2022
DOI: 10.1002/adts.202100612
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Formation of Linear Oligomers in Solid Electrolyte Interphase via Two‐Electron Reduction of Ethylene Carbonate

Abstract: Solid electrolyte interphase (SEI) plays a significant role in enhancing the stability and durability of lithium metal batteries (LMBs) by separating highly reactive lithium metal anode (LMA) from the electrolyte to avoid continuous degradation. However, the underlying reaction mechanism is still far from clear. Herein, a hybrid ab initio and reactive force field (HAIR) method is employed to extend the ab initio molecular dynamics (AIMD) to 1 ns, which provides crystal information about the reaction mechanism … Show more

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Cited by 5 publications
(5 citation statements)
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“…At 2.51 ps, in a Li + -rich environment, EC undergoes a one-electron reduction, breaking its C-O bond and transforming from a ring to a chain structure, forming OC2H4OCO − . Subsequently, OC2H4OCO − follows two pathways: It accepts another electron to form OC2H4O2 − , releasing one CO at 4.00 ps (Figure 3a), and releases CO2 while forming the free radical anion •C2H4O − , consistent with previous DFT calculations [52]. At 61.21 ps, •C2H4O − is further reduced by Li 0 and forms Li2O along with one electron transfer (Figure 3b).…”
Section: The Underlying Mechanism Of Electrolyte Reduction and Sei Fo...supporting
confidence: 87%
“…At 2.51 ps, in a Li + -rich environment, EC undergoes a one-electron reduction, breaking its C-O bond and transforming from a ring to a chain structure, forming OC2H4OCO − . Subsequently, OC2H4OCO − follows two pathways: It accepts another electron to form OC2H4O2 − , releasing one CO at 4.00 ps (Figure 3a), and releases CO2 while forming the free radical anion •C2H4O − , consistent with previous DFT calculations [52]. At 61.21 ps, •C2H4O − is further reduced by Li 0 and forms Li2O along with one electron transfer (Figure 3b).…”
Section: The Underlying Mechanism Of Electrolyte Reduction and Sei Fo...supporting
confidence: 87%
“…At 2.51 ps, in a Li +rich environment, EC undergoes a one-electron reduction, breaking its C-O bond and transforming from a ring to a chain structure, forming OC2H4OCO -. Subsequently, OC2H4OCO -follows two pathways: it accepts another electron to form OC2H4O2 -, releasing one CO at 4.00 ps (Figure 3a), and releases CO2 while forming the free radical anion •C2H4O -, consistenting with previous DFT [45]. At 61.21 ps, •C2H4O -is further reduced by Li 0 and forms Li2O along with one electron transfer (Figure 3b).…”
Section: Underlying Mechanism Of Electrolyte Reduction and Sei Formationsupporting
confidence: 87%
“…7c ) 41 47 . For example, EC is subjected to ring-opening and C − O breaking to generate RC = OLi, then recombining or decomposition to Li 2 CO 3 /ROCO 2 Li and ROLi 42 , while the latter reaction is partly hindered at the low temperature. Consequently, Li 2 CO 3 /ROCO 2 Li and ROLi are dominated in the SEI formed at 25 and 0 °C but much reduced at −20 °C replaced by its intermediate products RC = OLi as evidenced by the XPS (Fig.…”
Section: Resultsmentioning
confidence: 99%
“…Decreasing the temperature alters the thermodynamic reaction of electrolyte decomposition, resulting in different reaction pathways and products (Fig. 7c) [41][42][43][44][45][46][47] . For example, EC is subjected to ring-opening and C − O breaking to generate RC = OLi, then recombining or decomposition to Li 2 CO 3 /ROCO 2 Li and ROLi 42 , while the latter reaction is partly hindered at the low temperature.…”
Section: Sei Propertiesmentioning
confidence: 99%