@article{bibcite_36778, author = {Andrew Dopilka and Jonathan M Larson and Robert Kostecki}, title = {Operando Infrared Nanospectroscopy of the Silicon/Electrolyte Interface during Initial Stages of Solid-Electrolyte-Interphase Layer Formation}, abstract = {

The solid electrolyte interphase (SEI) is a critical component in Li-ion batteries; however, its nanoscale structure and composition and unstable nature make it difficult to characterize and ascertain primary functional mechanisms. We use operando nanoscale Fourier transform infrared spectroscopy (nano-FTIR) with a broadband synchrotron IR source to study the SEI formation on a thin-film Si electrode at nanometer-scale spatial resolution as a function of time and voltage. By probing the Si/carbonate electrolyte interface through a 25 nm-thick amorphous Si window/electrode, we detect molecular vibrational modes within a 10s of nanometers region adjacent to the Si surface and observe that PF6{\textendash} anions react to form LiF at 0.5 V. Spatially resolved nano-FTIR spectra showcase subtle nanoscale heterogeneities in the initial solid/liquid interface and the resulting deposited LiF. With its nanoscale resolution and high chemical specificity, operando nano-FTIR provides unique insights into the dynamics and heterogeneous formation of SEIs and opens opportunities for connecting nanoscale interfacial properties to bulk performance metrics.

}, year = {2025}, booktitle = {ACS Energy Letters}, journal = {ACS Energy Letters}, series = {ACS Energy Letters}, volume = {10}, pages = {410-419}, month = {10/01/2025}, institution = {American Chemical Society (ACS)}, publisher = {American Chemical Society (ACS)}, issn = {2380-8195, 2380-8195}, url = {https://doi.org/10.1021/acsenergylett.4c03255}, doi = {10.1021/acsenergylett.4c03255}, }