JP7337267B2 - 二次電池、及び該二次電池を備えた装置 - Google Patents
二次電池、及び該二次電池を備えた装置 Download PDFInfo
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- JP7337267B2 JP7337267B2 JP2022520094A JP2022520094A JP7337267B2 JP 7337267 B2 JP7337267 B2 JP 7337267B2 JP 2022520094 A JP2022520094 A JP 2022520094A JP 2022520094 A JP2022520094 A JP 2022520094A JP 7337267 B2 JP7337267 B2 JP 7337267B2
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- secondary battery
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- 239000000654 additive Substances 0.000 claims description 53
- 230000000996 additive effect Effects 0.000 claims description 51
- 239000003960 organic solvent Substances 0.000 claims description 34
- 239000008151 electrolyte solution Substances 0.000 claims description 28
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- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 20
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 20
- 239000007773 negative electrode material Substances 0.000 claims description 13
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 12
- 239000007774 positive electrode material Substances 0.000 claims description 12
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 10
- 229910052801 chlorine Inorganic materials 0.000 claims description 10
- 150000001875 compounds Chemical class 0.000 claims description 10
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- 125000006736 (C6-C20) aryl group Chemical group 0.000 claims description 4
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- 229910052744 lithium Inorganic materials 0.000 claims description 4
- 125000000027 (C1-C10) alkoxy group Chemical group 0.000 claims description 3
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical class [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims description 3
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical class [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 0.000 claims description 3
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical class [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 claims description 3
- 229910052739 hydrogen Inorganic materials 0.000 claims description 3
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 claims description 3
- 229910021382 natural graphite Inorganic materials 0.000 claims description 3
- QJMMCGKXBZVAEI-UHFFFAOYSA-N tris(trimethylsilyl) phosphate Chemical compound C[Si](C)(C)OP(=O)(O[Si](C)(C)C)O[Si](C)(C)C QJMMCGKXBZVAEI-UHFFFAOYSA-N 0.000 claims description 3
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 claims description 2
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 2
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910000676 Si alloy Inorganic materials 0.000 claims description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 2
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical class [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 2
- UMVBXBACMIOFDO-UHFFFAOYSA-N [N].[Si] Chemical class [N].[Si] UMVBXBACMIOFDO-UHFFFAOYSA-N 0.000 claims description 2
- 125000001931 aliphatic group Chemical group 0.000 claims description 2
- 229910021385 hard carbon Inorganic materials 0.000 claims description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 2
- 229910002102 lithium manganese oxide Inorganic materials 0.000 claims description 2
- ILXAVRFGLBYNEJ-UHFFFAOYSA-K lithium;manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[O-]P([O-])([O-])=O ILXAVRFGLBYNEJ-UHFFFAOYSA-K 0.000 claims description 2
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- 229910021384 soft carbon Inorganic materials 0.000 claims description 2
- VNLMVEHAAAAZPP-UHFFFAOYSA-N tris(triethylsilyl) phosphate Chemical compound CC[Si](CC)(CC)OP(=O)(O[Si](CC)(CC)CC)O[Si](CC)(CC)CC VNLMVEHAAAAZPP-UHFFFAOYSA-N 0.000 claims description 2
- XCGWLSWJFSFGKT-UHFFFAOYSA-N tris[ethenyl(dimethyl)silyl] phosphate Chemical compound C=C[Si](C)(C)OP(=O)(O[Si](C)(C)C=C)O[Si](C)(C)C=C XCGWLSWJFSFGKT-UHFFFAOYSA-N 0.000 claims description 2
- 125000003837 (C1-C20) alkyl group Chemical group 0.000 claims 1
- 125000003358 C2-C20 alkenyl group Chemical group 0.000 claims 1
- 125000003342 alkenyl group Chemical group 0.000 claims 1
- 125000000217 alkyl group Chemical group 0.000 claims 1
- 125000000304 alkynyl group Chemical group 0.000 claims 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 claims 1
- 229910001386 lithium phosphate Inorganic materials 0.000 claims 1
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 claims 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 claims 1
- TWQULNDIKKJZPH-UHFFFAOYSA-K trilithium;phosphate Chemical compound [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O TWQULNDIKKJZPH-UHFFFAOYSA-K 0.000 claims 1
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- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 2
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- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910015872 LiNi0.8Co0.1Mn0.1O2 Inorganic materials 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
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- 230000003446 memory effect Effects 0.000 description 1
- PQIOSYKVBBWRRI-UHFFFAOYSA-N methylphosphonyl difluoride Chemical group CP(F)(F)=O PQIOSYKVBBWRRI-UHFFFAOYSA-N 0.000 description 1
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- 229910052757 nitrogen Inorganic materials 0.000 description 1
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- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
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- YZYKZHPNRDIPFA-UHFFFAOYSA-N tris(trimethylsilyl) borate Chemical compound C[Si](C)(C)OB(O[Si](C)(C)C)O[Si](C)(C)C YZYKZHPNRDIPFA-UHFFFAOYSA-N 0.000 description 1
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- C07D307/00—Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom
- C07D307/02—Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings
- C07D307/34—Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members
- C07D307/56—Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D309/00—Heterocyclic compounds containing six-membered rings having one oxygen atom as the only ring hetero atom, not condensed with other rings
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D313/00—Heterocyclic compounds containing rings of more than six members having one oxygen atom as the only ring hetero atom
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- C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
- C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic Table
- C07F9/02—Phosphorus compounds
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- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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Description
で示される化合物から選択される1つ以上である。
で示される化合物から選択される1つ以上である。
で示される化合物から選択される1つ以上である。
で示される化合物から選択される1つ以上である。
正極活物質(LiNi0.8Co0.1Mn0.1O2)、導電剤Super P、及び接着剤であるフッ化ポリビニリデンを98:1:1の質量比で混合して、溶媒であるN-メチルピロリドンを加え、真空ミキサーにより系が均一な透明状となるまで撹拌し、正極スラリーを取得した。この正極スラリーを正極集電体としてのアルミ箔上に均一に塗布し、アルミ箔を室温で乾燥させた後にオーブンに移して乾燥させ、その後、コールドプレス、切断により正極板を得た。
負極活物質である一酸化ケイ素と人工黒鉛とを2:8の質量比で混合した後、導電剤であるSuper P、増粘剤であるカルボキシメチルセルロースナトリウム(CMC-Na)、及び接着剤であるスチレンブタジエンゴム(SBR)を92:2:2:4の質量比で混合して、脱イオン水を加え、真空ミキサーにより負極スラリーを取得した。この負極スラリーを負極集電体銅箔上に均一に塗布し、銅箔を室温で乾燥させた後にオーブンに移して乾燥させ、その後、コールドプレス、切断により負極板を得た。
含水量<10ppmのアルゴン雰囲気のグローブボックスにおいて、混合有機溶媒を製造した。続いて、十分に乾燥させた電解質塩をこの混合有機溶媒に溶解し、次に、添加剤を加え、均一に混合して電解液を取得した。電解液において使用した有機溶媒及び添加剤の具体的な種類及び含有量を表1に示す。表1において、各有機溶媒は有機溶媒の総質量に基づいて算出した質量百分率であり、各添加剤の含有量は電解液の総質量に基づいて算出した質量百分率である。
ポリエチレンフィルムをセパレータとして使用した。
セパレータが正極板と負極板との間に介在して離間作用を果たすように正極板、セパレータ、負極板を順に積層し、次に巻き取って電極組立体を得た。この電極組立体を外装に入れて、上述により製造した電解液を、乾燥した後の電池に注入し、真空パッケージ、静置、フォーメーション、サイジング等の工程により、二次電池を取得した。
25℃で、二次電池を0.5C定電流で4.25Vに充電し、次に、4.25V定電圧で電流が0.05Cになるまで充電し、ドレン法でこの時の二次電池の体積をテストしてV1とした。その後、この二次電池を60℃の恒温ボックスに入れ、30日間貯蔵した後に取り出し、この時の二次電池の体積をテストしてV2とした。
二次電池を60℃で30日間貯蔵した後の体積膨張率(%)=[(V2-V1)/V1]×100%
である。
45℃で、二次電池を1C定電流で4.25Vに充電し、4.25V定電圧で電流が0.05Cになるまで充電し、5分間静置し、次に、1C定電流で2.5Vに放電した。これらは二次電池の初回サイクル充電/放電過程であり、この時の放電容量は二次電池の初回サイクルの放電容量とし、上記過程で二次電池に対して800回のサイクル充電/放電のテストを行い、800回サイクル後の二次電池の放電容量を記録した。
二次電池を45℃で800回サイクルした後の容量保持率(%)=(二次電池の800サイクル後の放電容量/二次電池の初回サイクルの放電容量)×100%
である。
25℃で、二次電池を0.5C定電流/定電圧で50%SOCに充電し、10分間放置し、次に0.1C定電流(I1)で10秒間放電し、放電した後の二次電池の電圧を記録してU1とし、次に二次電池を4C定電流(I2)で30秒間放電し、放電した後の二次電池の電圧を記録してU2とした。
二次電池の直流インピーダンスDCR=(U1-U2)/(I2-I1)
である。
2・・・上筐体
3・・・下筐体
4・・・電池モジュール
5・・・二次電池
Claims (16)
- 負極板と、電解液とを備え、
前記負極板は、負極集電体と、負極集電体の少なくとも1つの表面上に設置され且つ負極活物質を含む負極シートとを備え、
前記電解液は、電解質塩と、有機溶媒と、添加剤とを含む、二次電池であって、
前記負極活物質は、シリコン系材料を含み、
前記有機溶媒は、前記有機溶媒中の質量比率20%以下の炭酸エチレン(EC)と、前記有機溶媒中の質量比率20%以下の炭酸ジエチル(DEC)とを含み、
前記有機溶媒は、炭酸エチルメチル(EMC)をさらに含み、前記有機溶媒中の前記炭酸エチルメチル(EMC)の質量比率は、50%よりも多く、
前記添加剤は、添加剤Aと、添加剤Bとを含み、
前記添加剤Aは、下記式1及び式2:
n1の値は0、1、2、3、4又は5であり、
n2の値は0、1、2、3、4、5、6、7、8又は9であり、
R11、R12、R13、R14、R21、R22、R23、及びR24は、それぞれ独立に、H、F、Cl、Br、I、置換又は非置換C1~C10の鎖状アルキル、置換又は非置換C1~C10の鎖状アルケニル、置換又は非置換C1~C10の鎖状アルキニル、C1~C10の脂肪族基、置換又は非置換C3~C9の環状アルキル、置換又は非置換C1~C10のアルコキシ、置換又は非置換C6~C20のアリール、及び置換又は非置換C3~C20のヘテロアリールから選択される1種であり、置換基はF、Cl、及びBrから選択される1つ以上である。)
で示される化合物から選択される1つ以上であり、
前記添加剤Bは、下記式3:
R31、R32、R33、R34、R35、R36、R37、R38、及びR39は、それぞれ独立に、置換又は非置換C1~C20のアルキル、置換又は非置換C2~C20のアルケニル、置換又は非置換C2~C20のアルキニル、及び置換又は非置換C6~C20のアリールから選択される1種であり、置換基はF、Cl、及びBrから選択される1つ以上である。)
で示される化合物から選択される1つ以上である、二次電池。 - 前記有機溶媒中の前記炭酸エチレン(EC)の質量比率は、10%~20%である、請求項1に記載の二次電池。
- 前記有機溶媒中の前記炭酸ジエチル(DEC)の質量比率は、10%~20%である、請求項1~2のいずれか一項に記載の二次電池。
- 前記電解液中の前記添加剤Aの質量比率は、1%以下である、請求項1~3のいずれか一項に記載の二次電池。
- 前記電解液中の前記添加剤Bの質量比率は、2%以下である、請求項1~4のいずれか一項に記載の二次電池。
- 前記有機溶媒中の前記炭酸エチルメチル(EMC)の質量比率は、55%~65%である、請求項1~5のいずれか一項に記載の二次電池。
- 前記添加剤Aは、以下の化合物:
- 前記添加剤Bは、トリス(トリメチルシリル)ホスフェート、トリス(トリエチルシリル)ホスフェート、及びトリス(ビニルジメチルシリル)ホスフェートから選択される1つ以上である、請求項1~7のいずれか一項に記載の二次電池。
- 前記添加剤は、フルオロエチレンカーボネート(FEC)をさらに含み、前記電解液中の前記フルオロエチレンカーボネート(FEC)の質量比率は、8%以下である、請求項1~8のいずれか一項に記載の二次電池。
- 前記添加剤は、エチレンスルファート(DTD)、1,3-プロパンスルトン(PS)、1,3-プロペニル-スルトン(PST)、ジフルオロ(オキサラト)ホウ酸リチウム(LiDFOB)、及びジフルオロビス(オキサラト)リン酸リチウム(LiDFOP)から選択される1つ以上をさらに含む、請求項1~9のいずれか一項に記載の二次電池。
- 前記二次電池は、以下の(1)~(3):
(1)前記電解液の25℃における導電率は、7mS/cm~9.5mS/cmである;
(2)前記電解液の25℃における粘度は、3mPa・s~4.5mPa・sである;
(3)前記電解液中の前記電解質塩の濃度は、1.0mol/L~1.3mol/Lである
から選択される1つ以上の条件をさらに満たす、請求項1~10のいずれか一項に記載の二次電池。 - 前記シリコン系材料は、単体シリコン、シリコン炭素化合物、シリコン酸素化合物、シリコン窒素化合物、及びシリコン合金から選択される1つ以上を含む、請求項1~11のいずれか一項に記載の二次電池。
- 前記負極活物質は、炭素材料をさらに含み、前記炭素材料は、天然黒鉛、人工黒鉛、ソフトカーボン、及びハードカーボンから選択される1つ以上を含む、請求項1~12のいずれか一項に記載の二次電池。
- 前記二次電池は、正極板をさらに含み、
前記正極板は、正極集電体と、正極集電体の少なくとも1つの表面上に設置され且つ正極活物質を含む正極シートとを備え、
前記正極活物質は、リチウム・ニッケル・コバルト・マンガン酸化物化合物、及びリチウム・ニッケル・コバルト・アルミニウム酸化物から選択される1つ以上を含む、請求項1~13のいずれか一項に記載の二次電池。 - 前記正極活物質は、リチウムニッケル酸化物、リチウムマンガン酸化物、リン酸鉄リチウム、リン酸マンガンリチウム、リン酸リチウム鉄マンガン、コバルト酸リチウム及びそれらの変性化合物から選択される1つ以上をさらに含む、請求項14に記載の二次電池。
- 請求項1~15のいずれか一項に記載の二次電池を備えた装置。
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KR102651812B1 (ko) | 2024-03-26 |
WO2021128002A1 (zh) | 2021-07-01 |
EP3913717B1 (en) | 2023-06-07 |
EP3913717A1 (en) | 2021-11-24 |
US20220037697A1 (en) | 2022-02-03 |
JP2022550421A (ja) | 2022-12-01 |
KR20220052980A (ko) | 2022-04-28 |
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