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Herein, we report a unique ternary sulfide compound, Cu<jats:sub>3<\/jats:sub>BiS<jats:sub>3<\/jats:sub>, in which all Cu atoms are coordinated within a two\u2010dimensional [CuS<jats:sub>3<\/jats:sub>] triangle plane. This local coordination leads to efficient out\u2010of\u2010plane phonon scattering and an ultralow thermal conductivity. Through DFT phonon spectrum calculations and analyses, we reveal that the lowest vibration frequency decreases from 2 THz for high\u2010dimensional [CuS<jats:sub>4<\/jats:sub>] tetrahedral coordinated Cu atoms in CuBiS<jats:sub>2<\/jats:sub> (CN=4, with an average Cu\u2212S bond length of 2.328\u2005\u00c5) to 1.5 THz for low\u2010dimensional [CuS<jats:sub>3<\/jats:sub>] triangular coordinated Cu atoms in Cu<jats:sub>3<\/jats:sub>BiS<jats:sub>3<\/jats:sub> (CN=3, with a shorter Cu\u2212S bond length of 2.285\u2005\u00c5). This is due to the out\u2010of\u2010plane thermal vibration of the Cu atoms in the latter. Consequently,Cu<jats:sub>3<\/jats:sub>BiS<jats:sub>3<\/jats:sub> exhibits one of the lowest values of <jats:italic>\u03ba<\/jats:italic><jats:sub>lat<\/jats:sub> (0.32\u2005W\/m\u2009K) among its peer, with a 36\u2009% reduction compared to CuBiS<jats:sub>2<\/jats:sub> (0.50\u2005W\/m\u2009K). This groundbreaking discovery highlights the significant role of 2D local coordination in reducing thermal conductivity through characteristic out\u2010of\u2010plane phonon scattering, while also contributing to a large Gr\u00fcneisen parameter (2.06) in Cu<jats:sub>3<\/jats:sub>BiS<jats:sub>3<\/jats:sub>.<\/jats:p>","DOI":"10.1002\/anie.202315642","type":"journal-article","created":{"date-parts":[[2023,11,7]],"date-time":"2023-11-07T04:14:09Z","timestamp":1699330449000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Cu<sub>3<\/sub>BiS<sub>3<\/sub>: Two\u2010Dimensional Coordination Induces Out\u2010of\u2010Plane Phonon Scattering Enabling Ultralow Thermal Conductivity"],"prefix":"10.1002","volume":"62","author":[{"given":"Fei","family":"Jia","sequence":"first","affiliation":[{"name":"Center for Advanced Materials Research Beijing Normal University, Zhuhai  Zhuhai 519087 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuang","family":"Zhao","sequence":"additional","affiliation":[{"name":"Center for Advanced Materials Research Beijing Normal University, Zhuhai  Zhuhai 519087 P. R. China"},{"name":"College of Chemistry Beijing Normal University  Beijing 100875 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Energy and Power Engineering Huazhong University of Science and Technology  Wuhan Hubei 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3693-4193","authenticated-orcid":false,"given":"Ling","family":"Chen","sequence":"additional","affiliation":[{"name":"College of Chemistry Beijing Normal University  Beijing 100875 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Te\u2010Huan","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Energy and Power Engineering Huazhong University of Science and Technology  Wuhan Hubei 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li\u2010Ming","family":"Wu","sequence":"additional","affiliation":[{"name":"Center for Advanced Materials Research Beijing Normal University, Zhuhai  Zhuhai 519087 P. R. China"},{"name":"College of Chemistry Beijing Normal University  Beijing 100875 P. R. 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