000014401 001__ 14401
000014401 005__ 20250117101314.0
000014401 02470 $$2doi$$ahttps://doi.org/10.1002/anie.202420680
000014401 037__ $$aTEXTUAL
000014401 037__ $$bArticle
000014401 041__ $$aeng
000014401 245__ $$aUnlocking Mesoscopic Disorder in Graphitic Carbon with Spectroelectrochemistry
000014401 269__ $$a2024-12-30
000014401 336__ $$aArticle
000014401 520__ $$aIntrinsic structural and oxidic defects activate graphitic carbon electrodes towards electrochemical reactions underpinning energy conversion and storage technologies. Yet, these defects can also disrupt the long-range and periodic arrangement of carbon atoms, thus, the characterization of graphitic carbon electrodes necessitates in-situ atomistic differentiation of graphitic regions from mesoscopic bulk disorder. Here, we leverage the combined techniques of in-situ attenuated total reflectance infrared spectroscopy and first-principles calculations to reveal that graphitic carbon electrodes exhibit electric-field dependent infrared activity that is sensitive to the bulk mesoscopic intrinsic disorder. With this platform, we identify graphitic regions from amorphous domains by discovering that they demonstrate opposing electric-field-dependent infrared activity under electrochemical conditions. Our work provides a roadmap for identifying mesoscopic disorder in bulk carbon materials under potential bias.
000014401 536__ $$oU.S. Department of Energy$$cDE-AC02-06CH11357$$aComputational Materials Sciences Program
000014401 536__ $$aBeckman Scholarship
000014401 536__ $$oUniversity of Chicago$$qhttps://ror.org/024mw5h28$$rROR$$astartup funds
000014401 536__ $$oUniversity of Chicago$$qhttps://ror.org/024mw5h28$$rROR$$aNeubauer Family Assistant Professorship
000014401 540__ $$a<p>© 2025 The Author(s)</p> <p>This is an open access article under the terms of the <a href="http://creativecommons.org/licenses/by-nc/4.0/" target="_blank">Creative Commons Attribution-NonCommercial License</a>, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.</p>
000014401 542__ $$fCC BY-NC
000014401 594__ $$aThe data that support the findings of this study are available in the supplementary material of this article.
000014401 6531_ $$aDisordered graphitic carbon electrodes
000014401 6531_ $$ain-situ infrared spectroscopy
000014401 6531_ $$afirst-principles calculations
000014401 690__ $$aPhysical Sciences Division
000014401 690__ $$aPritzker School of Molecular Engineering
000014401 691__ $$aChemistry
000014401 7001_ $$aPapadopoulos, Ry$$uUniversity of Chicago
000014401 7001_ $$aMasters, Benjamin$$uUniversity of Chicago
000014401 7001_ $$1https://orcid.org/0000-0001-5351-3254$$2ORCID$$aKundu, Arpan$$uUniversity of Chicago
000014401 7001_ $$aMaldonado, Nicholas$$uUniversity of Chicago
000014401 7001_ $$aFilatov, Alexander S.$$uUniversity of Chicago
000014401 7001_ $$aLiu, Yuzi$$uArgonne National Laboratory
000014401 7001_ $$aKim, Taemin$$uUniversity of Chicago
000014401 7001_ $$1https://orcid.org/0000-0002-8001-5290$$2ORCID$$aGalli, Giulia$$uUniversity of Chicago
000014401 7001_ $$aWuttig, Anna$$uUniversity of Chicago
000014401 773__ $$tAngewandte Chemie International Edition
000014401 8564_ $$uhttps://knowledge.uchicago.edu/record/14401/files/Unlocking-Mesoscopic-Disorder-in-Graphitic-Carbon-with-Spectroelectrochemistry.pdf$$yArticle$$97ca73c67-290c-4c77-8be3-fb6ab3a377cc$$s744980$$ePublic
000014401 8564_ $$uhttps://knowledge.uchicago.edu/record/14401/files/anie202420680-sup-0001-misc_information.pdf$$ySupporting information$$900671a83-f241-4ca1-8a3d-cb98aca1f1f4$$s3550994$$ePublic
000014401 908__ $$aI agree
000014401 909CO $$ooai:uchicago.tind.io:14401$$pGLOBAL_SET
000014401 983__ $$aArticle