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000894630 1001_ $$0P:(DE-HGF)0$$aBärmann, Peer$$b0$$eFirst author
000894630 245__ $$aMechanistic Insights into the Pre‐Lithiation of Silicon/Graphite Negative Electrodes in “Dry State” and After Electrolyte Addition Using Passivated Lithium Metal Powder
000894630 260__ $$aWeinheim$$bWiley-VCH$$c2021
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000894630 520__ $$aBecause of its high specific capacity, silicon is regarded as the most promising candidate to be incrementally added to graphite-based negative electrodes in lithium-ion batteries. However, silicon suffers from significant volume changes upon (de-)lithiation leading to continuous re-formation of the solid electrolyte interphase (SEI) and ongoing active lithium losses. One prominent approach to compensate for active lithium losses is pre-lithiation. Here, the “contact pre-lithiation” of silicon/graphite (Si/Gr) negative electrodes in direct contact with passivated Li metal powder (PLMP) is studied, focusing on the pre-lithiation mechanism in “dry state” and after electrolyte addition. PLMP is pressed onto the electrode surface to precisely adjust the degree of pre-lithiation (25%, 50%, and 75%). By in situ XRD and ex situ 7Li NMR studies, it is proven that significant lithiation of Si/Gr electrodes occurs by direct contact to Li metal, that is, without electrolyte. After electrolyte addition, de-lithiation of silicon and graphite is confirmed, resulting in SEI formation. The amount of Li metal highly impacts the presence and durability of the LixC and LixSi phases. Finally, the challenges for homogeneous pre-lithiation and SEI formation are identified, and the impact of electrolyte addition is assessed by analysis of the lateral and in-depth lithium distribution within the Si/Gr electrode.
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000894630 536__ $$0G:(EU-Grant)875548$$aSeNSE - Lithium-ion battery with silicon anode, nickel-rich cathode and in-cell sensor for electric vehicles (875548)$$c875548$$fH2020-LC-BAT-2019$$x1
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000894630 65027 $$0V:(DE-MLZ)SciArea-180$$2V:(DE-HGF)$$aMaterials Science$$x1
000894630 65017 $$0V:(DE-MLZ)GC-1603-2016$$2V:(DE-HGF)$$aChemical Reactions and Advanced Materials$$x0
000894630 7001_ $$0P:(DE-Juel1)187471$$aMohrhardt, Marvin$$b1$$ufzj
000894630 7001_ $$0P:(DE-HGF)0$$aFrerichs, Joop Enno$$b2
000894630 7001_ $$0P:(DE-HGF)0$$aHelling, Malina$$b3
000894630 7001_ $$0P:(DE-HGF)0$$aKolesnikov, Aleksei$$b4
000894630 7001_ $$0P:(DE-HGF)0$$aKlabunde, Sina$$b5
000894630 7001_ $$0P:(DE-HGF)0$$aNowak, Sascha$$b6
000894630 7001_ $$0P:(DE-HGF)0$$aHansen, Michael Ryan$$b7
000894630 7001_ $$0P:(DE-Juel1)166130$$aWinter, Martin$$b8$$eCorresponding author$$ufzj
000894630 7001_ $$00000-0002-2097-5193$$aPlacke, Tobias$$b9$$eCorresponding author
000894630 773__ $$0PERI:(DE-600)2594556-7$$a10.1002/aenm.202100925$$gVol. 11, no. 25, p. 2100925 -$$n25$$p2100925$$tAdvanced energy materials$$v11$$x1614-6840$$y2021
000894630 8564_ $$uhttps://onlinelibrary.wiley.com/doi/full/10.1002/aenm.202100925
000894630 8564_ $$uhttps://juser.fz-juelich.de/record/894630/files/Fullpaper.pdf$$yOpenAccess
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