CN114843450A - Sodium ion battery - Google Patents
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Abstract
Description
技术领域technical field
本发明属于二次电池技术领域,具体涉及一种钠离子电池。The invention belongs to the technical field of secondary batteries, and in particular relates to a sodium ion battery.
背景技术Background technique
由于锂资源全球储量有限,造成锂离子电池成本大幅增加。而钠资源丰度较高,其材料成本更低,而且技术上可实现与锂离子电池相似的功能,因此开发高性能的钠离子电池有助于缓解新能源行业的资源问题。与锂离子电池的石墨负极不同,钠离子电池负极通常使用比较面积较大的无定形碳材料作为负极,比如硬碳,由于电极活性材料比表面积越大,电解液在电池的消耗越多,因此钠离子电池的电解液设计与锂离子电池存在较大差异。Due to the limited global reserves of lithium resources, the cost of lithium-ion batteries has increased significantly. However, the abundance of sodium resources is higher, the material cost is lower, and it can technically achieve similar functions to lithium-ion batteries. Therefore, the development of high-performance sodium-ion batteries can help alleviate the resource problems in the new energy industry. Different from the graphite negative electrode of lithium ion battery, the negative electrode of sodium ion battery usually uses amorphous carbon material with a relatively large area as the negative electrode, such as hard carbon, because the larger the specific surface area of the electrode active material, the more electrolyte is consumed in the battery, so The electrolyte design of sodium-ion batteries is quite different from that of lithium-ion batteries.
钠离子电池由于使用比表面积较大的无定形碳作为负极,在电池化成阶段消耗较多电解液,成膜较厚,导致电池内阻较高、电池容量较低。Due to the use of amorphous carbon with a large specific surface area as the negative electrode, the sodium-ion battery consumes more electrolyte during the battery formation stage, and the film is thicker, resulting in higher battery internal resistance and lower battery capacity.
发明内容SUMMARY OF THE INVENTION
基于此,本发明的目的在于提供一种钠离子电池,其具有内阻低及循环稳定性好等优点。Based on this, the purpose of the present invention is to provide a sodium-ion battery, which has the advantages of low internal resistance and good cycle stability.
为达到上述目的,本发明采用如下技术方案。In order to achieve the above object, the present invention adopts the following technical solutions.
一种钠离子电池,所述钠离子电池包含正极、负极和非水电解液;所述负极包含负极活性材料,所述负极活性材料在负极的质量分数a、负极活性材料的比表面积b、非水电解液的密度x、非水电解液的摩尔电导率y满足0.3≤a×b×x/y≤1.5。A sodium ion battery, the sodium ion battery comprises a positive electrode, a negative electrode and a non-aqueous electrolyte; the negative electrode comprises a negative electrode active material, the mass fraction a of the negative electrode active material in the negative electrode, the specific surface area b of the negative electrode active material, the non-aqueous electrode active material The density x of the aqueous electrolyte and the molar conductivity y of the non-aqueous electrolyte satisfy 0.3≤a×b×x/y≤1.5.
在一些实施例中,所述a、b、x、和y满足0.4≤a×b×x/y≤1.3。In some embodiments, the a, b, x, and y satisfy 0.4≤a×b×x/y≤1.3.
在一些实施例中,所述负极活性材料在负极的质量分数a为90%~99%。In some embodiments, the mass fraction a of the negative electrode active material in the negative electrode is 90%-99%.
在一些实施例中,所述负极活性材料的比表面积b为3~7g/m2。In some embodiments, the specific surface area b of the negative electrode active material is 3˜7 g/m 2 .
在一些实施例中,所述非水电解液的密度x为0.8~1.4g/cm3。优选地,所述非水电解液的密度x为0.9~1.3g/cm3。In some embodiments, the density x of the non-aqueous electrolyte solution is 0.8˜1.4 g/cm 3 . Preferably, the density x of the non-aqueous electrolyte solution is 0.9˜1.3 g/cm 3 .
在一些实施例中,所述非水电解液的摩尔电导率y为5~12S·cm2/mol。优选地,所述非水电解液的摩尔电导率y为6~11S·cm2/mol。In some embodiments, the molar conductivity y of the non-aqueous electrolyte is 5-12 S·cm 2 /mol. Preferably, the molar conductivity y of the non-aqueous electrolyte is 6-11 S·cm 2 /mol.
在一些实施例中,所述负极活性材料选自硬碳、软碳、石墨、石墨烯、中间相碳微球中的至少一种。In some embodiments, the negative electrode active material is selected from at least one of hard carbon, soft carbon, graphite, graphene, and mesocarbon microspheres.
在一些实施例中,所述非水电解液含有电解液盐与溶剂。In some embodiments, the non-aqueous electrolyte contains an electrolyte salt and a solvent.
在一些实施例中,所述电解液盐选自六氟磷酸钠、双三氟甲烷磺酰亚胺钠、双氟磺酰亚胺钠、高氯酸钠、三氟甲基磺酸钠和四氟硼酸钠中的至少一种。In some embodiments, the electrolyte salt is selected from the group consisting of sodium hexafluorophosphate, sodium bistrifluoromethanesulfonimide, sodium bisfluorosulfonimide, sodium perchlorate, sodium trifluoromethanesulfonate, and tetrafluoromethanesulfonate At least one of sodium fluoroborate.
在一些实施例中,所述溶剂选自C3~C5的碳酸酯、C2~C6的羧酸酯和C4~C10的醚中的至少一种。In some embodiments, the solvent is selected from at least one of C3-C5 carbonates, C2-C6 carboxylates, and C4-C10 ethers.
在一些实施例中,所述正极包含正极活性材料,所述正极活性材料选自含钠的层状氧化物、含钠的聚阴离子化合物、含钠的普鲁士蓝化合物中的至少一种。In some embodiments, the positive electrode includes a positive electrode active material selected from at least one of sodium-containing layered oxides, sodium-containing polyanionic compounds, and sodium-containing Prussian blue compounds.
与现有技术相比,本发明具有以下有益效果:Compared with the prior art, the present invention has the following beneficial effects:
本发明针对钠离子电池内阻大和电池容量低的问题,创新性地提出从负极活性材料在负极的质量分数a、负极活性材料的比表面积b、非水电解液的密度x和非水电解液的摩尔电导率y多方面综合考虑来设计钠离子电池:对于比表面积较大的碳负极,减小非水电解液密度,可降低负极单位体积吸附的非水电解液含量,减少参与成膜过程中副反应消耗的非水电解液;增加非水电解液的摩尔电导率,有利于提升成膜过程的载流子利用率,减少阴离子参与成膜,形成更薄的界面膜。并进一步通过研究发现,当所述负极活性材料在负极中的质量分数a、负极活性材料的比表面积b、非水电解液的密度x、非水电解液的摩尔电导率y满足0.3≤a×b×x/y≤1.5时,可在有效降低钠离子电池内阻的同时增加电池容量,使其具有内阻低及循环稳定性好等优点。Aiming at the problems of high internal resistance and low battery capacity of sodium ion batteries, the present invention innovatively proposes to determine the mass fraction a of the negative electrode active material in the negative electrode, the specific surface area b of the negative electrode active material, the density x of the non-aqueous electrolyte and the non-aqueous electrolyte. The molar conductivity y is considered to design the sodium-ion battery comprehensively: for the carbon negative electrode with a large specific surface area, reducing the density of the non-aqueous electrolyte can reduce the content of the non-aqueous electrolyte adsorbed per unit volume of the negative electrode, and reduce the participation in the film formation process. The non-aqueous electrolyte consumed by side reactions; increasing the molar conductivity of the non-aqueous electrolyte is beneficial to improve the carrier utilization rate of the film formation process, reduce the participation of anions in the film formation, and form a thinner interface film. Through further research, it is found that when the mass fraction a of the negative electrode active material in the negative electrode, the specific surface area b of the negative electrode active material, the density x of the non-aqueous electrolyte, and the molar conductivity y of the non-aqueous electrolyte satisfy 0.3≤a× When b×x/y≤1.5, it can effectively reduce the internal resistance of the sodium-ion battery while increasing the battery capacity, making it have the advantages of low internal resistance and good cycle stability.
具体实施方式Detailed ways
本发明下列实施例中未注明具体条件的实验方法,通常按照常规条件,或按照制造厂商所建议的条件。实施例中所用到的各种常用化学试剂,均为市售产品。The experimental methods that do not specify specific conditions in the following examples of the present invention are usually in accordance with conventional conditions, or in accordance with the conditions suggested by the manufacturer. Various common chemical reagents used in the examples are all commercially available products.
除非另有定义,本发明所使用的所有的技术和科学术语与属于本发明的技术领域的技术人员通常理解的含义相同。本发明的说明书中所使用的术语只是为了描述具体的实施例的目的,不用于限制本发明。Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terms used in the description of the present invention are only for the purpose of describing specific embodiments, and are not used to limit the present invention.
本发明的术语“包括”和“具有”以及它们任何变形,意图在于覆盖不排他的包含。例如包含了一系列步骤的过程、方法、装置、产品或设备没有限定于已列出的步骤或模块,而是可选地还包括没有列出的步骤,或可选地还包括对于这些过程、方法、产品或设备固有的其它步骤。The terms "comprising" and "having" and any variations thereof of the present invention are intended to cover a non-exclusive inclusion. For example, a process, method, apparatus, product or device comprising a series of steps is not limited to the listed steps or modules, but optionally also includes unlisted steps, or optionally also includes steps for these processes, other steps inherent in the method, product or device.
在本发明中提及的“多个”是指两个或两个以上。“和/或”,描述关联对象的关联关系,表示可以存在三种关系,例如,A和/或B,可以表示:单独存在A,同时存在A和B,单独存在B这三种情况。字符“/”一般表示前后关联对象是一种“或”的关系。The "plurality" mentioned in the present invention means two or more. "And/or", which describes the association relationship of the associated objects, means that there can be three kinds of relationships, for example, A and/or B, which can mean that A exists alone, A and B exist at the same time, and B exists alone. The character "/" generally indicates that the associated objects are an "or" relationship.
本实施例提供了一种钠离子电池,所述钠离子电池包含正极、负极和非水电解液;所述负极包含负极活性材料,所述负极活性材料在负极的质量分数a、负极活性材料的比表面积b、非水电解液的密度x、非水电解液的摩尔电导率y满足0.3≤a×b×x/y≤1.5。This embodiment provides a sodium-ion battery, the sodium-ion battery includes a positive electrode, a negative electrode and a non-aqueous electrolyte; the negative electrode includes a negative electrode active material, the mass fraction a of the negative electrode active material in the negative electrode, the mass fraction of the negative electrode active material The specific surface area b, the density x of the non-aqueous electrolyte solution, and the molar conductivity y of the non-aqueous electrolyte solution satisfy 0.3≦a×b×x/y≦1.5.
发明人经过研究发现,当a×b×x/y值高于1.5时,负极单位体积吸附的电解液较多,电解液消耗较多;摩尔电导率较低,成膜动力学过程较慢,阴离子参与成膜较多,形成界面膜较厚,导致电池内阻较大;当a×b×x/y值低于0.3时,负极单位体积吸附的电解液过少,成膜不足,形成不稳定界面膜;电解液摩尔电导率较高,成膜动力学过程较快,阴离子参与成膜较少,形成界面膜机械强度不稳定,降低电池循环稳定性。After research, the inventor found that when the value of a×b×x/y is higher than 1.5, the negative electrode adsorbs more electrolyte per unit volume, and consumes more electrolyte; the molar conductivity is low, and the kinetic process of film formation is slow. Anions participate in the film formation more, forming a thicker interface film, resulting in a large internal resistance of the battery; when the value of a×b×x/y is lower than 0.3, the amount of electrolyte adsorbed per unit volume of the negative electrode is too small, the film formation is insufficient, and the formation of ineffective Stabilize the interface film; the molar conductivity of the electrolyte is higher, the kinetic process of film formation is faster, and the anions participate in the film formation less, the mechanical strength of the formed interface film is unstable, and the cycle stability of the battery is reduced.
在一些优选的实施例中,所述a、b、x、和y满足0.4≤a×b×x/y≤1.3。In some preferred embodiments, the a, b, x, and y satisfy 0.4≤a×b×x/y≤1.3.
具体地,所述a×b×x/y值为0.25、0.28、0.3、0.4、0.43、0.45、0.5、0.65、0.75、0.8、0.82、0.9、0.98、1、1.2、1.25、1.3、1.4、1.5、1.65、1.86。Specifically, the value of a×b×x/y is 0.25, 0.28, 0.3, 0.4, 0.43, 0.45, 0.5, 0.65, 0.75, 0.8, 0.82, 0.9, 0.98, 1, 1.2, 1.25, 1.3, 1.4, 1.5, 1.65, 1.86.
在一些实施例中,所述负极活性材料在负极的质量分数a为90%~99%。In some embodiments, the mass fraction a of the negative electrode active material in the negative electrode is 90%-99%.
在一些实施例中,所述负极活性材料的比表面积b为3~7g/m2。In some embodiments, the specific surface area b of the negative electrode active material is 3˜7 g/m 2 .
在一些实施例中,所述非水电解液的密度x为0.8~1.4g/cm3。In some embodiments, the density x of the non-aqueous electrolyte solution is 0.8˜1.4 g/cm 3 .
在一些优选的实施例中,所述非水电解液的密度x为0.9~1.3g/cm3。In some preferred embodiments, the density x of the non-aqueous electrolyte is 0.9-1.3 g/cm 3 .
在一些实施例中,所述非水电解液的摩尔电导率y为5~12S·cm2/mol。In some embodiments, the molar conductivity y of the non-aqueous electrolyte is 5-12 S·cm 2 /mol.
在一些优选的实施例中,所述非水电解液的摩尔电导率y为6~11S·cm2/mol。In some preferred embodiments, the molar conductivity y of the non-aqueous electrolyte is 6-11 S·cm 2 /mol.
在一些实施例中,所述负极活性材料选自硬碳、软碳、石墨、石墨烯、中间相碳微球中的至少一种。In some embodiments, the negative electrode active material is selected from at least one of hard carbon, soft carbon, graphite, graphene, and mesocarbon microspheres.
在一些实施例中,所述非水电解液含有电解液盐与溶剂。In some embodiments, the non-aqueous electrolyte contains an electrolyte salt and a solvent.
在一些实施例中,所述电解液盐选自六氟磷酸钠、双三氟甲烷磺酰亚胺钠、双氟磺酰亚胺钠、高氯酸钠、三氟甲基磺酸钠和四氟硼酸钠中的至少一种。In some embodiments, the electrolyte salt is selected from the group consisting of sodium hexafluorophosphate, sodium bistrifluoromethanesulfonimide, sodium bisfluorosulfonimide, sodium perchlorate, sodium trifluoromethanesulfonate, and tetrafluoromethanesulfonate At least one of sodium fluoroborate.
在一些实施例中,所述溶剂选自C3~C5的碳酸酯、C2~C6的羧酸酯和C4~C10的醚中的至少一种。In some embodiments, the solvent is selected from at least one of C3-C5 carbonates, C2-C6 carboxylates, and C4-C10 ethers.
在一些优选的实施例中,所述溶剂选自碳酸乙烯酯、碳酸丙烯酯、碳酸酯二甲酯、碳酸甲乙酯、丙酸乙酯、丙酸丙酯、γ-丁内酯、乙二醇二甲醚、乙二醇二乙醚、二乙二醇二甲醚、三乙二醇二甲醚、四乙二醇二甲醚中的至少一种。In some preferred embodiments, the solvent is selected from ethylene carbonate, propylene carbonate, dimethyl carbonate, ethyl methyl carbonate, ethyl propionate, propyl propionate, γ-butyrolactone, ethylene glycol At least one of glycol dimethyl ether, ethylene glycol diethyl ether, diethylene glycol dimethyl ether, triethylene glycol dimethyl ether, and tetraethylene glycol dimethyl ether.
在一些实施例中,所述正极包含正极活性材料,所述正极活性材料包括但不限于过渡金属氧化物、普鲁士类材料、磷酸盐、硫酸盐、钛酸盐材料中的至少一种。其中,所述过渡金属氧化物的化学式可为NazMxOy,M可选自Cr、Fe、Co、Ni、Cu、Mn、Sn、Mo、Sb、V中的至少一种,更为优选的,所述过渡金属氧化物为NaNimFenMnpO2(m+n+p=1,0≤m≤1,0≤n≤1,0≤p≤1)或NaNimConMnpO2(m+n+p=1,0≤m≤1,0≤n≤1,0≤p≤1);所述普鲁士类材料的分子式为NaxM[M′(CN)6]y·zH2O,其中M为过渡金属,M′为过渡金属,0<x≤2,0.8≤y<1,0<z≤20,更为优选的,所述普鲁士类材料为NaxMn[Fe(CN)6]y·nH2O(0<x≤2,0<y≤1,0<z≤10)或NaxFe[Fe(CN)6]y·nH2O(0<x≤2,0<y≤1,0<z≤10);所述磷酸盐的化学式为Na3(MO1- xPO4)2F1+2x,0≤x≤1,M选自Al、V、Ge、Fe、Ga中的至少一种,更为优选的,所述磷酸盐为Na3(VPO4)2F3或Na3(VOPO4)2F;所述磷酸盐的化学式为Na2MPO4F,M选自Fe、Mn中的至少一种,更为优选的,所述磷酸盐为Na2FePO4F或Na2MnPO4F;所述钛酸盐材料可选自Na2Ti3O7、Na2Ti6O13、Na4Ti5O12、Li4Ti5O12、NaTi2(PO4)3中的至少一种;所述硫酸盐的化学式为Na2M(SO4)2·2H2O,M可选自Cr、Fe、Co、Ni、Cu、Mn、Sn、Mo、Sb、V中的至少一种。In some embodiments, the positive electrode includes a positive active material including, but not limited to, at least one of transition metal oxides, Prussian-based materials, phosphates, sulfates, and titanate materials. Wherein, the chemical formula of the transition metal oxide can be Na z M x O y , M can be selected from at least one of Cr, Fe, Co, Ni, Cu, Mn, Sn, Mo, Sb, V, more Preferably, the transition metal oxide is NaNi m Fe n Mn p O 2 (m+n+p=1, 0≤m≤1, 0≤n≤1, 0≤p≤1) or NaNi m Co n Mn p O 2 (m+n+p=1, 0≤m≤1, 0≤n≤1, 0≤p≤1); the molecular formula of the Prussian material is Na x M[M'(CN) 6 ] y ·zH 2 O, wherein M is a transition metal, M' is a transition metal, 0<x≤2, 0.8≤y<1, 0<z≤20, more preferably, the Prussian material is Na x Mn[Fe(CN) 6 ] y ·nH 2 O (0<x≤2, 0<y≤1, 0<z≤10) or Na x Fe[Fe(CN) 6 ] y ·nH 2 O(0 <x≤2, 0<y≤1, 0<z≤10); the chemical formula of the phosphate is Na 3 (MO 1- x PO 4 ) 2 F 1+2x , 0≤x≤1, M is selected from At least one of Al, V, Ge, Fe, Ga, more preferably, the phosphate is Na 3 (VPO 4 ) 2 F 3 or Na 3 (VOPO 4 ) 2 F; the chemical formula of the phosphate is Na 2 MPO 4 F, M is selected from at least one of Fe and Mn, more preferably, the phosphate is Na 2 FePO 4 F or Na 2 MnPO 4 F; the titanate material can be selected from At least one of Na 2 Ti 3 O 7 , Na 2 Ti 6 O 13 , Na 4 Ti 5 O 12 , Li 4 Ti 5 O 12 , NaTi 2 (PO 4 ) 3 ; the chemical formula of the sulfate is Na 2 M(SO 4 ) 2 ·2H 2 O, M may be selected from at least one of Cr, Fe, Co, Ni, Cu, Mn, Sn, Mo, Sb, and V.
在一些实施例中,所述正极还包括有正极粘结剂和正极导电剂。In some embodiments, the positive electrode further includes a positive electrode binder and a positive electrode conductive agent.
所述正极粘结剂包括聚偏氟乙烯、偏氟乙烯的共聚物、聚四氟乙烯、偏氟乙烯-六氟丙烯的共聚物、四氟乙烯-六氟丙烯的共聚物、四氟乙烯-全氟烷基乙烯基醚的共聚物、乙烯-四氟乙烯的共聚物、偏氟乙烯-四氟乙烯的共聚物、偏氟乙烯-三氟乙烯的共聚物、偏氟乙烯-三氯乙烯的共聚物、偏氟乙烯-氟代乙烯的共聚物、偏氟乙烯-六氟丙烯-四氟乙烯的共聚物、热塑性聚酰亚胺、聚乙烯及聚丙烯等热塑性树脂;丙烯酸类树脂;以及苯乙烯丁二烯橡胶中的至少一种。The positive electrode binder includes polyvinylidene fluoride, vinylidene fluoride copolymer, polytetrafluoroethylene, vinylidene fluoride-hexafluoropropylene copolymer, tetrafluoroethylene-hexafluoropropylene copolymer, tetrafluoroethylene- Perfluoroalkyl vinyl ether copolymer, ethylene-tetrafluoroethylene copolymer, vinylidene fluoride-tetrafluoroethylene copolymer, vinylidene fluoride-trifluoroethylene copolymer, vinylidene fluoride-trichloroethylene copolymer Copolymers, vinylidene fluoride-vinyl fluoride copolymers, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene copolymers, thermoplastic polyimides, thermoplastic resins such as polyethylene and polypropylene; acrylic resins; and benzene At least one of ethylene butadiene rubber.
所述正极导电剂包括导电炭黑、导电碳球、导电石墨、导电碳纤维、碳纳米管、石墨烯或还原氧化石墨烯中的至少一种。The positive electrode conductive agent includes at least one of conductive carbon black, conductive carbon balls, conductive graphite, conductive carbon fibers, carbon nanotubes, graphene or reduced graphene oxide.
在一些实施例中,所述负极还包括有负极粘结剂和负极导电剂。所述负极粘结剂和负极导电剂可分别与所述正极粘接剂和正极导电剂相同,在此不再赘述。In some embodiments, the negative electrode further includes a negative electrode binder and a negative electrode conductive agent. The negative electrode binder and the negative electrode conductive agent may be the same as the positive electrode adhesive and the positive electrode conductive agent, respectively, and will not be repeated here.
在一些实施方式中,所述正极的制备方法为:将正极活性材料、正极粘结剂、正极导电剂和正极溶剂均匀混合,涂覆在基材上,除去正极溶剂,得到所述正极。所述正极溶剂为常规选择,例如可以是氮甲基吡咯烷基酮(NMP)。In some embodiments, the method for preparing the positive electrode is as follows: uniformly mixing the positive electrode active material, the positive electrode binder, the positive electrode conductive agent and the positive electrode solvent, coating the substrate on the substrate, and removing the positive electrode solvent to obtain the positive electrode. The cathode solvent is a conventional choice, for example, it can be nitrogen methyl pyrrolidone (NMP).
在一些实施方式中,所述负极的制备方法为:将负极活性材料、负极粘结剂、负极导电剂和负极溶剂均匀混合,涂覆在基材上,除去负极溶剂,得到所述负极。所述负极溶剂为常规选择,例如可以是纯水。In some embodiments, the preparation method of the negative electrode is as follows: the negative electrode active material, the negative electrode binder, the negative electrode conductive agent and the negative electrode solvent are uniformly mixed, coated on the substrate, and the negative electrode solvent is removed to obtain the negative electrode. The negative electrode solvent is a conventional choice, such as pure water.
在一些实施例中,所述钠离子电池中还包括有隔膜,所述隔膜位于所述正极和所述负极之间。In some embodiments, the sodium-ion battery further includes a separator, and the separator is located between the positive electrode and the negative electrode.
所述隔膜可为现有常规隔膜,可以是陶瓷隔膜、聚合物隔膜、无纺布、无机-有机复合隔膜等,包括但不限于单层PP(聚丙烯)、单层PE(聚乙烯)、双层PP/PE、双层PP/PP和三层PP/PE/PP等隔膜。The separator can be an existing conventional separator, which can be a ceramic separator, a polymer separator, a non-woven fabric, an inorganic-organic composite separator, etc., including but not limited to single-layer PP (polypropylene), single-layer PE (polyethylene), Diaphragms such as double-layer PP/PE, double-layer PP/PP and triple-layer PP/PE/PP.
在一些实施方式中,所述钠离子电池的制备方法为二次电池通用制备方法,即将正极、隔膜、负极组合,注入非水电解液,得到钠离子电池。In some embodiments, the preparation method of the sodium ion battery is a general preparation method of a secondary battery, that is, a positive electrode, a separator and a negative electrode are combined and injected into a non-aqueous electrolyte to obtain a sodium ion battery.
下面结合具体实施例进行说明。The following description will be given in conjunction with specific embodiments.
实施例1Example 1
本实施例提供一种钠离子电池,其包含正极、负极和非水电解液。This embodiment provides a sodium-ion battery, which includes a positive electrode, a negative electrode, and a non-aqueous electrolyte.
所述非水电解液制备方法如下:将碳酸乙烯酯、碳酸丙烯酯、碳酸酯二甲酯、碳酸甲乙酯按照质量比25:10:30:35配制成混合溶剂,将100g混合溶剂与14g六氟磷酸钠配制成溶液,获得密度x为1.2g/cm3、摩尔电导率y为7S·cm2/mol的溶液。The non-aqueous electrolyte preparation method is as follows: ethylene carbonate, propylene carbonate, dimethyl carbonate and ethyl methyl carbonate are prepared into a mixed solvent according to a mass ratio of 25:10:30:35, and 100 g of a mixed solvent is mixed with 14 g of a mixed solvent. Sodium hexafluorophosphate was prepared into a solution to obtain a solution with a density x of 1.2 g/cm 3 and a molar conductivity y of 7 S·cm 2 /mol.
所述负极包括负极活性材料、负极粘结剂和负极导电剂;所述负极活性材料为硬碳,硬碳在负极的质量分数a为95%,硬碳的比表面积b为6g/m2;所述负极粘结剂在负极的质量分数为3%;所述负极导电剂在负极的质量分数为2%。The negative electrode includes a negative electrode active material, a negative electrode binder and a negative electrode conductive agent; the negative electrode active material is hard carbon, the mass fraction a of the hard carbon in the negative electrode is 95%, and the specific surface area b of the hard carbon is 6 g/m 2 ; The mass fraction of the negative electrode binder in the negative electrode is 3%; the mass fraction of the negative electrode conductive agent in the negative electrode is 2%.
所述正极包括正极活性材料、正极粘结剂和正极导电剂;所述正极活性材料为NaNi1/3Fe1/3Mn1/3O2;所述正极活性材料、正极粘结剂和正极导电剂的质量比为96:2:2。The positive electrode includes a positive electrode active material, a positive electrode binder and a positive electrode conductive agent; the positive electrode active material is NaNi 1/3 Fe 1/3 Mn 1/3 O 2 ; the positive electrode active material, the positive electrode binder and the positive electrode are The mass ratio of the conductive agent is 96:2:2.
本实施例中,所述a×b×x/y值为0.98。In this embodiment, the value of a×b×x/y is 0.98.
实施例2Example 2
本实施例提供一种钠离子电池,其包含正极、负极和非水电解液。This embodiment provides a sodium-ion battery, which includes a positive electrode, a negative electrode, and a non-aqueous electrolyte.
所述非水电解液制备方法如下:将碳酸乙烯酯、碳酸丙烯酯、碳酸酯二甲酯、碳酸甲乙酯按照质量比25:10:30:35配制成混合溶剂,将100g混合溶剂与14.7g六氟磷酸钠配制成溶液,获得密度x为1.2g/cm3、摩尔电导率y为6.5S·cm2/mol的溶液。The preparation method of the non-aqueous electrolyte is as follows: ethylene carbonate, propylene carbonate, dimethyl carbonate and ethyl methyl carbonate are prepared into a mixed solvent according to a mass ratio of 25:10:30:35, and 100 g of the mixed solvent is mixed with 14.7 g sodium hexafluorophosphate was prepared into a solution to obtain a solution with a density x of 1.2 g/cm 3 and a molar conductivity y of 6.5 S·cm 2 /mol.
所述负极包括负极活性材料、负极粘结剂和负极导电剂;所述负极活性材料为硬碳,硬碳在负极的质量分数a为97%,硬碳的比表面积b为7g/m2;所述负极粘结剂在负极的质量分数为2%;所述负极导电剂在负极的质量分数为1%。The negative electrode includes a negative electrode active material, a negative electrode binder and a negative electrode conductive agent; the negative electrode active material is hard carbon, the mass fraction a of the hard carbon in the negative electrode is 97%, and the specific surface area b of the hard carbon is 7 g/m 2 ; The mass fraction of the negative electrode binder in the negative electrode is 2%; the mass fraction of the negative electrode conductive agent in the negative electrode is 1%.
所述正极同实施例1。The positive electrode is the same as that of Example 1.
本实施例中,所述a×b×x/y值为1.25。In this embodiment, the value of a×b×x/y is 1.25.
实施例3Example 3
本实施例提供一种钠离子电池,其包含正极、负极和非水电解液。This embodiment provides a sodium-ion battery, which includes a positive electrode, a negative electrode, and a non-aqueous electrolyte.
所述非水电解液制备方法如下:将碳酸乙烯酯、碳酸丙烯酯、碳酸酯二乙酯、碳酸甲乙酯按照质量比20:10:60:10配制成混合溶剂,将100g混合溶剂与9.5g六氟磷酸钠配制成溶液,获得密度x为1.1g/cm3、摩尔电导率y为9.5S·cm2/mol的溶液。The preparation method of the non-aqueous electrolyte is as follows: ethylene carbonate, propylene carbonate, diethyl carbonate and ethyl methyl carbonate are prepared into a mixed solvent in a mass ratio of 20:10:60:10, and 100 g of the mixed solvent is mixed with 9.5 g sodium hexafluorophosphate was prepared into a solution to obtain a solution with a density x of 1.1 g/cm 3 and a molar conductivity y of 9.5 S·cm 2 /mol.
所述负极包括负极活性材料、负极粘结剂和负极导电剂;所述负极活性材料为硬碳,硬碳在负极的质量分数a为93%,硬碳的比表面积b为4g/m2;所述负极粘结剂在负极的质量分数为4%;所述负极导电剂在负极的质量分数为3%。The negative electrode includes a negative electrode active material, a negative electrode binder and a negative electrode conductive agent; the negative electrode active material is hard carbon, the mass fraction a of the hard carbon in the negative electrode is 93%, and the specific surface area b of the hard carbon is 4 g/m 2 ; The mass fraction of the negative electrode binder in the negative electrode is 4%; the mass fraction of the negative electrode conductive agent in the negative electrode is 3%.
所述正极同实施例1。The positive electrode is the same as that of Example 1.
本实施例中,所述a×b×x/y值为0.43。In this embodiment, the value of a×b×x/y is 0.43.
对比例1:Comparative Example 1:
本对比例提供一种钠离子电池,其包含正极、负极和非水电解液。The present comparative example provides a sodium-ion battery comprising a positive electrode, a negative electrode and a non-aqueous electrolyte.
所述非水电解液制备方法如下:将碳酸乙烯酯、碳酸酯二甲酯、碳酸甲乙酯按照质量比80:5:15配制成混合溶剂,将100g混合溶剂与21.8g六氟磷酸钠配制成溶液,获得密度x为1.4g/cm3、摩尔电导率y为5S·cm2/mol的溶液。The preparation method of the non-aqueous electrolyte is as follows: ethylene carbonate, dimethyl carbonate and ethyl methyl carbonate are prepared into a mixed solvent according to a mass ratio of 80:5:15, and 100 g of the mixed solvent and 21.8 g of sodium hexafluorophosphate are prepared into a solution to obtain a solution with a density x of 1.4 g/cm 3 and a molar conductivity y of 5 S·cm 2 /mol.
所述负极包括负极活性材料、负极粘结剂和负极导电剂;所述负极活性材料为硬碳,硬碳在负极的质量分数a为95%,硬碳的比表面积b为7g/m2;所述负极粘结剂在负极的质量分数为3%;所述负极导电剂在负极的质量分数为2%。The negative electrode includes a negative electrode active material, a negative electrode binder and a negative electrode conductive agent; the negative electrode active material is hard carbon, the mass fraction a of the hard carbon in the negative electrode is 95%, and the specific surface area b of the hard carbon is 7 g/m 2 ; The mass fraction of the negative electrode binder in the negative electrode is 3%; the mass fraction of the negative electrode conductive agent in the negative electrode is 2%.
所述正极同实施例1。The positive electrode is the same as that of Example 1.
本对比例中a×b×x/y值为1.86。The value of a×b×x/y in this comparative example is 1.86.
对比例2:Comparative Example 2:
本对比例提供一种钠离子电池,其包含正极、负极和非水电解液。The present comparative example provides a sodium-ion battery comprising a positive electrode, a negative electrode and a non-aqueous electrolyte.
所述非水电解液制备方法如下:将碳酸丙烯酯、碳酸酯二乙酯、丙酸丙酯按照质量比10:5:85配制成混合溶剂,将100g混合溶剂与4g六氟磷酸钠配制成溶液,获得密度x为0.9g/cm3、摩尔电导率y为12S·cm2/mol的溶液。The non-aqueous electrolyte preparation method is as follows: propylene carbonate, diethyl carbonate, and propyl propionate are prepared into a mixed solvent according to a mass ratio of 10:5:85, and 100 g of a mixed solvent and 4 g of sodium hexafluorophosphate are prepared into a mixed solvent. solution to obtain a solution with a density x of 0.9 g/cm 3 and a molar conductivity y of 12 S·cm 2 /mol.
所述负极包括负极活性材料、负极粘结剂和负极导电剂;所述负极活性材料为硬碳,硬碳在负极的质量分数a为93%,硬碳的比表面积b为4g/m2;所述负极粘结剂在负极的质量分数为4%;所述负极导电剂在负极的质量分数为3%。The negative electrode includes a negative electrode active material, a negative electrode binder and a negative electrode conductive agent; the negative electrode active material is hard carbon, the mass fraction a of the hard carbon in the negative electrode is 93%, and the specific surface area b of the hard carbon is 4 g/m 2 ; The mass fraction of the negative electrode binder in the negative electrode is 4%; the mass fraction of the negative electrode conductive agent in the negative electrode is 3%.
所述正极同实施例1。The positive electrode is the same as that of Example 1.
本对比例中a×b×x/y值为0.28。The value of a×b×x/y in this comparative example is 0.28.
对实施例1~3及对比例1~2中的钠离子电池的性能进行测试:在电压范围1.50~3.95V进行循环充放电测试,记录电池内阻与循环200次的容量保持率。The performance of the sodium-ion batteries in Examples 1-3 and Comparative Examples 1-2 was tested: the cyclic charge-discharge test was performed in the voltage range of 1.50-3.95V, and the internal resistance of the battery and the capacity retention rate of 200 cycles were recorded.
结果如表1所示:The results are shown in Table 1:
表1性能测试结果Table 1 Performance test results
上述结果表明,本发明钠离子电池具有较低的内阻与较高的容量保持率,电池性能较优。The above results show that the sodium ion battery of the present invention has lower internal resistance and higher capacity retention rate, and has better battery performance.
与实施例1相比,对比例1钠离子电池使用的负极活性材料具有更高的比表面积,非水电解液密度较高、摩尔电导率较低,a×b×x/y值为1.86,大于1.50,负极单位体积吸附的电解液较多,非水电解液消耗较多;摩尔电导率较低,成膜动力学过程较慢,阴离子参与成膜较多,形成界面膜较厚,导致电池内阻较大。Compared with Example 1, the negative electrode active material used in the sodium-ion battery of Comparative Example 1 has higher specific surface area, higher density of non-aqueous electrolyte, lower molar conductivity, and a×b×x/y value of 1.86, If it is greater than 1.50, the negative electrode absorbs more electrolyte per unit volume, and consumes more non-aqueous electrolyte; the molar conductivity is low, the kinetics of film formation is slow, anions participate in film formation more, and the interface film is thicker, resulting in battery Internal resistance is large.
与实施例1相比,对比例2使用的负极活性材料具有更低的比表面积,非水电解液密度较低、摩尔电导率较高,a×b×x/y值为0.28,小于0.30,负极单位体积吸附的非水电解液过少,成膜不足,形成不稳定界面膜;非水电解液摩尔电导率较高,成膜动力学过程较快,阴离子参与成膜较少,形成界面膜机械强度不稳定,降低电池循环稳定性,电池容量保持率较低。Compared with Example 1, the negative electrode active material used in Comparative Example 2 has lower specific surface area, lower density of non-aqueous electrolyte, higher molar conductivity, a×b×x/y value of 0.28, less than 0.30, The amount of non-aqueous electrolyte adsorbed per unit volume of the negative electrode is too small, the film formation is insufficient, and an unstable interface film is formed; the molar conductivity of the non-aqueous electrolyte is higher, the kinetic process of film formation is faster, and the anions are less involved in film formation, forming an interface film. The mechanical strength is unstable, the battery cycle stability is reduced, and the battery capacity retention rate is low.
实施例2与对比例1进行比对,使用比表面积较高的负极活性材料时,降低x值,增加y值,使所述a、b、x、和y满足0.3≤a×b×x/y≤1.5,可获得更低的阻抗。Example 2 is compared with Comparative Example 1. When a negative electrode active material with a higher specific surface area is used, the value of x is decreased and the value of y is increased, so that the a, b, x, and y satisfy 0.3≤a×b×x/ y≤1.5, lower impedance can be obtained.
实施例3与对比例2进行比对,使用比表面积较低的负极活性材料时,增加x值,降低y值,使所述a、b、x、和y满足0.3≤a×b×x/y≤1.5,可获得更优的循环性能。Example 3 is compared with Comparative Example 2. When a negative electrode active material with a lower specific surface area is used, the value of x is increased and the value of y is decreased, so that the a, b, x, and y satisfy 0.3≤a×b×x/ y≤1.5, better cycle performance can be obtained.
综上所述,本发明通过优化钠离子电池负极活性材料在负极的质量分数a、负极活性材料的比表面积b、非水电解液的密度x、非水电解液的摩尔电导率y,使所述a、b、x、和y满足0.3≤a×b×x/y≤1.5,可有效提高钠离子电池循环稳定性并降低电池内阻。当a×b×x/y的值不在本发明范围内时,制备获得的钠离子电池性能明显降低。In summary, the present invention optimizes the mass fraction a of the negative electrode active material of the sodium ion battery in the negative electrode, the specific surface area b of the negative electrode active material, the density x of the non-aqueous electrolyte, and the molar conductivity y of the non-aqueous electrolyte, so that the Said a, b, x, and y satisfy 0.3≤a×b×x/y≤1.5, which can effectively improve the cycle stability of the sodium-ion battery and reduce the internal resistance of the battery. When the value of a×b×x/y is not within the scope of the present invention, the performance of the prepared sodium-ion battery is obviously reduced.
以上所述实施例的各技术特征可以进行任意的组合,为使描述简洁,未对以上实施例中的各个技术特征所有可能的组合都进行描述,然而,只要这些技术特征的组合不存在矛盾,都应当认为是本说明书记载的范围。The technical features of the above-described embodiments can be combined arbitrarily. In order to make the description concise, all possible combinations of the technical features in the above embodiments are not described. However, as long as there is no contradiction between the combinations of these technical features, All should be regarded as the scope described in this specification.
以上所述实施例仅表达了本发明的几种实施方式,其描述较为具体和详细,但并不能因此而理解为对本发明专利范围的限制。应当指出的是,对于本领域的普通技术人员来说,在不脱离本发明构思的前提下,还可以做出若干变形和改进,这些都属于本发明的保护范围。因此,本发明专利的保护范围应以所附权利要求为准。The above-mentioned embodiments only represent several embodiments of the present invention, and the descriptions thereof are specific and detailed, but should not be construed as a limitation on the scope of the patent of the present invention. It should be pointed out that for those of ordinary skill in the art, without departing from the concept of the present invention, several modifications and improvements can also be made, which all belong to the protection scope of the present invention. Therefore, the protection scope of the patent of the present invention shall be subject to the appended claims.
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WO2024046110A1 (en) * | 2022-09-02 | 2024-03-07 | 深圳新宙邦科技股份有限公司 | Sodium-ion secondary battery |
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