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Especially, oxychlorides rely mainly on layered structures, which suffer from low stability during photo(electro)catalytic processes. Herein we report a strategy to design a new polar 3D tetrahedral framework with composition Zn<jats:sub>4<\/jats:sub>Si<jats:sub>2<\/jats:sub>O<jats:sub>7<\/jats:sub>Cl<jats:sub>2<\/jats:sub>. We use a molten salt medium to enable low temperature crystallization of nanowires of this new compound, by relying on tetrahedral building units present in the melt to build the connectivity of the oxychloride. These units are combined with silicon\u2010based connectors from a non\u2010oxidic Zintl phase to enable precise tuning of the oxygen content. This structure brings high chemical and thermal stability, as well as strongly anisotropic hole mobility along the polar axis. These features, associated with the ability to adjust the transport properties by doping, enable to tune water splitting properties for photoelectrocatalytic H<jats:sub>2<\/jats:sub> evolution and water oxidation. This work then paves the way to a new family of mixed\u2010anion solids<\/jats:p>","DOI":"10.1002\/anie.202303487","type":"journal-article","created":{"date-parts":[[2023,4,12]],"date-time":"2023-04-12T14:55:03Z","timestamp":1681311303000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Molten Salts\u2010Driven Discovery of a Polar Mixed\u2010Anion 3D Framework at the Nanoscale: Zn<sub>4<\/sub>Si<sub>2<\/sub>O<sub>7<\/sub>Cl<sub>2<\/sub>, Charge Transport and Photoelectrocatalytic Water Splitting"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8044-5306","authenticated-orcid":false,"given":"Ram","family":"Kumar","sequence":"first","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Coll\u00e8ge de France Laboratoire de Chimie de la Mati\u00e8re Condens\u00e9e de Paris (CMCP)  4 place Jussieu 75005 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9921-0718","authenticated-orcid":false,"given":"Yang","family":"Song","sequence":"additional","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Coll\u00e8ge de France Laboratoire de Chimie de la Mati\u00e8re Condens\u00e9e de Paris (CMCP)  4 place Jussieu 75005 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6546-8742","authenticated-orcid":false,"given":"Anissa","family":"Ghoridi","sequence":"additional","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Coll\u00e8ge de France Laboratoire de Chimie de la Mati\u00e8re Condens\u00e9e de Paris (CMCP)  4 place Jussieu 75005 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2867-8986","authenticated-orcid":false,"given":"Philippe","family":"Boullay","sequence":"additional","affiliation":[{"name":"Normandie Universit\u00e9 ENSICAEN UNICAEN CNRS CRISMAT  14000 Caen France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8877-0015","authenticated-orcid":false,"given":"Gwenaelle","family":"Rousse","sequence":"additional","affiliation":[{"name":"PSL Research University Sorbonne Universit\u00e9 Coll\u00e8ge de France Chimie du Solide et de l'Energie UMR 8260 Coll\u00e8ge de France  11 place Marcelin Berthelot 75007 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7450-1738","authenticated-orcid":false,"given":"Christel","family":"Gervais","sequence":"additional","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Coll\u00e8ge de France Laboratoire de Chimie de la Mati\u00e8re Condens\u00e9e de Paris (CMCP)  4 place Jussieu 75005 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cristina","family":"Coelho Diogo","sequence":"additional","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Institut des Mat\u00e9riaux de Paris-Centre IMPC  75005 Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9081-3261","authenticated-orcid":false,"given":"Houria","family":"Kabbour","sequence":"additional","affiliation":[{"name":"Univ. 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