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A novel calculation strategy for optimized prediction of the reduction of electrochemical window at anode |
Guochen Sun(孙国宸)1,2, Jian Gao(高健)3,†, and Hong Li(李泓)1,‡ |
1 Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China; 2 College of Materials Sciences and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China; 3 College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China |
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Abstract The reduction of the electrochemical window (EW) of electrolytes plays a significant role in assessing their compatibility with the anode in lithium-ion batteries. However, the accurate calculation of the reduction of EW is still challenging due to missing the solvation effects, condensation effects, kinetic factors, and the passivation on anodes. The theoretical prediction of the intrinsic and apparent EW is confirmed by a comprehensive experimental analysis of ethylene carbonate-dimethyl carbonate (EC-DMC) electrolytes, combining linear sweep voltammetry (LSV) and gas chromatography-mass spectrometry (GC-MS). The proposed novel kinetic normal distribution theory model can quantitatively explain the current density from LSV and affirm acetaldehyde (MeCHO) as one of the primary reduction products of EC. The solvent effect restricts the intrinsic EW of EC-DMC without lithium salt to 2.6 V (vs. Li+/Li) arising from the Marcus-Gerischer theory and the passivation of MeCHO on the anode broadens the apparent EW to 0.3 V (vs. Li+/Li) arising from the normal distribution of the lowest unoccupied molecular orbital (LUMO) for MeCHO produced by thermal motion. In addition, the passivation on the anode depends intensively on the lithium salt, resulting in more complicated influences on the apparent EW.
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Received: 20 March 2023
Revised: 13 April 2023
Accepted manuscript online: 16 April 2023
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PACS:
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82.47.Aa
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(Lithium-ion batteries)
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82.45.Gj
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(Electrolytes)
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65.40.gk
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(Electrochemical properties)
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87.15.R-
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(Reactions and kinetics)
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Fund: Project supported by the National Natural Science Foundation of China (Grant Nos. U1964205 and 22109005), the National Key Research and Development Program of China (Grant No. 2016YFB0100100), and Beijing Municipal Science & Technology Commission, China (Grant No. Z191100004719001). |
Corresponding Authors:
Jian Gao, Hong Li
E-mail: gaojian@mail.buct.edu.cn;hli@iphy.ac.cn
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Cite this article:
Guochen Sun(孙国宸), Jian Gao(高健), and Hong Li(李泓) A novel calculation strategy for optimized prediction of the reduction of electrochemical window at anode 2023 Chin. Phys. B 32 078201
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[1] Harper G, Sommerville R, Kendrick E, et al. 2019 Nature 575 75 [2] Xu K 2014 Chem. Rev. 114 11503 [3] Severson K A, Attia P M, Jin N, et al. 2019 Nature Energy 4 383 [4] Qiao R X, Zhang M J, Liu Y D, et al. 2016 Chin. Phys. Lett. 33 078201 [5] Liu W, Liu P and Mitlin D 2020 Advanced Energy Materials 10 2002297 [6] Hou C, Han J, Liu P, et al. 2019 Advanced Energy Materials 9 1902675 [7] Xu K 2004 Chem. Rev. 104 4303 [8] Huang W, Attia P M, Wang H, et al. 2019 Nano Lett. 19 5140 [9] Han B, Zou Y, Xu G, et al. 2021 Energy Environ. Sci. 14 4882 [10] Parimalam B S, Macintosh A D, Kadam R, et al. 2017 The Journal of Physical Chemistry C 121 22733 [11] Shkrob I A, Zhu Y, Marin T W, et al. 2013 The Journal of Physical Chemistry C 117 19255 [12] Lee C H, Dura J A, Lebar A, et al. 2019 Journal of Power Sources 412 725 [13] Gachot G, Ribiere P, Mathiron D, et al. 2011 Anal. Chem. 83 478 [14] Ganesh P, Kent P R C and Jiang D E 2012 The Journal of Physical Chemistry C 116 24476 [15] Ushirogata K, Sodeyama K, Okuno Y, et al. 2013 J. Am. Chem. Soc. 135 11967 [16] Tasaki K 2005 J. Phys. Chem. B 109 2920 [17] Leung K 2013 Chem. Phys. Lett. 568-569 1 [18] Spotte-Smith E W C, Kam R L, Barter D, et al. 2022 ACS Energy Letters 7 1446 [19] Hossain M J, Pawar G, Liaw B, et al. 2020 J. Chem. Phys. 152 184301 [20] Martinez De La Hoz J M, Leung K and Balbuena P B 2013 ACS Appl. Mater. Interfaces 5 13457 [21] Liu Y, Wu Y, Sun Q, et al. 2022 Adv. Theory Simul. 5 2100612 [22] Ebadi M, Brandell D and Araujo C M 2016 J. Chem. Phys. 145 204701 [23] Ohba N, Ogata S and Asahi R 2019 The Journal of Physical Chemistry C 123 9673 [24] Borodin O 2019 Current Opinion in Electrochemistry 13 86 [25] Wang A, Kadam S, Li H, et al. 2018 npj Computational Materials 4 15 [26] Bard A J and Faulkner L R 2000 Electrochemical Methods: Fundamentals and Applications, 2nd Ed. (New York: John Wiley & Sons, Incorporated.) pp. 115-132 [27] Wang Y, Nakamura S, Ue M, et al. 2001 J. Am. Chem. Soc. 123 11708 [28] Leung K and Tenney C M 2013 The Journal of Physical Chemistry C 117 24224 [29] Wang D, He T, Wang A, et al. 2023 Advanced Functional Materials 33 2212342 [30] Wang A, Zou Z, Wang D, et al. 2021 Energy Storage Materials 35 595 [31] Stephens P J, Devlin F J, Chabalowski C F, et al. 1994 The Journal of Physical Chemistry 98 11623 [32] Hehre W J, Ditchfield R and Pople J A 1972 The Journal of Chemical Physics 56 2257 [33] Zade S S, Zamoshchik N and Bendikov M 2011 Accounts of Chemical Research 44 14 [34] Manzetti S and Lu T 2013 RSC Advances 3 25881 [35] Marcus R A 1956 The Journal of Chemical Physics 24 966 [36] Marcus R A 1968 Electrochimica Acta 13 995 [37] Pracht P, Bohle F and Grimme S 2020 Phys. Chem. Chem. Phys. 22 7169 [38] Bannwarth C, Ehlert S and Grimme S 2019 J. Chem. Theory Comput. 15 1652 [39] Grimme S 2019 J. Chem. Theory Comput. 15 2847 [40] Bannwarth C, Caldeweyher E, Ehlert S, et al. 2020 WIREs Comput Mol Sci. 11 e1493 [41] Neese F 2018 WIREs Comput Mol Sci. 8 e1327 [42] Weigend F and Ahlrichs R 2005 Phys. Chem. Chem. Phys. 7 3297 [43] Frisch M J, Trucks G W, Schlegel H B, et al. 2009 Gaussian 09 Rev. D.01. Wallingford, CT [44] Nelsen S F, Blackstock S C and Kim Y 1987 Journal of the American Chemical Society 109 677 [45] Hoffmann J S, O'connor R T, Magne F C, et al. 1956 J. Am. Oil Chem. Soc. 33 410 [46] Caldeweyher E, Bannwarth C and Grimme S 2017 J. Chem. Phys. 147 034112 [47] Dziewonski P M and Grzeszczuk M 2010 J. Phys. Chem. B 114 7158 [48] Winter M Barnett B and Xu K 2018 Chem. Rev. 118 11433 |
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