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This constitutes a crucial constraint on the performance of specific electrochemical devices, such as fuel cells and metal\u2013air batteries. To boost selectivity of metal nanoparticles, a novel methodology that harnesses the unique electrocatalytic properties of polyoxometalates (POM) to scavenge undesired intermediates of the ORR (such as HO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) promoting selectivity is proposed. It involves the covalent functionalization of metal nanoparticle's surface with an electrochemically active capping layer containing a new sulfur\u2010functionalized vanadium\u2010based POM (AuNP@POM). To demonstrate this approach, preformed thiolate Au(111) nanoparticles with a relatively poor ORR selectivity are chosen. The dispersion of AuNP@POM on the surface of carbon nanofibers (CNF) enhances oxygen diffusion, and therefore the ORR activity. The resulting electrocatalyst (AuNP@POM\/CNF) exhibits superior stability against impurities like methanol and a higher pH tolerance range compared to the standard commercial Pt\/C. The work demonstrates for the first time, the use of a POM\u2010based electrochemically active capping layer to switch on the selectivity of poorly selective gold nanoparticles, offering a promising avenue for the preparation of electrocatalyst materials with improved selectivity, performance, and stability for ORR\u2010based devices.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202301805","type":"journal-article","created":{"date-parts":[[2024,3,22]],"date-time":"2024-03-22T09:36:18Z","timestamp":1711100178000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Boosting Oxygen Reduction Reaction Selectivity in Metal Nanoparticles with Polyoxometalates"],"prefix":"10.1002","volume":"8","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3386-8685","authenticated-orcid":false,"given":"Eugenia Pilar","family":"Quir\u00f3s\u2010D\u00edez","sequence":"first","affiliation":[{"name":"Centro Singular de Investigaci\u00f3n en Qu\u00edmica Biol\u00f3xica e Materiais Moleculares (CiQUS) Departamento de Qu\u00edmica Inorg\u00e1nica Universidade de Santiago de Compostela  Santiago de Compostela 15782 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0619-3822","authenticated-orcid":false,"given":"Carlos","family":"Herreros\u2010Lucas","sequence":"additional","affiliation":[{"name":"Centro Singular de Investigaci\u00f3n en Qu\u00edmica Biol\u00f3xica e Materiais Moleculares (CiQUS) Departamento de Qu\u00edmica Inorg\u00e1nica Universidade de Santiago de Compostela  Santiago de Compostela 15782 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jos\u00e9 Manuel","family":"Vila\u2010Fungueiri\u00f1o","sequence":"additional","affiliation":[{"name":"Centro Singular de Investigaci\u00f3n en Qu\u00edmica Biol\u00f3xica e Materiais Moleculares (CiQUS) Departamento de Qu\u00edmica F\u00edsica Universidade de Santiago de Compostela  Santiago de Compostela 15782 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4003-5123","authenticated-orcid":false,"given":"Luc\u00eda","family":"Vizca\u00edno\u2010Anaya","sequence":"additional","affiliation":[{"name":"Centro Singular de Investigaci\u00f3n en Qu\u00edmica Biol\u00f3xica e Materiais Moleculares (CiQUS) Departamento de Qu\u00edmica Inorg\u00e1nica Universidade de Santiago de Compostela  Santiago de Compostela 15782 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7223-4138","authenticated-orcid":false,"given":"Yolanda","family":"Sabater\u2010Algarra","sequence":"additional","affiliation":[{"name":"Centro Singular de Investigaci\u00f3n en Qu\u00edmica Biol\u00f3xica e Materiais Moleculares (CiQUS) Departamento de Qu\u00edmica Inorg\u00e1nica Universidade de Santiago de Compostela  Santiago de Compostela 15782 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