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We demonstrate that the nature of the counter electrode and the resulting device configuration could drastically improve the long\u2010term stability of the ECD. We show that the replacement of the flat ITO glass electrode with a high surface area ITO electrode or the use of symmetrical working and counter electrode architecture leads to a much longer performance of the device. We propose a methodology to determine optimal operating conditions for ECDs by fine\u2010tuning the lower and upper operation potentials. In addition to using traditional cyclic voltammetry (CV), we utilize electrochemical impedance spectroscopy (EIS) to study the intrinsic properties of the devices and understand the factors that define the long\u2010term cycling stability, which is further described through the use of equivalent circuit models. The main reasoning behind decomposition processes in ECDs and ways to suppress them are discussed.<\/jats:p>","DOI":"10.1002\/celc.202100195","type":"journal-article","created":{"date-parts":[[2021,4,6]],"date-time":"2021-04-06T22:04:09Z","timestamp":1617746649000},"page":"2193-2204","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Probing the Influence of Counter Electrode Structure on Electrochromic\u2010Device Operating Potentials and Performance Using Electrochemical Impedance Spectroscopy"],"prefix":"10.1002","volume":"8","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8607-9853","authenticated-orcid":false,"given":"Rana","family":"Ahmad","sequence":"first","affiliation":[{"name":"Electrochemical Materials Lab Faculty of Science Ontario Tech University (University of Ontario Institute of Technology)  2000 Simcoe Street North L1G 0C5 Oshawa Ontario Canada"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6095-3522","authenticated-orcid":false,"given":"Nadia O.","family":"Laschuk","sequence":"additional","affiliation":[{"name":"Electrochemical Materials Lab Faculty of Science Ontario Tech University (University of Ontario Institute of Technology)  2000 Simcoe Street North L1G 0C5 Oshawa Ontario Canada"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2081-7598","authenticated-orcid":false,"given":"Iraklii I.","family":"Ebralidze","sequence":"additional","affiliation":[{"name":"Electrochemical Materials Lab Faculty of Science Ontario Tech University (University of Ontario Institute of Technology)  2000 Simcoe Street North L1G 0C5 Oshawa Ontario Canada"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2303-4620","authenticated-orcid":false,"given":"Olena V.","family":"Zenkina","sequence":"additional","affiliation":[{"name":"Electrochemical Materials Lab Faculty of Science Ontario Tech University (University of Ontario Institute of Technology)  2000 Simcoe Street North L1G 0C5 Oshawa Ontario Canada"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1493-0500","authenticated-orcid":false,"given":"E. 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