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Using enriched stable isotopes, we investigated the rates and dynamics of isotope exchange between 202Hg(0)aq and 201Hg(II) bound to organic and inorganic ligands with varying chemical structures and binding affinities. Time-dependent exchange reactions were followed by isotope compositional changes using both inductively coupled plasma mass spectrometry and Zeeman cold vapor atomic absorption spectrometry. Rapid, spontaneous isotope exchange (&amp;lt;1 h) was observed between 202Hg(0)aq and 201Hg(II) bound to chloride (Cl\u2013), ethylenediaminetetraacetate (EDTA), and thiols, such as cysteine (CYS), glutathione (GSH), and 2,3-dimercaptopropanesulfonic acid (DMPS) at a thiol ligand-to-Hg(II) molar ratio of 1:1. Without external reductants or oxidants, the exchange resulted in transfer of two electrons and redistribution of Hg isotopes bound to the ligand but no net changes of chemical species in the system. However, an increase in the ligand-to-Hg(II) ratio decreased the exchange rates due to the formation of 2:1 or higher thiol:Hg(II) chelated complexes, but had no effects on exchange rates with 201Hg(II) bound to EDTA or Cl\u2013. The exchange between 202Hg(0)aq and 201Hg(II) bound to dissolved organic matter (DOM) showed an initially rapid followed by a slower exchange rate, likely resulting from Hg(II) complexation with both low- and high-affinity binding functional groups on DOM (e.g., carboxylates vs bidentate thiolates). These results demonstrate that Hg(0)aq readily exchanges with Hg(II) bound to various ligands and highlight the importance of considering exchange reactions in experimental enriched Hg isotope tracer studies or in natural abundance Hg isotope studies in environmental matrices.<\/jats:p>","DOI":"10.1021\/acs.est.0c06229","type":"journal-article","created":{"date-parts":[[2020,11,16]],"date-time":"2020-11-16T12:28:49Z","timestamp":1605529729000},"page":"15534-15545","source":"Crossref","is-referenced-by-count":36,"title":["Rates\nand Dynamics of Mercury Isotope Exchange between\nDissolved Elemental Hg(0) and Hg(II) Bound to Organic and Inorganic\nLigands"],"prefix":"10.1021","volume":"54","author":[{"given":"Quanying","family":"Wang","sequence":"first","affiliation":[{"name":"Northeast Institute of Geography and Agroecology, Chinese Academy of Sciences , , ,","place":["Changchun, China, 130102"]},{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lijie","family":"Zhang","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xujun","family":"Liang","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangping","family":"Yin","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaoling","family":"Zhang","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3413-9700","authenticated-orcid":true,"given":"Wang","family":"Zheng","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]},{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4951-1931","authenticated-orcid":true,"given":"Eric M.","family":"Pierce","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7299-2956","authenticated-orcid":true,"given":"Baohua","family":"Gu","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37830"]},{"name":"University of Tennessee , , , ,","place":["Knoxville, Tennessee, United States, 37996"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2020,11,16]]},"reference":[{"key":"2026090202182876800_cit1","doi-asserted-by":"publisher","first-page":"101","DOI":"10.1016\/j.envres.2012.03.013","article-title":"Mercury\nbiogeochemical cycling in the ocean and policy implications","volume":"119","author":"Mason","year":"2012","journal-title":"Environ. 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