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Treatment of a naphthalene complex with N<jats:sub>2<\/jats:sub> gave an end\u2010on bridging dinitrogen complex featuring a [Ti<jats:sub>2<\/jats:sub>K<jats:sub>2<\/jats:sub>N<jats:sub>2<\/jats:sub>] core. The dinitrogen complex underwent insertion of CO<jats:sub>2<\/jats:sub> into each Ti\u2212NN bond to afford an <jats:italic>N<\/jats:italic>,<jats:italic>N<\/jats:italic>\u2032\u2010dicarboxylated hydrazido complex. Stepwise nitrogen\u2010carbon bond formation at coordinated N<jats:sub>2<\/jats:sub> proceeded to afford an unsymmetric hydrazido complex upon sequentially treating the dinitrogen complex with CS<jats:sub>2<\/jats:sub> and CO<jats:sub>2<\/jats:sub>. Addition of Me<jats:sub>3<\/jats:sub>SiCl to the dicarboxylated hydrazido complex resulted in partial silylation of the carboxylate groups but did not lead to removal of the functionalized N<jats:sub>2<\/jats:sub> unit from the metal centers. However, reduction of the dicarboxylated hydrazido complex with potassium naphthalenide afforded an oxo\u2010bridged dinuclear complex along with release of free potassium cyanate.<\/jats:p>","DOI":"10.1002\/anie.202304700","type":"journal-article","created":{"date-parts":[[2023,6,7]],"date-time":"2023-06-07T07:42:11Z","timestamp":1686123731000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Dinitrogen Functionalization with Carbon Dioxide and Carbon Disulfide Giving Symmetric and Unsymmetric Hydrazido Complexes"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5282-1220","authenticated-orcid":false,"given":"Yutaka","family":"Ishida","sequence":"first","affiliation":[{"name":"Department of Chemistry Tokyo Institute of Technology  Ookayama, Meguro-ku 152-8551 Tokyo 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