Development status and research progress of power battery for pure electric vehicles
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摘要: 現階段, 鋰離子電池已經成為電動汽車最重要的動力源, 其發展經歷了三代技術的發展(鈷酸鋰正極為第一代, 錳酸鋰和磷酸鐵鋰為第二代, 三元技術為第三代).隨著正負極材料向著更高克容量的方向發展和安全性技術的日漸成熟、完善, 更高能量密度的電芯技術正在從實驗室走向產業化.本文從鋰離子電池產學研結合的角度, 從電池正負極材料, 電池設計和生產工藝來分析動力電池行業最新動態和科學研究的前沿成果, 并結合市場需求與政策導向來闡述動力電池的發展方向和技術路線的實現途徑.Abstract: Compared to the traditional electrochemical power source, lithium ion batteries (LIBs) have the advantages of higher energy density, longer life, and absence of any memory effect, and thus have attracted widespread research interest around the world. After Sony Inc. invented and produced the first commercial 18650 cell, many domestic and international research centers and companies have promoted the industrialization of LIBs. With the development of LIB technology, its application scope has extended from traditional consumer electronics to the new energy vehicles (NEVs) and energy storage fields. NEVs include pure electric vehicles (PEVs), hybrid electric vehicles (HEVs), and plug-in hybrid electric vehicles (PHEVs). LIBs have been the main driving force for PEVs to date, and their cathode technology development process has had three generations, i.e., the first using LiCoO2, the second using LiMn2O4 and LiFePO4, and the third generation using Li(NixCoyMn1-x-y)O2. With the development of cathode and anode materials with higher capacities and the increased reliability of LIB safety technology (including separators with higher temperature resistance, electrolytes with higher voltage resistance, and other protection methods), cells with higher energy densities and longer lives can be developed and applied in the future. These improvements will enable PEVs to travel longer distances, which is the most critical issue to customers. This paper provides a review of the development status of the power battery industry and an analysis of the direction of LIB technology with respect to the following: (1) the cathode/anode materials used, including the higher Ni content in Li(NixCoyMn1-x-y)O2, along with its structural modification, and the stability of silicon and improvements in its efficiency and cycle life; (2) the design technology, including the electrode and structure designs developed using simulation technology, theoretical modeling, and experimental methods based on Taguchi design; and (3) advances in process technology, including mixing and coating processes. Based on the above information, a clear picture of the technical direction was provided for LIBs in the PEV field.
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圖 1 不同類型電池的比功率/比能量曲線圖[1]
Figure 1. Ragone plot of different battery chemistries for electric vehicles
圖 4 動力電池發展規劃. (a) 不同國家純電動車動力電池發展規劃; (b) 我國動力電池相關技術指標規劃情況
Figure 4. Development planning for power batteries: (a) development planning in various countries; (b) development planning in China regarding critical technical indicators of power batteries
圖 6 不同正極材料電池的裝機量. (a) 市場總裝機量；(b) 2017年國內銷量前十的企業裝機量
Figure 6. LIBs installed capacities for electric vehicles using various positive materials: (a) overall installed capacity; (b) installed capacity of the top ten enterprises, based on 2017 sales
圖 11 單晶與多晶的三元材料顆粒的對比圖. (a) 單晶材料(A, a)與多晶材料(B, b)的掃描電鏡對比圖[30]；(b) 電化學和界面上的穩定性對比的示意圖[32]
Figure 11. Comparison between polycrystalline and single crystalline NCM cathodes: (a) SEM morphologies of single-crystalline (A, a) and polycrystalline (B, b) NCM cathode[30]; (b) electrochemical and interfacial stability of polycrystalline and single-crystalline cathodes[32]
圖 17 動力電池的三種封裝形狀[56]. (a) 圓柱卷繞式；(b) 軟包疊片式；(c) 方形卷繞式
Figure 17. Three package structures of power batteries: (a) cylindrical type; (b) laminated type; (c) prismatic type
圖 18 軟包疊片式電池的兩種極耳布置方式. (a) 同側布置；(b) 對側布置(單位：mm)
Figure 18. Two tab layouts of laminated power batteries: (a) the same side; (b) the opposite side (unit: mm)
圖 19 鋰離子電池生產工藝流程圖(以軟包電池為例)
Figure 19. Process flow diagram of lithium ion batteries production (pouch cell)
圖 20 活性顆粒表面導電網絡分布[67]. (a) 有無干法混料的導電劑分布示意圖；(b) 掃描電子顯微鏡下顆粒表面導電劑分布圖
Figure 20. Conductive network on the surface of active material particles[67]: (a) diagram of conductive agent coating on particles with and without dry mixing; (b) diagram of conductive agent coating on particles with dry mixing, characterized by SEM
表 1 全球動力電池企業發展現狀(數據截止2017年)
Table 1. Development status of global power battery enterprises (up to 2017)
銷量排名 動力電池企業 國家 電池銷量/(GW·h) 產品類型 能量密度/(W·h·kg-1) 主要客戶 1 寧德時代 中國 12 方型 200~250 寶馬，奔馳，大眾 2 松下 日本 10 圓柱 250~340 特斯拉 3 比亞迪 中國 7.2 方型 150~200 比亞迪 4 沃特瑪 中國 5.5 圓柱 145 奇瑞，金龍 5 LG化學 韓國 4.5 軟包 240 通用，現代，大眾 6 國軒高科 中國 3.2 方型 150~200 北汽，江鈴，長安 7 三星SDI 韓國 2.8 方型 250 寶馬 8 北京國能 中國 1.9 軟包 160~200 金龍，安凱 9 比克 中國 1.6 圓柱 220~232 眾泰，一汽，江淮 10 孚能科技 中國 1.3 軟包 220 北汽，長安 
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表 2 不同正極材料在電動汽車上的典型應用
Table 2. Application of positive materials in batteries for electric vehicles
汽車廠商 正極材料 電池供應商 電池總容量/(kW·h) 續航里程/km 特斯拉Model S NCA 松下 85.0 480 現代Kona NCM LG化學 64.0 470 寶馬i3 NCM 三星SDI 33.2 277 比亞迪e6 LFP 比亞迪 60.0 300 日產Leaf LMO+NCA AESC 24.0 160
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表 3 目前商業化負極材料性能分析及應用情況
Table 3. Performance analysis and application of commercialized anode materials
材料 克容量/(mA·h·g-1) 首次效率/% 壓實密度/(g·m-3) 工作電壓/V 循環壽命(次) 安全性 倍率性能 應用方向 天然石墨 340~370 90~93 1.6~1.85 0.2 >1000 一般 差 數碼/動力 人造石墨 310~370 90~96 1.5~1.8 0.2 >1500 良好 良好 數碼/動力 中間相碳微球 280~340 90~94 1.5~1.7 0.2 >1000 良好 優秀 動力 軟碳 250~300 80~85 1.3~1.5 ~0.5 >1000 良好 優秀 動力/儲能 硬碳 250~400 80~85 1.3~1.5 ~0.5 >1000 良好 優秀 動力/儲能 鈦酸鋰 160~170 98~99 1.8~2.3 1.55 >30000 優秀 優秀 動力/儲能 硅/氧化硅 1000~4000 60~90 0.9~1.1 0.3~0.5 < 1000 一般 一般 動力
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表 4 硅基材料制備工藝對比
Table 4. Comparison of various synthetic procedures for silicon-based materials
制備工藝 優勢 劣勢 高溫熱解法 1.工藝簡單，生產難度小
2.產品一致性較好1.顆粒不易分散，碳層包覆一致性不高
2.高溫處理過程顆粒易團聚，影響性能機械球磨法 1.可調控粒徑分布
2.生產成本較低1.需要根據硅與石墨的親和性選擇合適研磨條件
2.產生較多微晶顆粒，易引發副反應化學氣相沉積法 1.碳包覆層均勻性好
2.對材料性能提升明顯1.工藝設備投入復雜，成本高
2.需要與其他方法組合使用
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表 5 硅基材料對比
Table 5. Performance comparison of different silicon-based materials
硅基材料 優勢 劣勢 氧化硅 1、可逆容量高，體積膨脹低
2、循環和倍率性能相比硅負極較好1、首次效率低(< 80%)
2、制備工藝復雜，成本較高硅 1、克容量發揮高，首次效率更高
2、工藝成熟，原材料便宜1、體積膨脹率大，循環性能差
2、熱安全性差硅合金 1、可逆容量高，體積膨脹低
2、體積和質量能量密度較低1、工藝制備復雜，成本高
2、首次效率和循環性能有待提高
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表 6 不同商業化的圓柱型動力電池型號及極耳設計方式
Table 6. Various tab layouts of cylindrical power batteries
表 7 高比能量電池設計思路
Table 7. Design concepts of high-energy cells
電池設計 途徑 實現方法 高克容量 高鎳三元材料+硅碳材料 材料配方 高主材占比 高導電性導電劑、高黏度黏結劑 微觀電極 高電壓 單晶材料、特殊電解液 面密度 提高料區面密度 提高料區涂覆量，降低箔材面密度 孔隙率 高壓實 單晶或粒徑分布合理范圍的三元材料 構型 極片組裝和封裝方式 軟包疊片式 宏觀結構 極片總面積 單位面積/電極數量 增加電極面積、卷繞圈數或疊片數 比例 箔材、隔膜和極耳 箔材和隔膜減薄，極耳結構優化
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表 8 不同廠商的高比能量電池研究現狀
Table 8. Current research on high-energy cells by various battery manufacturers
廠商 構型 容量/(A·h) 能量密度/(W·h·kg-1) 體系 應用 松下 圓柱 4.1 242 NCA-硅碳 Model 3 比克 圓柱 2.9 220 811-石墨 云度π1、π3 CATL 方形 51 220 622-石墨 蔚來ES8 LG 軟包 56.7 212 532(4.3V)-石墨 通用
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久色视频表 9 動力電池生產企業采用的涂布技術的優缺點
Table 9. Advantages and disadvantages of coatings adopted by mainstream LIB companies
涂布技術 優點 缺點 刮刀轉移式涂布 設備成本低
維護成本很低涂布速度慢
膜厚難以控制
涂布缺陷多
黏度范圍窄涂布速度高狹縫擠壓式涂布 膜厚一致性好
黏度范圍廣
涂布缺陷少
漿料利用率高設備成本高
安裝和操作要求高
模頭維護成本高
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