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在惰性气氛Ar和还原性气氛H2中通过高温裂解含苯环的聚硅氧烷分别制备了硅氧碳化物Si-O-C复合负极材料,并且采用了元素分析element analysis、广角粉末X射线衍射XRD、傅里叶激光拉曼光谱Raman等手段表征了二者组成和结构的差别.实验发现,在H2气氛中裂解制备的Si-O-C复合负极含有较高的可逆、较低的不可逆容量,而且可逆容量随温度的增加而增长.其中H2气氛中1000 ℃情况下制备的Si-O-C复合负极的可逆容量622 mAh/g,首次库仑效率59%.Si-O-C复合负极的不可逆容量与氧的含量相关,可逆容量可能与碳含量及碳结构,以及SiOC中硅的结构相关.在H2气氛中制备的Si-O-C负极材料是一种潜在的锂离子电池的负极材料.Silicon Oxycarbide (Si-O-C) composite anode materials are prepared by pyrolysis of polysiloxane containing phenyl under argon and hydrogen atmospheres, separately. They are characterized by element analysis, wide-angle powder X-ray diffraction, Raman spectroscopy for comparison with each other. It is found that the silicon oxycarbide composite anode pyrolyzed under a hydrogen atmosphere demonstrates lower irreversible capacity and larger reversible capacity which increases with temperature rising. The one pyrolyzed at 1000 ℃ shows a reversible capacity of 622 mAh/g, and first coulombic efficiency of 59%.The magnitude of the irreversible capacity is correlated with the content of oxygen, and the reversible capacity is related to the content and structure of free carbon, and also the structure of Si-O-C. It is believed that Si-O-C composite materials pyrolyzed under a hydrogen atmosphere could be promising anode materials for lithium ion batteries.
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Keywords:
- silicon oxycarbide /
- anode material /
- lithium ion battery
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[65] -
[1] Hou Z F, Liu H Y, Zhu Z Z, Huang M C, Yang Y 2003 Acta Phys. Sin. 52 952(in Chinese)[侯柱锋、刘慧英、朱梓忠、黄美纯、杨 勇 2003 物理学报 52 952]
[2] Hou X H, Hu S J, Li W S, Zhao L Z, Yu H W, Tan C L 2008 Acta Phys. Sin. 57 2375(in Chinese)[侯贤华、胡社军、李伟善、赵灵智、余洪文、谭春林 2008 物理学报 57 2375]
[3] [4] [5] Lee H Y, Lee S M 2004 Electrochem. Commun. 6 465
[6] Zhang X W, Patil P K, Wang C, Appleby A J, Little F 2004 J. Power Sources 125 206
[7] [8] Chan C K, Peng H, Liu G, McIlwrath K, Zhang X F, Huggins R A, Cui Y 2007 Nat.Nanotechnol. 3 31
[9] [10] Kasavajjula U, Wang C, Appleby A J 2007 J. Power Sources 163 1003
[11] [12] [13] Maranchi J P, Hepp A F, Kumta P N 2003 Electrochem. Solid-State Lett. 6 A198
[14] Lee K L, Jung J Y, Lee S W, Moon H S, Park J W 2004 J. Power Sources 129 270
[15] [16] [17] Ohara S, Suzuki J, Sekine K, Takamura T 2004 J. Power Sources 136 303
[18] [19] Uehara M, Suzuki J, Tamura K, Sekine K, Takamura T 2005 J. Power Sources 146 441
[20] Chen L, Wang K, Xie X, Xie J 2006 Electrochem. Solid-State Lett. 9 A512
[21] [22] Chen L B, Yu H C, Xu C M, Wang T H 2009 Acta Phys. Sin. 58 5029 (in Chinese)[陈立宝、虞红春、许春梅、王太宏 2009 物理学报 58 5029]
[23] [24] Dimov N, Kugino S, Yoshio M 2003 Electrochim. Acta 48 1579
[25] [26] [27] Wen Z S, Yang J, Wang B F, Wang K, Liu Y 2003 Electrochem. Commun. 5 165
[28] Wang G X, Ahn J H, Yao J, Bewlay S, Liu H K 2004 Electrochem. Commun. 6 689
[29] [30] [31] Wang G X, Yao J, Liu H K 2004 Electrochem. Solid-State Lett. 7 A250
[32] Datta M K, Kumta P N 2006 J. Power Sources 158 557
[33] [34] Xing W, Wilson A M, Zank G, Dahn J R 1997 Solid State Ionics 93 239
[35] [36] [37] Wilson A M, Xing W, Zank G, Yates B, Dahn J R 1997 Solid State Ionics 100 259
[38] [39] Wilson A M, Reimers J N, Fuller E W, Dahn J R 1994 Solid State Ionics 74 249
[40] Wilson A M, Zank G, Eguchi K, Xing W, Dahn J R 1997 J. Power Sources 68 195
[41] [42] [43] Ning L, Wu Y, Wang L, Fang S, Holze R 2005 J. Solid State Electrochem. 9 520
[44] Shen J, Ahn D, Raj R 2010 J. Power Sources 196 2875
[45] [46] Ahn D, Raj R 2011 J. Power Sources 196 2179
[47] [48] [49] Ahn D, Raj R 2010 J. Power Sources 195 3900
[50] Fukui H, Ohsuka H, Hino T, Kanamura K 2009 Chem. Lett. 38 86
[51] [52] Konno H, Morishita T, Wan C, Kasashima T, Habazaki H, Inagaki M 2007 Carbon 45 477
[53] [54] [55] Fukui H, Ohsuka H, Hino T, Kanamura K 2010 ACS Appl. Mater. Interfaces 2 998
[56] Ferrari A C, Robertson J 2000 Phys. Rev. B 61 14095
[57] [58] Soraru G D, DAndrea G, Campostrini R, Babonneau F, Mariotto G 1995 J. Am. Ceram. Soc. 78 379
[59] [60] [61] Wilson A M 1994 Ph. D. Dissertation (Ottawa:Simon Fraser University)
[62] Wang S, Matsumura Y, Maeda T 1995 Synth. Met. 71 1759
[63] [64] Buiel E, George A E, Dahn J R 1998 J. Electrochem. Soc. 145 2252
[65]
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