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Yet, finding effective material combinations and identifying the reactive site remains challenging and an obstacle for rational catalyst\/sensor design. Here, the low\u2010temperature oxidation of formaldehyde with CuO<jats:sub>x<\/jats:sub> clusters on Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> nanoparticles is demonstrated yielding an excellent sensor for this critical air pollutant. When fabricated by flame\u2010aerosol technology, such CuO<jats:sub>x<\/jats:sub> clusters are finely dispersed, while some Cu ions are incorporated into the Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> lattice enhancing thermal stability. Importantly, infrared spectroscopy of adsorbed CO, near edge X\u2010ray absorption fine structure spectroscopy and temperature\u2010programmed reduction in H<jats:sub>2<\/jats:sub> identified Cu<jats:sup>+<\/jats:sup> and Cu<jats:sup>2+<\/jats:sup> species in these clusters as active sites. Remarkably, the Cu<jats:sup>+<\/jats:sup> surface concentration correlated with the apparent activation energy of formaldehyde oxidation (Spearman's coefficient <jats:italic>\u03c1<\/jats:italic> = 0.89) and sensor response (0.96), rendering it a performance descriptor. At optimal composition, such sensors detected even the lowest formaldehyde levels of 3 parts\u2010per\u2010billion (ppb) at 75\u00b0C, superior to state\u2010of\u2010the\u2010art sensors. Also, selectivity to other aldehydes, ketones, alcohols, and inorganic compounds, robustness to humidity and stable performance over 4 weeks are achieved, rendering such sensors promising as gas detectors in health monitoring, air and food quality control.<\/jats:p>","DOI":"10.1002\/advs.202308224","type":"journal-article","created":{"date-parts":[[2023,12,24]],"date-time":"2023-12-24T23:14:27Z","timestamp":1703459667000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["Structure\u2010Function Relationship of Highly Reactive CuO<sub>x<\/sub> Clusters on Co<sub>3<\/sub>O<sub>4<\/sub> for Selective Formaldehyde Sensing at Low Temperatures"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8775-1573","authenticated-orcid":false,"given":"Matteo","family":"D'Andria","sequence":"first","affiliation":[{"name":"Human\u2010centered Sensing Laboratory, Department of Mechanical and Process Engineering, ETH Zurich  Zurich CH\u20108092 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5625-1536","authenticated-orcid":false,"given":"Frank","family":"Krumeich","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences Laboratory of Inorganic Chemistry, ETH Zurich  Zurich CH\u20108093 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhangyi","family":"Yao","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering University College London  London WC1E 7JE UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2475-606X","authenticated-orcid":false,"given":"Feng Ryan","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering University College London  London WC1E 7JE UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4127-752X","authenticated-orcid":false,"given":"Andreas T.","family":"G\u00fcntner","sequence":"additional","affiliation":[{"name":"Human\u2010centered Sensing Laboratory, Department of Mechanical and Process Engineering, ETH Zurich  Zurich CH\u20108092 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,12,24]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201902136"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202204810"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.snb.2014.10.091"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0TC00387E"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565-021-01022-y"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202003300"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202008370"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.1c04854"},{"key":"e_1_2_8_9_1","first-page":"90","author":"G\u00fcntner A. 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