TWI600203B - Composite lithium secondary battery - Google Patents
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- TWI600203B TWI600203B TW104135532A TW104135532A TWI600203B TW I600203 B TWI600203 B TW I600203B TW 104135532 A TW104135532 A TW 104135532A TW 104135532 A TW104135532 A TW 104135532A TW I600203 B TWI600203 B TW I600203B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Description
本發明係有關於一種鋰二次電池,特別是指一種正極表面設有複數區域以塗佈不同正極活性材料的複合式鋰二次電池。The present invention relates to a lithium secondary battery, and more particularly to a composite lithium secondary battery having a plurality of regions on the surface of the positive electrode to coat different positive active materials.
近年來,如攝影機、數字靜態照相機、行動電話和筆記型電腦等便攜式電子裝置被廣泛地使用,為了便於攜帶及增長使用時間,如何縮減前述電子裝置的尺寸、重量並延長其使用壽命成為必需克服的主要技術問題。因此,電池領域開發了能夠提供高能量密度的輕量型二次電池,作為用於這些便攜式電子裝置的電源,以符合前述使用要求。In recent years, portable electronic devices such as cameras, digital still cameras, mobile phones, and notebook computers have been widely used. In order to facilitate carrying and increasing the use time, how to reduce the size, weight and extend the service life of the aforementioned electronic devices has become a necessity. The main technical issues. Therefore, in the field of batteries, lightweight secondary batteries capable of providing high energy density have been developed as power sources for these portable electronic devices to meet the aforementioned usage requirements.
鋰二次電池是一種利用鋰離子的嵌入和脫嵌而達到充電和放電反應的二次電池,由於鋰二次電池能夠提供比鉛電池和鎳鎘電池更高能量密度,而被廣泛地使用。如圖1A、圖1B所示,目前鋰二次電池A的裝配是在正極片與負極片之間設置隔離膜後,卷繞成一卷芯A1,再設置於常見的圓筒型(圖1A)或方型(圖1B)電池殼體A2中。鋰二次電池中包括電解質、正極與負極;其中,前述正極係在正極集流板/片上塗佈有包括正極活性材料的正極活性材料層而構成,前述負極係在負極集流板/片上塗佈有包括負極活性材料的負極活性材料層,電解質則包括溶解有電解質鹽的溶劑。其中,正極材料及負極材料對於提高鋰二次電池電容量密度和低化影響最大,也最為關鍵。A lithium secondary battery is a secondary battery that achieves charging and discharging reactions by intercalation and deintercalation of lithium ions, and is widely used because it can provide higher energy density than lead batteries and nickel-cadmium batteries. As shown in FIG. 1A and FIG. 1B, the current lithium secondary battery A is assembled by providing a separator between the positive electrode sheet and the negative electrode sheet, and then wound into a core A1 and then placed in a common cylindrical shape (FIG. 1A). Or square (Fig. 1B) in the battery case A2. The lithium secondary battery includes an electrolyte, a positive electrode, and a negative electrode. The positive electrode is formed by coating a positive electrode active material layer including a positive electrode active material on a positive electrode current collecting plate/sheet, and the negative electrode is coated on a negative electrode current collecting plate/sheet. An anode active material layer including a negative electrode active material is disposed, and the electrolyte includes a solvent in which an electrolyte salt is dissolved. Among them, the positive electrode material and the negative electrode material have the greatest influence on improving the capacitance density and the reduction of the lithium secondary battery, and are also the most critical.
在負極材料部分,由於碳材料在嵌入和脫嵌鋰離子時晶體結構變化非常小,因此目前負極材料係廣泛採用例如石墨等碳材料,以使鋰二次電池在電池容量等特性上具有穩定的表現。在正極材料部分,常見批量應用於鋰電池的正極材料主要有鈷酸鋰(LiCoO2 )、鎳酸鋰(LiNiO2 )、錳酸鋰(LiMn2 O4 、LiMnO2 )、鈷鎳錳酸鋰(三元材料,LiNiCoMnO2 ,LNCM)、鎳鈷鋁酸鋰(三元材料,LiNix Coy Al1-x-y O2 ,LNCA)以及磷酸鐵鋰(LiFePO4 ,LFP)等鋰氧化物。In the negative electrode material portion, since the crystal structure changes very little when the carbon material is intercalated and deintercalated with lithium ions, the current negative electrode material widely uses a carbon material such as graphite to make the lithium secondary battery stable in characteristics such as battery capacity. which performed. In the positive electrode material part, the positive electrode materials commonly used in lithium batteries are lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), lithium manganate (LiMn 2 O 4 , LiMnO 2 ), lithium cobalt nickel manganese oxide. Lithium oxides such as (ternary materials, LiNiCoMnO 2 , LNCM), nickel cobalt cobalt aluminate (ternary materials, LiNi x Co y Al 1-xy O 2 , LNCA), and lithium iron phosphate (LiFePO 4 , LFP).
值得注意的是,目前正極的製備是將單一種類的正極材料塗佈於電池中所有正極集流板/片的兩側面上,然而,各種正極材料在效能的表現上各有優缺點,例如,鋰錳氧化物(LiMn2 O4 )電容量雖然較低,但熱安全性較高,適合應用在強調高功率性能及安全考量的中大型鋰電池或動力電池(High Power Battery);而磷酸鋰鐵(LiFePO4 ),相較於鋰錳氧化物(LiMn2 O4 )具有更高的熱穩定性,不會有爆炸或過熱等安全問題,適合應用在強調高功率、對電容量要求較低的動力電池或大型電池;當使用單一種類正極材料時,鋰二次電池只能在部分特性上產生較佳的效能表現,而有所不足。It is worth noting that the current positive electrode is prepared by coating a single type of positive electrode material on both sides of all positive current collecting plates/sheets in the battery. However, various positive electrode materials have advantages and disadvantages in performance performance, for example, Lithium manganese oxide (LiMn 2 O 4 ) has a low thermal capacity, but it is suitable for medium and large lithium batteries or high power batteries that emphasize high power performance and safety considerations. Iron (LiFePO 4 ) has higher thermal stability than lithium manganese oxide (LiMn 2 O 4 ) and does not have safety problems such as explosion or overheating. It is suitable for applications with high power and low capacity requirements. A power battery or a large battery; when a single type of positive electrode material is used, the lithium secondary battery can only produce better performance in some characteristics, and is insufficient.
有鑑於上述習知鋰二次電池因正極塗佈單一種類正極材料所導致的效能表現受限問題,本發明目的在於,經由將磷酸鐵鋰(LiFePO4 ,LFP)及選自含鋰三元系氧化物之不同的正極材料塗佈於同一正極表面的不同區域上,以在鋰二次電池充電、放電過程中,獲得不同正極材料之優點,達到提供一種具有高電壓、高電容量且安全性高的複合式鋰二次電池。 In view of the above-described problem that the lithium secondary battery has limited performance performance due to the application of a single type of positive electrode material to the positive electrode, the present invention aims to pass lithium iron phosphate (LiFePO 4 , LFP) and a lithium-containing ternary system. The different positive electrode materials of the oxide are coated on different regions of the same positive electrode surface to obtain the advantages of different positive electrode materials during charging and discharging of the lithium secondary battery, thereby providing a high voltage, high capacitance and safety. High composite lithium secondary battery.
緣是,為達上述目的,依據本發明所提供之一種複合式鋰二次電池,包含有至少一正極層、至少一負極層及複數隔設於該正極層及負極層之間的隔離膜,令該正極層、該負極層及該隔離膜層疊後捲繞形成該複合式鋰二次電池;該正極層包括能夠嵌入和脫嵌電極反應物的正極材料,該正極層的一側端上具有至少一正極極耳,且該正極層的兩側面上塗佈有該正極材料,定義該正極層經卷繞後位於中央之一端為一內側端,位於外側之一端為一外側端;該負極層包括能夠嵌入和脫嵌該電極反應物的負極材料,該負極層的一側端上具有至少一負極極耳,且其兩側面上塗佈有該負極材料;其中,該正極層之兩側面、上相對應地設有複數個區域及至少一空白區,該每一區域均塗佈有正極材料,該正極層兩側面上的正極材料為相對應地塗佈配置者,各該區域及其上的正極材料之間為該空白區隔開,該空白區的間隔寬幅D為大於等於0.5mm(D≧0.5mm);在該正極層的同一側面上具有至少一區域所塗佈之正極材料與其他區域所塗佈的正極材料不同,該正極材料係選自磷酸鋰鐵(LiFePO4,LFP)與含鋰三元系氧化物之組合。 In order to achieve the above object, a composite lithium secondary battery according to the present invention comprises at least one positive electrode layer, at least one negative electrode layer, and a plurality of separators interposed between the positive electrode layer and the negative electrode layer. The positive electrode layer, the negative electrode layer and the separator are laminated and wound to form the composite lithium secondary battery; the positive electrode layer includes a positive electrode material capable of intercalating and deintercalating the electrode reactant, and the positive electrode layer has one side end At least one positive electrode tab, and the positive electrode material is coated on both sides of the positive electrode layer, and the positive electrode layer is defined as an inner end at one end of the center after winding, and an outer end at one end of the outer layer; And comprising a negative electrode material capable of inserting and extracting the electrode reactant, the negative electrode layer has at least one negative electrode tab at one end thereof, and the negative electrode material is coated on both sides thereof; wherein the two sides of the positive electrode layer, Correspondingly, a plurality of regions and at least one blank region are disposed, each of which is coated with a positive electrode material, and the positive electrode materials on both sides of the positive electrode layer are correspondingly coated, each region and above The positive electrode material is separated by the blank region, and the gap width D of the blank region is 0.5 mm or more (D≧0.5 mm); at least one region coated with the positive electrode material on the same side surface of the positive electrode layer The positive electrode material coated in other regions is different, and the positive electrode material is selected from the group consisting of lithium iron phosphate (LiFePO 4 , LFP) and a lithium-containing ternary oxide.
進一步地,本發明複合式鋰二次電池中,該正極材料係橄欖石結構之磷酸鋰鐵(LFP)與選自鎳鈷鋁酸鋰(LNCA)或鈷鎳錳酸鋰(LNCM)之組合。其中,LFP+LNCA複合式鋰二次電池的工作電壓範圍可達4.5V~2.7V,電容量可達到175mAh/g以上;LFP+LNCM複合式鋰二次電池的工作電壓範圍可達4.4V~2.6V,電容量可達到185mAh/g以上。 Further, in the composite lithium secondary battery of the present invention, the positive electrode material is a combination of olivine-structured lithium iron phosphate (LFP) and lithium nickel cobalt aluminate (LNCA) or lithium cobalt nickel manganate (LNCM). Among them, the working voltage range of LFP+LNCA composite lithium secondary battery can reach 4.5V~2.7V, and the capacitance can reach 175mAh/g or more; the working voltage range of LFP+LNCM composite lithium secondary battery can reach 4.4V~ 2.6V, the capacitance can reach 185mAh / g or more.
進一步地,本發明複合式鋰二次電池中,該空白區的間隔寬幅D係小於等於5cm且大於等於0.5mm(5cm≧D≧0.5mm),以避免各區域上的塗層重疊增厚而顯響卷芯的放電效能。 Further, in the composite lithium secondary battery of the present invention, the gap width D of the blank region is less than or equal to 5 cm and greater than or equal to 0.5 mm (5 cm ≧ D ≧ 0.5 mm) to avoid overlapping and thickening of the coating on each region. It also shows the discharge performance of the core.
進一步地,本發明複合式鋰二次電池中,該負極材料係選自石墨系或焦碳系的碳材料。 Further, in the composite lithium secondary battery of the present invention, the negative electrode material is selected from a graphite-based or coke-based carbon material.
進一步地,本發明複合式鋰二次電池中,塗佈該正極層最接近外側端之區域的正極材料為磷酸鋰鐵(LFP)。 Further, in the composite lithium secondary battery of the present invention, the positive electrode material to which the region of the positive electrode layer closest to the outer end is applied is lithium iron phosphate (LFP).
進一步地,本發明複合式鋰二次電池中,定義連接該正極層之兩側端的空白區為一縱向空白區,連接該正極層之內側端與外側端的空白區為一橫向空白區,斜向連接該正極層之兩側端或內側端與外側端的空白區為一斜向空白區,令該正極層之側面上相對應地設有該縱向空白區、該橫向空白區及/或該斜向空白區而隔設出該複數個區域。 Further, in the composite lithium secondary battery of the present invention, the blank area connecting the both ends of the positive electrode layer is defined as a longitudinal blank area, and the blank area connecting the inner end and the outer end of the positive electrode layer is a horizontal blank area, obliquely a blank area connecting the two side ends or the inner side and the outer side of the positive electrode layer is an oblique blank area, such that the longitudinal blank area, the horizontal blank area and/or the oblique direction are correspondingly provided on the side surface of the positive electrode layer The blank area is separated by the plurality of areas.
有關於本發明為達成上述目的,所採用之技術、手段及其他功效,茲舉數較佳可行實施例並配合圖式詳細說明如后。 The preferred embodiments of the present invention have been described in detail with reference to the accompanying drawings.
請以圖2配合參閱圖3A至圖6C所示,說明本發明複合式鋰二次電池的實施方式。 An embodiment of the composite lithium secondary battery of the present invention will be described with reference to FIG. 3 as shown in FIG. 3A to FIG. 6C.
本發明複合式鋰二次電池的卷芯係包括至少一正極層10、至少一負極層20及複數用以隔設於該正極層10及該負極層20之間的隔離膜30,經將該正極層10、該負極層20及該隔離膜30層疊後捲繞形成卷芯,令卷芯裝入電池殼體後形成本發明的複合式鋰二次電池。於本實施例中,如圖2所示,該卷芯可以由一層正極層10、一層內部隔離膜30、一層負極層20及一層外部隔離膜30組成一電極組,也可以視電容量需求增加前述電極組。 The core of the composite lithium secondary battery of the present invention comprises at least one positive electrode layer 10, at least one negative electrode layer 20, and a plurality of separators 30 interposed between the positive electrode layer 10 and the negative electrode layer 20, The positive electrode layer 10, the negative electrode layer 20, and the separator 30 are laminated and wound to form a core, and the core is placed in a battery case to form the composite lithium secondary battery of the present invention. In this embodiment, as shown in FIG. 2, the core may be composed of a positive electrode layer 10, an inner isolation film 30, a negative electrode layer 20, and an outer isolation film 30 to form an electrode group, or may increase the capacitance requirement. The aforementioned electrode group.
如圖2所示,該正極層10具有相對二側面11、12,該二側面11、12之間具有沿長邊之相對二側端13、14以及沿短邊之相對二端,定義該二沿短邊之端,於該正極10經卷繞後位於中央之一端為一內側端15,位於外側之一端為一外側端16;其一沿長邊的側端13上具有至少一正極極耳17,該二側面11、12上設有一塗佈區,用以塗佈能夠嵌入和脫嵌例如鋰離子之電極反應物的正極材料,且該塗佈區分隔設有複數區域18及至少一空白區19,該每一區域18均塗佈有正極材料,該正極層10兩側面11、12上的正極材料為相對應地塗佈配置者,各該區域18及其上的正極材料之間為該空白區19隔開;在該正極層10的同一側面11/12上具有至少一區域18所塗佈之正極材料與其他區域18所塗佈的正極材料不同。 As shown in FIG. 2, the positive electrode layer 10 has opposite side faces 11, 12, and the opposite side ends 13 and 14 along the long side and the opposite ends along the short side are defined between the two side faces 11, 12. Along the end of the short side, after the positive electrode 10 is wound, one end of the center is an inner end 15 and one end of the outer side is an outer end 16; and a side end 13 along the long side has at least one positive electrode tab. 17. The two sides 11, 12 are provided with a coating zone for coating a positive electrode material capable of intercalating and deintercalating an electrode reactant such as lithium ions, and the coating zone is provided with a plurality of regions 18 and at least one blank. a region 19, each of which is coated with a positive electrode material, and a positive electrode material on both side faces 11 and 12 of the positive electrode layer 10 is correspondingly applied to the device, and between the region 18 and the positive electrode material thereon The blank regions 19 are spaced apart; the positive electrode material coated with at least one region 18 on the same side 11/12 of the positive electrode layer 10 is different from the positive electrode material coated by the other regions 18.
於本實施例中,該正極層10上的空白區19主要成形為長條形區域地間設於各區域18之間,用於避免正極材料塗層重疊而增加重疊處厚度,進而使電極間難以伏貼層疊,導致影響電池放電效能的問題。該空白區19的間隔寬幅D為大於等於0.5mm(D≧0.5mm),且可視所應用之鋰二次電池形態、尺寸而調整間隔寬幅D範圍為小於等於5cm且大於等於0.5mm(5cm≧D≧0.5mm),以符合實際的電池設計及使用需求。 In this embodiment, the blank region 19 on the positive electrode layer 10 is mainly formed as an elongated region between the regions 18 for avoiding overlap of the positive electrode material coating and increasing the thickness of the overlap, thereby further inter-electrode spacing. It is difficult to laminate the laminates, resulting in problems affecting the discharge performance of the battery. The gap width D of the blank region 19 is 0.5 mm or more (D ≧ 0.5 mm), and the interval width D can be adjusted to be less than or equal to 5 cm and greater than or equal to 0.5 mm depending on the shape and size of the applied lithium secondary battery. 5cm≧D≧0.5mm) to meet the actual battery design and use requirements.
本發明複合式鋰二次電池的正極材料係選自橄欖石結構之磷酸鋰鐵(LiMxPO4,以下簡稱LFP)與含鋰三元系氧化物之組合。該含鋰三元系氧化物較佳選自鎳鈷鋁酸鋰(LiNixCoyAl1-x-yO2,以下簡稱LNCA)或鈷鎳錳酸鋰(LiNiCoMnO2,以下簡稱LNCM),以形成磷酸鋰鐵與鎳鈷鋁酸鋰(LFP+LNCA)或磷酸鋰鐵與鈷鎳錳酸鋰(LFP+LNCM)之組合。 The positive electrode material of the composite lithium secondary battery of the present invention is selected from the group consisting of lithium iron phosphate (LiM x PO 4 , hereinafter abbreviated as LFP) and a lithium-containing ternary oxide. The lithium-containing ternary oxide is preferably selected from lithium nickel cobalt aluminate (LiNi x Co y Al 1-xy O 2 , hereinafter referred to as LNCA) or lithium cobalt nickel manganese oxide (LiNiCoMnO 2 , hereinafter referred to as LNCM) to form A combination of lithium iron phosphate and nickel cobalt cobalt aluminate (LFP+LNCA) or lithium iron phosphate with lithium cobalt nickel manganese oxide (LFP+LNCM).
進一步地,本發明正極層10係由正極材料塗佈於一片狀鋁基體(例如鋁箔)表面所構成者,該正極材料另可包括導電劑、粘合劑,用以將前述鋰 氧化物組成之活性物質塗佈於鋁基體表面。該粘合劑可以是樹脂粘合劑,但不限於此。 Further, the positive electrode layer 10 of the present invention is composed of a positive electrode material coated on a surface of a piece of aluminum substrate (for example, an aluminum foil), and the positive electrode material may further include a conductive agent and a binder for using the lithium as described above. The active material of the oxide composition is coated on the surface of the aluminum substrate. The adhesive may be a resin adhesive, but is not limited thereto.
該負極層20具有相對二側面21、22,該二側面21、22之間具有沿長邊之二相對側端23、24以及沿短邊之相對二端,定義該二沿短邊之端,於該負極層20經卷繞後位於中央之一端為一內側端25,位於外側之一端為一外側端26;其一沿長邊的側端23上具有至少一負極極耳27,該二側面21、22上設有一塗佈區,用以塗佈能夠嵌入和脫嵌例如鋰離子之電極反應物的負極材料。 The negative electrode layer 20 has two opposite side faces 21, 22 having opposite sides 23, 24 along the long sides and opposite ends along the short sides, defining the ends of the short sides. After the negative electrode layer 20 is wound, one end of the center is an inner end 25, and one end of the outer side is an outer end 26; and a side end 23 along the long side has at least one negative electrode tab 27, the two sides 21, 22 is provided with a coating zone for coating a negative electrode material capable of intercalating and deintercalating electrode reactants such as lithium ions.
本發明複合式鋰二次電池的負極材料可以選自石墨系或焦碳系的碳材料;進一步地,本發明負極層20係由負極材料塗佈於一片狀銅基體(例如銅箔)表面所構成者,該負極材料另可包括導電劑、粘合劑,用以將前述碳材料塗佈於鋁基體表面;該粘合劑可以是樹脂粘合劑,但不限於此。另,本發明的隔離膜30為一微孔性及多孔性之薄膜,材質可以選自PP或PE材料但不限於此,用以關閉或阻斷通道,以確實隔離正極層10及負極層20。 The negative electrode material of the composite lithium secondary battery of the present invention may be selected from a graphite or coke-based carbon material; further, the negative electrode layer 20 of the present invention is coated on the surface of a piece of copper substrate (for example, copper foil) by a negative electrode material. The anode material may further include a conductive agent and a binder for coating the carbon material on the surface of the aluminum substrate; the binder may be a resin binder, but is not limited thereto. In addition, the separator 30 of the present invention is a microporous and porous film, and the material may be selected from PP or PE materials, but is not limited thereto, for closing or blocking the channels to surely isolate the positive electrode layer 10 and the negative electrode layer 20 .
以上係本發明複合式鋰二次電池的正極層10、負極層20以及隔離膜30的結構及材料說明;以下請配合參閱圖3A至圖6C所示,逐一說明本發明正極層10之塗佈區域的具體實施例。其中,本發明分區塗佈的正極材料較佳為橄欖石結構的磷酸鐵鋰(LFP)或選自鎳鈷鋁酸鋰(LNCA)或鈷鎳錳酸鋰(LNCM)之含鋰三元系氧化物的組合;又,塗佈於本發明正極層10最接近外側端16之區域18的正極材料較佳為磷酸鐵鋰。 The above is the structure and material description of the positive electrode layer 10, the negative electrode layer 20, and the separator 30 of the composite lithium secondary battery of the present invention; the coating of the positive electrode layer 10 of the present invention will be described one by one with reference to FIGS. 3A to 6C. A specific embodiment of the area. Wherein, the partition coated positive electrode material of the present invention is preferably an olivine-structured lithium iron phosphate (LFP) or a lithium-containing ternary oxidation selected from lithium cobalt cobalt aluminate (LNCA) or lithium cobalt manganese oxide (LNCM). Further, the positive electrode material applied to the region 18 of the positive electrode layer 10 of the present invention which is closest to the outer end 16 is preferably lithium iron phosphate.
為便於解說以下塗佈實施例,定義塗佈含鋰三元系氧化物(LNCA或LNCM)者為區域18A,塗佈磷酸鐵鋰(LFP)者為區域18B。該空白區19主要成形為長條形區域而可以呈縱向設置、橫向設置或斜向設置,以將正極層10的 塗佈區分隔成複數個區域18;其中,定義如圖3A垂直連接正極層10的兩側端13、14的空白區形態為一縱向空白區19A,如圖5B垂直連接正極層10的內、外側端15、16的空白區形態為一橫向空白區19B,如圖4C傾斜連接正極層10的側端13、14的空白區形態為一斜向空白區19C。 In order to facilitate the explanation of the following coating examples, it is defined that the coating of the lithium-containing ternary oxide (LNCA or LNCM) is the region 18A, and the coating of the lithium iron phosphate (LFP) is the region 18B. The blank region 19 is mainly formed into an elongated strip region and may be disposed in a longitudinal direction, a lateral direction, or an oblique direction to sandwich the positive electrode layer 10 The coating region is divided into a plurality of regions 18; wherein, the blank region defined as the side ends 13 and 14 of the positive electrode layer 10 vertically connected to each other as shown in FIG. 3A is defined as a longitudinal blank region 19A, which is vertically connected to the positive electrode layer 10 as shown in FIG. 5B. The blank area of the outer ends 15, 16 is in the form of a lateral blank area 19B, and the blank area of the side ends 13, 14 obliquely connected to the positive electrode layer 10 as shown in Fig. 4C is an oblique blank area 19C.
需被理解的是,前述「垂直」是指包括接近垂直或完全垂直的狀態;「垂直連接」、「連接」是指包括空白區延伸後呈連接的情況,如圖6A;前述用語僅用於解釋空白區的設置狀態,但空白區的設置形態並不以此為限。此外,本發明實施例圖式所繪製的正極層10尺寸、厚度係用於標示及便於解釋塗佈形態之簡圖,圖式所繪製的層結構尺寸及厚度不應該被用於解釋或限制本案的技術。 It should be understood that the above-mentioned "vertical" refers to a state of being nearly vertical or completely vertical; "vertical connection" and "connection" refer to a case where a blank area is extended and connected, as shown in FIG. 6A; the foregoing term is only used for Explain the setting status of the blank area, but the setting form of the blank area is not limited to this. In addition, the size and thickness of the positive electrode layer 10 drawn by the embodiment of the present invention are used to indicate and facilitate the explanation of the coating form. The layer structure size and thickness drawn by the drawing should not be used to explain or limit the case. Technology.
實施例一:Embodiment 1:
如圖3A、圖3B所示,顯示正極層10的塗佈區由內側端15朝向外側端16依序設有一區域18A、一縱向空白區19A及一區域18B,該二區域依序設有含鋰三元系氧化物及磷酸鐵鋰,且正極層10的兩側面11、12設有位置及正極材料相對應的區域18A、縱向空白區19A及區域18B。於本實施例中,該區域18A與該區域18B所佔面積比例可以在兩側面11、12位置對應的前提下,視電池設計需求進行調整面積比例,或者,也可以透過在兩側面11、12上相對應的區域18中可以塗佈相同或不同的正極材料達到調整面積比例之目的。 As shown in FIG. 3A and FIG. 3B, the coating region of the positive electrode layer 10 is sequentially provided with an area 18A, a longitudinal blank area 19A and an area 18B from the inner end 15 toward the outer end 16, and the two areas are sequentially provided. A lithium ternary oxide and lithium iron phosphate are provided, and the side faces 11 and 12 of the positive electrode layer 10 are provided with a region 18A corresponding to the position of the positive electrode material, a longitudinal blank region 19A, and a region 18B. In this embodiment, the ratio of the area occupied by the area 18A and the area 18B may be adjusted according to the battery design requirements on the premise that the positions of the two sides 11 and 12 correspond to each other, or may be transmitted through the two sides 11 and 12 The same or different positive electrode materials may be coated in the corresponding regions 18 for the purpose of adjusting the area ratio.
藉此,透過前述塗佈區域及正極材料之配置,令本發明複合式鋰二次電池於初始的放電電壓表現出含鋰三元系氧化物的特性,即具有較高的工作電壓,並在放電後期同時表現出含鋰三元系氧化物及磷酸鐵鋰的特性,即具有較高的電容量、安全性以及耐深度放電,達到提供一種兼具磷酸鐵鋰與含鋰三元系氧化物優點的鋰二次電池。Thereby, the composite lithium secondary battery of the present invention exhibits the characteristics of the lithium-containing ternary oxide at the initial discharge voltage through the arrangement of the coating region and the positive electrode material, that is, has a high operating voltage, and In the later stage of discharge, it also exhibits the characteristics of lithium-containing ternary oxides and lithium iron phosphate, which have high capacitance, safety and deep discharge resistance, and provide a combination of lithium iron phosphate and lithium-containing ternary oxides. Advantages of lithium secondary batteries.
實施例二 : Embodiment 2 :
如圖4A、圖4B所示,顯示正極層10的側面11、12上由內側端15朝向外側端16依序設有二縱向空白區19A以及為其隔開的三個塗佈區域,並在正極層10的側面11及側面12上的相對應的區域設置不對應的正極材料。如圖4B,側面11上依序設有一區域18B、一區域18A及一區域18B,即該三區域依序設有磷酸鐵鋰、含鋰三元系氧化物及磷酸鐵鋰,而側面12上則依序設有一區域18A、一區域18B及一區域18A,即該三區域依序設有含鋰三元系氧化物、磷酸鐵鋰及含鋰三元系氧化物。於本實施例中,該三區域所佔面積比例可以視電池的設計需求進行調整,且正極材料的塗佈位置亦可視需求調整。As shown in FIG. 4A and FIG. 4B, the side faces 11, 12 of the positive electrode layer 10 are sequentially provided with two longitudinal blank regions 19A from the inner end 15 toward the outer end 16, and three coated regions separated therefrom, and A corresponding region on the side surface 11 and the side surface 12 of the positive electrode layer 10 is provided with a non-corresponding positive electrode material. As shown in FIG. 4B, a side region 18B, a region 18A and a region 18B are sequentially disposed on the side surface 11, that is, the three regions are sequentially provided with lithium iron phosphate, lithium-containing ternary oxide and lithium iron phosphate, and the side 12 is A region 18A, a region 18B and a region 18A are sequentially disposed, that is, the three regions are sequentially provided with a lithium-containing ternary oxide, lithium iron phosphate and a lithium-containing ternary oxide. In this embodiment, the proportion of the area occupied by the three regions can be adjusted according to the design requirements of the battery, and the coating position of the positive electrode material can also be adjusted according to requirements.
如圖4C所示,顯示將圖4A的縱向空白區19A改變為斜向空白區19C的形態。該斜向空白區19C的設置並不限於此,亦可以視實際需求呈連接正極層10之內、外側端15、16的態樣。As shown in Fig. 4C, the form in which the vertical blank area 19A of Fig. 4A is changed to the oblique blank area 19C is shown. The arrangement of the oblique blank area 19C is not limited thereto, and the inner and outer ends 15 and 16 of the positive electrode layer 10 may be connected according to actual needs.
實施例三 : Embodiment 3 :
如圖5A、圖5B所示,顯示正極層10的側面11、12上設有一橫向空白區19B以及為其隔開的二個塗佈區域,並在正極層10的側面11及側面12上的相對應區域設置部分不對應的正極材料。如圖5B,側面11上由側端13朝向側端14依序設有一區域18A及一區域18B,即該二區域依序設有含鋰三元系氧化物及磷酸鐵鋰,而側面12上則依序設有一區域18B及一區域18B,即該二區域皆設置了磷酸鐵鋰。於本實施例中,該二區域所佔面積比例可以視電池的設計需求進行調整,且正極材料的塗佈位置亦可視需求調整。其中,由於側面12上的二個區域的正極材料相同,因此可視狀況消除側面12上的橫向空白區19B,以簡化塗佈工序。As shown in FIG. 5A and FIG. 5B, the side surfaces 11 and 12 of the positive electrode layer 10 are provided with a lateral blanking region 19B and two coating regions spaced apart therefrom, and are disposed on the side surface 11 and the side surface 12 of the positive electrode layer 10. The corresponding region does not correspond to the positive electrode material. As shown in FIG. 5B, a region 18A and a region 18B are sequentially disposed from the side end 13 toward the side end 14 on the side surface 11, that is, the two regions are sequentially provided with a lithium-containing ternary oxide and lithium iron phosphate, and the side 12 is provided. A region 18B and a region 18B are sequentially disposed, that is, lithium phosphate is disposed in the two regions. In this embodiment, the proportion of the area occupied by the two regions can be adjusted according to the design requirements of the battery, and the coating position of the positive electrode material can also be adjusted according to requirements. Wherein, since the positive electrode materials of the two regions on the side surface 12 are the same, the lateral blank region 19B on the side surface 12 can be eliminated in a visual manner to simplify the coating process.
實施例四 : Embodiment 4 :
如圖6A、圖6B、圖6C所示,顯示正極層10的側面11、12上設有一橫向空白區19B、連接於該橫向空白區19B及側端14之間的二縱向空白區19A,而將塗佈區隔開成一上三下排列形態的四個塗佈區域,並在正極層10的側面11及側面12上的相對應區域設置部分不對應的正極材料。如圖6B、圖6C,側面11上鄰近正極極耳17處設有一區域18A,其下的三個區域由內而外設有一區域18B、區域18A及一區域18B,而側面12上鄰近正極極耳17處設有一區域18A,其下的三個區域由內而外設有一區域18A、一區域18B及一區域18A。於本實施例中,該四區域所佔面積比例可以視電池的設計需求進行調整,且正極材料的塗佈位置亦可視需求調整。As shown in FIG. 6A, FIG. 6B, and FIG. 6C, the side surfaces 11, 12 of the positive electrode layer 10 are provided with a lateral blank area 19B, and two longitudinal blank areas 19A connected between the lateral blank area 19B and the side end 14, and The coating zone is divided into four coating regions in a top three-down arrangement, and a portion of the positive electrode material that does not correspond to the corresponding region on the side surface 11 and the side surface 12 of the positive electrode layer 10 is provided. As shown in FIG. 6B and FIG. 6C, a region 18A is disposed on the side surface 11 adjacent to the positive electrode tab 17, and the lower three regions are surrounded by a region 18B, a region 18A and a region 18B, and the side surface 12 is adjacent to the positive electrode. An area 18A is provided at the ear 17, and the lower three areas are surrounded by an area 18A, an area 18B and an area 18A. In this embodiment, the proportion of the area occupied by the four regions can be adjusted according to the design requirements of the battery, and the coating position of the positive electrode material can also be adjusted according to requirements.
應被理解的是,本發明所提出之正極材料塗佈形態並不限於前述,是可依據實際狀況進行調整,只要塗佈區域及正極材料之配置能夠達到提升鋰二次電池工作效能之塗佈形態,皆屬於本發明之範疇。It should be understood that the coating form of the positive electrode material proposed by the present invention is not limited to the foregoing, and may be adjusted according to actual conditions, as long as the configuration of the coating region and the positive electrode material can achieve coating for improving the working efficiency of the lithium secondary battery. Forms are all within the scope of the invention.
請配合參閱圖7、圖8,顯示本發明複合式鋰二次電池與其他正極塗佈單一正極材料之鋰二次電池的特性曲線。Please refer to FIG. 7 and FIG. 8 to show the characteristic curves of the lithium secondary battery of the composite lithium secondary battery of the present invention and other positive electrode coated single positive electrode materials.
如圖7的LNCA曲線及圖8的LNCM曲線,依序顯示鎳鈷鋁酸鋰及鈷鎳錳酸鋰兩種三元系正極材料的放電特性。其中,三元系正極材料具有高工作電壓以及高能量密度的優點,其工作電壓範圍約為3.2V~4.5V(常態約為3.7),電容量則約為175~190 mAh/g;然而,三元系正極材料的放電截止電壓較高,約在3V~2.7V,當過度放電時(電壓小於3.0V時放電),過量嵌入的鋰離子會永久固定於晶格中,無法再釋放,因而導致電池壽命縮短,存在無法深度放電的缺點。As shown in the LNCA curve of FIG. 7 and the LNCM curve of FIG. 8, the discharge characteristics of the two ternary positive electrode materials of nickel cobalt aluminum aluminate and lithium cobalt nickel manganate are sequentially shown. Among them, the ternary cathode material has the advantages of high working voltage and high energy density, and its working voltage range is about 3.2V~4.5V (normal state is about 3.7), and the capacitance is about 175~190 mAh/g; however, The discharge cut-off voltage of the ternary positive electrode material is relatively high, about 3V~2.7V. When over-discharged (discharge when the voltage is less than 3.0V), the excessively embedded lithium ions are permanently fixed in the crystal lattice and cannot be released any more. This leads to a shortened battery life and the disadvantage of not being able to discharge deeply.
如圖7、圖8的LFP曲線,顯示的是磷酸鐵鋰正極材料的放電特性。其中,磷酸鐵鋰在工作電壓及能量密度的表現皆不如前述的三元系正極材料,其工作電壓範圍約為2.5V~3.8V(常態約為3.2),電容量則約為130~150 mAh/g;然而,磷酸鐵鋰的放電截止電壓明顯較三元系正極材料為低,可達到2V,而具有耐深度放電,且過度放電後立即充電即可恢復的優勢。As shown in the LFP curves of Figs. 7 and 8, the discharge characteristics of the lithium iron phosphate positive electrode material are shown. Among them, lithium iron phosphate does not perform as well as the above-mentioned ternary cathode material, and its working voltage range is about 2.5V~3.8V (normally about 3.2), and the capacitance is about 130~150 mAh. /g; However, the discharge cut-off voltage of lithium iron phosphate is significantly lower than that of the ternary cathode material, which can reach 2V, and has the advantage of being resistant to deep discharge and being charged immediately after overdischarge.
是以,本發明通過將磷酸鐵鋰與鎳鈷鋁酸鋰之組合(圖7的曲線LFP+LNCA)、磷酸鐵鋰與鈷鎳錳酸鋰之組合(圖8的曲線LFP+LNCM)的不同正極材料塗佈於同一正極表面的不同區域上,從而形成複合式鋰二次電池,並於實測前述正極材料組合後,測得如圖7的LFP+LNCA曲線以及如圖8的LFP+LNCM曲線,分別用以表示LFP+LNCM複合式鋰二次電池以及LFP+LNCA複合式鋰二次電池的放電特性。Therefore, the present invention differs in the combination of the combination of lithium iron phosphate and lithium nickel cobalt aluminate (curve LFP+LNCA of FIG. 7), lithium iron phosphate and lithium cobalt nickel manganate (curve LFP+LNCM of FIG. 8). The positive electrode material is coated on different regions of the same positive electrode surface to form a composite lithium secondary battery, and after the combination of the foregoing positive electrode materials is measured, the LFP+LNCA curve as shown in FIG. 7 and the LFP+LNCM curve as shown in FIG. 8 are measured. They are used to indicate the discharge characteristics of the LFP+LNCM hybrid lithium secondary battery and the LFP+LNCA composite lithium secondary battery, respectively.
由圖7的LFP+LNCA曲線可知,本發明複合式鋰二次電池透過其LNCA正極材料,在放電前期的工作電壓明顯高於僅塗佈LFP的鋰二次電池,且工作電壓呈平緩下降而非瞬間降低,前期工作電壓以及電容量的表現近似LFP+LNCA曲線。在放電後期,LFP正極材料雖使本發明複合式鋰二次電池的工作電壓趨近於LFP曲線,但具有使本發明複合式鋰二次電池的放電截止電壓下探至約2.6V,已明顯低於並超出LNCA曲線的放電截止電壓範圍。由圖可知,本發明LFP+LNCA複合式鋰二次電池具有4.5V~2.7V的工作電壓範圍,大於175mAh/g的電容量,而具有高工作電壓、高電容量且耐深度放電及過度放電後立即充電即可恢復的技術功效。It can be seen from the LFP+LNCA curve of FIG. 7 that the composite lithium secondary battery of the present invention passes through its LNCA positive electrode material, and the working voltage in the pre-discharge period is significantly higher than that in the lithium secondary battery coated only with LFP, and the working voltage is gently lowered. Non-instantaneous reduction, the performance of the previous working voltage and capacitance is similar to the LFP+LNCA curve. In the late stage of discharge, the LFP cathode material makes the working voltage of the composite lithium secondary battery of the present invention approach the LFP curve, but has the discharge cut-off voltage of the composite lithium secondary battery of the present invention down to about 2.6V, which is obvious. Below and beyond the discharge cut-off voltage range of the LNCA curve. As can be seen from the figure, the LFP+LNCA composite lithium secondary battery of the present invention has an operating voltage range of 4.5V to 2.7V, a capacitance greater than 175 mAh/g, and has a high operating voltage, high capacitance, and resistance to deep discharge and overdischarge. The technical effect of recovery can be restored immediately after charging.
由圖8的LFP+LNCM曲線可知,本發明複合式鋰二次電池透過其LNCM正極材料,在放電前期的工作電壓明顯高於僅塗佈LFP的鋰二次電池,且工作電壓呈平緩下降而非瞬間降低,前期工作電壓以及電容量的表現近似LFP+LNCM曲線。在放電後期,LFP正極材料雖使本發明複合式鋰二次電池的工作電壓趨近於LFP曲線,但具有使本發明複合式鋰二次電池的放電截止電壓下探至約2.5V,已明顯低於並超出LNCM曲線的放電截止電壓範圍。由圖可知,本發明LFP+LNCM複合式鋰二次電池具有4.4V~2.6V的工作電壓範圍,大於185mAh/g的電容量,而具有高工作電壓、高電容量且耐深度放電及過度放電後立即充電即可恢復的技術功效。It can be seen from the LFP+LNCM curve of FIG. 8 that the composite lithium secondary battery of the present invention passes through its LNCM positive electrode material, and the working voltage in the pre-discharge period is significantly higher than that in the lithium secondary battery coated only with LFP, and the working voltage is gently lowered. Non-instantaneous reduction, the performance of the previous working voltage and capacitance is similar to the LFP+LNCM curve. In the late stage of discharge, the LFP positive electrode material makes the working voltage of the composite lithium secondary battery of the present invention approach the LFP curve, but has the discharge cutoff voltage of the composite lithium secondary battery of the present invention down to about 2.5V, which is obvious. Below and beyond the discharge cut-off voltage range of the LNCM curve. As can be seen from the figure, the LFP+LNCM composite lithium secondary battery of the invention has an operating voltage range of 4.4V~2.6V, a capacitance greater than 185mAh/g, and has a high working voltage, high capacitance and resistance to deep discharge and overdischarge. The technical effect of recovery can be restored immediately after charging.
綜上所述,本發明透過上述複合式鋰二次電池之說明,確實可達到上述諸項功效,誠已符合專利申請要件,爰依法提出專利申請,祈請惠予審查並早日賜准專利,實感德便。In summary, the present invention can achieve the above-mentioned various effects through the description of the above-mentioned composite lithium secondary battery, and has already met the patent application requirements, and has filed a patent application according to law, praying for review and early granting of patents. Real sense of virtue.
〔先前技術〕
A‧‧‧鋰二次電池
A1‧‧‧卷芯
A2‧‧‧電池殼體
〔本發明〕
10‧‧‧正極層
11、12‧‧‧側面
13、14‧‧‧側端
15‧‧‧內側端
16‧‧‧外側端
17‧‧‧正極極耳
18‧‧‧區域
18A‧‧‧區域
18B‧‧‧區域
18C‧‧‧區域
19‧‧‧空白區
19A‧‧‧縱向空白區
19B‧‧‧橫向空白區
19C‧‧‧斜向空白區
D‧‧‧間隔寬幅
20‧‧‧負極層
21、22‧‧‧側面
23、24‧‧‧側端
25‧‧‧內側端
26‧‧‧外側端
27‧‧‧負極極耳
28‧‧‧塗佈區
30‧‧‧隔離膜[prior art]
A‧‧‧Lithium secondary battery
A1‧‧‧core
A2‧‧‧ battery case (present invention)
10‧‧‧ positive layer
11, 12‧‧‧ side
13, 14‧‧‧ side
15‧‧‧Inside
16‧‧‧Outside
17‧‧‧ positive pole
18‧‧‧Area
18A‧‧‧Area
18B‧‧‧Area
18C‧‧‧Area
19‧‧‧Blank area
19A‧‧‧ Vertical blank area
19B‧‧‧Horizontal blank area
19C‧‧‧ oblique blank area
D‧‧‧ spaced wide
20‧‧‧negative layer
21, 22‧‧‧ side
23, 24‧‧‧ side
25‧‧‧Inside
26‧‧‧Outside
27‧‧‧Negative pole
28‧‧‧ Coating area
30‧‧‧Separator
圖1A係習知鋰二次電池的卷芯卷繞於圓筒型電池殼體之立體示意圖。 Fig. 1A is a schematic perspective view showing a winding core of a conventional lithium secondary battery wound around a cylindrical battery case.
圖1B係習知鋰二次電池的卷芯卷繞於方型電池殼體之立體示意圖。 1B is a schematic perspective view showing a winding core of a conventional lithium secondary battery wound around a square battery case.
圖2係本發明複合式鋰二次電池的卷芯在卷繞前之立體示意圖。 Fig. 2 is a perspective view showing the core of the composite lithium secondary battery of the present invention before winding.
圖3A係本發明複合式鋰二次電池的正極塗佈形態第一實施例正視示意圖。 Fig. 3A is a front elevational view showing a first embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖3B係本發明複合式鋰二次電池正極塗佈形態的第一實施例底視示意圖。 Fig. 3B is a bottom plan view showing a first embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖4A係本發明複合式鋰二次電池正極塗佈形態的第二實施例正視示意圖。 Fig. 4A is a front elevational view showing a second embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖4B係本發明複合式鋰二次電池正極塗佈形態的第二實施例底視示意圖。 Fig. 4B is a bottom view showing a second embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖4C係本發明複合式鋰二次電池正極塗佈形態的第二實施例側視示意圖。 Fig. 4C is a side elevational view showing a second embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖5A係本發明複合式鋰二次電池正極塗佈形態的第三實施例正視示意圖。 Fig. 5A is a front elevational view showing a third embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖5B係本發明複合式鋰二次電池正極塗佈形態的第三實施例側視示意圖。 Fig. 5B is a side elevational view showing a third embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖6A係本發明複合式鋰二次電池正極塗佈形態的第四實施例正視示意圖。 Fig. 6A is a front elevational view showing a fourth embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖6B係本發明複合式鋰二次電池正極塗佈形態的第四實施例側視示意圖。 Fig. 6B is a side elevational view showing a fourth embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖6C係本發明複合式鋰二次電池正極塗佈形態的第二實施例底視示意圖。 Fig. 6C is a bottom view showing a second embodiment of a positive electrode coating form of the composite lithium secondary battery of the present invention.
圖7係本發明複合式鋰二次電池(LFP+LNCA)與塗佈單一正極材料(LFP、LNCA)之電池特性曲線圖。 Fig. 7 is a graph showing the battery characteristics of the composite lithium secondary battery (LFP+LNCA) of the present invention and a single positive electrode material (LFP, LNCA).
圖8係本發明複合式鋰二次電池(LFP+LNCM)與塗佈單一正極材料(LFP、LNCM)之電池特性曲線圖。 Fig. 8 is a graph showing the battery characteristics of the composite lithium secondary battery (LFP+LNCM) of the present invention and a single positive electrode material (LFP, LNCM).
10‧‧‧正極層 10‧‧‧ positive layer
13、14‧‧‧側端 13, 14‧‧‧ side
15‧‧‧內側端 15‧‧‧Inside
16‧‧‧外側端 16‧‧‧Outside
17‧‧‧正極極耳 17‧‧‧ positive pole
18A‧‧‧區域 18A‧‧‧Area
18B‧‧‧區域 18B‧‧‧Area
19A‧‧‧縱向空白區 19A‧‧‧ Vertical blank area
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