系统表征并揭示了其高电压循环稳定的机理, 为开发出高性能钠离子正极材料提供了重要参考.

关键词:

Abstract

Driven by global demand for new energy, Li-ion batteries (LIBs) have developed rapidly due to their competitive performance. Although LIBs show the advantages of high capacity and good cycling stability, their disadvantages such as uneven distribution of lithium resources are gradually exposed. Therefore, with abundant reserves, Na-ion batteries (NIB) have become one of the most promising solutions to make up for the deficiency of Li-ion battery. The NIBs layered oxide cathodes have the most potential applications of cathode material due to their high specific capacity (167 mAh·g^–1 in 2.4–4.3 V) and simple synthesis method. However, improving the cycling stability of layered cathode materials is one of the keys to their large-scale industrialization. To develop high capacity and cycling stability cathode materials, the Mg²⁺ is substituted for Ni²⁺ in NaNi_0.4Cu_0.1Mn_0.4Ti_0.1O₂ (NCMT), thereby obtaining a NaNi_0.35Mg_0.05Cu_0.1Mn_0.4Ti_0.1O₂ (NCMT-Mg) cathode material. The NCMT-Mg has a high reversible specific capacity of 165 mAh·g^–1 in a voltage window of 2.4–4.3 V. The reversible specific capacity of about 110 mAh·g^–1 at 0.1 C after 350 cycles with a capacity retention of 67.3% is about 13% higher than the counterpart of NCMT. The irreversible reaction is suppressed from P'3 phase to X phase for NCMT. The ex-XRD spectrometers further prove that the NCMT-Mg shows a P3 and X mixed phase after being initially charged to 4.3 V, but the NCMT shows an X phase. The irreversible phase transition is suppressed to increase the cycling stability. The inactive Mg²⁺ replaces Ni²⁺, reducing the charge compensation and stabilizing the structure, the inactive Mg²⁺ can activate the charge compensation of Ni²⁺/Cu²⁺. The electrochemical activity increases from 77% to 86%. The high capacity and excellent cycling stability prove that the NCMT-Mg structure remains intact after various current rates have been tested. The long cycling stability mechanism is further systematically studied by using various technologies. The present work will provide an important reference for developing high-performance Na-ion cathode materials.

Keywords:

作者及机构信息

1.
盐城工学院机械工程学院, 盐城　224051

2.
中国科学院物理研究所, 北京凝聚态物理国家研究中心, 北京　100190

3.
中国石油勘探开发研究院新能源研究中心, 北京　100083

通信作者: 容晓晖, rong@iphy.ac.cn ; 洪捐, jameshong@ycit.cn ; 许宁, xuning196402@163.com ;

基金项目: 国家自然科学基金(批准号: 51805466)和中国石油研究基金资助的课题.

Authors and contacts

1.
College of Mechanical Engineering, Yancheng Institute of Technology, Yancheng 224051, China

2.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

3.
Research Center of New Energy, Research Institute of Petroleum Exploration and Development (RIPED) PetroChina, Beijing 100083, China

Corresponding author: Rong Xiao-Hui, rong@iphy.ac.cn ; Hong Juan, jameshong@ycit.cn ; Xu Ning, xuning196402@163.com ;

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51805466) and the R&D Department of PetroChina.

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 样品NCMT (a)和NCMT-Mg (b)粉末材料的XRD衍射谱图. 样品NCMT (c)和NCMT-Mg (d)的SEM图以及对应于方框中颗粒表面不同元素的EDS分布图

Fig. 1. XRD diffraction patterns of NCMT (a) and NCMT-Mg powder (b). SEM images of NCMT (c) and NCMT-Mg (d) particles, with EDS images of different elements with particles marked with squares.

下载: 全尺寸图片幻灯片

图 2 (a)—(d) 材料NCMT各元素轨道(Mn 3s, C 1s, Mn 2p, Ni 2p)的XPS测试结果图; (e)—(i) 材料NCMT-Mg各元素轨道(Mn 3s, C 1s, Mn 2p, Ni 2p, Mg 1s)的XPS测试结果图

Fig. 2. The XPS spectra of (a)–(d) Mn 3s, C 1s, Mn 2p and Ni 2p of NCMT, and (e)–(i) Mn 3s, C 1s, Mn 2p, Ni 2p, Mg 1s of NCMT-Mg.

下载: 全尺寸图片幻灯片

图 3 NCMT和NCMT-Mg两种正极材料的电化学性能. 使用不同正极组装的电池NCMT (a)和NCMT-Mg (b) 的第1周, 和第10周、第50周、第100周和第350周充放电曲线((c), (d)); 在0.1 C电流倍率下两材料的循环性能((e), (f))

Fig. 3. Electrochemical performance of NCMT and NCMT-Mg based batteries. The batteries are assembled using different samples NCMT (a) and NCMT-Mg (b) initial charge and discharge curves. The batteries are assembled using different samples (c) NCMT and (d) NCMT-Mg charge and discharge curves for the, 10 th, 50 th, 100 th, and 350 th cycles. Cycling performance of the (e) NCMT and (f) NCMT-Mg at 0.1 C.

下载: 全尺寸图片幻灯片

图 4 使用NCMT (a), NCMT-Mg (b) 组装的电池在2.4—4.3 V范围内前两周循环dQ/dV曲线; 使用NCMT (c), NCMT-Mg (d) 组装的电池充电至4.3 V的非原位XRD衍射图谱

Fig. 4. dQ/dV curves of the first two cycles between 2.4 and 4.3 V of batteries assembled using different samples NCMT (a) and NCMT-Mg (b). Ex-XRD curves of the first to fifth cycles charge to 4.3 V of NCMT (c) and NCMT-Mg (d).

下载: 全尺寸图片幻灯片

图 5 两正极材料的倍率性能NCMT (a), NCMT-Mg (b); 使用不同样品NCMT (c), NCMT-Mg (d)组装的电池的第一周、第二周、第五周、第十周循环后的EIS结果

Fig. 5. Rate capability of the NCMT (a) and NCMT-Mg (b) at various current densities. EIS results after the first, second, fifth, and tenth cycles of NCMT (c) and NCMT-Mg (d).

下载: 全尺寸图片幻灯片

[1]	陆雅翔, 赵成龙, 容晓晖, 陈立泉, 胡勇胜 2018 物理学报 67 120601 Google Scholar Lu Y X, Zhao C L, Rong X H, Chen L Q, Hu Y S 2018 Acta Phys. Sin. 67 120601 Google Scholar
[2]	Li Y, Lu Y, Zhao C, Hu Y S, Titirici M M, Li H, Yong-Sheng H, Chen L 2017 Energy Storage Mater 7 130 Google Scholar
[3]	Ding F, Li J, Deng F, Xu G, Liu Y, Yang K, Kang F 2017 ACS Appl. Mater. Interfaces 9 27936 Google Scholar
[4]	Braconnier J, Delmas C, Fouassier C, Hagenmuller P 1980 Mater. Res. Bull. 15 1797 Google Scholar
[5]	Nagelberg A, Worrell W 1979 J. Solid State Chem. 29 345 Google Scholar
[6]	Whittingham M 1978 Prog Solid State Chem. 12 41 Google Scholar
[7]	Whittingham M S 1976 Science 192 1126 Google Scholar
[8]	Sun Y, Guo S, Zhou H 2019 Energy Environ. Sci. 12 825 Google Scholar
[9]	Kubota K, Kumakura S, Yoda Y, Kuroki K, Komaba S 2018 Adv. Energy Mater. 8 1703415 Google Scholar
[10]	Liu Q, Hu Z, Chen M, Zou C, Jin H, Wang S, Chou S L, Dou S X 2019 Small 15 1805381 Google Scholar
[11]	Bauer A, Song J, Vail S, Pan W, Barker J, Lu Y 2018 Adv. Energy Mater. 8 1702869 Google Scholar
[12]	Wang L, Lu Y, Liu J, Xu M, Cheng J, Zhang D, Goodenough J B 2013 Angew. Chem. Int. Ed. 52 1964 Google Scholar
[13]	Wang S, Wang L, Zhu Z, Hu Z, Zhao Q, Chen J. 2014 Angew. Chem. Int. Ed. 53 5892 Google Scholar
[14]	Wang Q, Zhao C, Lu Y, Li Y, Zheng Y, Qi Y, Rong X, Jiang L, Qi X, Shao Y, Pan D, Li B, Hu Y S, Chen L 2017 Small 13 1701835 Google Scholar
[15]	Wang Y S, Xiao R J, Hu Y S, Avdeev M, Chen L Q 2015 Nat. Commun. 6 6954 Google Scholar
[16]	Wu F, Zhao C, Chen S, Lu Y, Hou Y, Hu Y S, Maier J, Yu Y 2018 Mater. Today 21 960 Google Scholar
[17]	Xu S Y, Wu X Y, Li Y M, Hu Y S, Chen L Q 2014 Chin. Phys. B 23 118202 Google Scholar
[18]	Li Y, Yang Z, Xu S, Mu L, Gu L, Hu Y S, Li H, Chen L 2015 Adv. Sci. 2 1500031 Google Scholar
[19]	Delmas C, Fouassier C, Hagenmuller P 1980 Physica B & C 99 81
[20]	穆林沁, 戚兴国, 胡勇胜, 李泓, 陈立泉, 黄学杰. 2016 储能科学与技术 5 324 Mu L Q, Qi X G, Hu Y S, Li H, Chen L Q, Huang X J 2016 Energy Storage Sci. Technol. 5 324
[21]	Su D, Wang C, Ahn H J, Wang G 2013 Chem. Eur. J. 19 10884 Google Scholar
[22]	Caballero A, Hernan L, Morales J, Sanchez L, Pena J S, Aranda M A G 2002 J. Mater. Chem. 12 1142 Google Scholar
[23]	Rai A K, Anh L T, Gim J, Mathew V, Kim J 2014 Ceram. Int. 40 2411 Google Scholar
[24]	Xia X, Dahn J R 2012 J. Electrochem. Soc. 159 A1048 Google Scholar
[25]	Yang L, Sun S, Du K, Zhao H, Yan D, Yang H Y, Bai Y 2021 Ceram. Int. 47 28521 Google Scholar
[26]	Huang J Y, Yu T Y, Sun Y K 2018 J. Mater. Chem. A 6 16854 Google Scholar
[27]	Hong N, Wu K, Peng Z, Zhu Z, Jia G, Wang M 2020 J. Phys. Chem. C 124 22925 Google Scholar
[28]	Pang W L, Zhang X H, Guo J Z, Li J Y, Yan X, Hou B H, Wu X L 2017 J. Power Sources 356 80 Google Scholar
[29]	Lee E, Lu J, Ren Y, Luo X, Zhang X, Wen J, Johnson C S 2014 Adv. Energy Mater. 4 1400458 Google Scholar
[30]	Zheng S, Zhong G, McDonald M J, Gong Z, Liu R, Wen W, Yang Y 2016 J. Mater. Chem. A 4 9054 Google Scholar
[31]	Natasha A C, Ma M, Xiao J, et al. 2006 MRS Online Proceedings Library 972 1
[32]	Yuan D D, Wang Y X, Cao Y L, Ai X P, Yang H X 2015 ACS Appl. Mater. Interfaces 7 8585 Google Scholar
[33]	Yabuuchi N, Yano M, Yoshida H, Kuze S, Komaba S 2013 J. Electrochem. Soc. 160 A3131 Google Scholar
[34]	Zhao H, Li J, Liu W, Xu H, Gao X, Shi J, Ding X 2021 Electrochim. Acta 388 138561 Google Scholar
[35]	Kubota K, Fujitani N, Yoda Y, Kuroki K, Tokita Y, Komaba S 2021 J. Mater. Chem. A 9 12830 Google Scholar
[36]	Zhang X, Zhou Y N, Yu L, Zhang S Y, Xing X X, Wang W, Xu S 2021 Mater. Chem. Front. 5 5344 Google Scholar
[37]	Yao H R, Wang P F, Gong Y, Zhang J, Yu X, Gu L, Wan L J 2017 J. Am. Chem. Soc. 139 8440 Google Scholar
[38]	Wang Q, Mariyappan S, Vergnet J, Abakumov A M, Rousse G, Rabuel F 2019 Adv. Energy Mater. 9 1901785 Google Scholar
[39]	Zhao C, Wang Q, Yao Z, Wang J, Sánchez-Lengeling B, Ding F, Hu Y S 2020 Science 370 708
[40]	Dang R, Li N, Yang Y, Wu K, Li Q, Lee Y L, Liu X F, Hu Z B, Xiao X 2020 J. Power Sources 464 228190 Google Scholar
[41]	彭佳悦, 祖晨曦, 李泓 2013 储能科学与技术 2 55 Google Scholar Peng J Y, Zu C X, Li H 2013 Energy Storage Sci. Technol. 2 55 Google Scholar

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[20]	何济洲, 王磊, 李俊彬. 量子简并性对气体斯特林制冷循环性能的影响. 物理学报, 2005, 54(1): 24-29. doi: 10.7498/aps.54.24

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Mg掺杂提升钠离子电池正极材料高电压循环性能