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CN102947976B - 可充电、高密度的电化学设备 - Google Patents

可充电、高密度的电化学设备 Download PDF

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CN102947976B
CN102947976B CN201180028013.4A CN201180028013A CN102947976B CN 102947976 B CN102947976 B CN 102947976B CN 201180028013 A CN201180028013 A CN 201180028013A CN 102947976 B CN102947976 B CN 102947976B
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CN102947976A (zh
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S·W·斯奈德
B·J·纽德克尔
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Abstract

公开了可充电的、高密度的电化学设备。这些电化学设备可，例如，包括高能量密度，在没有任何液态或凝胶型电池组件的情况下，相比其他电池，可在给定、受限的体积中存储更多能量，且仍表现出可接受的功率或电流率容量。特定实施例可涉及，例如，除了阴极之外的所有电池组件具有较小的体积或质量，同时在正阴极内获得较高的电化学有效质量。

Description

可充电、高密度的电化学设备
相关申请
本申请要求根据35U.S.C.§119(e)在2010年6月7日提交的美国临时专利申请系列号为No.61/352,082的优先权，该申请通过引用整体结合于此。
技术领域
本发明涉及可充电、高密度的电化学设备。特定地，本发明的特定实施例涉及，例如，具有高能量密度的全固态、可充电电池，且在没有任何液态、或凝胶型电池组件的情况下，其具有在有限体积中存储更多能量的容量并仍显示出可接受的功率或电流率能力。
背景技术
通过正阴极和负阳极来界定可充电和不可充电电池的容量。在使用可基于硅或锡的金属锂阳极（如，在Li-MnO2纽扣电池中）或大容量（capacity rich）Li-离子阳极时，电池的容量受控或受限于正阴极的特定容量（用mAh/g或mAh/ccm计量）。减少所有其他电池组件的体积，这对于小电池而言是最有用的，或者减少所有其他电池组件的质量，这对于较大电池（如，在电动车中）而言是最有用的，而对于给定阴极-阳极化学，同时增加正阴极内电化学有效质量是增加能量密度（例如，用Wh/liter来计量）最有效的方法。
增加正阴极内电化学有效质量意味着减少阴极中的任何辅助相（诸如机械粘合剂（binder）、或离子或电子传导增强剂（enhancer））、或使得该阴极对于给定阴极面积而言更厚。当阴极厚度变得非常大（>>20μm）时由于限制的扩散运动和相关联的受限的电流率或功率容量，高能量密度室温电池，诸如手机和膝上计算机电池，需要高传导、基于液态有机溶剂的锂离子电解液来刺穿这些电池的阴极。然而，液态有机溶剂的存在是这样的电池在最近二十年所经历的最多的问题的起源，问题诸如，例如，一旦分解的热逸出、或一旦遇到与热有关的故障引起的断路、一旦遇到特定电池故障模式引起的火/气味/烟/爆炸、早期电化学循环中的气体析出和压力增大、受限于300-1000次循环的充放电循环、受限的操作温度范围（在很多情况下是0°C—60°C）、以及其他。此外，约束挥发性液态有机溶剂要求特定的封装体系架构和电池封装，其经常配备有孔或阀门避免在早期电化学循环过程中的电池过压。
在这个行业中需要具有更高能量密度的电池。特定地，存在对于全固态可充电电池的需要，其没有用于在有限体积中存储更多能量的任何液态或凝胶型电池组件，仍然显示出可接受的功率和/或电流率能力。这导致更安全的电池且允许使用简化的封装，以及操作与存储的更高更低的温度范围。
发明概述
本发明的特定示例性实施例可包括对于给定阴极-阳极化学，具有较高能量密度的电池。如下文进一步详细讨论地，特定实施例可涉及，例如，除了阴极之外的所有电池组件具有较小的体积或质量，同时在正阴极内获得较高的电化学有效质量。
具有正复合阴极的可充电电化学设备的实施例可包括固态电化学活性材料、在电化学活性材料被初始化充电前具有的电子传导率比所述电化学活性材料的电子传导率至少高出三倍(three times higher than)的固态导电材料、和在电化学活性材料被初始化充电前具有的离子传导率比所述电化学活性材料的离子传导率至少高出三倍的固态、无机、离子传导的材料。
可选地，具有正复合阴极的可充电电化学设备的实施例可包括至少一个固态电化学活性材料、不同于该电化学活性材料的至少一个固态、离子传导的材料、且可不包含液态或胶状溶剂。
可充电电化学设备的可选实施例可包括固态正阴极、负阳极、和夹在该阴极和该阳极之间的固态电解质；其中该电化学设备包含单个电化学电池，其基于正阴极的几何占用面积(footprint)优选地具有例如，至少2mAh/cm2的额定容量。
附图说明
图1示出可被用于手机中的示例性Li-离子或Li-聚合物电池的截面图。
图2示出具有三个固相的示例性电化学设备，包括电化学活性阴极材料、离子传导率增强剂、和电子传导率增强剂。
图3示出具有两个固相的示例性电化学设备，包括电化学活性阴极材料、和电子传导率增强剂。
具体实施方式
要理解本发明不限于在此所描述的特定方法学、混合物、材料、制造技术、用途、以及应用，因为这些可有变化。还要理解本文中所使用的术语仅出于描述特定实施的目的，而不旨在限定本发明范围。必需注意到，如本文以及所附权利要求书中所使用地，单数形式的“一”、“一个”以及“该”包括复数引用，除非上下文另外明确地指出相反情况。因此，例如对“一个要素”的引用是对一个或多个要素的引用，并包括本领域内技术人员所熟知的其等效物。同样，对于另一示例，对“一个步骤”或“一个装置”的引用是对一个或多个步骤或装置的引用，并可包括子步骤或辅助性装置。所使用的所有连接词要以可能的最大涵盖方式来理解。因此，词语“或”应当理解为具有逻辑“或”的定义而非逻辑“异或”的定义，除非在上下文中另外明确指出相反情况。本文中所描述的结构应理解为也提及这种结构的功能性等效物。可解释为表示近似的语言应当如此理解，除非上下文中另外明确指出相反情况。
除非另外定义，否则在本文中所使用的所有技术和科学术语具有与本发明所属技术领域的一名普通技术人员所通常理解相同的含义。描述了优选方法、技术、装置和材料，但是在本发明的实践或测试中可使用与那些所描述的相似或等效的任何方法、技术、装置、或材料。本文中所描述的结构应理解为也提及这种结构的功能性等效物。
通过引用结合于本文中的所有专利和其它出版物出于描述和公开的目的，举例而言在这种出版物中描述的方法学可与本发明相结合而使用。在本发明的申请日之前，这些出版物单独地提供其公开内容。在这一点上不能解释为承认发明人不具备资格由于现有发明或者出于任何其它原因预料这种公开内容。
本发明的特定实施例，例如，包括全固态、高能量密度电池组，其与传统的手机电池和纽扣电池不同，不含有任何液态或胶状组件。胶状组件包括，例如，具有如此高的粘性以使它们不像常见液体那样流动的溶剂。可通过各特征的组合完成较高的能量密度，特征诸如是，例如：
1.在最大化每单元阴极面积的阴极厚度的同时，将充电和放电电流能力维持在可接受的性能极限内；
2.优化阴极内部的电化学有效质量的载荷或体积百分比，这可包括复合的而非单相电化学活性材料来构成阴极体积的100%；
3.使用包含全固态锂离子传导和电子传导增强相的合成电化学活性材料；和/或
4.最小化所有其他电池组的组件（诸如衬底、电解质、负阳极、电流集电器、和端子以及封装）的体积分数。
关于第1项，本发明的特定实施例，例如，可包括具有约100-1000μm阴极厚度的电化学设备，而手机类型电池的阴极厚度可，例如约100μm。关于第2项，示例性电化学设备可优选地使用高于约50%体积比的电化学活性材料的载荷。为了增强电池的功率和电流率能力（第1项和第3项），合成阴极的剩余例如50%的体积比可由两种材料填充：(a)锂离子传导增强材料，在制造和电池操作和存储过程中，该材料与电化学活性阴极材料是化学稳定的，同时表现出的离子传导率比电化学活性材料的离子传导率至少高出三倍；和(b)电子传导增强材料，其具有的电子传导率比电化学活性材料的电子传导率至少高出三倍。关于第4项，本发明的特定实施例的设备可被配置为，除了其他部件外，具有：(i)较薄的金属阴极电流集电器，诸如，例如10μm Al箔，其还用作任选的衬底（或如果正阴极沿其可连接正端子的外部表面具有足够的传导率，则没有这样的电流集电器）；(ii)较薄的电解质，诸如，例如，1-3μm厚的Lipon；和(iii)较薄的金属阴极，诸如，例如10-50μm的金属锂。使用易于获得的Li箔，通过物理气相沉积（PVD）工艺或热压层压，第4项的一个或多个元件可被制为本发明的特定实施例的设备。最后，本发明的特定实施例的设备可，例如，使用厚度约3μm的薄膜封装来包装，如以前所公开的，例如，在美国专利申请公开No.2009/0181303中，其整体通过引用而结合至此。
在特定实施例中，在复合阴极和/或电解质中没有任何挥发性液态有机溶剂的存在可高度有益于该电化学设备的安全以及操作和存储的更高温度极限，这包括无铅回流焊情况，其中高达265°C的温度漂移可发生达若干分钟。
本发明的特定实施例的高容量电池的更低成本的版本可包括含有更厚的陶瓷层、或多层陶瓷层的电解质替代物，其可完全地或部分地通过非PVD或非化学气相沉积（CVD）法制成，诸如传统的陶瓷或湿法化学处理。
这些电解质替代物的示例可包括Li2S-SiS2或Li2S-P2S5基的玻璃电解质粉末的压缩（~100μm层厚）、Li3N-LiTi2(PO4)3双层陶瓷板(~100μm厚)、单侧Lipon保护的LiAl2Ti(PO4)3或Li0.35La0.55TiO3板(~100μm厚)或压缩的（压制的）Li7La3Zr2O12粉末(~50μm厚)。类似于复合阴极，对于本发明的特定实施例，可使用复合阳极，且复合阳极可包括陶瓷压缩的、LiySn-活性的、纳米大小的Li4Ti5O12粉末(1.5V相对Li+/Li;相比于采用金属锂阳极的那些4V电池，结果包括本发明的特定实施例的完全制造的电化学电池的1.5V伏特的减少)，其中在体积不变化的LixTi5O12(4≤x≤7)阳极相中LiySn用作锂离子和电子传导增强第二相。还可采用其他复合阳极。
尽管制造固态的、具有陶瓷和/或湿法化学制造的电解质和/或阳极的高容量电池可能是具有吸引力的，但是由于这些电池的成本和制造吞吐量，，它们并不包含根据本发明的特定实施例的电池的功率和密度性能，其中根据本发明的特定实施例的电池使用薄膜电解质和完全由电池的电化学活性品类（诸如Li离子电池的金属锂）构成的金属阳极。这些较低成本的电池是较为不理想的，因为陶瓷和/或湿法化学制成的电解质和/或复合阳极一般较厚（其可增加电池电阻并对电池增加不含能量的体积，这两者均是不期望的特性）并提供了较低的电池电压（这可导致较低的能量和较低的功率，这两者均是不期望的特性）。
本发明的特定实施例的良好阴极性能（对于纯阴极和复合阴极）可要求，例如，阴极内的较高的、有效的扩散系数。阴极内的这样的扩散系数允许，一旦电池放电，尽可能多的电化学活性品类（离子和电子）在尽可能最短的时间内被插入阴极且插入最为远离扩散起源平面（是阴极-电解质界面）的阴极位置。在简化的画面中，根据如下式，可使用扩散的菲克第二定律的一维解，其中对于给定扩散系数D，在扩散周期t之后，扩散品类（diffusingspecies）的波前刺穿了本体（body）达深度X（有时称为扩散长度）：
X=2(D*t)1/2 (1)
式（1）是对于离子和电子的组合的扩散的准确估算。在很多实用的电化学活性阴极材料中，电子传导率大大高于电化学活性离子的传导率。例如，充电的LixCo02(x<0.7)的电子传导率为环境温度下为约1S/cm，而锂离子的传导率为小于10-7S/cm。因此，有益的是，通过掺混入合适的锂离子传导增强材料、藉此形成阴极复合，来增强阴极的锂离子传导率。
在特定实施例中，使用离子传导率作为式（1）的确定的、独立的变量，扩散系数可由菲克扩散定律的一部分所替代，这是
D=RT/(c*z*F2*dE/dx)*j (2)
这将D相关于气体常数R、绝对温度T、扩散品类的局部浓度c、这些品类的电荷数量（charge number）z（对于Li+离子而言z=1）、法拉第常数F、局部电场强度dE/dx、和扩散品类的电流密度j。在将式（2）插入式（1）并在所得式两侧求平方后所得式为
X2=4*RT/(c*z*F2*dE/dx)*t*j (3)
其中扩散周期t还可被解释为在给定电流密度j需要来放电或充电阴极的额定容量的连续的放电或充电时间，其中额定容量与给定阴极复合的阴极的厚度X成比例，该给定阴极复合为电化学活性阴极材料、离子传导率增强材料、和电子传导率增强材料。阴极的额定容量为，例如，在完全电池充电后的环境条件下所提供的电池的放电容量。使用欧姆定律用电阻R和整个阴极上的电压E（其进而具有截面扩散面积A）将电流密度j转换为传导率G后所得式，
R=E/(j*A) (4)
且传导率G（=电阻率的逆）的定义
G=1/R*X/A (5)
是
j＝E*G/X (6)
在将式（6）插入式（2）并考虑跨阴极的整个厚度X的电压降后所得式为
X2=4*RT/(c*z*F2*dE/dX)*t*E*G/X (7)
或，在重新排列式（7）后，
X3=4*RT/(c*z*F2*dE/dX)*t*E*G (8)
对于整个阴极上不变的电场梯度（这可能是导电良好的阴极的情况），dE/dx变成E/X，从而式（8）简化为
X2=4*RT/(c z*F2)*t*G (9)
因此，
X2~t*G (10)
式（10）可被认为是阴极的设计规则，如果，例如，对于通过电化学电池的厚度X的给定扩散周期（或放电或充电时间）t，在可努力倍增阴极的厚度X从而在其他参数不变的情况下（即，相同的电化学活性材料、电化学活性材料的相同容量负荷、阴极的相同截面积，和其他）倍增每占用面积的容量前，阴极的离子传导率G可被增加四倍。电池的放电时间容量可被给出其倒数值，所谓C-率，在数学上忽略放电之间的充电周期时，C-率定义了电池或电化学电池每隔多久（how often）能在一小时内数学地放电其额定容量。
式（10）还表示对于阴极内的给定传导率G，增加阴极厚度可导致慢得多（即，更长）的放电时间容量（更低的C-率）。例如，在倍增阴极厚度时，给定额定容量的全部放电的放电时间可大约增至四倍（C-率降至约25%）。维持给定额定容量的同时倍增阴极厚度暗示着，可通过向阴极增加电化学惰性材料、倍增其多孔性或者改变阴极内电活性材料来完成厚度增加。
式（10）进一步教导向阴极添加电化学惰性材料，诸如不存储电化学容量或能量的纯离子或电子传导率增强剂，因此仅增加了阴极厚度达ΔX，而不增加阴极的容量或能量，式（10）伴随的代价是：因此在特定实施例中，如果将（复合）阴极的离子传导率增加为G*(X+ΔX)2/X2从而维持，或甚至更佳地，缩短了放电或充电时间，则此举是合适的，因为：
(X+ΔX)2~t*G[(X+ΔX)2/X2] (11)
在特定实施例的阴极内较大的离子传导率的重要性和需要是明显的。由于电化学活性阴极材料，诸如，例如，商业可获得的LiCoO2，本身可不提供充分高的锂离子传导率（如，在从4.2V-2.0V相对Li+/Li之间的整个电化学活性范围上，在环境温度可表现出<10- 7S/cm，），例如，可用锂离子传导率增强材料（锂离子传导率基本高于电化学活性阴极材料的传导率）制造复合阴极。
在选择合适的锂离子传导增强材料后，诸如，例如钛酸镧锂（在25°C时Li0.35La0.55TiO3具有G=10-3S/cm(块状物)和G=2*10-5S/cm(晶界)，其示例在Y.Inaguma等人的Solid State Communications 86(1993)689页中有讨论，该文献通过参考整体并入此处）、锆酸镧锂（在25°C时Li7La3Zr2O12表现出7.7*10-4S/cm，其示例在R.Murugan等的Angewandte ChemieInternational Edition 46(2007)7778中有讨论，该文献通过参考整体并入此处）、磷酸钛铝锂（在25°C时Li1.3Til.7A10.3(PO4)3表现出7*10-4S/cm,其示例在G.Adachi等人的U.S.Pat.No.4,985,317中有讨论，该文献通过参考整体并入此处）、或硫代磷酸锂（在25°C时80at%Li2S—20at%P2S5[＝Li8P2S9;"Thio-LISICON II"]表现出7.4*10-4S/cm，其示例在Senga Minoru等人的美国专利申请公开No.2007/0160911中有讨论，该文献通过参考整体并入此处），在特定环境下是重要的，来确保锂离子传导率增强材料的形态（包括颗粒大小和颗粒大小分布）被调整为在复合引进该电化学活性阴极材料的颗粒大小和分布。这个方法可在所述复合阴极内提供锂离子传导率的正三维网络。由于欠佳的传导路径或晶粒间接触面积，复合阴极内的多孔性可能抵销具有很好传导率（应用至离子和电子）的材料的效能，传导率继而可被最大化来优化晶粒之间和整个复合阴极上的传导。这个目的可通过如下完成，对于阴极内的离子传导率增强材料和电化学活性材料二者，颗粒大小优选在约0.1-10μm范围内，且最优选为0.5-5μm。远大于10μm的颗粒可承担遮蔽或阻挡离子网络内的离子传导路径、和电子网络内的电子传导路径的风险。
可选地或附加地，可增强电化学活性材料本身的离子传导率。此举可通过，例如，将其块状晶粒（晶粒内）部分与其他、合适的化学元素混合，和/或通过化学地或机械地修改其晶界（这是固态阴极内晶粒之间的首选离子传导通路）来实现。经由与合适的化学物质反应的化学改性可以是根据本发明的特定实施例的优选方法。快速离子晶界传导在提供离子进/出位于晶粒块状物内的负责容量和能量存储的电化学反应位置是最有效的。如果在阴极内在晶粒块状物和/或晶界内的被这样增强的电化学活性材料，例如LiCoO2，表现出充分高的锂离子传导率，则仅提供添加增强的锂离子传导率的惰性相，诸如，例如钛酸镧锂（Li0.35La0.55TiO3），可能变得没有必要了。然而，可重要的是确保该阴极电子传导良好，例如，具有远高于阴极内锂离子传导率的电子传导率。否则，当应用于电子而非离子时，根据式（9），阴极的电子传导率可限制锂离子传导率的有效性，且因此仅在限制电子传导率的速度下可发生通过阴极的离子扩散。
电子传导率增强材料相对是不昂贵的，诸如例如，碳或镍粉末。使用普遍选择的电化学活性材料（如，LiCoO2）和所选择的离子传导率增强材料（诸如，例如钛酸镧锂（Li0.35La0.55TiO3）或锆酸镧锂（Li7La3Zr2O12）），这些材料相当稳定达至少500°C。根据本发明的特定实施例，优选的是使得这些电子传导率增强材料以合适的颗粒大小分布（这有助于最大化复合阴极的电子传导率）可用，最优选的是以电子传导率增强材料的最低添混容量分数可用。如果使用了较大的颗粒，诸如，50μm Ni，则这些颗粒可为复合阴极提供良好的电子传导率，但是可能不必要地移除了复合阴极内宝贵的体积，这些体积没有被填充更为重要的电化学活性阴极材料（其提供能量）和/或任选的锂离子传导率增强材料（可在那个能级增强功率容量）。
可选地或附加地，电化学活性材料本身的电子传导率可被增强。此举可通过，例如，将其块状晶粒（晶粒内）部分与其他、合适的化学元素混合，和/或通过化学地或机械地修改其晶界（这是固态阴极内晶粒之间的首选电子传导通路）来实现。经由与合适的化学物质反应的化学改性可以是根据本发明的特定实施例的优选方法。快速电子晶界传导在提供电子进/出位于晶粒块状物内的负责容量和能量存储的电化学反应位置是最有效的。如果在阴极内在晶粒块状物和/或晶界内的被这样增强的电化学活性材料，例如LiCoO2，表现出充分高的电子传导率，则在正阴极中添加基本电化学存储容量的情况下添加仅提供增强的电子传导率的惰性相，诸如，例如，镍或碳粉末，可变得没有必要。
例如，可使用高能球磨研磨（可将原始粉末碾磨至纳米/亚微米大小的颗粒）产生合适的颗粒大小和分布。可通过将应用了不同碾磨参数的分别被碾磨的粉末批次混合起来，完成对给定材料的特定颗粒大小分布。由于一种材料（如，锂离子传导率增强材料）的这样获得的粉末具有特定的颗粒大小分布，这个粉末可与具有以类似方式创建的颗粒大小分布的另一种材料（如，电化学活性阴极材料）相混合。最终，电子传导率增强材料（以与为锂离子传导率增强材料所采用的方式类似的方式制成的特定颗粒大小分布）可被添加至该粉末混合物。然后，可以各种方式实现该粉末混合物的均质化，诸如，例如，通过使用低浓度的低密度碾磨媒质（诸如Si3N4或Al2O3，这可或不可进一步改变该粉末混合物中一个或多个材料的颗粒大小分布）进行的低能球磨研磨。
本发明的示例性实施例
示例1：根据本发明的实施例，在初始化充电之前，可使用商业可获得的LiCoO2粉末，通过(a)冷压合7吨的厚度0.5mm且直径10mm的粉末小粒（此举可获得5.06g/ccm理论密度的76%），和（b）冷压合7吨的厚度0.5mm且直径10mm的粉末小粒且之后通过在空气中在900°C烧结该小粒（pellet）达1小时（此举可获得5.06g/ccm理论密度的72%），来确定环境条件下它的电子传导率。然后这样获得的小粒，在两侧小粒表面上可被涂覆0.3μm厚的、PVD制造的、锂离子阻挡的金电极，并接受使用电化学阻抗谱法和10mV幅值的电阻测量。示例性被冷压合的LiCoO2小粒的电子传导率获得2.7*10-5S/cm，而可在900°C被退火的小粒表现出7.1*10-4S/cm的电子传导率。
示例2：根据本发明的实施例，可从被冷压合的0.5mm厚且直径10mm的7吨Ni小粒中确定商业可获得的Ni粉末（2-3μm晶粒大小）的电子传导率。该密度可以是理论密度（8.91g/ccm）的80%。这样获得的Ni小粒可被夹在两个铜电极之间并经受10m VDC。然而，电阻抗可以如此低（<<1Ohm）以致电流落在测试仪器能力（10A）之外。替代确定精确的电子传导率，可通过Ni的文献值（在25°C时在约105S/cm）来近似该电子传导率。在初始化充电之前，这个值大于LiCoO2的10个数量级。
示例3：根据本发明的实施例，在初始化充电之前，可使用来自示例1的商业可获得的LiCoO2粉末，通过(a)冷压合7吨的厚度0.5mm且直径10mm的粉末小粒、和（b）冷压合7吨的厚度0.5mm且直径10mm的粉末小粒且之后通过在空气中在700℃烧结该小粒达1小时（此举可获得5.06g/ccm理论密度的73%），来确定环境条件下它的离子传导率。这样获得的小粒，在每一个小粒表面上，可被涂覆有3μm厚的电子阻挡Lipon电解质层。此外，两个金属Li电极可被PVD制造在与被夹持的LiCoO2小粒相对的Lipon电解质层上。通过对在发生锂涂镀或剥离的锂电极应用1-5VDC之间的各种电压，这个离子传导率测试单元可经受欧姆电阻测量。在这个设置中，仅锂离子可传导通过LiCoO2小粒，而其电子传导完全被阻止。所引起的瞬时电流可表现出欧姆行为且被计算到电阻中。减去串联连接的两个3μm Lipon层的已知、组合电阻（来自其他独立的试验）能在初始化充电前提取到LiCoO2的离子传导率。当在25°C测量时，示例性冷压合LiCoO2小粒和之后在空气中在700°C被退火达1小时的冷压合LiCoO2小粒二者的离子传导率均为2*10-8S/cm，这比25°C时LiCoO2的离子传导率低三个数量级。因此，在这个示例中的LiCoO2表现为主要电子传导的材料，具有欠佳的锂离子传导率。
示例4：根据本发明的实施例，通过起始化合物LiOH、La203、和TiO2的标准粉末反应，可合成Li0.35La0.55TiO3。最终粉末Li0.35La0.55TiO3，经XRD验证，可实际上没有杂质相。然后这个粉末可(a)冷压合7吨、0.4mm厚度和10mm直径粉末小粒（此举获得4.99g/ccm理论密度的64%），和(b)冷压合7吨、0.4mm厚度和10mm直径粉末小粒且之后在空气中在1100°C烧结达1小时（此举获得4.99g/ccm理论密度的70%）。如此获得的小粒，可在每一个小粒表面上被应用PVD制造的金电极。通过电化学阻抗谱法，可确定Li0.35La0.55TiO3小粒的离子传导率，其可显示，对于被冷压合的小粒在25°C测得5.6*10-8S/cm的晶界（晶粒内）传导率，而由于测试设置的受限的频率容量，不可确定块状物（晶粒内）传导率，这继而可需要约10MHz范围的频率。当在25°C被测量时，在700°C在空气中被退火达1小时的Li0.35La0.55TiO3小粒的晶界传导率被确定为约1.8*104S/cm。然而，在1100°C被制造的小粒，而可允许反卷积（deconvolution）为块状物（晶粒间）和晶界（晶粒内）传导率，这可分别总计5.6*10-4S/cm和2.4*10-6S/cm。在其初始化充电前，这些传导率可大于LiCoO2的锂离子传导率的两个数量级（见示例3）。
实施例5：根据本发明的实施例，可用例如，80wt%LiCoO2和20wt%Ni的混合物且没有添加诸如Li0.35La0.55TiO3之类的离子传导增强剂，来制造复合阴极。该混合物可被冷压合为大小为0.3mm x 10mm直径的复合阴极小粒。通过在空气中在700°C烧结这些小粒达1小时，可进一步处理其他小粒。所得被冷压合或被烧结的复合阴极小粒可保留良好的电子传导（>10-2S/cm）。当被制造为包含1.5μm厚Lipon电解质和10μm金属Li阳极的全电化学电池时，可发现有两种小粒类型早在常压4.2V的初始化充电步骤过程中就经受了严厉的电流率限制。在25°C，数分钟内电流可衰减为约1μA，在10mAh电池的情况下，这可引起大于10,000小时(大于1年)的充电时间。这样的电池，例如，可包含83mg的LiCo02。电化学活性阴极材料（LiCoO2）的纯复合，对于例如较小阴极厚度（诸如，小于30μm，在本发明的特定实施例中常规地被构建为薄膜形式），表现出充分的离子和电子导电率。进一步，当为了高容量电池（>1mAh/cm2）使用相当厚的厚度（>>30μm）时，电子传导增强剂（Ni）可能不会导致电化学良好活性的复合阴极。因此，至少一个关键组件可从复合阴极中移去，来实现有用的电池性能。
示例6：这个示例表现出优于示例5的示例性潜在改进。根据本发明的实施例，在示例1-4中使用的粉末可被以如下重量百分比混合：40wt%LiCoO2(理论密度=5.06g/ccm),40wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)。该粉末混合物可被冷压合为直径0.3mm x10mm的复合阴极小粒，具有80%的理论密度，这可从式（12）中被计算：
复合阴极小粒的理论密度(g/ccm)=100%/(40wt%/5.06g/ccm+40wt%/4.99g/ccm+20wt%/8.91g/ccm)=5.50g/ccm (12)
使用两个夹持的铜板的示例性复合阴极的电子传导率大于10-2S/cm，而通过XRD检测出没有除了原始要素LiCoO2,Li0.35La0.55TiO3、和Ni外的新的相。可从复合阴极中Li0.35La0.55TiO3的体积分数来估算复合阴极的离子传导率，这由式（13）给出：
vol% of Li0.35La0.55TiO3=40wt%*5.50g/ccm/4.99g/ccm=44vol% (13)
在第一近似中，可假设在复合阴极内小粒的以下近似是正确的：
复合阴极的密度/Li0.35La0.55TiO3的实际密度≈复合阴极的理论密度/Li0.35La0.55TiO3的理论密度 (14)
所以，式（13）为复合阴极内的Li0.35La0.55TiO3的实际vol%提供了良好的估算。可进一步假设，根据下式，通过主导锂离子导体的vol%确定复合阴极内理想晶粒大小复合的锂离子传导率：
Actual vol% Li0.35La0.55TiO3*5.6*10-8S/cm=2.5*10-8S/cm (15)
例如基于被冷压合为复合阴极小粒且没有被进一步热处理的Li0.35La0.55TiO3锂离子晶界传导率的锂离子传导率，对于实际应用目的而言太低，且可能类似于纯LiCoO2(见示例3)的锂离子传导率。因此，复合阴极小粒可在700°C被热处理，在此温度可提供0.44*1.8*10-7S/cm=7.9*10-8S/cm的复合阴极。这对于实践应用，仍然不是足够的锂离子传导率（见示例14）。在900°C退火该复合阴极小粒可使得LiCoO2与Ni的某些反应来形成NiO和LiCoO2分解侧相（decomposition side phase）。锂离子传导率的改进可以是很小的和/或可上升至约4*10-7S/cm。
明显的是，当在复合阴极内时，可改进增强剂材料的锂离子晶界传导率。复合电极，在可于复合电极的构成要素之间设置不期望的化学反应之前，例如，不可高于特定温度（如，900°C）被处理。
通过将锂离子传导增强剂的粉末碾磨和粉碎为较小晶粒大小（<2μm）和/或通过机械地或化学地合适地修改其晶粒表面增加其锂离子晶界传导率，来完成这些特定示例性改进。这样的被表面修改的锂离子传导率增强剂材料，当被冷压合为复合阴极小粒和之后在空气中在700°C达1小时的退火步骤时，可展现出约10-4S/cm的晶界传导率。约10-4S/cm的示例性复合阴极的总体锂离子传导率可允许C/30的连续电流汲取，对于具有300μm厚的复合阴极的6mAh电池，这转换为0.2mA（见示例13）。
示例7：根据本发明的实施例，基于正阴极的几何占用面积提供2mAh/cm2容量的10mm直径电化学电池，可用包含40wt%LiCoO2(理论密度=5.06g/ccm),40wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。阴极的几何占用面积是，例如，当沿其表面法向或沿设备的主轴面对着表面时获得的表面积，该表面具有当假设是非常平坦的表面时测得的几何面积。利用电化学活性阴极材料（LiCoO2）的这个载荷，可由11.2mg LiCoO2制成该复合阴极，藉此导致厚度优选为约28mg/(0.785cm2*80%*5.50g/ccm)=81μm。
示例8：根据本发明的实施例，提供2mAh/cm2容量的10mm直径电化学电池，可用包含20wt%LiCoO2(理论密度=5.06g/ccm),60wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。采用电化学活性阴极材料（LiCoO2）的这个载荷，可由11.2mg LiCoO2制成该复合阴极，藉此导致厚度为约56mg/(0.785cm2*80%*5.49g/ccm)=162μm。
示例9：根据本发明的实施例，提供4mAh/cm2容量的10mm直径电化学电池，可用包含40wt%LiCoO2(理论密度=5.06g/ccm),40wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。利用电化学活性阴极材料（LiCoO2）的这个载荷，可由22.4mg LiCoO2制成该复合阴极，藉此导致厚度为约56mg/(0.785cm2*80%*5.50g/ccm)=162μm。
示例10：根据本发明的实施例，提供4mAh/cm2容量的10mm直径电化学电池，可用包含20wt%LiCoO2(理论密度=5.06g/ccm),60wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。利用电化学活性阴极材料（LiCoO2）的这个载荷，可由22.4mg LiCoO2制成该复合阴极，藉此导致厚度为约112mg/(0.785cm2*80%*5.49g/ccm)=325μm。
示例11：根据本发明的实施例，提供5mAh/cm2容量的10mm直径电化学电池，可用包含40wt%LiCoO2(理论密度=5.06g/ccm),40wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。利用电化学活性阴极材料（LiCoO2）的这个载荷，可由28mgLiCoO2制成该复合阴极，藉此导致厚度为约70mg/(0.785cm2*80%*5.50g/ccm)=203μm。
示例12：根据本发明的实施例，提供5mAh/cm2容量的10mm直径电化学电池，可用包含20wt%LiCoO2(理论密度=5.06g/ccm),60wt%Li0.35La0.55TiO3(理论密度=4.99g/ccm),和20wt%Ni(理论密度=8.91g/ccm)的复合阴极制造。利用电化学活性阴极材料（LiCoO2）的这个载荷，可由28mgLiCoO2制成该复合阴极，藉此导致厚度为约140mg/(0.785cm2*80%*5.49g/ccm)=406μm。
示例13：根据本发明的实施例，示例11的电池，其中28mg的LiCoO2材料可由28mg的Li1.2Ni0.175Co0.10Mn0.525O2(见例如，美国专利申请公开No.2010/086853,整体通过引用并入此处)所替代，当在4.6-2.0V之间循环时，这可改进电池的容量达70%，且同时伴随着将每单位面积的容量从5mAh/cm2增强至约8.5mAh/cm2。由于LiCoO2和Li1.2Ni0.175Co0.10Mn0.525O2的理论密度类似，电池中所制造的复合阴极小粒的实际密度也类似，且因此两个复合阴极小粒厚度可约为200μm。
示例14：根据本发明的实施例，在将式（9）重新排列，
X2=4*RT/(c*z*F2)*t*G (16)
为
X2*c*z*F2/(4*RT)＝t*G (17)
之后，其中
c=复合阴极中活性阴极负载的vol%*给定活性阴极材料中移动离子品类的浓度 (18)
对于其中活性阴极材料是LiCoO2,的情况，c=复合阴极中活性阴极负载的vol%*2.3*10-2mol/ccm(假设100%致密复合阴极),z=1,F=96485C/mol,R=8.3143J/(K*mol),T=298K，且
(复合阴极的厚度)2*复合阴极中活性阴极负载的vol%*2.2*104秒/(Ohm*ccm)=放电时间*复合阴极中的锂离子传导率 (19)
在具有40vol%载荷的500μm厚的复合阴极的情况下，例如，10小时（36,000秒）放电或充电时间（C/10率）要求在复合阴极内最小的约6*104S/cm的锂离子传导率，而C/30率(30小时的放电或充电时间)仅要求约2*10-4S/cm。
倍增阴极载荷（80vol%有效负载），例如，同时维持给定容量，允许复合阴极被制造为约1/2的阴极厚度或250μm。作为结果，C/10率容量可仅要求约3*104S/cm，而C/30的情况可仅要求约1*104S/cm。
由于创建具有在例如104S/cm的较高的锂离子传导率的复合阴极是困难的，对于给定复合已近中的给定容量和对于在给定温度处的给定放电和充电时间，一个选项可以是最大化复合阴极内活动电化学材料的vol%载荷，且同时最小化复合阴极的厚度。
对于具有给定离子传导率的给定复合阴极中的给定容量Q，放电或充电时间t根据下式确定了最大连续放电或充电电流
最大连续放电或充电电流=Q/t (20)
示例15：根据本发明的实施例，类似于示例7中的电池，不过其中Li0.35La0.55TiO3粉末具有小于2μm的平均晶粒大小，可具有改进的晶界传导率，其方式为使得电池在其4.2-2.0V的可逆性范围（reversibility range）内在10小时或更少时间内被连续放电至约2mAh/cm2。可逆性范围是，例如，通常可被接受的电压范围，在该范围中，在给定温度，给定电极“基本”稳定。较高的温度一般可减少电极的可逆性范围。例如，在25°C，LiCoO2的可逆性范围通常可被接收为4.2—2.0V相对Li+/Li，这等同于从约Li1.0CoO2(2.0V相对Li+/Li)到约Li0.5CoO2(4.2V相对Li+/Li)的化学计算（stoichiometry）范围。
示例16：根据本发明的实施例，类似于示例9中的电池，不过其中Li0.35La0.55TiO3粉末具有小于lμm的平均晶粒大小，可具有改进的晶界传导率，使得电池在4.2-2.0V内在10小时或更少时间内被连续放电至约4mAh/cm2。
示例17：根据本发明的实施例，类似于示例11中的电池，不过其中Li0.35La0.55TiO3粉末具有小于0.5μm的平均晶粒大小，可具有改进的晶界传导率，使得电池在4.2-2.0V内在10小时或更少时间内被连续（且完全地）放电至约5mAh/cm2。
示例18：根据本发明的实施例，示例7的电化学电池可被配置为具有1.5μm厚的Lipon电解质、10μm厚的金属Li阳极、10μm Al阴极电流集电器箔片、10μm Cu阳极电流集电器箔片、和位于该电化学电池之上和之下的100μm壁厚的聚合物袋状封装（pouchencapsulation）。当电池被充电至4.2V时，在考虑了Li阳极将其厚度增加至全部约22μm且全部复合阴极的厚度为约82μm之后，这样的特性提供了在完全包装的状态下约59Ah/升的体积容量密度（例如，通过将额定容量除以完全包装的电池体积计算得到）、和约236Wh/升的体积能量密度（例如，通过将额定容量与额定电压的乘积处于完全包装的电池体积计算得到）。“完全包装的状态”，例如，是将所有外围部件包括在电池内的电池的状态，包括，例如，电流集电器、端子、主要封装（如果外壳没有被包括在该封装内）、和外壳。
示例19：根据本发明的实施例，示例9的电化学电池可被配置为具有1.5μm厚的Lipon电解质、10μm厚的金属Li阳极、10μm Al阴极电流集电器箔片、10μm Cu阳极电流集电器箔片、和位于该电化学电池之上和之下的100μm壁厚的聚合物袋状封装。当电池被充电至4.2V时，在考虑了Li阳极将其厚度增加至全部约34μm且全部复合阴极的厚度为约163μm之后，这样的特性提供了在完全包装的状态下约92Ah/升的体积容量密度、和约368Wh/升的体积能量密度。
示例20：根据本发明的实施例，示例11的电化学电池可被配置为具有1.5μm厚的Lipon电解质、10μm厚的金属Li阳极、10μm Al阴极电流集电器箔片、10μm Cu阳极电流集电器箔片、和位于该电化学电池之上和之下的100μm壁厚的聚合物袋状封装。当电池被充电至4.2V时，在考虑了Li阳极将其厚度增加至全部约40μm且全部复合阴极的厚度为约205μm之后，这样的特性提供了在完全包装的状态下约103Ah/升的体积容量密度、和约412Wh/升的体积能量密度。
示例21：根据本发明的实施例，当在示例18、19、20的每一个示例中将电化学活性阴极材料（LiCoO2）的载荷从约40wt%增至60wt%且将锂传导增强材料（Li0.35La0.55TiO3，与LiCoO2具有非常类似的密度，从而复合阴极的厚度基本保持一样）从40wt%减少至20wt%，示例18、19、20中给出的能量密度分别增加至约354Wh/升、约552Wh/升、和约618Wh/升。
示例22：根据本发明的实施例，来自示例21的618Wh/升的电池包含约5.89mAh且可被配置为具有50μm厚的电解质、50μm厚的LiySn-活性的、纳米大小的Li4Ti5O12阳极、10μm Al阴极电流集电器箔片、10μm Cu阳极电流集电器箔片、和位于该电化学电池之上和之下的100μm壁厚的聚合物袋状封装。当电池被充电至4.2V时，这个配置提供了在完全包装的状态下具有约135Ah/升的体积容量密度和约338Wh/升的体积能量密度的电池，同时阳极厚度大约保持不变在约50μm，且复合阴极可到达约约205μm的全部厚度。然而，中间点电压，可从4.0V（示例21）变化至约2.5V。
示例23：根据本发明的实施例，复合阴极可被制造为包括60wt%LiCoO2,20wt%Ni、和20wt%化学表面改性的Li0.35La0.55TiO3的混合物。通过分别与LiIO4*2H2O、聚吡咯、Li3N、Ni、或碳在250°C-900°C的温度范围内进行前期反应，可实现Li0.35La0.55TiO3的化学表面改性。然后该混合物可被冷压合至直径0.3mm x 10mm大小的复合阴极小粒，且随后在空气中在250°C-500°C被退火。所得被退火的复合阴极小粒可保留良好的电子传导（>10-2S/cm）。当被制造为包含1.5μm厚Lipon电解质和10μm金属Li阳极的全电化学电池时，该复合阴极可为该电池提供在4.2—2.0V之间的大于C/30的连续充电和放电电流。该化学表面改性基本增强了离子传导率增强剂材料（Li0.35La0.55TiO3）的锂离子电导率达约三个数量级，从10-7S/cm的锂离子晶界（晶粒内）电导率到接近10-4S/cm的锂离子晶界传导率值。
示例24：根据本发明的实施例，可制成包含约80wt%化学表面改性的LiCoO2和20约wt%Ni的混合物且没有添加诸如Li0.35La0.55TiO3之类的任何离子传导增强剂的混合物的复合阴极。通过与LiIO4*2H2O、或聚吡咯在约250°C—900°C的温度范围内进行的独立和前期反应，可实现LiCoO2的化学表面改性。然后该混合物可被冷压合至直径0.3mm x 10mm大小的复合阴极小粒，且随后在空气中在约250°C-500°C被退火。所得被退火的复合阴极小粒可保留良好的电子传导（>10-2S/cm）。当被制造为包含1.5μm厚Lipon电解质和10μm金属Li阳极的全电化学电池时，这些电池中的这些复合阴极可维持4.2—2.0V之间的大于C/30的连续充电和放电电流。明显的是该化学表面改性基本增强了电化学活性材料（LiCoO2）的锂离子传导率达大于约3个数量级，从约2*10-8S/cm到接近约10-4S/cm的值。这个方法允许复合阴极的制造，该复合阴极具有离子传导率增强剂，其可以是电化学活性材料本身，藉此呈现出不具有电化学存储容量（如，Li0.35La0.55TiO3）冗余的被分开提供的离子传导率增强剂。
示例25：根据本发明的实施例，可制造使用来自示例24的复合阴极的10mm直径的电化学电池。该复合阴极可具有约4.43g/ccm的实际冷压合的密度（这是约5.54g/ccm的理论密度的约80%）、和约350μm的厚度。这个复合阴极为电池提供约13.7mAh的容量。这个电池可进一步被配置为具有1.5μm厚Lipon电解质、10μm厚金属Li阳极、10μm Al阴极电流集电器箔片、10μmCu阳极电流集电器箔片、和位于该电化学电池之上和之下的100μm壁厚的聚合物袋状封装。当电池被充电至4.2V时，在考虑了Li阳极将其厚度增加至全部约92μm且全部复合阴极的厚度为全部约355μm之后，这个结构提供了在完全包装的状态下约254Ah/升的体积容量密度、和约1018Wh/升的体积能量密度。这样的电化学电池可具有改进的晶界传导率，且在4.2-2.0V范围内，能使电池在10小时或更少时间内被连续（且完全地）放电至约17mAh/cm2。
图1示出被用在手机电池中的Li-离子或Li-聚合物电池的现有技术的截面示图。复合阴极110一般是约100μm厚且包括四个相，其中三个相是固态相，且第四个是液相。电化学活性阴极材料111可以是固态LiCoO2（或衍生物）粉末且电子传导率增强剂113可以是石墨碳。聚合物粘合剂114，诸如PVDF，将之前两个固态相粘合至Al箔片衬底130。非水液体电解质112，其为具有溶解的锂盐的有机溶剂，渗入复合阴极110的小孔中。当100%的测量体积是电解质时，液体电解质112在25°C时具有10-2-10-3S/cm的较高的锂离子传导率。液体电解质112可到达复合电极内几乎每一个体积元素，除了已经被电化学活性阴极材料111、电子传导率增强剂113、和，某种程度上，聚合物键114，所占据的那些体积元素。假设电解质112可存在于，例如仅约30%的复合阴极体积中，且附加地例如，可具有弯曲的路径来克服小孔中的困难，以发挥其锂传导，复合阴极110，在25°C在其大部分上具有约10-3-10-4S/cm的有效整体锂离子传导率。
进一步如图1中所示，非水液态电解质112渗入、穿透聚合物衬底120（一般13-50μm厚）和一般Li-离子或Li-聚合物阳极140。Li-离子或Li-聚合物阳极140一般约100μm厚且包括一般通过石墨碳提供的电化学阳极材料141、为石墨碳而优化的聚合物键142、和非水液态电解质112。存在附加的电池组件，诸如Cu阳极电流集电器箔片和电池包装，但没有被包括在图1中。
图2示出本发明的示例性实施例中的一个。复合阴极210可包括，例如至少三个固态相（没有任何液态相出现）：（1）诸如，例如LiCoO2之类的至少一个固态电化学活性阴极材料211；(2)诸如例如Ni之类的至少一个固态电子传导材料213，且在其初始化充电前具有的电子传导率比所述电化学活性阴极材料211的电子传导率至少高出三倍；和(3)诸如例如Li0.35La0.55TiO3之类的至少一个固态、无机、离子传导材料212，且在其初始化充电前具有的离子传导率比所述电化学活性阴极材料211的离子传导率至少高出三倍。
本发明的特定实施例的复合阴极210可不需要用于液态非水电解质的任何小孔，且因此可被以更为致密的方式制造（如，一般是少于20%的剩余多孔性）且为了改进的晶界结合在更高的温度被退火。本发明的特定实施例的复合阴极210可易于被制造为具有增加的厚度（如，100-1000μm）和良好的机械性质。在本发明的特定实施例中，复合阴极210可具有充分的刚性，从而它能用作自身的衬底或其他电池组件的衬底，诸如，例如，1.5μm厚固态薄膜电解质220和薄膜金属锂阳极240。
图3示出本发明的另一个可选的优选实施例。复合阴极310可包括，至少两个固态相（没有任何液态相存在）：（1）诸如，例如具有被极大地增强的锂离子晶界传导率的表面改性的LiCoO2之类的至少一个固态电化学活性阴极材料311；和(2)诸如例如Ni之类的至少一个固态电子传导材料313，且在其初始化充电前具有的电子传导率比所述电化学活性阴极材料311的电子传导率至少高出三倍。提供具有被极大地增强的锂离子晶界传导率的表面改性的LiCoO2可消除对于独立的、固态、无机、离子传导材料（诸如图2中的元件212）的需要。
本发明的特定实施例的复合阴极310可不需要用于液态非水电解质的任何小孔，且因此可被以更为致密的方式制造（如，一般少于20%的剩余多孔性）且在更高的温度被退火用于改进的晶界结合。本发明的特定实施例的复合阴极310可易于被制造为具有增加的厚度（如，100-1000μm）和良好的机械性质。在大多数情况下，本发明的特定实施例的复合阴极310可具有充分的刚性，从而它能用作自身的衬底或其他电池组件的衬底，例如，1.5μm厚固态薄膜电解质320和薄膜金属锂阳极340。
上述实施例和示例仅为示例性。本领域普通技术人员可认识到本文详细描述的实施例的变体意味着落入本公开和发明的范围。因此，本发明仅由以下权利要求来限制。因此，本发明旨在涵盖本发明的所有这些修改，只要它们落在所附权利要求书及其等效方案的范围中即可。

Claims (30)

1.一种可充电的电化学设备，包括：
正复合阴极，所述正复合阴极包括：
固态电化学活性材料，在该电化学活性材料的预充电状态中具有电子传导率和晶粒内离子传导率，
固态电子传导材料，其所具有的相应的电子传导率至少是所述电化学活性材料在其预充电状态中的电子传导率的三倍高，和
固态无机的离子传导材料，其具有的相应的晶粒内离子传导率至少是所述电化学活性材料在其预充电状态中的晶粒内离子传导率的三倍高，
其中所述固态电化学活性材料或者所述固态无机的离子传导材料包括具有增强的晶粒间离子传导率的表面改性的晶界，并且所述电化学活性材料和所述离子传导材料的颗粒尺寸在0.1-10μm之间，以及
其中所述电化学设备不包含液体、胶状溶剂或聚合物粘合剂的残余。
2.如权利要求1所述的电化学设备，其特征在于，所述电化学活性材料，相比所述正复合阴极中的任何其他材料，为所述正复合阴极提供更多的电子传导率。
3.一种可充电的电化学设备，包括：
正复合阴极，其包括：
具有电子传导率和晶粒内离子传导率的固态电化学活性材料，
和
固态离子传导材料，包括与所述电化学活性材料不同的材料，并且其所具有的相应的晶粒内离子传导率至少为所述固态电化学活性材料在其预充电状态中的晶粒内离子传导率的三倍高，
其中所述固态电化学活性材料或者所述固态离子传导材料包括具有增强的晶粒间离子传导率的表面改性的晶界，并且其中所述电化学活性材料和所述离子传导材料的颗粒尺寸在0.1-10μm之间，
其中所述电化学设备不包含液体、胶状溶剂或聚合物粘合剂的残余。
4.如权利要求3所述的电化学设备，其特征在于，所述电化学活性材料，相比所述正复合阴极中的任何其他材料，为所述正复合阴极提供更多的电子传导率。
5.如权利要求3所述的电化学设备，其特征在于，还包括电子传导材料，其包括的电子传导率至少是所述电化学活性材料在其预充电状态中的电子传导率的三倍高。
6.如权利要求3所述的电化学设备，其特征在于，还包括固态电解质，所述固态电解质不包括液体且不包括胶状溶剂。
7.如权利要求3所述的电化学设备，其特征在于，所述正复合阴极仅包括固态电化学活性相。
8.如权利要求3所述的电化学设备，其特征在于，基于所述正复合阴极的几何占用面积，所述电化学设备具有至少2mAh/cm2的额定容量。
9.如权利要求3所述的电化学设备，其特征在于，基于所述正复合阴极的几何占用面积，所述电化学设备包括至少4mAh/cm2的额定容量。
10.如权利要求3所述的电化学设备，其特征在于，基于所述正复合阴极的几何占用面积，所述电化学设备包括至少17mAh/cm2的额定容量。
11.如权利要求3所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于30小时内能够被完全放电。
12.如权利要求3所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于10小时内能够被完全放电。
13.如权利要求7所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于30小时内能够被完全放电。
14.如权利要求7所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于10小时内能够被完全放电。
15.如权利要求8所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于30小时内能够被完全放电。
16.如权利要求8所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于10小时内能够被完全放电。
17.如权利要求9所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于30小时内能够被完全放电。
18.如权利要求9所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于10小时内能够被完全放电。
19.如权利要求10所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于30小时内能够被完全放电。
20.如权利要求10所述的电化学设备，其特征在于，在其可逆性范围内，所述电化学设备在少于10小时内能够被完全放电。
21.如权利要求3所述的电化学设备，其特征在于，包括在完全包装的状态中的至少60Ah/升的体积容量密度。
22.如权利要求3所述的电化学设备，其特征在于，包括在完全包装的状态中的至少240Wh/升的体积能量密度。
23.如权利要求7所述的电化学设备，其特征在于，包括在完全包装的状态中的至少90Ah/升的体积容量密度。
24.如权利要求7所述的电化学设备，其特征在于，包括在完全包装的状态中的至少360Wh/升的体积能量密度。
25.如权利要求8所述的电化学设备，其特征在于，包括在完全包装的状态中的至少100Ah/升的体积容量密度。
26.如权利要求8所述的电化学设备，其特征在于，包括在完全包装的状态中的至少400Wh/升的体积能量密度。
27.如权利要求10所述的电化学设备，其特征在于，包括在完全包装的状态中的至少250Ah/升的体积容量密度。
28.如权利要求10所述的电化学设备，其特征在于，包括在完全包装的状态中的至少1000Wh/升的体积能量密度。
29.如权利要求3所述的电化学设备，其特征在于，在其初始化充电之前，所述正复合阴极包括复合物。
30.如权利要求3所述的电化学设备，其特征在于，在其初始化充电之前，所述正复合阴极包括单相。
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