『Abstract
Laboratory experiments were carried out continuously for 30-35
days at 25 and 5℃ in three different buffer solutions of pH 4.0,
2.2 and 8.4 to calculate dissolution rates of two minerals, calcite
(CC) and dolomite (DM) and two rocks, leucogranite (LG) and gneiss
(GN) from the Himalayan range. Calculated rates in terms of release
of targeted elements versus time (Ca for CC; Mg for DM; Si for
LG and GN) demonstrate direct correlation with temperature. Dissolution
rates are higher at 25℃ compared to 5℃. CC and DM were experimented
only at pH 8.4 and results show that both undergo congruent dissolution
with CC dissolving 〜5 times faster than DM. Ca and Mg exhibit
average apparent activation energies (Ea)
of 13.98 and 9.98 kcal mol-1 respectively at pH 8.4
which reflects greater sensitivity of CC dissolution than DM dissolution
towards an increase in temperature. Scanning Electron Microscope
attached with Energy Dispersive X-ray Analyser (SEM-EDX) data
indicates that dissolution is controlled primarily by surface-reaction
processes, with dislocation sites contributing maximum to the
dissolution. As compared to CC and DM dissolution, LG and GN undergo
relatively slower incongruent dissolution with precipitation of
some secondary minerals as revealed from X-ray diffractometer
(XRD) results. Rates of dissolution of LG is maximum at pH 2.2,
moderate at pH 8.4 and least at pH 4.0, whereas GN shows maximum
dissolution at pH 2.2, moderate at pH 4.0 and least at pH 8.4.
A comparison in dissolution behavior of LG and GN at experimental
conditions reveals that increase in Si-release rate in the temperature
range between 5 and 25℃ is maximum at pH 8.4 (〜3.4-4.5 time),
moderate at pH 4.0 (〜3-1.8 times) and least at pH 2.2 (〜1.0-1.5
times). Within the experimental temperature range, calculated
values of Ea for Si release during LG and
GN dissolution advocates positive correlation with pH. A substantial
decrease in initial values of Brunauer-Emmett-Teller (BET) surface
area of DM, LG, and GN has been encountered at the end of the
experiment, except for CC for which an increase is observed. The
study clearly demonstrates the dissolution behavior of pure minerals
and rocks under controlled conditions. The dissolution rates assume
enormous significance for the release of trace elements from rocks/minerals
to the reacting water.
Keywords: Calcite; Dolomite; Leucogranite; Gneiss; Dissolution
rates; Kinetics』
Introduction
Materials and methods
Sample characterization, preparation and analytical techniques
Surface area measurement
Experimental solutions
Dissolution experiments
Activation energy and dissolution rate calculations
Results and discussion
Mechanism of calcite (CC) and dolomite (DM) dissolution
Mechanism of leucogranite (LG) and gneiss (GN) dissolution
Post-experiment decrease in surface area
Conclusion
Acknowledgments
References