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The study of the ternary system Li\u2010Si\u2010P revealed a series of new compounds, two of which, Li<jats:sub>8<\/jats:sub>SiP<jats:sub>4<\/jats:sub> and Li<jats:sub>2<\/jats:sub>SiP<jats:sub>2<\/jats:sub>, are presented. Both phases represent members of a new family of Li ion conductors that display Li ion conductivity in the range from 1.15(7)\u00d710<jats:sup>\u22126<\/jats:sup> Scm<jats:sup>\u22121<\/jats:sup> at 0\u2009\u00b0C to 1.2(2)\u00d710<jats:sup>\u22124<\/jats:sup> Scm<jats:sup>\u22121<\/jats:sup> at 75\u2009\u00b0C (Li<jats:sub>8<\/jats:sub>SiP<jats:sub>4<\/jats:sub>) and from 6.1(7)\u00d710<jats:sup>\u22128<\/jats:sup> Scm<jats:sup>\u22121<\/jats:sup> at 0\u2009\u00b0C to 6(1)\u00d710<jats:sup>\u22126<\/jats:sup> Scm<jats:sup>\u22121<\/jats:sup> at 75\u2009\u00b0C (Li<jats:sub>2<\/jats:sub>SiP<jats:sub>2<\/jats:sub>), as determined by impedance measurements. Temperature\u2010dependent solid\u2010state <jats:sup>7<\/jats:sup>Li NMR spectroscopy revealed low activation energies of about 36\u2005kJ\u2009mol<jats:sup>\u22121<\/jats:sup> for Li<jats:sub>8<\/jats:sub>SiP<jats:sub>4<\/jats:sub> and about 47\u2005kJ\u2009mol<jats:sup>\u22121<\/jats:sup> for Li<jats:sub>2<\/jats:sub>SiP<jats:sub>2<\/jats:sub>. Both compounds were structurally characterized by X\u2010ray diffraction analysis (single crystal and powder methods) and by <jats:sup>7<\/jats:sup>Li, <jats:sup>29<\/jats:sup>Si, and <jats:sup>31<\/jats:sup>P\u2005MAS NMR spectroscopy. Both phases consist of tetrahedral SiP<jats:sub>4<\/jats:sub> anions and Li counterions. Li<jats:sub>8<\/jats:sub>SiP<jats:sub>4<\/jats:sub> contains isolated SiP<jats:sub>4<\/jats:sub> units surrounded by Li atoms, while Li<jats:sub>2<\/jats:sub>SiP<jats:sub>2<\/jats:sub> comprises a three\u2010dimensional network based on corner\u2010sharing SiP<jats:sub>4<\/jats:sub> tetrahedra, with the Li ions located in cavities and channels.<\/jats:p>","DOI":"10.1002\/chem.201602903","type":"journal-article","created":{"date-parts":[[2016,10,27]],"date-time":"2016-10-27T05:37:08Z","timestamp":1477546628000},"page":"17635-17645","source":"Crossref","is-referenced-by-count":85,"title":["Lithium Ion Mobility in Lithium Phosphidosilicates: Crystal Structure, <sup>7<\/sup>Li, <sup>29<\/sup>Si, and <sup>31<\/sup>P\u2005MAS NMR Spectroscopy, and Impedance Spectroscopy of Li<sub>8<\/sub>SiP<sub>4<\/sub> and Li<sub>2<\/sub>SiP<sub>2<\/sub>"],"prefix":"10.1002","volume":"22","author":[{"given":"Lorenzo","family":"Toffoletti","sequence":"first","affiliation":[{"name":"Department of Chemistry 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