CN101507018A - 基于原硅酸盐衍生物的嵌锂电极材料 - Google Patents
基于原硅酸盐衍生物的嵌锂电极材料 Download PDFInfo
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Abstract
本发明提供一种基于原硅酸盐结构的嵌锂型正极材料以及该材料的发电器和可变光传输装置。
Description
本专利申请要求2006年8月21日提交的美国临时申请序列号60/839,026的优先权益,其内容以全文引入作为参考。
技术领域
本发明提供一种有序的Li3PO4结构的电极材料,其中氧形成可能变形的六方密排排列,且其中全部阳离子元素处于四面体配位中。还提供具有包含该材料的至少一个电极的发电器和可变光传输装置。
背景技术
具有橄榄石结构LiFePO4的电极材料(锂蓝铁矿)和拟同晶型的脱锂材料□FePO4(其中□表示Li空位;从LiFePO4中除掉Li后,Fe(2+)转变为Fe(3+)以维持电荷平衡)具有有利的工作电压3.5V,相对于Li+/Li°,也就是说,在液体和聚合物电解质的稳定性窗口中,但具有平坦的充电/放电(锂插入)平台。可逆性和显著的快速动力学的有利性能被认为与Li和两种氧化态的Fe在八面体环境中的制约有关。锰衍生物LiMnPO4,其在相对于Li+/Li°为4.2V时有活性,更理想地适合用于液体电解质。对于铁和锰衍生物二者来说,室温下在两相之间缺少可混性,这在相当程度上限制了通过过渡金属位置上的小极化子的电子电导率。
发明内容
现在已经发现,将过渡金属离子和锂离子制约到八面体位置,就像在LiMPO4橄榄石结构中(M=Fe或Mn或它们的固溶体),并不是有利的电极性能的先决条件。
本发明提供用于电极的材料,其属于有序的Li3PO4结构,以Li2FeSiO4和Li2MnSiO4和它们的固溶体为例,其中氧形成可能变形的六方密排排列,且其中全部的阳离子元素处于四面体配位中。另外,这些材料的结构通过异价或等电荷置换在阴离子或阳离子位置或这两种位置上可进行修改,以提供更好的锂离子扩散率和电子电导率。例如,这些置换能使在两种不同氧化态下的铁或锰在同一相中共存,或者引入与氧化还原水平接近于Fe和Mn的其他元素的特定相互作用(例如 等等),这两者都有利于电子电导率,同时在阴离子位置上的无序为Li+提供优先扩散位置。类似地,硅被磷、钒和/或铝部分置换,能够控制晶格参数以及因此的瓶颈尺寸,通过该瓶颈发生锂扩散。在钒的情况下,发生的额外氧化还原态增加了电极容量。另外,和LiMPO4相反,其中每个过渡金属离子中电子的数量限于一个,而本发明的材料有可能每个过渡金属离子交换一个以上的电子,尤其是用锰和钒。
因此,本发明提供了基于原硅酸盐结构的嵌锂型正极材料,其通式,式I,包括
Lix+yM1-(y+d+t+q+r)DdTtQqRr[SiO4]1-(p+s+v+a+b)[SO4]s[PO4]p[VO4]v[AlO4]a[BO4]b
其中
M是Mn2+或Fe2+或其组合;
D是+2氧化态的金属,选自Mg2+、Ni2+、Co2+、Zn2+、Cu2+、Ti2+和Ca2+;
T是+3氧化态的金属,选自Al3+、Ti3+、Cr3+、Fe3+、Mn3+、Ga3+、Zn2+和V3+;
Q是+4氧化态的金属,选自Ti4+、Ge4+、Sn4+和V4+;和
R是+5氧化态的金属,选自V5+、Nb5+和Ta5+。
此外,M、D、T、Q、R是位于Li2FeSiO4中Fe离子的四面体位置中的所有元素。V5+、Al3+和B3+的计量系数,分别是v,a和b,每个都位于Li2FeSiO4的四面体Si位置。计量系数x、y、d、t、q、r、p、s、v、a和b全部在0(包括本数)和1之间。或者,
0≤x≤2,
y+d+t+q+r<1,
p+s+v+a+b<1,和/或
3+2y+a+b=y+t+2q+3r+2s+p+v
其中x是电极材料工作期间的插入度。
本发明还提供一种发电器,其包括至少一个正极和至少一个负极,其中所述至少一个正极包含式I的材料,所述至少一个负极是高化学活性的锂离子源。
用于本发明的发电器负极中的锂离子源实例包括但不限于:金属锂、锂合金、锂-碳插层化合物、锂-钛尖晶石Li4+zTi5O12(0≤z≤3)以及它与其他尖晶石的固溶体、锂-过渡金属混合氮化物、及其混合物。
本发明发电器的正极可以进一步包含导电添加剂。用于本发明正极的导电添加剂的实例是碳。
替代地或此外,该正极可以进一步包含具有快速扩散动力学的插层材料。用于本发明正极的具有快速扩散动力学的插层材料实例包括层状的二硫族化合物(dichalcognenide),钒氧化合物VOx(2.1≤x≤2.5),Nasicon相关材料比如Li3Fe2(PO4)3,和碳涂覆的LiFe1-αMnαPO4,0≤α≤1。
此外,本发明发电器的正极可以进一步包含聚合粘合剂。优选该聚合粘合剂具有离子导电性。用于本发明的聚合粘合剂实例包括但不限于:聚酯,基于甲基丙烯酸甲酯的聚合物,基于丙烯腈的聚合物,基于偏氟乙烯的聚合物,四氟乙烯的均聚物或共聚物以及乙烯-丙烯-二烯三元共聚物。另外的聚合粘合剂的非限制实例包括羧甲基纤维素和聚苯乙烯磺酸,两者均为其氢形式,其锂盐、钠盐或钾盐形式。在一个实施方案中,该聚合粘合剂是交联或非交联的聚醚,并且溶解于盐中,其阳离子至少部分是Li+。另一个实施方案中,该聚合粘合剂被非质子溶剂溶胀并包含有盐,盐中的阳离子至少部分是Li+。用于该实施方案的非质子溶剂实例包括但不限于:碳酸亚乙酯,碳酸亚丙酯,碳酸二甲酯,碳酸二乙酯,碳酸甲乙酯,γ-丁内酯,四烷基氨基磺酰胺(tetraalkylsulfamide),分子量小于或等于2000的一、二、三、四或更高的低聚乙二醇的二烷基醚,及其混合物。
本发明还提供了可变光传输装置,包括涂覆透明半导体的玻璃或塑料以及被固体或凝胶电解质隔开的两个电极,其中至少一个电极包含式I的材料。在一个实施方案中,该电极通过真空淀积技术、溅射或由溶胶-凝胶前体在涂覆透明半导体的玻璃或塑料上铺设式I材料的薄膜来获得。
Claims (19)
1.一种基于原硅酸盐结构的嵌锂型正极材料,具有式I:
Lix+yM1-(y+d+t+q+r)DdTtQqRr[SiO4]1-(p+s+v+a+b)[SO4]s[PO4]p[VO4]v[AlO4]a[BO4]b
其中
M选自Mn2+和Fe2+及其组合;
D是+2氧化态的金属,选自Mg2+、Ni2+、Co2+、Zn2+、Cu2+、Ti2+和Ca2+;
T是+3氧化态的金属,选自Al3+、Ti3+、Cr3+、Fe3+、Mn3+、Ga3+、Zn2+和V3+;
Q是+4氧化态的金属,选自Ti4+、Ge4+、Sn4+和V4+;
R是+5氧化态的金属,选自V5+、Nb5+和Ta5+;和
M、D、T、Q、R是位于Li2FeSiO4中Fe离子的四面体位置中的元素;且
其中x、y、d、t、q、r、p、s、v、a和b在0和1之间;或
其中x在0和2之间,y+d+t+q+r小于1,p+s+v+a+b小于1,3+2y+a+b=y+t+2q+3r+2s+p+v。
2.一种包括至少一个正极和至少一个负极的发电器,其中所述至少一个正极包含权利要求1的嵌锂型正极材料,所述至少一个负极是高化学活性的锂离子源。
3.如权利要求2所述的发电器,其中所述至少一个负极包括金属锂、锂合金、锂-碳插层化合物、锂-钛尖晶石Li4+zTi5O12(0≤z≤3)以及它与其他尖晶石的固溶体、锂-过渡金属混合氮化物、或它们的混合物。
4.如权利要求2所述的发电器,其中所述至少一个正极还包含导电添加剂。
5.如权利要求4所述的发电器,其中所述导电添加剂包括碳。
6.如权利要求2所述的发电器,其中所述至少一个正极还包含具有快速扩散动力学的插层材料。
7.如权利要求6所述的发电器,其中所述具有快速扩散动力学的插层材料包括层状的二硫族化合物、钒氧化物VOx(2.1≤x≤2.5)或Nasicon相关材料或碳涂覆的LiFe1-αMnαPO4,0≤α≤1。
8.如权利要求7所述的发电器,其中所述Nasicon相关材料是Li3Fe2(PO4)3。
9.如权利要求2到5中任一项所述的发电器,其中所述至少一个正极还包含聚合粘合剂。
10.如权利要求9所述的发电器,其中所述聚合粘合剂包括四氟乙烯的均聚物或共聚物,或乙烯-丙烯-二烯三元共聚物。
11.如权利要求9或10所述的发电器,其中所述聚合粘合剂具有离子导电性。
12.如权利要求7所述的发电器,其中所述至少一个正极还包含聚合粘合剂。
13.如权利要求12所述的发电器,其中所述聚合粘合剂是交联或非交联的聚醚,且溶解于盐中,所述盐的阳离子至少部分是Li+。
14.如权利要求12所述的发电器,其中所述聚合粘合剂被非质子溶剂溶胀,并包含有盐,所述盐的阳离子至少部分是Li+。
15.如权利要求9所述的发电器,其中所述聚合粘合剂是聚醚、聚酯、基于甲基丙烯酸甲酯的聚合物、基于丙烯腈的聚合物或基于偏氟乙烯的聚合物。
16.如权利要求12所述的发电器,其中所述聚合粘合剂是羧甲基纤维素或聚苯乙烯磺酸,两者均为其氢形式,其锂盐、钠盐或钾盐形式。
17.如权利要求14所述的发电器,其中所述非质子溶剂是碳酸亚乙酯,碳酸亚丙酯,碳酸二甲酯,碳酸二乙酯,碳酸甲乙酯,γ-丁内酯,四烷基氨基磺酰胺,分子量为2000以下的一、二、三、四或更高的低聚乙二醇的二烷基醚,或它们的混合物。
18.一种可变光传输装置,包括:涂覆透明半导体的玻璃或塑料,以及由固体或凝胶电解质隔开的两个电极,其中至少一个电极包含权利要求1的嵌锂型正极材料。
19.如权利要求18所述的可变光传输装置,其中包括嵌锂型正极材料的电极通过如下而获得:通过真空淀积技术、溅射或由溶胶-凝胶前体在涂覆透明半导体的玻璃或塑料上铺设所述材料的薄膜。
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US3090094A (en) | 1961-02-21 | 1963-05-21 | Gen Motors Corp | Method of making porous ceramic articles |
US5976454A (en) | 1996-04-01 | 1999-11-02 | Basf Aktiengesellschaft | Process for producing open-celled, inorganic sintered foam products |
DE19612985A1 (de) | 1996-04-01 | 1997-10-02 | Basf Ag | Sinterschäume und Verfahren zu ihrer Herstellung |
US6514640B1 (en) * | 1996-04-23 | 2003-02-04 | Board Of Regents, The University Of Texas System | Cathode materials for secondary (rechargeable) lithium batteries |
JP3007868B2 (ja) | 1997-03-11 | 2000-02-07 | マツダ株式会社 | 金属多孔体および軽合金複合部材並びにこれらの製造方法 |
US6085015A (en) * | 1997-03-25 | 2000-07-04 | Hydro-Quebec | Lithium insertion electrode materials based on orthosilicate derivatives |
WO1999063612A1 (fr) * | 1998-06-04 | 1999-12-09 | Mitsubishi Chemical Corporation | Batterie secondaire contenant une solution electrolytique non aqueuse |
CA2270771A1 (fr) | 1999-04-30 | 2000-10-30 | Hydro-Quebec | Nouveaux materiaux d'electrode presentant une conductivite de surface elevee |
CA2271354C (en) * | 1999-05-10 | 2013-07-16 | Hydro-Quebec | Lithium insertion electrode materials based on orthosilicate derivatives |
DE19928997C2 (de) | 1999-06-24 | 2001-05-17 | Fraunhofer Ges Forschung | Verfahren und Vorrichtung zum Schäumen von Metallen |
DE60039748D1 (de) | 2000-03-14 | 2008-09-18 | Centre Nat Rech Scient | Neue Elektrodenmaterialen mit Lithium Interkalation auf Basis von Orthosilikatsderivaten |
US6852272B2 (en) | 2001-03-07 | 2005-02-08 | Advanced Ceramics Research, Inc. | Method for preparation of metallic and ceramic foam products and products made |
JP3960193B2 (ja) * | 2001-12-20 | 2007-08-15 | 株式会社デンソー | リチウム二次電池用電極及びリチウム二次電池並びにその製造方法 |
-
2007
- 2007-08-17 CN CNA2007800311526A patent/CN101507018A/zh active Pending
- 2007-08-17 WO PCT/EP2007/007288 patent/WO2008022750A1/en active Application Filing
- 2007-08-17 CA CA002661453A patent/CA2661453A1/en not_active Abandoned
- 2007-08-17 US US12/377,884 patent/US8236450B2/en not_active Expired - Fee Related
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN107666010A (zh) * | 2016-07-29 | 2018-02-06 | 比亚迪股份有限公司 | 一种锂离子电池固态电解质、其制备方法及锂离子电池 |
Also Published As
Publication number | Publication date |
---|---|
WO2008022750A1 (en) | 2008-02-28 |
CA2661453A1 (en) | 2008-02-28 |
US8236450B2 (en) | 2012-08-07 |
US20100104943A1 (en) | 2010-04-29 |
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