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HSNO and HSSNO with their conjugate bases <jats:sup>\u2212<\/jats:sup>SNO and <jats:sup>\u2212<\/jats:sup>SSNO form in the reaction of H<jats:sub>2<\/jats:sub>S with NO as well as S\u2010nitrosothiols (RSNO) and nitrite (NO<jats:sub>2<\/jats:sub><jats:sup>\u2212<\/jats:sup>) that serve as NO reservoirs. While HSNO and HSSNO are elusive, their conjugate bases form isolable zinc complexes <jats:sup>Ph,Me<\/jats:sup>TpZn(SNO) and <jats:sup>Ph,Me<\/jats:sup>TpZn(SSNO) supported by tris(pyrazolyl)borate ligands. Reaction of Na(15\u2010C\u20105)SSNO with <jats:sup>Ph,Me<\/jats:sup>TpZn(ClO<jats:sub>4<\/jats:sub>) provides <jats:sup>Ph,Me<\/jats:sup>TpZn(SSNO) that undergoes S\u2010atom removal by PEt<jats:sub>3<\/jats:sub> to give <jats:sup>Ph,Me<\/jats:sup>TpZn(SNO) and S=PEt<jats:sub>3<\/jats:sub>. Unexpectedly stable at room temperature, these Zn\u2010SNO and Zn\u2010SSNO complexes release NO upon heating. <jats:sup>Ph,Me<\/jats:sup>TpZn(SNO) and <jats:sup>Ph,Me<\/jats:sup>TpZn(SSNO) quickly react with acidic thiols such as C<jats:sub>6<\/jats:sub>F<jats:sub>5<\/jats:sub>SH to form N<jats:sub>2<\/jats:sub>O and NO, respectively. Increasing the thiol basicity in p\u2010substituted aromatic thiols <jats:sup>4\u2212X<\/jats:sup>ArSH in the reaction with <jats:sup>Ph,Me<\/jats:sup>TpZn(SNO) turns on competing S\u2010nitrosation to form <jats:sup>Ph,Me<\/jats:sup>TpZn\u2010SH and RSNO, the latter a known precursor for NO.<\/jats:p>","DOI":"10.1002\/anie.202104906","type":"journal-article","created":{"date-parts":[[2021,6,28]],"date-time":"2021-06-28T07:51:02Z","timestamp":1624866662000},"page":"21184-21188","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":28,"title":["Thionitrite and Perthionitrite in NO Signaling at Zinc"],"prefix":"10.1002","volume":"60","author":[{"given":"Valiallah","family":"Hosseininasab","sequence":"first","affiliation":[{"name":"Department of Chemistry Georgetown University  Box 571227 Washington DC 20057-1227 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3419-5163","authenticated-orcid":false,"given":"Jeffery A.","family":"Bertke","sequence":"additional","affiliation":[{"name":"Department of Chemistry Georgetown University  Box 571227 Washington DC 20057-1227 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9217-8890","authenticated-orcid":false,"given":"Timothy H.","family":"Warren","sequence":"additional","affiliation":[{"name":"Department of Chemistry Georgetown University  Box 571227 Washington DC 20057-1227 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2021,8,23]]},"reference":[{"key":"e_1_2_2_1_1","unstructured":"\u00a0"},{"key":"e_1_2_2_2_2","volume-title":"Nitric Oxide: Biology and Pathobiology","author":"Ignarro L. 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