Determination of Metal (Bi)Sulfide Stability Constants of Mn2+, Fe2+, Co2+, Ni2+, Cu2+, and Zn2+by Voltammetric Methods
Abstract
The stoichiometry as well as the conditional and thermodynamic stability constants for the (bi)sulfide complexes of the +2 cations of Mn, Fe, Ni, Co, Cu, and Zn have been determined by voltammetric methods in seawater and chloride solutions of varying ionic strength. Acid−base titrations allowed for the determination of the proton stoichiometry of the complexes. Mn, Fe, Ni, and Co form bisulfide, HS -, complexes of stoichiometry MSH +, M 2 (SH) 3+, and M 3 (SH) 5+, which are labile under diffusion control conditions, in seawater at pH values > 7. These complexes dissociate below pH = 7, releasing H 2 S from solution. Evidence for sulfide-rich complexes of form M(SH) 2 was not found. Cu and Zn form sulfide, S 2 -, complexes of stoichiometry MS and M 2 S 3 2 -, which are inert (nonlabile) under diffusion control conditions, in seawater at pH values > 7. There is no evidence for metal-rich sulfide complexes of stoichiometry [M x S] 2 x - 2 from the titration data. The M 2 S 3 2 - complexes are tetrameric structures (M 4 S 6 ) with tetrahedral metal coordination based on known thiolate complex and mineral geometries. The Zn complexes dissociate below pH = 6.7, releasing H 2 S from solution. However, the Cu complex does not fully dissociate below pH = 2 because of Cu(II) reduction and production of polysulfide, which do not appear to be quantitative. At seawater pH, both Zn and Cu sulfide complexes can be deposited on a mercury drop, indicating that these metal complexes are likely responsible for the presence of nanomolar levels of sulfide in oxic seawater.
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MnHS− is likely abundant in pore water in sulfidic sediments.
“The solubility of iron sulfide from Rickard (2006) was added to the database as well as MnHS C as a solute (Luther et al., 1996) because it is likely abundant in pore water in sulfidic sediments (Heiser et al., 2001).”
From Are recent changes in sediment manganese sequestration in the euxinic basins of the Baltic Sea linked to the expansion of hypoxia? (2015) · cites this paper as Luther et al., 1996
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- Authors
- Luther, G. W., Rickard, D. T., Theberge, S., & Olroyd, A.
- Affiliations
- University of Delaware (US)
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 1996-01-01
- Volume
- 30
- Issue
- 2
- Pages
- 671-679
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W4253009332
- Cited by
- 155
- References
- 35
- Citations by year
- 2026: 1 · 2025: 2 · 2024: 4 · 2023: 3 · 2022: 3 · 2021: 4 · 2020: 6 · 2019: 3 · 2018: 6 · 2017: 4 · 2016: 7 · 2015: 7 · 2014: 8 · 2013: 4 · 2012: 8
- FWCI
- 6.12
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- ORCA Online Research @Cardiff (Cardiff University) (submittedVersion)
- Topics
- Physical Sciences › Chemistry › Electrochemistry › Electrochemical Analysis and Applications
- Physical Sciences › Earth and Planetary Sciences › Geochemistry and Petrology › Geochemistry and Elemental Analysis
- Physical Sciences › Chemical Engineering › Filtration and Separation › Chemical and Physical Properties in Aqueous Solutions
- Keywords
- sulfide complexes, stability constants, conditional stability constants, proton stoichiometry, manganese, iron, cobalt, nickel, copper, zinc, seawater, chloride solutions, ionic strength, acid-base titration, hydrogen sulfide release, polysulfides, copper(II) reduction, tetrahedral coordination, metal sulfide precipitation
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