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石墨烯吸附Li团簇的第一性原理计算

杨光敏 梁志聪 黄海华

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石墨烯吸附Li团簇的第一性原理计算

杨光敏, 梁志聪, 黄海华

The first-principle calculation on the Li cluster adsorbed on graphene

Yang Guang-Min, Liang Zhi-Cong, Huang Hai-Hua
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  • 构建了单层六方石墨烯超晶胞结构,以吸附不同尺寸的Li团簇,Li:C摩尔比例皆为1:6.采用基于密度泛函理论的第一性原理,计算了其态密度、差分电荷密度、能带,分析了Li团簇与石墨烯吸附前后的电荷分布情况及Li-C成键类型,二者之间的电荷分布决定了两者的相互作用.使用热力学的方法及成核机制进行分析,得出成核的可能性与团簇尺寸的关系,研究了一定浓度下的锂在石墨烯上的成核问题.相应的计算结果有助于理论上深入理解锂电池储能机理.
    As a stable single sheet of carbon atoms with a honeycomb lattice, graphene has become attractive for its potential applications in electrochemical storage devices, such as anodes for rechargeable Li batteries. Since both sides of it can hold adsorbents, a graphene sheet is expected to have extra storage sites and therefore it has a possibly higher capacity than graphite. However, certain shortcomings of Li battery, such as instability lead to battery failure under overcharging or overvoltage conditions. The limit to capacity results in a short time of discharge. Thus, more attention should be paid to the stabilities of electrode materials, such as Li cluster nucleation on graphene leading to dendrite formation and failure of the Li-ion battery. In this work, we build a supercell model of single layer graphene with hexagonal structure, and then change the size of Li cluster which is used to be adsorbed on graphene, with keeping m Li:C ratio at 1:6. Using the first principle based on density functional theory, we calculate the density of states, charge density difference and energy band structure. The interaction between Li and pristine graphene is studied in detail by analyzing the electronic properties and charge distribution of the isolated Li clusters and Li clusters adsorbed on graphene. It is found that the ionic bonding can be formed at the interface between Li clusters and graphene, and the charge transfer controls the interaction of the Li-carbon nanostructure. Combing thermodynamics method with the nucleation mechanism, the relationship between the cluster size and nucleation probability is analyzed, and the nucleation on graphene of Li with a certain concentration is also investigated. We estimate the nucleation barrier for Li on graphene and investigate the stability of Li adsorption on graphene by considering the effects of Li concentration and temperature. The Li concentration of 16.7% is considered for the formation of clusters with different sizes on graphene. With the size of Li cluster increasing, the cluster adsorbed on the graphene begins to be more stable than the single Li atom. The formation energy for the cluster is found to increase with the increase of temperature, and it is negative, meaning that Li cluster can be formed. It is expected that the corresponding calculation results from this atomistic simulation will shed some light on the in-depth understanding of Li-storage on graphene and the cycling stability and dendrite formation in Li-ion batteries with graphene-based materials serving as the anode.
      通信作者: 杨光敏, yangguangmin@cncnc.edu.cn
    • 基金项目: 长春师范大学自然科学基金(批准号:2015-010)资助的课题.
      Corresponding author: Yang Guang-Min, yangguangmin@cncnc.edu.cn
    • Funds: Project supported by the Natural Science Foundation of Changchun Normal University, China (Grant No. 2015-010).
    [1]

    Yoo E, Kim J, Hosono E, Zhou H, Kudo T, Honma I 2008Nano Lett. 8 2277

    [2]

    Lian P C, Zhu X F, Liang S Z, Li Z, Yang W S, Wang H H 2010Electrochim.Acta 55 3909

    [3]

    Jaber-Ansari L, Puntambekar K P, Tavassol H, Yildirim H, Kinaci A, Kumar R, Saldana S J, Gewirth A A, Greeley J P, Chan M K, Hersam M C 2014ACS Appl.Mater.Interfaces 6 17626

    [4]

    Zhao X, Hayner C M, Kung M C, Kung H H 2011ACS Nano 5 8739

    [5]

    Jang B Z, Liu C G, Neff D, Yu Z N, Wang M C, Xiong W, Zhamu A 2011Nano Lett. 11 3785

    [6]

    Wang D, Choi D, Li J, Yang Z, Nie Z, Kou R, Hu D, Wang C, Saraf L V, Zhang J, Aksay I A, Liu J 2009ACS Nano 3 907

    [7]

    Zheng J, Ren Z, Guo P, Fang L, Fan J 2011Appl.Surf Sci 258 1651

    [8]

    Lv W, Tang D M, He Y B, You C H, Shi Z Q, Chen X C, Chen C M, Hou P X, Liu C, Yang Q H 2009ACS Nano 3 3730-6

    [9]

    Wang G X, Shen X D, Yao J, Park J 2009Carbon 47 2049

    [10]

    Pan D, Wang S, Zhao B, Wu M, Zhang H, Wang Y, Jiao Z 2009Chem.Mater. 21 3136

    [11]

    Bhardwaj T, Antic A, Pavan B, Barone V, Fahlman B D J 2010Am.Chem.Soc. 132 12556

    [12]

    Ferre-Vilaplana A 2008J.Phys.Chem.C 112 3998

    [13]

    Froudakis G E 2001Nano Lett. 1 531

    [14]

    Garay-Tapia A M, Romero A H, Barone V 2012J.Chem.Theory Comput. 8 1064

    [15]

    Khantha M, Cordero N A, Molina L M, Alonso J A, Girifalco L A 2004Phys.Rev.B 70 125422

    [16]

    Chan K T, Neaton J B, Cohen M L 2008Phys.Rev.B 77 235430

    [17]

    Yang C K 2009Appl.Phys.Lett. 94 163115

    [18]

    Medeiros P V C, Mota F D, Mascarenhas A J S, de Castilho C M C 2010Nanotechnology 21 115701

    [19]

    Klintenberg M, Lebegue S, Katsnelson M I, Eriksson O 2010Phys.Rev.B 81 085433

    [20]

    Tarascon J M, Armand M 2001Nature 414 359

    [21]

    Mayers M Z, Kaminski J W, Miller Ⅲ T F 2012J.Phys.Chem.C 116 26214

    [22]

    Harris S J, Timmons A, Baker D R, Monroe C 2010Chem.Phys.Lett. 485 265

    [23]

    Kresse G, Furthmller J 1996J.Comput.Mater.Sci. 6 15

    [24]

    Blchl P E 1994Phys.Rev.B 50 17953

    [25]

    Perdew J P, Chevary J A, Vosko S H, Jackson K A, Pederson M R, Singh D J, Fiolhais C 1992Phys.Rev.B 46 6671

    [26]

    Yang G M, Zhang H Z, Fan X F, Zheng W T 2015J.Phys.Chem.C 119 6464

    [27]

    Fan X F, Liu L, Kuo J L, Shen Z X 2010J.Phys.Chem.C 114 14939

    [28]

    Henkelman R, Arnaldsson A, Jonsson H J 2006Comput.Mater.Sci. 36 354

    [29]

    Liu M, Kutana A, Liu Y, Yakobson B I 2014J.Phys.Chem.Lett. 5 1225

    [30]

    Pollak E, Geng B, Jeon K J, Lucas I T, Richardson T J, Wang F, Kostecki R 2010Nano Lett. 10 3386

  • [1]

    Yoo E, Kim J, Hosono E, Zhou H, Kudo T, Honma I 2008Nano Lett. 8 2277

    [2]

    Lian P C, Zhu X F, Liang S Z, Li Z, Yang W S, Wang H H 2010Electrochim.Acta 55 3909

    [3]

    Jaber-Ansari L, Puntambekar K P, Tavassol H, Yildirim H, Kinaci A, Kumar R, Saldana S J, Gewirth A A, Greeley J P, Chan M K, Hersam M C 2014ACS Appl.Mater.Interfaces 6 17626

    [4]

    Zhao X, Hayner C M, Kung M C, Kung H H 2011ACS Nano 5 8739

    [5]

    Jang B Z, Liu C G, Neff D, Yu Z N, Wang M C, Xiong W, Zhamu A 2011Nano Lett. 11 3785

    [6]

    Wang D, Choi D, Li J, Yang Z, Nie Z, Kou R, Hu D, Wang C, Saraf L V, Zhang J, Aksay I A, Liu J 2009ACS Nano 3 907

    [7]

    Zheng J, Ren Z, Guo P, Fang L, Fan J 2011Appl.Surf Sci 258 1651

    [8]

    Lv W, Tang D M, He Y B, You C H, Shi Z Q, Chen X C, Chen C M, Hou P X, Liu C, Yang Q H 2009ACS Nano 3 3730-6

    [9]

    Wang G X, Shen X D, Yao J, Park J 2009Carbon 47 2049

    [10]

    Pan D, Wang S, Zhao B, Wu M, Zhang H, Wang Y, Jiao Z 2009Chem.Mater. 21 3136

    [11]

    Bhardwaj T, Antic A, Pavan B, Barone V, Fahlman B D J 2010Am.Chem.Soc. 132 12556

    [12]

    Ferre-Vilaplana A 2008J.Phys.Chem.C 112 3998

    [13]

    Froudakis G E 2001Nano Lett. 1 531

    [14]

    Garay-Tapia A M, Romero A H, Barone V 2012J.Chem.Theory Comput. 8 1064

    [15]

    Khantha M, Cordero N A, Molina L M, Alonso J A, Girifalco L A 2004Phys.Rev.B 70 125422

    [16]

    Chan K T, Neaton J B, Cohen M L 2008Phys.Rev.B 77 235430

    [17]

    Yang C K 2009Appl.Phys.Lett. 94 163115

    [18]

    Medeiros P V C, Mota F D, Mascarenhas A J S, de Castilho C M C 2010Nanotechnology 21 115701

    [19]

    Klintenberg M, Lebegue S, Katsnelson M I, Eriksson O 2010Phys.Rev.B 81 085433

    [20]

    Tarascon J M, Armand M 2001Nature 414 359

    [21]

    Mayers M Z, Kaminski J W, Miller Ⅲ T F 2012J.Phys.Chem.C 116 26214

    [22]

    Harris S J, Timmons A, Baker D R, Monroe C 2010Chem.Phys.Lett. 485 265

    [23]

    Kresse G, Furthmller J 1996J.Comput.Mater.Sci. 6 15

    [24]

    Blchl P E 1994Phys.Rev.B 50 17953

    [25]

    Perdew J P, Chevary J A, Vosko S H, Jackson K A, Pederson M R, Singh D J, Fiolhais C 1992Phys.Rev.B 46 6671

    [26]

    Yang G M, Zhang H Z, Fan X F, Zheng W T 2015J.Phys.Chem.C 119 6464

    [27]

    Fan X F, Liu L, Kuo J L, Shen Z X 2010J.Phys.Chem.C 114 14939

    [28]

    Henkelman R, Arnaldsson A, Jonsson H J 2006Comput.Mater.Sci. 36 354

    [29]

    Liu M, Kutana A, Liu Y, Yakobson B I 2014J.Phys.Chem.Lett. 5 1225

    [30]

    Pollak E, Geng B, Jeon K J, Lucas I T, Richardson T J, Wang F, Kostecki R 2010Nano Lett. 10 3386

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出版历程
  • 收稿日期:  2016-09-17
  • 修回日期:  2016-12-04
  • 刊出日期:  2017-03-05

石墨烯吸附Li团簇的第一性原理计算

  • 1. 长春师范大学物理学院, 长春 130032;
  • 2. 吉林大学材料科学与工程学院, 长春 130012
  • 通信作者: 杨光敏, yangguangmin@cncnc.edu.cn
    基金项目: 长春师范大学自然科学基金(批准号:2015-010)资助的课题.

摘要: 构建了单层六方石墨烯超晶胞结构,以吸附不同尺寸的Li团簇,Li:C摩尔比例皆为1:6.采用基于密度泛函理论的第一性原理,计算了其态密度、差分电荷密度、能带,分析了Li团簇与石墨烯吸附前后的电荷分布情况及Li-C成键类型,二者之间的电荷分布决定了两者的相互作用.使用热力学的方法及成核机制进行分析,得出成核的可能性与团簇尺寸的关系,研究了一定浓度下的锂在石墨烯上的成核问题.相应的计算结果有助于理论上深入理解锂电池储能机理.

English Abstract

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