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    Revisiting the Ethylene Carbonate-Propylene Carbonate Mystery with Operando Characterization

    Year: 2022

    Journal: Adv. Mater. Interfaces, Volume 9, MAR

    Authors: Melin, Tim; Lundstrom, Robin; Berg, Erik J.

    Organizations: Knut and Alice Wallenberg (KAW) Foundation [2017.0204]; Swedish Research Council [2016-04069]; StandUp for Energy

    Keywords: electrochemical quartz crystal microbalance with dissipation monitoring; Li-ion batteries; online electrochemical mass spectrometry; operando; solid electrolyte interphases

    The ethylene carbonate (EC)-propylene carbonate (PC) mystery has puzzled electrochemists for decades. Surprisingly, the minor structural difference between PC and EC, a methyl vis-a-vis a proton, prevents PC unlike EC to form a stable solid electrolyte interphase (SEI) on carbon (C), which along with the popularity of PC has impeded the development of Li-ion batteries with many years. Despite several hypotheses, the fundamental reason remains debated largely due to the lack of sufficient experimental evidence. Herein, SEI formed as a result of EC and PC reductions are analyzed by two state-of-the-art operando techniques, online electrochemical mass spectrometry and electrochemical quartz crystal microbalance with dissipation monitoring. Although both EC- and PC-based electrolytes appear to have virtually identical reaction pathways, PC is reduced much more extensively than EC and forms a much thicker SEI. However, while the SEI derived from EC remains on the electrode, PC reduction products redissolve in the electrolyte leaving the bare C electrode behind. The presented study illustrates the complex scheme of competing electro-/chemical reactions behind SEI formation and provides further scientific details needed to eventually form a consensus of the processes governing electrode/electrolyte interphases in Li-ion batteries.
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