Journal
GEOCHIMICA ET COSMOCHIMICA ACTA
Volume 69, Issue 5, Pages 1111-1121Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.gca.2004.07.036
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Methylmercury cation (CH3Hg+) is known to have a strong affinity for organic matter in soil, sedimentary, and aquatic environments. The objective of this study is to determine the dominant ligands binding CH3Hg+ in humic acids by evaluating several CH3Hg+-Iigand complexation models, using mercury L-III-edge extended X-ray absorption fine structure (EXAFS). The model CH3Hg+ binding ligands examined in this study include thiol (-SH), hydrogen polysulfide (-SSH or -SSSH), sulfide (-S-), disulfide (-SS-), carboxyl (-COOH), and amine (-NH2). Based on the atomic geometry around mercury in each model structure, we distinguished CH3Hg+-bindihg ligands in two different humic acids (soil and aquatic). We observed CH3Hg+ preferentially binds to thiol ligands. After saturating reactive thiol ligands, the majority of CH3Hg+ binds to carboxyl ligands rather than to amine or other reduced sulfur ligands than thiol. We found no evidence of significant CH3Hg+-sulfide/disulfide or CH3Hg+-hydrogen polysulfide complexes in any samples. When CH3Hg+ binds to a humic ligand, the C-Hg bond in CH3Hg+ remains intact. Some heavy atoms are proximately coordinated around the mercury atom in the sample containing the highest CH3Hg+ levels used in this study. Copyright (c) 2005 Elsevier Ltd.
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