摘 要：以纳米LiFePO4锂离子电池为研究对象，在50～450 A和-18～50 ℃范围内，对其充放电特性、Peuk" />
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基于Peukert模型的车用纳米磷酸铁锂电池性能研究
2015年6期目录
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　　摘 要：以纳米LiFePO4锂离子电池为研究对象，在50～450 A和-18～50 ℃范围内，对其充放电特性、Peukert模型与温度的关系进行了讨论，利用Ragone曲线对阀控式密封铅酸动力电池、镍氢动力电池及锰酸锂离子电池的能量功率特性进行了对比分析。研究表明，该纳米LiFePO4锂离子电池的快速放电能力和能量功率特性都得到很大改善，尤其适合于高温工况；低温性能依然还是纳米LiFePO4锂离子电池的弱点，亟待进一步提高。 中国论文网 /1/view-7240869.htm　　关键词：电动汽车；锂离子电池；纳米磷酸铁锂；温度；Peukert 　　中图分类号：TM 912.9文献标文献标识码：A文献标DOI：10.3969/j.issn.15.06.05 　　Abstract：In the range of 50～450 A and -18～50℃， the paper investigated the discharge characteristics of the lithium-ion battery with nano-LiFePO4 and discussed the relation between Peukert's equation and temperature. The capacity， resistance， and efficiency of the battery were studied as well. A Ragone plot was used to analyze the relationship between energy and power of the lithium-ion battery with nano-LiFePO4， and to compare the power performance of the battery with VRLA battery， NiMH battery and LiMn2O4 lithium-ion battery. The results show that for high temperature conditions， the lithium-ion battery with nano-LiFePO4 has better power performance， including more rapid discharging and better energy and power capability. However， its low-temperature performances need to be further promoted. 　　Key words：electric vehicle； lithium-ion battery； nano-LiFePO4； temperature； Peukert 　　锂离子电池是电动汽车研究的关键技术。LiFePO4（橄榄石型磷酸铁锂）正极材料以其优良的热耐受性、环境友好性及成本低、安全性高和循环寿命长等优点，成为锂离子电池正极材料研究领域的热点。锂离子电池充放电过程是一种两相反应，即LiFePO4/FePO4两相的转化过程，充放电过程中体积的变化很小，避免了晶体结构崩塌，使LiFePO4正极具有良好的循环性能和安全性。LiFePO4晶体结构的限制导致电子电导率和锂离子扩散系数较低[1]，使动力电池的倍率特性差，大电流可用电量衰减较大，严重制约了LiFePO4材料的应用和发展，因此改善电子导电率以及锂离子扩散率成为研究的关键点。目前包覆、掺杂、纳米化是最主要的改良方法。 　　锂离子在LiFePO4正极中的嵌入和脱嵌受很多因素影响。碳包覆和体相掺杂虽然可以提高 LiFePO4材料的电子导电率，但较低的锂离子迁移速率仍然是制约目前非纳米LiFePO4材料性能的关键因素。纳米级颗粒的粒径比较小，减小了充放电过程中锂离子嵌入和脱出的路程；其次纳米颗粒较大的比表面积，使反应的活性位显著增加，提供较多扩散通道[2]，可有效提高锂离子扩散系数。此外纳米颗粒聚集起来产生的间隙，极大程度缓解了锂离子嵌入脱出产生的应力，能够提高锂离子电池材料的循环寿命[3]。 　　研究实践证明，降低LiFePO4颗粒尺寸可以提高大倍率放电能力及充放循环的稳定性[4-7]。 　　Liu H.等人[8]基于阻抗谱的理论，利用式（1）计算LiFePO4正极内锂离子扩散系数，可见温度升高对锂离子扩散有很大促进作用。 　　式中，R为气体常数；T为绝对温度，K；A为电极表面积，m2；n为每摩尔物质参与电极氧化反应的转移电子数；F为法拉第常数；C为电极中的锂离子浓度，mol/L； σ是Warburg因子。 　　在大电流或高功率的应用工况中，动力电池的温度会剧烈变化，所以温度是至关重要的影响因素。本文以温度为着眼点，在-18～50 ℃范围内，对国产纳米LiFePO4锂离子电池的充放电特性（50～450 A）、能量功率特性进行分析和特性研究。 　　1 试验 　　试验对象为国产纳米LiFePO4锂离子电池，如图1所示，标称容量为150 Ah，正极材料（纳米级磷酸铁锂材料）的颗粒中位粒径D50=70 nm。电池试验设备为美国AeroVironment公司的AV-900电池试验台，试验数据通过SmartGuard系统采集。高低温试验设备是WD4025（F）恒温箱。 　　充放电试验描述：（1）在室温下以50 A恒流充电至4.2 V，恒流转恒压充电，充电截止电流为2 A，此时电池SOC=100%。（2）电池温度标定：先将恒温箱调至设定温度并将电池放入恒温箱静置，试验温度点分别为-18 ℃，-10 ℃，0 ℃，18 ℃，35 ℃，50 ℃，对应的静置时间见表2。（3）将该锂离子电池以50 A恒流放电至截止电压2.5 V。
　　2 充放电特性及Peukert模型分析 　　Zhang[9]认为颗粒尺寸在50～400 nm 之间时，LiFePO4材料的比容量与尺寸大小并没有明显的相关性。但Gaberscek等人[10]却认为LiFePO4正极材料的比容量只取决于活性物质颗粒的平均尺寸。Padhi等人[11]针对磷酸铁锂离子电池的充放电过程提出了收缩核模型（Shrinking Core Model），他认为在放电过程中LiFePO4/FePO4界面自外向内径向移动，两相界面的面积逐渐减小，在充电过程中则相反。在恒流充放电过程中，存在着临界两相界面面积，这个临界面积是指当界面不能再承受更多的锂离子通过时的界面面积。在充放电过程中，电流越大，相应的容量损失就越大。 　　Ceder等人[12]认为LiFePO4充放电过程中的相变有可能是晶格弹性模量不匹配而导致的，当颗粒尺寸小到LiFePO4 的表面能足够大，体相弹性模量引起的晶格应力不占优势地位时，充放电过程有可能成为单相固溶充放电过程。Gibot等人[13]采用低温沉淀法制备了40 nm的LiFePO4粒子作为正极材料，他们发现该电极在充放电过程中表现出“S”形曲线，减小粒子尺寸实际上影响了材料的结构和成分，是典型的单相充放电机制（固溶机制）。 　　图2所示为该纳米型LiFePO4锂离子电池不同电流下的充放电电压曲线族，可以清晰看出不同电流对应的充放电容量及曲线形状。当放电电流在50～300 A之间时，电池温度变化不大，容量损失基本是符合收缩核模型的。但该动力电池在初始温度为50℃时进行450 A恒流放电，放电时间为19.8 min，放出电量148.14 Ah，放电结束时极柱温度升至110℃，电池壁温度升至70℃，放出电量超过100～300 A的恒流放电电量。可见由于温度的升高，提高了锂离子电导率，可用容量也随之增加。可见电池充放电特性与温度之间也有强相关性影响。但图中显示，中位粒径为70 nm的纳米铁锂电池的充放电曲线形状并不符合单相固溶机制的特征，在大部分充放电时间内呈现很明显的电压平台。 　　Andersson等人[14]利用原位穆斯堡尔谱研究了LiFePO4的充放电过程，提出了锂离子迁移模型“Radial Model”和“Mosaic Mdoel”，由于纳米级LiFePO4颗粒较小，减少了锂离子的扩散路径，提高了扩散速率，保证了大电流时的可用电量不发生衰减。Meethong等人[15]研究发现随着LiFePO4颗粒的减小，LiFePO4/FePO4两相的不相混溶区也会变小，当颗粒减小到一定程度时不相混溶区会消失，同时会使可用电量增大，这种现象与温度升高对纳米LiFePO4锂离子电池可用电量的影响是一致的。 　　Peukert模型是用来表征电池放电特性的电化学经验模型，可以描述可用电量与放电电流的关系，但没有考虑温度因素，见式（2）。仝猛等人[16]以11 Ah LiFePO4锂离子电池为研究对象，对常温1.1～88 A恒流放电时的可用电量进行分析，对Peukert模型在常温下倍率放电过程的应用进行了讨论，建立了基于二阶段放电法的Peukert修正模型。 　　式中，I为放电电流，A；t为放电至截止电压2.5 V时的放电时间，h；n为Peukert系数，与电池的化学体系、材料和结构有关，通过试验数据计算；C为常数，通过试验确定。 　　图3为该纳米LiFePO4锂离子电池在不同温度50 A恒流放电的单体电压曲线。 　　对式（3）两边取对数，可得Peukert系数n的计算公式，见式（4）。 　　将锂离子电池试验数据代入式（4）即可求得Peukert模型系数。图4为该纳米LiFePO4锂离子电池在50 ℃时，恒流放电t - I在对数域内的线性关系，得到Peukert系数后将放电数据代入式（2），计算得到常数C的数值，见式（5）。 　　值得注意的是，该型LiFePO4锂离子电池50 ℃的Peukert系数 n =0.998 36，远小于铅酸电池的1.27～1.34和镍镉电池的1.14。说明该锂离子电池在大电流放电时其容量损失很小，库伦效率较高，大电流放电性能良好。 　　分别计算0℃、25℃、35℃和50℃的Peukert系数，同时结合图5对Peukert模型的温度适用性进行分析，结果见表3。 　　Peukert模型的应用与温度有很大关系。随着温度从50℃开始降低，Peukert系数逐渐增大，到0℃时Peukert系数增加至1.220 9，在50～300 A范围内符合Peukert模型。 　　电池在低于-10℃进行100～300 A恒流放电时，随着放电时间增加，可用容量会呈非线性形式加速衰减，使Peukert模型不再成立，见图5中-10℃和-18℃两种温度下的数据。该纳米型LiFePO4锂离子电池Peukert模型的适用电流范围变窄，-18℃时的放电特性不再适用Peukert模型。 　　通过对该LiFePO4锂离子电池的恒流放电分析可知，当初始温度在25℃或以上的大电流放电过程中温升明显。温度升高会加快锂离子的迁移速率，降低扩散阻力，使其在橄榄石型磷酸铁锂晶体和石墨层状结构中的嵌入与脱嵌及扩散变得容易[17]，所以大电流下的可用电量会有所上升。纳米LiFePO4锂离子电池在50℃时的Peukert系数n=0.998 4<1，这种现象在铅酸电池的倍率放电特性中是不会出现的，在小容量磷酸铁锂离子电池的常温倍率放电特性中也不会出现，这得益于其正极材料（橄榄石型磷酸铁锂晶体）优良的高温特性。所以Andersson等人[14]认为LiFePO4锂离子电池具有优良的高温循环可逆性，而且由于LiFePO4/FePO4的高温耐受性强，可提高温度以改善其高倍率放电性能。 　　温度与内阻和效率特性也有很大关系。图6所示为电池内阻与温度的关系。内阻的步骤和测算方法参见《FreedomCAR电池试验手册》中的混合动力脉冲功率特性（HPPC）试验。
　　图7为该纳米LiFePO4锂离子电池的库伦效率和能量效率与温度的相关性关系。随着温度的升高，纳米材料电导率比低温时有了很大的改善，离子移动速度增大，化学反应速度加快，浓差极化和电化学极化减轻，极化内阻减小，所以当温度从-18℃升至35℃时，库伦效率和能量效率显著提高，在35～50℃温度范围内库伦效率基本稳定。值得注意的是，当温度超过35℃后，电池内部化学反应热增多，电解液可能发生副反应，导致能量损耗增加[18]，电池能量效率出现下降趋势。 　　3 能量功率特性 　　Ragone图[19]可以描述各类储能器件的能量功率特性，图8所示为五种动力电池的Ragone曲线，其中曲线B和D分别为50℃和0℃时纳米磷酸铁锂离子电池的Ragone曲线。 　　VRLA65 Ah动力电池（曲线F）为Optima黄顶铅酸动力电池，支持短时大电流放电，低温性能较为优秀，但是放电比功率和比能量相对镍氢电池和锂离子电池都比较低，无法满足现代电动汽车的大功率及高能量需求。80 Ah镍氢动力电池的Ragone曲线（曲线E）表明其恒功率放电能力不如锂离子电池，按厂家要求工作温度不能超过40℃，高温特性较差，对电池管理系统要求较高。 　　200 Ah聚合物锰酸锂离子电池（曲线A）的比能量是最高的，但是恒功率放电能力较差，恒功率放电特性并不突出。曲线B和曲线D分别是纳米LiFePO4锂离子电池在50℃和0℃的Ragone曲线，温度的升高大大促进了该电池的恒功率放电能力。曲线C为尖晶石型（LiMn2O4）锰酸锂离子电池的Ragone曲线，呈现近似竖直分布，放电比功率增加的同时，比能量基本保持稳定，具有在大功率放电时仍能提供较多电能的优点。 　　4 结论 　　（1）LiFePO4材料的纳米化可以有效改善其电化学性能，经过表面碳包覆改性的纳米LiFePO4锂离子电池具有优异的充放电性能，尤其是充放电特性和能量功率特性都有显著提升。 　　（2）温度在25～50℃时，Peukert模型适用于该纳米LiFePO4锂离子电池，具备了优秀的倍率放电特性和恒功率放电能力。随着温度降低，倍率放电特性逐渐恶化，Peukert系数增大，Peukert模型最终失效。 　　（3）温度对锂离子在纳米LiFePO4正极材料中的扩散速度有重大影响，提高温度可显著改善放电容量、倍率放电和恒功率放电能力。嵌入脱嵌反应加速，是其放电容量与倍率放电特性显著改善的主要原因，但低温下放电性能及能量功率特性依然亟待提高。 　　参考文献（References）： 　　ZHANG W J. Structure and Performance of LiFePO4 Cathode Materials：A Review [J]. Journal of Power Sources，（6）：. 　　GORIPARTI S，MIELE E，DE ANGELIS F，et al. Review on Recent Progress of Nanostructured Anode Materials for Li-ion Batteries [J]. Journal of Power Sources，（0）：421-443. 　　周鑫，赵新兵，余红明，等. F掺杂 LiFePO4/C 的固相合成及电化学性能 [J]. 无机材料学报，）： 587-591. 　　Zhou Xin，Zhao Xinbing，Yu Hongming，et al. Electro-chemical Properies of F-doped LiFePO4/C Prepared by Solid-State Synthesis [J]. Journal of Inorganic Materials，）：587-591.（in Chinese） 　　DELACOURT C，POIZOT P，LEVASSEUR S，et al. Size Effects on Carbon-Free LiFePO4 Powders The Key to Superior Energy Density [J]. Electrochemical and Solid-State Letters，）：A352-A355. 　　KANG B，CEDER G. Battery Materials for Ultrafast Charging and Discharging [J]. Nature，（23）：190-193. 　　SIDES C R，CROCE F，YOUNG V Y，et al. A High-Rate， 　　Nanocomposite LiFePO4/Carbon Cathode [J]. Electro-chemical and Solid-State Letters，）：A484-A487. 　　FEY G T，TU H J，HUANG K P，et al. Particle Size Effects of Carbon Sources on Electrochemical Properties of LiFePO4/C composites [J]. Journal of Solid State Elec-trochemistry，）：. 　　LIU H，LI C，ZHANG H P，et al. Kinetic Study on LiFePO4/C Nanocomposites Synthesized by Solid State Technique [J]. Journal of Power Sources，（1）：717-720.
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日前，广汉高新区企业广汉牧甫锂动力材料有限公司已成功完成设备修复、调试和试生产工作，目前形成了年产1500吨磷酸铁锂的规模化产能，将于3月初正式投产。
广汉牧甫董事长、总经理黄铭教授经过多年研究，发明了“用多溶剂制备磷酸铁锂方法”等系列专利技术，一举打破日韩的技术垄断。秉承“技术报效国家，产业回馈社会”的理念，他创办了广汉牧甫锂动力材料有限公司，为行业提供质优价廉的纳米磷酸铁锂产品。
新年伊始，产品即获得市场热烈响应，多家大型电池企业订单纷至沓来。公司将在赢得丰盈的市场收益的同时，向建设全球最大的纳米磷酸铁锂基地稳步迈进。
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其他题材概念
磷酸铁锂电池概念股磷酸铁锂电池上市公司
市场关注度：
较昨天&+12.5%
龙头个股：相关题材：驱动事件：
&&&&&&&&&&&&磷酸铁锂
各股票与磷酸铁锂电池概念的相关程度
相关性越接近100%，就越有可能成为龙头股！
磷酸铁锂电池概念简介
科技部网站6月25日报道，在“十二五”国家863计划支持下，“高能量锂离子电池系统和电池组技术开发”项目取得重大进步。项目以研制磷酸铁锂正极材料的高能量型锂离子电池为目标，开展锂离子电池原材料和电池单体设计技术等研究。
铅酸电池的循环寿命一般在300次左右,最高也就500次左右,锰酸锂电池目前寿命也就能达到500次,而铁锂电池,在标准充放电下循环寿命达到2800次以上,电池组循环寿命预计2500次以上。以上数据我们已经在公司实验室得到验证.铁锂电池不仅仅是代表动力电池的发展方向，它的安全性、可靠性已获重大技术突破。超级大题材在酝酿之中！
中国锂离子电池总产量已经过了前期的爆发式增长过程，现已进入平稳增长的阶段。目前中国生产的锂离子电池产品基本以用于手机的方形电池为主。受到金融危机的影响， 2008 年中国锂离子电池产量增长率下降到4.8%。锂离子电池的应用领域十分广泛，目前在手机、笔记本电脑、电动工具、数码相机、音频设备和游戏机等领域都有重要应用。手机市场和手提电脑市场一直是锂离子电池的最主要市场，这一趋势在短期内仍然不会改变。但长期来看，未来随着新能源汽车的推广，汽车用锂离子动力电池将迎来高速增长，锂离子市场的传统格局或将被打破。锂电池行业的市场竞争力很大程度依赖于长期发展的技术积累，而非单纯的资金投资，同样，锂电池材料具有较高的技术壁垒，各细分行业领先企业大多为较早进入行业者。谁掌握了规模化生产磷酸铁锂和磷酸铁锂电池技术的企业，谁就将在未来的电动汽车产业竞争中处于领先地位。
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