Chemical reactivity of aprotic electrolytes on a solid Li2O2 surface: screening solvents for Li-air batteries

被引:29
作者
Laino, Teodoro [1 ]
Curioni, Alessandro [1 ]
机构
[1] IBM Res Zurich, CH-8803 Ruschlikon, Switzerland
来源
NEW JOURNAL OF PHYSICS | 2013年 / 15卷
关键词
GENERALIZED GRADIENT APPROXIMATION; ELASTIC BAND METHOD; LITHIUM PEROXIDE; LI-O-2; BATTERY; CARBONATE; STABILITY; ETHER; CHEMISTRY;
D O I
10.1088/1367-2630/15/9/095009
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Nowadays, simulation techniques are routinely used to generate accurate models of the structures of crystalline and amorphous solids, to study surfaces, defects and the properties of complex systems, and to screen possible candidate materials for the most diverse types of technological applications. The screening of novel molecular structures has been so far pursued by calculation of intrinsic properties with first-principle methods. Still, the use of intrinsic properties as scoring functions may not always be optimal for systems of high complexity. In these cases, increasingly detailed and realistic simulations that take into account the interaction with the surrounding molecules are of crucial importance. In this paper, we present an effective way to screen different solvents with respect to their chemical stability versus Li2O2 solid particles. To achieve this, the minimum energy paths for different types of reactions of a series of aprotic solvents (acetonitrile and pivalonitrile, dimethyl sulphoxide, N-methyl-2-pyrrolidone and some of its derivatives, penta ethylene glycol (PEG-5) and a fluorinated derivative) with solid Li2O2 are computed and reported. From these data, we can extract the reaction energy barriers, which compare extremely well with the available experimental data and offer a convenient way for screening and designing suitable solvents for Li-air batteries from first-principle calculations.
引用
收藏
页数:21
相关论文
共 41 条
  • [1] A polymer electrolyte-based rechargeable lithium/oxygen battery
    Abraham, KM
    Jiang, Z
    [J]. JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1996, 143 (01) : 1 - 5
  • [2] Toward reliable density functional methods without adjustable parameters: The PBE0 model
    Adamo, C
    Barone, V
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (13) : 6158 - 6170
  • [3] Computational Studies of Polysiloxanes: Oxidation Potentials and Decomposition Reactions
    Assary, Rajeev S.
    Curtiss, Larry A.
    Redfern, Paul C.
    Zhang, Zhengcheng
    Amine, Khalil
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (24) : 12216 - 12223
  • [4] The Identification of Stable Solvents for Nonaqueous Rechargeable Li-Air Batteries
    Bryantsev, Vyacheslav S.
    Uddin, Jasim
    Giordani, Vincent
    Walker, Wesley
    Addison, Dan
    Chase, Gregory V.
    [J]. JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2013, 160 (01) : A160 - A171
  • [5] Predicting Autoxidation Stability of Ether- and Amide-Based Electrolyte Solvents for Li-Air Batteries
    Bryantsev, Vyacheslav S.
    Faglioni, Francesco
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2012, 116 (26) : 7128 - 7138
  • [6] Predicting Solvent Stability in Aprotic Electrolyte Li-Air Batteries: Nucleophilic Substitution by the Superoxide Anion Radical (O2•-)
    Bryantsev, Vyacheslav S.
    Giordani, Vincent
    Walker, Wesley
    Blanco, Mario
    Zecevic, Strahinja
    Sasaki, Kenji
    Uddin, Jasim
    Addison, Dan
    Chase, Gregory V.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2011, 115 (44) : 12399 - 12409
  • [7] Computational Study of the Mechanisms of Superoxide-Induced Decomposition of Organic Carbonate-Based Electrolytes
    Bryantsev, Vyacheslav S.
    Blanco, Mario
    [J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2011, 2 (05): : 379 - 383
  • [8] Reactivity of Electrolytes for Lithium-Oxygen Batteries with Li2O2
    Chalasani, Dinesh
    Lucht, Brett L.
    [J]. ECS ELECTROCHEMISTRY LETTERS, 2012, 1 (02) : A38 - A42
  • [9] Li-O2 Battery with a Dimethylformamide Electrolyte
    Chen, Yuhui
    Freunberger, Stefan A.
    Peng, Zhangquan
    Barde, Fanny
    Bruce, Peter G.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (18) : 7952 - 7957
  • [10] On the structure of lithium peroxide, Li2O2
    Cota, LG
    de la Mora, P
    [J]. ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS, 2005, 61 : 133 - 136