『Abstract
Cinnabar (HgS) dissolution rates were measured in the presence
of 12 different natural dissolved organic matter (DOM) isolates
including humic, fulvic, and hydrophobic acid fractions. Initial
dissolution rates varied by 1.3 orders of magnitude, from 2.31×10-13
to 7.16×10-12 mol Hg (mg C)-1 m-2
s-1. Rates correlate positively with three DOM characteristics:
specific ultraviolet absorbance (R2 = 0.88), aromaticity
(R2 = 0.80), and molecular weight (R2 =
0.76). Three experimental observations demonstrate that dissolution
was controlled by the interaction of DOM with the cinnabar surface:
(1) linear rates of HgS release with time, (2) significantly reduced
rates when DOM was physically separated from the surface by dialysis
membranes, and (3) rates that approached constant values at a
specific ratio of DOM concentration to cinnabar surface area,
suggesting a maximum surface coverage by dissolution-reactive
DOM. Dissolution rates for the hydrophobic acid fractions correlate
negatively with sorbed DOM concentrations, indicating the presence
of a DOM component that reduced the surface area of cinnabar that
can be dissolved. When two hydrophobic acid isolates that enhanced
dissolution to different extents were mixed equally, a 20% reduction
in rate occurred compared to the rate with the more dissolution-enhancing
isolate alone. Rates in the presence of the more dissolution enhancing
isolate were reduced by as much as 60% when cinnabar was prereacted
with the isolate that enhanced dissolution to a lesser extent.
The data, taken together, imply that the property of DOM that
enhances cinnabar dissolution is distinct from the property that
causes it to sorb irreversibly to the cinnabar surface.』
1. Introduction
2. Materials and methods
2.1. Materials
2.2. Experimental methods
2.2.1. Dissolution experiments
2.2.2. Dialysis experiments
2.2.3. Sorption experiments
3. Results
3.1. Dissolution rates in the presence of single DOM isolates
3.2. Dissolution in dialysis experiments
3.3. Sorption of DOM to the cinnabar surface
3.4. Dissolution rates in the presence of two DOM isolates
4. Discussion
4.1. Qualitative dissolution model
4.2. Chemical controls on the dissolution rate of cinnabar
4.3. Enhancement of dissolution via interaction of DOM with the
cinnabar surface
4.4. Slowing of dissolution via interaction of DOM with the cinnabar
surface
4.5. Nature of dissolution-enhancing and dissolution-slowing
components of DOM
4.6. Possible role of competitive sorption during dissolution
5. Conclusions
Acknowledgments
References