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Engineering this catalytically active periphery, where kinetically relevant surface intermediates are efficiently turned over, offers a pathway to optimized performance, yet it remains challenging due to the need for precise control over nanospatial catalyst features. Herein, we address this subject for the relevant case of methanol synthesis by CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation on Cu\/ZrO\n                    <jats:sub>2<\/jats:sub>\n                    catalysts. The methanol synthesis rate reaches a maximum at a surface\u2010to\u2010surface Cu interparticle distance of ca. 15\u00a0nm.\n                    <jats:italic>Operando<\/jats:italic>\n                    modulation\u2013excitation diffuse reflectance infrared spectroscopy reveals that this optimal spacing maximizes the fraction of surface\u2010bound HCOO* intermediates, stabilized on coordinatively unsaturated Zr(IV) Lewis acid sites on the ZrO\n                    <jats:sub>2<\/jats:sub>\n                    support, which are dynamically involved in catalysis. This particle spacing represents a shift in the reaction's kinetic control regime and the apparent activation energy for methanol synthesis. Engineering Cu interparticle spacing to the optimal value results in exceptionally high metal\u2010specific methanol formation rates under industrially relevant reaction conditions. More broadly, our findings highlight that, beyond metal particle size, interparticle spacing is a key design parameter for catalyst systems featuring functional metal\u2010oxide interfaces.\n                  <\/jats:p>","DOI":"10.1002\/anie.202420126","type":"journal-article","created":{"date-parts":[[2025,7,30]],"date-time":"2025-07-30T05:35:57Z","timestamp":1753853757000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Engineering Peripheral Metal\u2010Oxide Catalysis: Interparticle Spacing in Cu\/ZrO\n                    <sub>2<\/sub>\n                    Catalysts for Methanol Synthesis by CO\n                    <sub>2<\/sub>\n                    Hydrogenation"],"prefix":"10.1002","volume":"64","author":[{"given":"Iv\u00e1n","family":"L\u00f3pez\u2010Luque","sequence":"first","affiliation":[{"name":"ITQ Instituto de Tecnolog\u00eda Qu\u00edmica Universitat Polit\u00e8cnica de Val\u00e8ncia\u2010Consejo Superior de Investigaciones Cient\u00edficas (UPV\u2010CSIC)  Av. 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Los Naranjos s\/n Valencia 46022 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wilson","family":"Henao","sequence":"additional","affiliation":[{"name":"ITQ Instituto de Tecnolog\u00eda Qu\u00edmica Universitat Polit\u00e8cnica de Val\u00e8ncia\u2010Consejo Superior de Investigaciones Cient\u00edficas (UPV\u2010CSIC)  Av. Los Naranjos s\/n Valencia 46022 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0608-2070","authenticated-orcid":false,"given":"Bernat","family":"Mundet","sequence":"additional","affiliation":[{"name":"Institut Catal\u00e0 de Nanoci\u00e8ncia i Nanotecnolog\u00eda (ICN2) Campus UAB  Bellaterra (Cerdanyola del Vall\u00e8s) Barcelona 08193 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-2217-8814","authenticated-orcid":false,"given":"Prathamesh","family":"Patil","sequence":"additional","affiliation":[{"name":"Centre for Electrochemistry and Surface Technology TFZ\u2013Wiener Neustadt  Viktor\u2010Kaplan\u2010Strasse 2 Wr. 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