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Despite its postulated significant influence on  activity, direct spectroscopic evidence of the complex interplay between EDL structure and reaction kinetics has remained elusive. Here, we introduce Dynamic Response Spectroscopy (DRS), a novel approach that isolates spectroscopic signatures of key physicochemical features of the EDL, including the compact (interfacial) layer and the diffuse double layer based on their time\u2010variance profiles. By analyzing multi\u2010dimensional time\u2010variance within a matrix of time\u2010resolved infrared spectral data recorded during sequential potential steps, we reveal that EDL equilibration is not continuous but involves discrete restructuring events. We provide spectroscopic evidence that these sudden EDL reorganizations correlate with the rapid adsorption and conversion of  to CO. Furthermore, we show that saturation of aqueous NaHCO\n                    <jats:sub>3<\/jats:sub>\n                    electrolytes with , as opposed to Ar, induces more frequent and pronounced water reorientation in the diffuse double layer, characterized by less ice\u2010like ordering and increased randomness. These findings provide novel insights into the dynamic nature of the EDL and its synergistic role in electrocatalysis, establishing a paradigm to better understand, and thus optimize, electrochemical\u00a0systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202423177","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T08:46:26Z","timestamp":1741682786000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Decoding Double Layer Dynamics for CO2 Electroreduction over Cu"],"prefix":"10.1002","volume":"64","author":[{"given":"Daniel","family":"Sinausia","sequence":"first","affiliation":[{"name":"Schulich Faculty of Chemistry, Resnick Sustainability Center for Catalysis, and Grand Technion Energy Program Technion \u2010 Israel Institute of Technology  Haifa 3200002 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Noam","family":"Zisser","sequence":"additional","affiliation":[{"name":"Schulich Faculty of Chemistry, Resnick Sustainability Center for Catalysis, and Grand Technion Energy Program Technion \u2010 Israel Institute of Technology  Haifa 3200002 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thierry Kilian","family":"Slot","sequence":"additional","affiliation":[{"name":"Schulich Faculty of Chemistry, Resnick Sustainability Center for Catalysis, and Grand Technion Energy Program Technion \u2010 Israel Institute of Technology  Haifa 3200002 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"Eisenberg","sequence":"additional","affiliation":[{"name":"Schulich Faculty of Chemistry, Resnick Sustainability Center for Catalysis, and Grand Technion Energy Program Technion \u2010 Israel Institute of Technology  Haifa 3200002 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Florian","family":"Meirer","sequence":"additional","affiliation":[{"name":"Inorganic Chemistry and Catalysis Group Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science Utrecht University  Universiteitsweg 99 Utrecht 3584 CG The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0562-3237","authenticated-orcid":false,"given":"Charlotte","family":"Vogt","sequence":"additional","affiliation":[{"name":"Schulich Faculty of Chemistry, Resnick Sustainability Center for Catalysis, and Grand Technion Energy Program Technion \u2010 Israel Institute of Technology  Haifa 3200002 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,6,13]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aad4998"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-019-0244-4"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-27909-x"},{"key":"e_1_2_7_4_1","volume-title":"Electrochemical Methods: Fundamentals and Applications","author":"Bard A. 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