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Inspired by the structural stability of aminophosphonium compounds, here we report the first A<jats:sub>3<\/jats:sub>BX<jats:sub>6<\/jats:sub>type cyanometallate [Ph<jats:sub>2<\/jats:sub>(<jats:sup>i<\/jats:sup>PrNH)<jats:sub>2<\/jats:sub>P]<jats:sub>3<\/jats:sub>[Fe(CN)<jats:sub>6<\/jats:sub>] (<jats:bold>1<\/jats:bold>), which shows a ferroelectric saturation polarization (<jats:italic>P<jats:sub>s<\/jats:sub><\/jats:italic>) of 3.71\u2005\u03bcC\u2009cm<jats:sup>\u22122<\/jats:sup>. Compound<jats:bold>1<\/jats:bold>exhibits a high electrostrictive coefficient (<jats:italic>Q<jats:sub>33<\/jats:sub><\/jats:italic>) of 0.73\u2005m<jats:sup>4<\/jats:sup>\u2005C<jats:sup>\u22122<\/jats:sup>, far exceeding those of piezoceramics (0.034\u20130.096\u2005m<jats:sup>4<\/jats:sup>\u2005C<jats:sup>\u22122<\/jats:sup>). Piezoresponse force microscopy (PFM) analysis demonstrates the polarization switching and domain structure of<jats:bold>1<\/jats:bold>further confirming its ferroelectric nature. Furthermore, thermoplastic polyurethane (TPU) polymer composite films of<jats:bold>1<\/jats:bold>were prepared and employed as piezoelectric nanogenerators. Notably, the 15\u2005wt\u2009%<jats:bold>1<\/jats:bold>\u2010TPU device gave a maximum output voltage of 13.57\u2005V and a power density of 6.03\u2005\u03bcW\u2009cm<jats:sup>\u22122<\/jats:sup>.<\/jats:p>","DOI":"10.1002\/anie.202214984","type":"journal-article","created":{"date-parts":[[2022,11,21]],"date-time":"2022-11-21T11:43:45Z","timestamp":1669031025000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["A Ferroelectric Aminophosphonium Cyanoferrate with a Large Electrostrictive Coefficient as a Piezoelectric Nanogenerator"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4456-5655","authenticated-orcid":false,"given":"Thangavel","family":"Vijayakanth","sequence":"first","affiliation":[{"name":"Department of Chemistry and Centre for Energy Science Indian Institute of Science Education and Research, Pune Dr. Homi Bhabha Road Pune 411008 India"},{"name":"Present address: The Shmunis School of Biomedicine and Cancer Research George S. Wise, Faculty of Life Sciences Tel Aviv University Tel Aviv 6997801 Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6896-7168","authenticated-orcid":false,"given":"Supriya","family":"Sahoo","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Centre for Energy Science Indian Institute of Science Education and Research, Pune Dr. Homi Bhabha Road Pune 411008 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Premkumar","family":"Kothavade","sequence":"additional","affiliation":[{"name":"Polymer Science and Engineering Division and Academy of Scientific and Innovative Research CSIR-National Chemical Laboratory Dr. Homi Bhabha Road Pune 411008 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vijay","family":"Bhan Sharma","sequence":"additional","affiliation":[{"name":"Department of Physics Indian Institute of Technology Mumbai 400076 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dinesh","family":"Kabra","sequence":"additional","affiliation":[{"name":"Department of Physics Indian Institute of Technology Mumbai 400076 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6117-6876","authenticated-orcid":false,"given":"Jan K.","family":"Zar\u0119ba","sequence":"additional","affiliation":[{"name":"Institute of Advanced Materials Wroc\u0142aw University of Science and Technology 50-370 Wroc\u0142aw Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kadhiravan","family":"Shanmuganathan","sequence":"additional","affiliation":[{"name":"Polymer Science and Engineering Division and Academy of Scientific and Innovative Research CSIR-National Chemical Laboratory Dr. Homi Bhabha Road Pune 411008 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5933-4414","authenticated-orcid":false,"given":"Ramamoorthy","family":"Boomishankar","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Centre for Energy Science Indian Institute of Science Education and Research, Pune Dr. Homi Bhabha Road Pune 411008 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