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Hg<jats:sup>II<\/jats:sup> is considered to be enclosed in the \u03b1 and \u03b2 domains as tetrahedral \u03b1\u2010type Hg<jats:sub>4<\/jats:sub>Cys<jats:sub>11\u201012<\/jats:sub> and \u03b2\u2010type Hg<jats:sub>3<\/jats:sub>Cys<jats:sub>9<\/jats:sub> clusters similar to Cd<jats:sup>II<\/jats:sup> and Zn<jats:sup>II<\/jats:sup>. However, neither the four\u2010fold coordination of Hg nor the existence of Hg\u2013Hg atomic pairs have ever been demonstrated, and the Hg<jats:sup>II<\/jats:sup> partitioning among the two protein domains is unknown. Using high energy\u2010resolution XANES spectroscopy, MP2 geometry optimization, and biochemical analysis, evidence for the coexistence of two\u2010coordinate Hg\u2010thiolate complex and four\u2010coordinate Hg\u2010thiolate cluster with a metacinnabar\u2010type (\u03b2\u2010HgS) structure in the \u03b1 domain of separate metallothionein molecules from blue mussel under in vivo exposure is provided. The findings suggest that the CXXC claw setting of thiolate donors, which only exists in the \u03b1 domain, acts as a nucleation center for the polynuclear complex and that the five CXC motifs from this domain serve as the cluster\u2010forming motifs. Oligomerization is driven by metallophilic Hg\u22c5\u22c5\u22c5Hg interactions. Our results provide clues as to why Hg has higher affinity for the \u03b1 than the \u03b2 domain. More generally, this work provides a foundation for understanding how metallothioneins mediate mercury detoxification in the cell under in vivo conditions.<\/jats:p>","DOI":"10.1002\/chem.201804209","type":"journal-article","created":{"date-parts":[[2018,11,14]],"date-time":"2018-11-14T02:48:30Z","timestamp":1542163710000},"page":"997-1009","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Mercury(II) Binding to Metallothionein in <i>Mytilus edulis<\/i> revealed by High Energy\u2010Resolution XANES Spectroscopy"],"prefix":"10.1002","volume":"25","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0845-611X","authenticated-orcid":false,"given":"Alain","family":"Manceau","sequence":"first","affiliation":[{"name":"ISTerre Univ. 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