CN104795547A - 结构化颗粒及其在锂可再充电电池组中的使用 - Google Patents

结构化颗粒及其在锂可再充电电池组中的使用 Download PDF

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CN104795547A
CN104795547A CN201510080927.5A CN201510080927A CN104795547A CN 104795547 A CN104795547 A CN 104795547A CN 201510080927 A CN201510080927 A CN 201510080927A CN 104795547 A CN104795547 A CN 104795547A
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M·格林
刘峰名
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Abstract

硅或包括硅的材料的柱状颗粒及其制造方法。这些颗粒可被用于产生具有聚合物粘结剂、导电添加剂和金属箔集电体的复合阳极结构以及电极结构。所述颗粒的结构克服了充电/放电容量损失的问题。

Description

结构化颗粒及其在锂可再充电电池组中的使用
本申请是申请日为2008年7月17日、申请号为200880025163.8、发明名称为“制造由硅或基于硅的材料构成的结构化颗粒的方法及其在锂可再充电电池组中的使用”的申请的分案申请。
技术领域
本发明涉及包括硅的颗粒、制造颗粒的方法、包含颗粒作为其活性材料的电极、电化学电池(cell)、锂可再充电电池阳极、电池、由电池供电的装置、产生复合电极的方法、制造锂可再充电电池的方法以及制造含硅纤维的方法。
背景技术
最近对于诸如移动电话和笔记本电脑的便携式电子装置的使用的增加和在混合电动车辆中使用可再充电电池组(battery)的新兴趋势,已经产生了对用于向上述装置和其他电池组供电装置提供电力的更小、更轻、更长寿命的可再充电电池组的需求。在20世纪90年代期间,锂可再充电电池组(特别地,锂离子电池组)变得流行,就售出数量而言,现在其统治着便携式电子设备市场并被用来应用于新的、对成本敏感的应用。然而,由于越来越多的耗电功能(例如,移动电话中的照相机)被加入到上述装置中,因此需要每单位质量和每单位体积存储更多能量的改进的且成本更低的电池组。
公知可以使用硅作为可再充电锂离子电化学电池组电池(battery cell)的活性阳极材料(参见,例如,Insertion Electrode Materials for Rechargeable Lithium Batteries,M.Winter,J.O.Besenhard,M.E.Spahr,and P.Novak in Adv.Mater.1998,10,No.10)。图1示出了常规锂离子可再充电电池组电池的基本构成,其包括基于石墨的阳极电极,该部件将被基于硅的阳极所取代。该电池组电池包括单个电池,还可包括多于一个的 电池。
电池组电池通常包括用于阳极的铜集电体(current collector)10和用于阴极的铝集电体12,集电体10和12可根据需要而被外部连接到负载或连接到再充电电源。基于石墨的复合阳极层14覆盖集电体10,并且基于含锂金属氧化物的复合阴极层16覆盖集电体12。在基于石墨的复合阳极层14与基于含锂金属氧化物的复合阴极层16之间设置多孔塑性间隔物或分离物20,并且液体电解质材料被分散在多孔塑性间隔物或分离物20、复合阳极层14以及复合阴极层16内。在一些情况下,可以用聚合物电解质材料取代多孔塑性间隔物或分离物20,并且在这些情况下,聚合物电解质材料存在于复合阳极层14和复合阴极层16二者内。
当电池组电池完全充满电时,锂经由电解质而从含锂金属氧化物输运到基于石墨的层中,在该处,锂与石墨反应生成化合物LiC6。作为复合阳极层中的电化学活性材料,石墨具有372mAh/g的最大容量。注意,在负载两端设置电池组的意义上使用术语“阳极”和“阴极”。
通常认为,当将硅用作锂离子可再充电电池中的活性阳极材料时,硅提供的容量显著高于当前所使用的石墨。当通过在电化学电池中硅与锂反应而转变为化合物Li21Si5时,硅具有4200mAh/g的最大容量,该容量显著高于石墨的最大容量。因此,如果在锂可再充电电池组中可用硅来取代石墨,便可以实现所希望的每单位质量和每单位体积的存储的能量的增加。
在锂离子电化学电池中使用硅或基于硅的活性阳极材料的现有方法不能在经过了所需数目的充电/放电循环之后维持容量,因此在商业上是不可用的。
本领域中公开的一种方法使用粉末形式的硅(例如,具有10μm直径的颗粒或球基元(element)),在某些实例中其被制造为复合物(具有或不具有电子添加剂)并包含涂敷在铜集电体上的诸如聚偏氟乙烯的适宜的粘结剂。然而,该电极系统在经受重复的充电/放电循环时不能维持容量。认为该容量损失归因于硅粉末块(mass)的由与锂插入/抽离宿主硅相关联的体积膨胀/收缩导致的局部机械隔离。这反过来又引起硅基元与铜集电体 和其自身的电隔离。此外,体积膨胀/收缩使球基元破裂,从而导致在球基元本身内部的电接触的损失。
为处理在连续循环期间的大的体积变化的问题而设计的本领域中公知的另一方法为使构成硅粉末的硅基元的尺寸非常小,即,使用具有1-10nm范围的直径的球形颗粒。该方案假设纳米尺寸的基元可以经受与锂插入/抽离相关联的大的体积膨胀/收缩,而不会被破裂或损坏。然而,该方法具有的问题在于,其需要处理非常精细的纳米尺寸的粉末(这造成健康和安全风险),并且由于硅粉末要经受与锂插入/抽离相关的体积膨胀/收缩,因此不能防止球基元与铜集电体及其自身的电隔离。重要的是,纳米尺寸的基元的大表面积会导致含锂表面膜的产生,这会在锂离子电池组电池中引入大的不可逆容量。此外,对于给定质量的硅,大量的小尺寸的硅颗粒产生了大量的颗粒到颗粒接触,并且每一接触都具有接触电阻,由此导致硅块的电阻太高。上述问题由此使硅颗粒不能在商业上取代锂可再充电电池组组以及具体的锂离子电池组中的石墨。
在由Ohara等人在Journal of Power Sources 136(2004)303-306中的描述的另一方法中,将硅蒸发到镍箔集电体上作为薄膜,然后使用该结构形成锂离子电池的阳极。然而,虽然该方法提供了良好的容量保持,但这仅仅是使用非常薄的膜(例如,~50nm)的情况,并且由此这些电极结构不能提供可使用的量的每单位面积容量。增加膜厚度(例如,>250nm)会导致良好容量保持的消除。本发明的发明人认为这些薄膜的良好的容量保持归因于薄膜吸收与锂插入/抽离宿主硅相关联的体积膨胀/收缩而不会破裂或损坏膜的能力。并且,该薄膜具有比相等质量的纳米尺寸的颗粒低得多的表面积,由此减小了由含锂表面膜的形成而导致的不可逆容量的量。上述问题由此使在金属箔集电体上的硅薄膜不能在商业上取代锂可再充电电池组以及具体的锂离子电池组中的石墨。
在US2004/0126659中描述的另一方法中,将硅蒸发到镍纤维上,然后使用该镍纤维形成锂电池组的阳极。
然而,发现该方法在镍纤维上提供了不均匀的硅分布,由此显著影响 了操作。此外,这些结构具有镍集电体质量对活性硅质量的高比率,由此不能提供可使用的量的每单位面积或每单位质量的容量。
Kasavajjula等人(J.Power Sources(2006),doi:10.1016/jpowsour.2006.09.84)提供了对用于锂离子二次电池的基于纳米和体硅的插入电极的回顾,在此通过引用并入其内容。
在英国专利申请GB2395059A中描述的另一方法使用包括在硅衬底上制造的硅柱的规则或不规则阵列的硅电极。这些结构化的硅电极在经受重复的充电/放电循环时呈现良好的容量保持,本发明的发明人认为该良好的容量保持归因于硅柱吸收与锂插入/抽离宿主硅相关联的体积膨胀/收缩而不会破裂或损坏柱的能力。然而,在上述公开中描述的该结构化的硅电极是通过使用高纯度、单晶硅晶片而制成,因此制造的电极具有潜在的高成本。
发明内容
本发明的第一方面提供一种包括硅的颗粒,其具有颗粒核和从所述颗粒核延伸的包括硅的柱的阵列。
所述柱是规则或不规则的。本发明的柱的一个维度为0.08到0.70微米,优选0.1到0.5微米,更优选0.2到0.4微米,最优选0.3微米或更高。在第二维度,所述柱为4到100微米,优选10到80微米,更优选30微米或更高。所述柱由此具有大于20:1的纵横比。所述柱具有基本上圆形的截面或基本上非圆形的截面。
柱状颗粒包括未掺杂的硅、掺杂的硅、或混合物,例如硅-锗混合物。特别地,所述颗粒的硅纯度为90.00质量%到99.95质量%,优选90.0质量%到质量99.5%。可以用任何材料(例如磷、铝、银、硼和/或锌)来掺杂所述硅。所述颗粒为相对低纯度的冶金级的硅。
所述颗粒的截面是规则或不规则的,并且所述颗粒的直径为10μm到1mm,优选20μm到150μm,更优选25μm到75μm。
本发明的第二方面提供一种制造第一方面的颗粒的方法,包括蚀刻包 括硅的颗粒的步骤。特别地,通过化学反应蚀刻或电化交换蚀刻(galvanic exchange etching)来产生所述柱。
本发明的第三方面提供一种复合电极,其包含在本发明的第一方面中限定的颗粒作为其活性材料之一。特别地,第三方面提供了一种复合电极,其使用铜作为集电体。在第三方面的特征中,所述电极可以为阳极。
因此本发明的第三方面还提供一种包含上述的电极的电化学电池。特别地,提供一种电化学电池,其中阴极包括含锂化合物作为其活性材料,所述含锂化合物能够释放和再次吸收锂离子。具体而言,提供一种电化学电池,其中阴极包括基于锂的金属氧化物或磷酸盐作为其活性材料,优选LiCoO2、或LiMnxNixCo1-2xO2或LiFePO4
本发明还提供一种包括第一方面的颗粒的锂可再充电电池阳极。具体而言,提供一种阳极,其中颗粒为复合物的一部分。
第三方面还提供一种包括阳极和阴极的电池,其中所述阴极优选包括基于锂的材料,更优选地,锂钴二氧化物。
还提供一种由上述电池供电的装置。
本发明的第四方面提供一种产生复合电极的方法,包括以下步骤:制备包含柱状颗粒的基于溶剂的浆料;将所述浆料涂敷到集电体上;以及使所述溶剂蒸发以产生复合膜。
本发明还提供一种制造锂可再充电电池的方法,包括以下步骤:产生上述电极;以及添加阴极和电解质。具体地,该方法还包括在阴极与所述阳极之间添加分离物。围绕所述电池提供壳体。
还提供一种制造包括硅的纤维的方法,其中,通过刮、搅拌或化学蚀刻中的一种或多种使柱从第一方面的颗粒分离。
使用本发明的结构化的颗粒来制造阳极电极结构进一步克服了硅与锂的可逆反应的问题。具体地,通过在复合结构中设置颗粒,该复合结构为颗粒、聚合物粘结剂和导电添加剂的混合物,或者,通过直接将结构化的颗粒接合到集电体,充电/放电过程变为是可逆和可重复的,由此获得良好的容量保持。本发明的发明人认为该良好的可逆性归因于结构化的硅颗粒 的硅柱形成部分的吸收与锂插入/抽离宿主硅相关联的体积膨胀/收缩而不会破裂或损坏柱的能力。重要的是,本发明中描述的硅电极是通过使用低纯度、冶金级硅制成,因此制造的电极具有潜在的低成本。
附图说明
将通过实例并参考附图来描述本发明的实施例,其中:
图1是示出了电池组电池的部件的示意图;
图2是根据本发明的实施例的柱状颗粒的电子显微图;
图3示出了总的电化交换蚀刻机制;以及
图4示出了电化交换蚀刻处理中的分电流形式的假想动力学曲线。
具体实施方式
总体上,本发明允许产生硅或包括硅的材料的柱状颗粒,并使用这些颗粒产生具有聚合物粘结剂、导电添加剂(如果需要)和金属箔集电体的复合阳极结构和电极结构。特别地,认为,构成复合物的所述颗粒的结构克服了充电/放电容量损失的问题。通过提供具有多个狭长的或细长柱的颗粒,可以减轻充电/放电容量损失的问题。
典型地,所述柱将具有约20:1的长度对直径比率。锂在柱中的插入和移出虽然会造成体积膨胀和体积收缩,但不会造成对柱的毁坏,因此保持了纤维内的导电性。
通过湿法蚀刻/使用例如在共同待审的具有共同受让人的名称为“Method of etching a silicon-based material”的申请GB 0601318.9(在此通过引用并入其内容)中描述的化学电化交换方法,制造所述柱。还可以使用的相关方法已在Peng K-Q,Yan,Y-J Gao,S-P,Zhu J,Adv.Materials,14(2004),1164-1167(“Peng”);K.Peng等,Angew.Chem.Int.Ed.,442737-2742;以及K.Peng等,Adv.Funct.Mater.,16(2006),387-394;K.Peng,Z.Huang and J.Zhu,Adv.Mater.,16(2004),127-132;以及T.Qui,L.Wu,X.Yang,G.S.Huang and Z.Y.Zhang,Appl.Phys. Lett.,84(2004),3867-3869中公开。上述方法用于由高纯度的硅晶片制造柱。
在本发明的优选实施例中,在诸如冶金级硅的相对低纯度硅的晶体颗粒上制造柱。该方法包括五个步骤:研磨和筛选;清洗;成核;蚀刻;以及银去除,随后将仅以实例的方式来解释。图2示出了根据本发明制造的柱状颗粒的电子显微图。
任何合适的研磨工艺是适用的,例如,粉末研磨或球磨。本领域的技术人员可以理解,将存在这样的最小颗粒尺寸,如果小于该尺寸,则柱不能被蚀刻到表面上而是会均匀地蚀刻掉颗粒。具有小于0.5μm直径的颗粒将太小。
通过在蚀刻之前成核,产生就密度和高度而言更均匀的柱阵列。该步骤产生银核/岛(核组合和形成作为柱生长的部位的银岛)的均匀分布。
银岛勾画出柱的形成和{100}面的电化氟化物蚀刻,参见图3。参考图3,示出了具有柱307的硅表面301。电子305从氟化物离子303转移到硅表面301。氟与硅301和氟化物离子的反应产生了氟硅酸盐离子305。这是阳极蚀刻过程。阴极过程是银离子309的放电以形成金属银311。
通过假设硅-氟化物键的形成是在蚀刻过程中的主要步骤来解释该结构。此外,Si-F(单氟化物)的结构是稳定的,并且F-Si-F(双氟化物)的结构和Si[-F]3(三氟化物)的结构是不稳定的。这是因为对最邻近基团的Si表面的位阻干扰。在{111}面的情况为,单氟化物表面(除边缘处之外是稳定的)不可避免地会行进到三氟化物表面,因此是不稳定的。{110}表面是硅的唯一的稳定的主晶面,将只具有单氟化物键,因此是稳定的,并且蚀刻速率比率[蚀刻速率<100>]:[蚀刻速率<110>]为约三个数量级。所以柱的侧面将终结在{110}面。
使用柱表面密度来定义在颗粒的表面上的柱的密度。这里,其被定义为F=P/[R+P],其中,F为柱表面密度,P为颗粒的被柱占据的总表面积,R为颗粒的未被柱占据的总表面积。
柱表面密度越大,硅颗粒电极的每单位面积的锂容量越大,并且可用 于产生纤维的可收获的柱的量越大。
例如,使用来自Elken of Norway的具有400×300×200μm的蚀刻前尺寸的上述硅粉末,在整个表面上产生的柱具有约25到30μm的柱高度,约200到500nm的直径,以及10-50%,更典型地,30%的柱表面密度F。
例如,发现具有约63-80×50×35μm的蚀刻前尺寸的颗粒可以制造高度为约10到15μm,覆盖率为约30%且直径为约200到500nm的柱。
在优选的实施例中,可以在包括硅的颗粒上且由包括硅的颗粒制造例如长度为100μm并且直径为0.2μm的柱。更一般地,由具有10到1000μm的初始尺寸的颗粒可以制成长度范围为4到100微米并且直径或横向尺寸的范围为0.08到0.70微米的柱。
根据该方法,硅颗粒主要为n或p型,并且,根据化学方法,可以在任何暴露的(100)、(111)或(110)晶面上蚀刻。因为蚀刻沿晶面进行,因此产生的柱为单晶。由于该结构特征,柱将基本上是直的,有助于大于20:1的长度对直径比率。
然后,使用柱状颗粒形成复合电极,如下面所述。可替代地,使柱从颗粒分离,并使用柱形成基于纤维的电极。分离的柱还可以描述为纤维。
本发明包括从颗粒分离柱。可将附有柱的颗粒置于烧杯或任何合适的容器中,使其覆盖在诸如乙醇或水的惰性液体中,并对其进行超声搅拌。发现在几分钟内,观察到液体是浑浊的,并且通过电子显微检测观察到在该阶段所述柱已经从颗粒去除。
在一个实施例中,在两阶段处理中从颗粒去除柱。在第一阶段,在水中多次清洗颗粒,并且如果需要,在低真空系统中干燥以去除水。在第二阶段,在超声浴中搅拌颗粒以使柱分离。它们悬浮在水中,然后使用不同的各种过滤纸尺寸进行过滤,以收集硅纤维。
应该理解,用于“收获”柱的可替代的方法包括刮颗粒表面以分离柱或化学地分离柱。一种适用于n型硅材料的化学方法包括在存在背侧照射的条件下在HF溶液中蚀刻颗粒。
一旦制成了柱状颗粒,就可将其用作锂离子电化学电池的复合阳极中 的活性材料。为了制造复合电极,将柱状颗粒与聚偏氟乙烯混合,制成具有浇注(casting)溶剂(例如,n-甲基吡咯烷二酮)的浆料。然后,例如,用刮刀或以任何其他合适的方式物理地将该浆料施加到或涂敷到金属板或金属箔或其他导电衬底上,以获得所需厚度的涂敷的膜,然后使用合适的干燥系统使浇注溶剂从该膜蒸发,以留下没有或基本没有浇注溶剂的复合膜,其中该合适的干燥系统采用范围为50摄氏度到140摄氏度的升高的温度。产生的复合膜具有多孔结构,其中基于硅的柱状颗粒的质量典型地在70%到95%之间。该复合膜的百分比孔隙容量为10-30%,优选约20%。
此后,以任何合适的方式,例如,按照图1示出的常规结构,进行锂离子电池组电池的制造,但却使用包括硅的活性阳极材料而不是石墨活性阳极材料。例如,通过多孔隔离物18覆盖基于硅颗粒的复合阳极层,将电解质添加到最终的结构中,浸透所有的可利用的孔隙容量。电解质添加在将电极置于合适的壳体中之后实施,且可包括阳极的真空填充,以确保用液体电解质填充孔隙容量。
一些实施例提供了包含多个柱状硅颗粒作为其活性材料的电极。容量保持性被改善,因为硅的柱状结构允许适应与锂的插入/抽离(充电和放电)相关联的体积膨胀。有利地,通过蚀刻低纯度的硅(称为冶金级硅)的团块(lump)而产生柱状颗粒,以便硅核保持为被直径在0.08μm与0.5μm之间并且长度在4μm与150μm之间的柱覆盖。
这里描述的方法的具体优点为,与目前在锂离子电池组电池的基于石墨的阳极的情况一样地,可以制造大的基于硅的阳极的片,然后对其进行轧制(roll),或者随后冲压成型,意味着可以利用现有的制造能力改造这里描述的方法。
将通过参考一个或多个下面的非限制性的实例来示例本发明。
研磨和筛选
在第一阶段,研磨并筛选广泛可得的冶金级硅(例如,来自Elkem of Norway的“Silgrain”),以产生范围在10到1000μm,优选30到300μm,更优选50到100μm的颗粒。
清洗
第二阶段包括在水中清洗研磨和筛选后的颗粒以去除附着在大颗粒上的任何细颗粒。然后,在稀释的HNO3(1mol·L)或H2SO4/H2O2(体积比1:2)或H2O2/NH3H2O/H2O2(体积比1:1:1)中处理清洗后的颗粒10分钟,以除去可能的有机或金属杂质。
成核
在第三阶段,在室温(~23℃)下,使用约400×300×200μm尺寸的0.1g的硅颗粒,在17.5ml HF(40%)+20ml AgNO3(0.06mol/l)+2.5ml EtOH(97.5%)+10ml H2O的溶液中进行成核反应7~10分钟。对于相同重量的硅,硅颗粒越小,由于表面积对体积的比率的增加,因此需要的溶液体积越大。
室温下乙醇的作用为减慢化学过程,这提供更均匀分布的银岛。时间(尤其是上限)要足以消耗显著量的溶液银。
蚀刻
第四阶段包括蚀刻。在室温(~23℃)下,使用约400×300×200μm尺寸的0.1g的硅颗粒,在17.5ml HF(40%)+12.5ml Fe(NO3)3(0.06mol·l)+2ml AgNO3(0.06mol·l)+18ml H2O的溶液,进行蚀刻反应1~1.5小时。对于相同重量的硅,硅颗粒越小,由于表面积对体积的比率的增加,因此需要的溶液体积越大。此外,当颗粒尺寸减小时,越小的硅颗粒需要的时间越短,例如,对于100~120μm(筛选尺寸)样品为30分钟,对于63~80μm样品为20分钟。
在进一步的修改例中,搅拌使蚀刻速率增大,这可能因为释放了氢。这里,氟硅酸盐离子的外扩散是速率限制。
技术人员将理解,除Ag+之外的氧化剂同样适用。例如,K2PtCl6、Cu(NO3)2、Ni(NO3)2、Mn(NO3)2、Fe(NO3)3、Co(NO3)2、Cr(NO3)2、Mg(NO3)2。包括具有高于氢的电势的Cu和Pt的化合物提供金属沉积(Cu和Pt),但除镍之外的其他金属却不可以。
可以使用图3和4示例总的电化交换蚀刻机制。在图3中,阳极过程:
Si+6F-=SiF6 2-+4e-   (-1.24伏特)
是硅的局部蚀刻。而与银离子放电相伴的电子去除是阴极过程:
Ag++e-=Ag   (+0.8伏特)
在标准条件下,总的电池电压为2.04伏特。所关注的其他阴极偶对(couple)为Cu/Cu2+(+0.35V)、PtCl6 2-/PtCl4 2-+(+0.74V)、Fe3+/Fe2+(+0.77V),这是因为他们相对于氢都是正的。比H+/H2负性更强的偶对将与氢竞争,因此在很大程度上是无效的。图4示出了部分电极反应的示意图。
银去除
处理的最终阶段包括去除遗留在来自第三和第四阶段的蚀刻后的硅颗粒上的银。使用15%的HNO3溶液以5~10分钟的时间去除(并回收)银。
当然,应该理解,可以采用任何合适的方法来实现上述的方法和装置。例如,柱分离操作可以包括振动、刮、化学或其他操作中的任何一种,只要可以从颗粒去除柱。颗粒可以具有任何合适的尺寸并且可以为例如纯硅或掺杂的硅或其他包括硅的材料,例如硅-锗混合物或任何其他合适的混合物。产生柱的颗粒为n型或p型,范围从100到0.001欧姆·cm,或为合适的硅合金,例如,SixGe1-x。所述颗粒是冶金级硅。
所述颗粒和/或分离的柱可以用于任何适宜的目的,例如,制造通常包括阴极的电极。阴极材料可以为任何适宜的材料,典型地为基于锂的金属氧化物或磷酸盐材料,例如,LiCoO2、LiMnxNixCo1-2xO2或LiFePO4。不同实施例的特征可以根据需要而互换或并列,并且可以以任何适宜的次序实施方法步骤。
虽然可以蚀刻硅的相对高纯度的单晶晶片来制造具有希望的参数的柱,但由于其高的纯度,晶片自身是非常昂贵的。此外,难以将柱状晶片设置成电极几何形状。本发明的实施例是有利的,这是因为冶金级硅相对便宜,并且柱状颗粒自身可以并入到复合电极中而无需进一步的处理。并且,柱状颗粒是硅纤维的良好的源,并且其自身可以被用作电池组电极中的“活性”成分。
用于蚀刻的颗粒可以为晶体,例如具有等于或大于所需柱高度的微晶尺寸的单晶或多晶。多晶颗粒包括任何数目的晶体,例如两个或更多。
有利地,由于相对高的缺陷密度(与半导体工业中使用的硅晶片相比),冶金级硅特别适合作为电池组电极。这使得电阻低,且因此电导率高。
技术人员将理解,n型和p型硅二者都可以被蚀刻,并且,如果材料不显著退化,则任何电荷载流子密度都是适宜的。

Claims (36)

1.一种包括硅的颗粒,所述颗粒具有颗粒核和从所述颗粒核延伸的包括硅的柱的阵列。
2.根据权利要求1的颗粒,其中所述阵列是规则的。
3.根据权利要求1的颗粒,其中所述阵列是不规则的。
4.根据上述权利要求中的任一项的颗粒,其中所述柱具有范围为0.08到0.70微米的第一维度。
5.根据上述权利要求中的任一项的颗粒,其中所述柱具有范围为4到100微米的第二维度。
6.根据权利要求1到5中的任一项的颗粒,其中所述柱具有大于20:1的纵横比。
7.根据权利要求1到6中的任一项的颗粒,其中所述柱具有基本上圆形的截面。
8.根据权利要求1到7中的任一项的颗粒,其中所述柱具有基本上非圆形的截面。
9.根据上述权利要求中的任一项的颗粒,其中所述颗粒和/或柱包括未掺杂的硅、掺杂的硅或硅锗混合物。
10.根据上述权利要求中的任一项的颗粒,其中所述硅含量为90.00质量%到99.95质量%,优选90.0质量%到99.5质量%。
11.根据上述权利要求中的任一项的颗粒,其中所述颗粒为冶金级硅。
12.根据上述权利要求中的任一项的颗粒,其具有规则的截面。
13.根据上述权利要求中的任一项的颗粒,其具有不规则的截面。
14.根据上述权利要求中的任一项的颗粒,其第一维度为10μm到1mm,优选20μm到150μm,更优选25μm到75μm。
15.根据上述权利要求中的任一项的颗粒,其中所述颗粒核为晶体的或多晶的。
16.根据上述权利要求中的任一项的颗粒,其中所述颗粒核的被柱所占据的表面积的分数为0.10到0.50,优选0.20到0.40,更优选0.25到0.35。
17.一种制造根据权利要求1到16中的任一项的颗粒的方法,包括蚀刻包括硅的颗粒的步骤。
18.根据权利要求17的方法,其中通过化学反应蚀刻产生所述柱。
19.根据权利要求17的方法,其中通过电化交换蚀刻产生所述柱。
20.一种电极,其包含根据权利要求1到16中的任一项的颗粒作为其活性材料之一。
21.根据权利要求20的电极,其使用铜作为集电体。
22.根据权利要求20的复合电极,其中所述电极是阳极。
23.一种电化学电池,其包含根据权利要求20到22中的任一项的电极。
24.根据权利要求23的电化学电池,其中所述阴极包括含锂化合物作为其活性材料,所述含锂化合物能够释放和再吸收锂离子。
25.根据权利要求24的电化学电池,其中所述阴极包括基于锂的金属氧化物、硫化物或磷酸盐作为其活性材料。
26.一种锂可再充电电池阳极,其包括根据权利要求1到16中的任一项的颗粒作为其活性材料之一。
27.根据权利要求26的阳极,其中所述颗粒为复合膜的一部分。
28.一种电池,其包括阴极和根据权利要求26或27中任一项的阳极。
29.根据权利要求28的电池,其中所述阴极包括基于锂的材料。
30.根据权利要求29的电池,其中所述阴极包括锂钴二氧化物。
31.一种装置,其通过根据权利要求23到30中的任一项的电池供电。
32.一种产生复合电极的方法,其包括以下步骤:制备包含根据权利要求1到16中的任一项的颗粒的基于溶剂的浆料;将所述浆料涂敷到集电体上;以及蒸发所述溶剂以产生复合膜。
33.一种制造锂可再充电电池的方法,包括以下步骤:产生根据权利要求26或27的阳极;以及添加阴极和电解质。
34.根据权利要求33的方法,还包括在所述阴极与所述阳极之间添加分隔物。
35.根据权利要求33或34的方法,还包括围绕所述电池提供壳体。
36.一种制造包括硅的纤维的方法,其中通过刮、搅拌或化学蚀刻中的一种或多种使所述柱从根据权利要求1到16中的任一项的颗粒分离。
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