高镍正极材料微裂纹诱导容量衰减的应对策略研究进展

doi:10.16085/j.issn.1000-6613.2021-2138

化工进展 ›› 2022, Vol. 41 ›› Issue (8): 4277-4287.DOI: 10.16085/j.issn.1000-6613.2021-2138

高镍正极材料微裂纹诱导容量衰减的应对策略研究进展

李想¹(), 葛武杰²(), 马先果², 彭工厂³

^1.河南科技大学化工与制药学院，河南洛阳 471000
^2.贵州理工学院化学工程学院，贵州贵阳 550003
^3.中国科学院成都有机化学有限公司，四川成都 610041

收稿日期:2021-10-18 修回日期:2021-11-16 出版日期:2022-08-25 发布日期:2022-08-22
通讯作者: 葛武杰
作者简介:李想（1990—），男，博士，讲师，研究方向为锂离子电池正负极材和光催化。E-mail：lixiang@haust.edu.cn。
基金资助:
河南省高等学校重点科研项目计划(21A150018);国家自然科学基金(21805053);贵州理工学院高层次人才科研启动项目(XJGC20190901);贵州省科技计划(黔科合基础[2019]1132号);郑州市基础与应用基础研究专项基金(ZZSZX202001)

Research progress on countermeasures for microcrack-induced capacity degradation of Ni-rich cathode materials

LI Xiang¹(), GE Wujie²(), MA Xianguo², PENG Gongchang³

^1.Chemical Engineering & Pharmaceutics School, Henan University of Science & Technology, Luoyang 471000, Henan, China
^2.School of Chemical Engineering, Guizhou Institute of Technology, Guiyang 550003, Guizhou, China
^3.Chengdu Organic Chemicals Company Limited, Chinese Academy of Sciences, Chengdu 610041, Sichuan, China

Received:2021-10-18 Revised:2021-11-16 Online:2022-08-25 Published:2022-08-22
Contact: GE Wujie

摘要/Abstract

摘要：

随着锂离子电池在电动汽车、储能等领域的广泛应用，其正极材料尤其是钴酸锂、镍钴锰酸锂及镍钴铝酸锂三元正极材料的需求量也随之剧增。然而由于钴资源稀缺，“高镍低钴化”成为近年来锂离子电池行业的重要关注点和发展方向。高镍正极材料（Ni的摩尔分数大于60%）凭借着容量高、成本低廉等优势获得了广泛的关注和研发，其产业化步伐逐渐加快。然而其仍然面临着诸多限制其大规模应用的问题，其中微裂纹的产生诱发的快速容量衰减问题被越来越多的研究证明是常规球状高镍正极材料容量衰减的首要因素。本文综述了近年来针对这一问题的几种典型应对策略的研究进展，包括填隙包覆处理、径向有序设计以及采用高镍单晶正极材料。本文对以上典型应对策略的技术手段、工艺参数和电化学性能进行了总结和归纳。最后对于进一步的研究方向进行了展望。

关键词: 再生能源, 电化学, 高镍正极材料, 稳定性, 填隙包覆, 径向有序设计, 高镍单晶正极, 微裂纹

Abstract:

With the wide application of lithium-ion batteries in the fields of electric vehicles and energy storage, the demand for cathode materials, especially lithium cobalt oxide, lithium nickel-cobalt-manganese oxide and lithium nickel-cobalt-aluminum oxide cathode materials, have increased dramatically. However, due to the scarcity of cobalt resources, “Ni-rich and Co-poor” has become an important concern and direction of development of the lithium-ion battery industry in recent years. Ni-rich cathode materials (Ni mole content higher than 60%) have attracted wide attention due to the advantages of high energy density and cost efficiency, and the pace of industrialization of the materials has accelerated over time. The conventional spherical Ni-rich cathode materials are faced with the problem of rapid capacity fading caused by microcrack formation due to anisotropic volume change. The problem is considered as the dominant factor of capacity fading of spherical Ni-rich cathode materials. In this paper, several strategies to deal with this problem in recent years are reviewed, including interstitial coating, design and synthesis of radially ordered primary particles, and the use of Ni-rich single-crystal cathode materials. These methods are analyzed, evaluated and summarized in detail, and further research direction is prospected.

Key words: renewable energy, electrochemistry, Ni-rich cathode materials, stability, interstitial coating, radially aligned design, Ni-rich single-crystal cathode materials, micro-crack

中图分类号:

李想, 葛武杰, 马先果, 彭工厂. 高镍正极材料微裂纹诱导容量衰减的应对策略研究进展[J]. 化工进展, 2022, 41(8): 4277-4287.

LI Xiang, GE Wujie, MA Xianguo, PENG Gongchang. Research progress on countermeasures for microcrack-induced capacity degradation of Ni-rich cathode materials[J]. Chemical Industry and Engineering Progress, 2022, 41(8): 4277-4287.

图/表 5

参考文献 56

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方法	解决的关键问题	优点	缺陷	技术手段	典型改性原料及工艺参数
填隙包覆	保护晶界，避免开裂后与电解液直接接触，减少阻碍锂离子传导的惰性相的形成	承袭表面包覆技术方法，较为简便，利于规模化应用	仍停留在表面，无法从根本上减弱应力应变的程度；改性物质选择范围有限，对其含量要求苛刻，使用过多会导致容量明显下降	①湿法共混-球磨-烧结； ②干法共混-球磨-烧结	①乙酸钴+乙酸锂（NCM622）^［7］，4-乙烯苯硼酸（NCA）^［8］，硝酸钴+硼氢化钠（NCM811）^［9］；②磷酸钴（NCA）^［10］，磷酸锂（ALD，LiNi_0.76Mn_0.14Co_0.1O₂）^［11］，磷酸锂（ALD，NCM811）^［12］
径向有序设计	调整各向异性应力应变方向，减弱开裂的程度	可以大幅度减弱应力应变的累积，提高电压稳定性	合成过程较为复杂，工艺难度较大	①水/溶剂热法；②控制结晶-共沉淀法；③烧结助剂法	①硝酸镍+硝酸钴+聚乙烯吡咯烷酮^［15］；②pH=11.5，NH₃/TM=1（NCA）^［16］；pH=11.2，NH₃/TM=2（NCM811）^［17］；pH=10.5，NH₃/TM=3（NCM622）^［18］③氧化硼^{［23-25， 49］}，硼酸^［50］，五氧化二钽^{［25， 51］}，三氧化钨^{［25，52］}，三氧化钼^［25］，三氧化二锑^{［25， 53］}，五氧化二铌（LiNi_0.9Co_0.1O₂）^［25］
单晶制备	进一步减弱一次颗粒之间的应力应变作用，极大减少开裂现象	可以从根本上避免球形二次颗粒内部出现应力应变累积现象，极大提高整体稳定性；同时能避免加工过程的挤压破碎	单晶颗粒内部锂离子传导距离较长，对倍率性能有较大影响；需要较长煅烧时间和较多的烧结助剂	①成品球磨-烧结；②共沉淀-助剂-烧结法；③熔盐法；④喷雾热解法	①碳酸锂，Li/TM=1.05，940℃-5h（NCM622）^［42］；氢氧化锂，Li/TM=0.98，870℃6h→Li/TM=1.08，830℃-12h（NCM811）^［54］；②偏钨酸铵+钼酸铵+氢氧化锂，Li/TM=1.05，800℃-12h （LiNi_0.92Co_0.06Mn_0.01Al_0.01O₂）^［47］；硫酸锂+氢氧化锂，Li/TM=1.5，900℃-10h（NCM622）^［45］；③硝酸盐+KCl/CsCl/LiCl，Li/TM=2~4，800~900℃，8~12h（NCM622/811）^［55］；碳酸锂，Li/TM=1.3，775℃（NCM811）^［56］；④氯化镍+氯化钴+氯化锰+氢氧化锂，Li/TM=1.05（800℃，NCM811）^［46］

方法	解决的关键问题	优点	缺陷	技术手段	典型改性原料及工艺参数
填隙包覆	保护晶界，避免开裂后与电解液直接接触，减少阻碍锂离子传导的惰性相的形成	承袭表面包覆技术方法，较为简便，利于规模化应用	仍停留在表面，无法从根本上减弱应力应变的程度；改性物质选择范围有限，对其含量要求苛刻，使用过多会导致容量明显下降	①湿法共混-球磨-烧结； ②干法共混-球磨-烧结	①乙酸钴+乙酸锂（NCM622）^［7］，4-乙烯苯硼酸（NCA）^［8］，硝酸钴+硼氢化钠（NCM811）^［9］；②磷酸钴（NCA）^［10］，磷酸锂（ALD，LiNi_0.76Mn_0.14Co_0.1O₂）^［11］，磷酸锂（ALD，NCM811）^［12］
径向有序设计	调整各向异性应力应变方向，减弱开裂的程度	可以大幅度减弱应力应变的累积，提高电压稳定性	合成过程较为复杂，工艺难度较大	①水/溶剂热法；②控制结晶-共沉淀法；③烧结助剂法	①硝酸镍+硝酸钴+聚乙烯吡咯烷酮^［15］；②pH=11.5，NH₃/TM=1（NCA）^［16］；pH=11.2，NH₃/TM=2（NCM811）^［17］；pH=10.5，NH₃/TM=3（NCM622）^［18］③氧化硼^{［23-25， 49］}，硼酸^［50］，五氧化二钽^{［25， 51］}，三氧化钨^{［25，52］}，三氧化钼^［25］，三氧化二锑^{［25， 53］}，五氧化二铌（LiNi_0.9Co_0.1O₂）^［25］
单晶制备	进一步减弱一次颗粒之间的应力应变作用，极大减少开裂现象	可以从根本上避免球形二次颗粒内部出现应力应变累积现象，极大提高整体稳定性；同时能避免加工过程的挤压破碎	单晶颗粒内部锂离子传导距离较长，对倍率性能有较大影响；需要较长煅烧时间和较多的烧结助剂	①成品球磨-烧结；②共沉淀-助剂-烧结法；③熔盐法；④喷雾热解法	①碳酸锂，Li/TM=1.05，940℃-5h（NCM622）^［42］；氢氧化锂，Li/TM=0.98，870℃6h→Li/TM=1.08，830℃-12h（NCM811）^［54］；②偏钨酸铵+钼酸铵+氢氧化锂，Li/TM=1.05，800℃-12h （LiNi_0.92Co_0.06Mn_0.01Al_0.01O₂）^［47］；硫酸锂+氢氧化锂，Li/TM=1.5，900℃-10h（NCM622）^［45］；③硝酸盐+KCl/CsCl/LiCl，Li/TM=2~4，800~900℃，8~12h（NCM622/811）^［55］；碳酸锂，Li/TM=1.3，775℃（NCM811）^［56］；④氯化镍+氯化钴+氯化锰+氢氧化锂，Li/TM=1.05（800℃，NCM811）^［46］

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高镍正极材料微裂纹诱导容量衰减的应对策略研究进展

Research progress on countermeasures for microcrack-induced capacity degradation of Ni-rich cathode materials

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