{"title":"将乙酰化锂(Li2C2)确立为锂离子电池中固体电解质相间层的功能元素","authors":"Viviane Maccio-Figgemeier , Gebrekidan Gebresilassie Eshetu , Damian Mroz , Hyunsang Joo , Egbert Figgemeier","doi":"10.1016/j.powera.2024.100152","DOIUrl":null,"url":null,"abstract":"<div><p>Previously, lithium-acetylide (Li<sub>2</sub>C<sub>2</sub>) had been identified as electrolyte degradation product on lithium-metal based electrodes using Raman spectroscopy. This raised the question, if Li<sub>2</sub>C<sub>2</sub> is also be formed on graphitic electrodes in lithium-ion batteries without lithium metal present. In order to shed light on this research question, we performed a series of in situ Raman experiments with graphitic electrodes in half- and full-cell configuration. The recorded cell potential dependent spectra clearly prove the presence of Li<sub>2</sub>C<sub>2</sub> in the lithiated state of the electrodes, but the according peak vanishes when delithiating. This observation indicates a somewhat reversible process involving Li<sub>2</sub>C<sub>2</sub>. Several chemical/electrochemical reactions are in question to contribute to this effect. With respect to its properties and potential role in the solid-electrolyte interphase (SEI) DFT calculations of Li<sub>2</sub>C<sub>2</sub>-nanoclusters were performed, which revealed an exceptionally low energy band gap, hence a remarkable electric conductivity. In conjunction with a relatively high ionic conductivity, Li<sub>2</sub>C<sub>2</sub> appears to play a key role in the degradation of lithium-ion batteries, which had not yet been revealed nor taken into account in simulations of the interphase.</p></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666248524000180/pdfft?md5=841d9ceaf9a647e74a350bdfb42703d7&pid=1-s2.0-S2666248524000180-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Establishing Li-acetylide (Li2C2) as functional element in solid-electrolyte interphases in lithium-ion batteries\",\"authors\":\"Viviane Maccio-Figgemeier , Gebrekidan Gebresilassie Eshetu , Damian Mroz , Hyunsang Joo , Egbert Figgemeier\",\"doi\":\"10.1016/j.powera.2024.100152\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Previously, lithium-acetylide (Li<sub>2</sub>C<sub>2</sub>) had been identified as electrolyte degradation product on lithium-metal based electrodes using Raman spectroscopy. This raised the question, if Li<sub>2</sub>C<sub>2</sub> is also be formed on graphitic electrodes in lithium-ion batteries without lithium metal present. In order to shed light on this research question, we performed a series of in situ Raman experiments with graphitic electrodes in half- and full-cell configuration. The recorded cell potential dependent spectra clearly prove the presence of Li<sub>2</sub>C<sub>2</sub> in the lithiated state of the electrodes, but the according peak vanishes when delithiating. This observation indicates a somewhat reversible process involving Li<sub>2</sub>C<sub>2</sub>. Several chemical/electrochemical reactions are in question to contribute to this effect. With respect to its properties and potential role in the solid-electrolyte interphase (SEI) DFT calculations of Li<sub>2</sub>C<sub>2</sub>-nanoclusters were performed, which revealed an exceptionally low energy band gap, hence a remarkable electric conductivity. In conjunction with a relatively high ionic conductivity, Li<sub>2</sub>C<sub>2</sub> appears to play a key role in the degradation of lithium-ion batteries, which had not yet been revealed nor taken into account in simulations of the interphase.</p></div>\",\"PeriodicalId\":34318,\"journal\":{\"name\":\"Journal of Power Sources Advances\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-06-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2666248524000180/pdfft?md5=841d9ceaf9a647e74a350bdfb42703d7&pid=1-s2.0-S2666248524000180-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Power Sources Advances\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2666248524000180\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Power Sources Advances","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2666248524000180","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Establishing Li-acetylide (Li2C2) as functional element in solid-electrolyte interphases in lithium-ion batteries
Previously, lithium-acetylide (Li2C2) had been identified as electrolyte degradation product on lithium-metal based electrodes using Raman spectroscopy. This raised the question, if Li2C2 is also be formed on graphitic electrodes in lithium-ion batteries without lithium metal present. In order to shed light on this research question, we performed a series of in situ Raman experiments with graphitic electrodes in half- and full-cell configuration. The recorded cell potential dependent spectra clearly prove the presence of Li2C2 in the lithiated state of the electrodes, but the according peak vanishes when delithiating. This observation indicates a somewhat reversible process involving Li2C2. Several chemical/electrochemical reactions are in question to contribute to this effect. With respect to its properties and potential role in the solid-electrolyte interphase (SEI) DFT calculations of Li2C2-nanoclusters were performed, which revealed an exceptionally low energy band gap, hence a remarkable electric conductivity. In conjunction with a relatively high ionic conductivity, Li2C2 appears to play a key role in the degradation of lithium-ion batteries, which had not yet been revealed nor taken into account in simulations of the interphase.