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TWI246212B - Anode material for lithium secondary cell with high capacity - Google Patents

Anode material for lithium secondary cell with high capacity Download PDF

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TWI246212B
TWI246212B TW093118302A TW93118302A TWI246212B TW I246212 B TWI246212 B TW I246212B TW 093118302 A TW093118302 A TW 093118302A TW 93118302 A TW93118302 A TW 93118302A TW I246212 B TWI246212 B TW I246212B
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carbon layer
anode material
metal core
core layer
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TW093118302A
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TW200501469A (en
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You-Min Kim
Ki-Young Lee
Seo-Jae Lee
Suk-Myung Roh
Ou-Jung Kwon
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Lg Chemical Ltd
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Description

1246212 九、發明說明： 【發明所屬之技術領域】 以及一種利 本發明係關於一種鋰二次電池之陽極材料 用此陽極材料之鋰二次電池。 【先前技術】 目前，碳質（carbonaceous)材料常作為鋰二次電池之陽 ㈣才料。然而，使用一具有較高容量之陽極材料以增加鋰二 -欠電池之電容是刻不容緩的。 10 15 為了達成這個目的，與鋰離子電化學地形成合金，且具 有高度充電/放電容量之金屬，如石夕、銘等，可被考慮作為 陽極=料。然而，此類以金屬為基礎的陽極材料，在鋰離子 進行嵌入/去嵌入（intercalation/deintercalati〇n)過程中，合谔 經極大的體積變化，因此該等活性材料終將彼此分離，= 離子電池具有低落的電池壽命特; 日本公開之申請案版2__297757揭露了一種陽極材 枓，其陽極材料包括1_相（例如：石夕）且具有至少一元辛 可進行鐘離子嵌入/去极入；以及一 β_相其係為一介金屬 (mtermetallic)化合物或一元素與另—以素組成之固能 20液。 心/ 然而，該習知技藝之陽極材料無法提供足夠且可接受的 電池壽命特徵’因此無法實際作為—鋰二次電池之陽：材 料0 1246212 【發明内容】 因此為了解決上述習知問題，本發 供一種链二次電池之陽極材料，俾能使該電池具有的^f充提/ 放電容量，以及較長的電池壽命特徵。 又充 5 10 15 本發明之另-目的係在提供—種鐘二次 料’其中包括-金屬層（核心層）具有鋰離子二二％:材 /去甘入之月匕力，其表面部分地或全部地依序覆 (a,〇« 〇 可:抑制一金屬在輯子嵌入/去嵌入過程中所造成之體積 改維持陽極材料粒子的高導電性，因而提m 放电合里以及良好的電池壽命特徵。 又 本發明之又一目的係在提供一-上述之陽極材料。μ、軸一二人電池，其係利用 為達成上述目的，本發明提供一種陽極 一金屬核心層，具備鋰齙孚舌、—山 具包括· 糸石山s计 重複嵌入及去後入能力；—非晶 二、、係塗佈於該金屬核心層之表面；以及—… 二、、係塗佈於該非晶系碳層之表面。根據本發明之另二二 。’本發明係提供_種利用上述陽極材料之鐘二次電'、也。 本發明之金屬核心層能夠提供高度充/放電容量。’ 此外’本發明之非晶系碳層與該晶質碳層可 在鐘離子嵌入/去嵌 卩利孟屬 較佳的電池壽命特徵私中所造成之體積變化，因而提供 力愈即使一金屬層（例如-由矽所構成之金屬層）且有導. 力與鋰離子僖導鈐士少 曰^ 百¥電 專V此力，而允許鋰離子之嵌入/去 20 1246212 順地使鋰離子嵌入/去嵌入之電子導電力依然太低。因此， 藉由形成一晶質碳層以降低在活性金屬層與集電體（current collector)之間、各金屬材料粒子之間之接觸阻力，而可提高 其鐘離子嵌入/去嵌入性質。 5 所形成的覆蓋層包括非晶系碳層以及晶質碳層，二者部 分地或全部地塗佈於於金屬核心層之表面。 同日守，忒1¼極材料從核心往外較佳依序包括了金屬核心 層、非晶系碳層、以及晶質碳層。 圖1係本發明一較佳實施例之陽極材料之剖面圖。從圖i 10中可見，該具有電化學充/放電能力之金屬表面，其表層覆 盍包括一非晶系碳層以及一晶質石炭層。 形成金屬核心層之金屬可包括至少一金屬選自一群組 包括：矽（S1)、鋁（A1)、錫（Sn)、銻（sb)、鉍（B1)、砷（As)、、 鍺（Ge)、鉛（Pb)、以及上述之合金。然而金屬之材質並無特 15殊限制，只要其能夠進行電化學及可逆之鋰離子嵌入/去嵌 入即可。 人 此非晶系碳層可包括從煤焦瀝f、石油瀝t及多種有機 物之中經由熱處理而獲得之含碳材料。 此晶質碳層可包括高度石墨化之天然石墨、人造石墨 2〇等，且以此石墨為基礎之材質可包括介穩相碳微粒ς (MesoCarbon MicroBead)、碳纖維及天然石墨。 金屬核心層、非晶系碳層與晶質碳層之較佳比例係為 9〇〜U)wt% : 〇·i〜50wt% : 9〜9〇_。若金屬核心層之含量低 於總量之1〇wt%時，充電容量低’因此不可能成為具有高電 1246212 容量之陽極材料。若曰片 非曰系π M ^，則不能有效抑制金屬之膨脹，而當 及Ϊ電^日之含量高於總量之5Gwt%時，則可能降低電容量 ίο 15 :::月，陽極材料可藉由以下步驟製備。此非晶系碳I ，輪沈積製程（如化學氣相沈積法、物理氣相沈積 2)直接形成於金屬層之上。或者，先在金屬核心層表面 各種有機前驅材料，如石油瀝青、煤焦瀝青、酚醛樹脂、 ^a^^(p〇iyvinyl chloride) ^^^SKpoiyvi^ alc〇h^ 等，接著將該前驅材料在惰性氣體下，在5〇〇〜13〇〇。〇下進行 30刀1里至3小日守之熱處理，以完成碳化，藉以將此非晶系石夏 =形成於金屬核心層之表面。接著，在一含有9〇〜98以％晷 質碳材料以及2〜l〇wt%之黏著劑（選擇性地含有5%或更少之 導電劑）之混合物中，加入足量的溶劑，參勻混合以得到4 泥狀聚體。將此泥狀漿體塗佈於非晶系碳層之上並乾燥之， 以付到晶質碳層。 在一種變化形式中，形成核心層的金屬先與晶質碳以^ 預定比例混合，例如金屬比晶質碳為10〜9〇wt%^ 90〜l〇wt%。接著，非晶系碳層以及晶質碳層可以同時藉由 如球磨法（ball mill)、機械融合法（meck^no-fusion)或其他機 械合金法（mechanical alloying)來形成。 機械合金法係藉由機械施力而使得生成物具有均一的 組成。 20

Claims (1)

  1. 5 十、申請專利範圍： 1 · 一種陽極材料，包括·· 二金屬核心層，具備雜子重複嵌人及去嵌入能力； 二^系碳層，其係覆蓋於該金屬核心層之表面；以及 -晶質碳層，其係覆蓋於該非晶系碳層之表面。 如申請專利範圍第1項所述之陽極材料，其中該金屬 核二係由—金屬或—合金所構成，該金屬或該合金係包括 ”、-金屬選自一由：矽、鋁、錫、銻、鉍、砷、鍺、以及 鉛組成之群組。 10 如申請專利範圍第1項所述之陽極材料，其中該金屬 核心層，表面係部分地或全部地被-塗佈層所覆蓋，該塗佈 層包括该非晶系碳層及該晶質碳層。 =如申請專利範圍第i項所述之陽極材料，其中該金屬 核心層、該非晶系碳層與該晶質碳層之比例係為9〇〜10重量 15百分比.（M〜50重量百分比：9〜9〇重量百分比。 …5·如中料利範圍第丨項所述之陽極材料，其中該非晶 糸石厌層包括有一碳原子層間距（㈣2)其係等於或大於 0.34nm ’且該非晶系碳層之厚度係等於或大於5·。 中請專利範圍第1項所述之陽極材料，其中該晶質 20石厌θ匕括有-碳原子層間距_2)其係、介於my麵至 〇/5麵之間’ j_該晶f碳層之厚度係介於1微米至職米之 17 1246212 7· —種鋰二次電池，其包括一陰極，一陽極，一非水 相電解液以及一隔離片，其中該陽極係使用申請專利範圍第 1貝至弟6項中任一項所述之陽極材料，該陽極材料係含： 一金屬核心層，具備鋰離子重複嵌入及去嵌入能力； 一非晶系碳層，其係覆蓋於該金屬核心層之表面；以及 一晶質碳層，其係覆蓋於該非晶系碳層之表面。 8· —種陽極材料之製備方法，該陽極材料係如申請專 利範圍第1項至第6項中任一項所述，該製備方法包括以^步 10 15 20 *、在一金屬核心層之表面形成一非晶系碳層，其係利用 膜沈積製程、或者先在該金屬核心層之表面塗佈瀝青或 前驅材料並熱處理以進行碳化，以塗佈—非晶系❹於1金 屬核心層之表面;以及塗佈一層含有晶質碳材質之; 於该非晶系碳層之表面’並乾燥之，以形成一晶質碳層-久-種陽極材料之製備方法，該陽極材料係如申曰 ^圍弟旧至第6項中任—項所述，該製備方法包括以^步 以及進行-機械合 質碳層於該金屬核 將一金屬形成一核心層並與晶質碳混合，· 金製程，以同時形成一非晶系碳層與一晶 心層之上。 ι〇·如中請專利範圍第9項所述之製備方法， 對δ亥晶質碳之混合比例為1 〇〜9〇 : 〜1 〇。 ζ盅屬 18
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