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Title: | Lithium nitrate mediated dynamic formation of solid electrolyte interphase revealed by in situ Fourier transform infrared spectroscopy | Authors: | Wu, Longsheng Hu, Jingping Chen , Sijing Yang , Xiaorong Liu , Lu Foord, John S. POBEDINSKAS, Paulius HAENEN, Ken Hou, Huijie Yang , Jiakuan |
Issue Date: | 2023 | Publisher: | PERGAMON-ELSEVIER SCIENCE LTD | Source: | ELECTROCHIMICA ACTA, 466 (Art N° 142973) | Abstract: | A stable solid electrolyte interphase (SEI) plays a vital role in the cyclic stability and Coulombic efficiency (CE) of high-performance lithium-sulfur (Li-S) batteries. It is recognized that the LiNO3 additive can stabilize the SEI of the lithium electrode. However, the exact mechanism of the LiNO3 additive on the SEI of the lithium electrode remains unclear. In this work, we first revealed the mediation mechanism of LiNO3 additive on the dynamic evolution of the SEI on a lithium anode surface through in situ Fourier transform infrared (FTIR) spectroscopy and ab initio molecular dynamics (AIMD) methods. The FTIR and AIMD results directly proved that LiNO3 can accelerate the reduction of lithium bis(trifluoromethyl sulfonyl)imide (LiTFSI) into small molecules rich in Li2O on lithium anode, thus forming a compact and stable SEI after immersing in the LiNO3-containing electrolyte. Moreover, the decomposition of LiTFSI and the solvent is hindered in the subsequent lithium deposition stripping process due to the stable SEI, thus leading to higher Coulombic efficiency and long-term cyclic stability. In addition, an ROSO2Li-like intermediate is also observed during the lithium deposition process while decomposing or diffusing away during the lithium stripping process, maintaining a dynamic formation/dissolution equilibrium of the SEI. This research provides a new insight into understanding the role of LiNO3 in stabilizing lithium electrode. | Notes: | Hu, JP (corresponding author), Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Hubei, Peoples R China. hujp@hust.edu.cn |
Keywords: | Solid electrolyte interphase;LiNO3;Lithium electrode;In situ Fourier transform infrared spectroscopy;Ab initio molecular dynamics | Document URI: | http://hdl.handle.net/1942/40880 | DOI: | 10.1016/j.electacta.2023.142973 | ISI #: | 001059102300001 | Rights: | 2023 Elsevier Ltd. All rights reserved. | Category: | A1 | Type: | Journal Contribution |
Appears in Collections: | Research publications |
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Lithium nitrate mediated dynamic formation of solid electrolyte interphase revealed by in situ Fourier transform infrared spectroscopy.pdf Restricted Access | Published version | 5.82 MB | Adobe PDF | View/Open Request a copy |
EA23-0780_Revised.pdf Until 2025-10-20 | Peer-reviewed author version | 1.74 MB | Adobe PDF | View/Open Request a copy |
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