Labradorite (Ca 0.6Na 0.4Al 1.6Si 2.4O 8) dissolution rates were measured using a mixed flow reactor from 30 to 130°C as a function of dissolved CO 2 (1.2×10 −5 and 0.6 M), and aluminum (10 −6 to 10 −3 M) at pH 3.2. Over these experimental conditions, labradorite dissolution can be described with a single rate expression that accounts for observed increases in dissolution rate with increasing temperature and decreases in dissolution rate with increasing dissolved aluminum: (A1) Si Rate ( mol Labradorite cm − 2 s − 1 ) = k × 10 − E a / 2.303 R T [ ( a H + 3 n / a Al 3 + n ) K T / ( 1 + K T ( a H + 3 n / a Al 3 + n ) ) ] Si Rate where the apparent dissolution rate constant, k=10 −5.69 (mol Labradorite cm −2 s −1) and the net activation energy, E a=10.06 (kcal mol −1). This temperature-dependent rate expression is partly based on the model proposed by Oelkers et al. (1994) [Oelkers, E.H., Schott, J., Devidal, J., 1994. The effect of aluminum, pH, and chemical affinity on the rates of aluminosilicate dissolution reactions. Geochim. Cosmochim. Acta, 58, 2011–2024.] in which the dependence of silicate dissolution rates on dissolved aluminum in acidic solutions is attributed to H +–Al 3+ exchange at the mineral surface and formation of silica-rich surface complexes. For this exchange reaction, regression of the experimental data yield a stoichiometric coefficient n=0.31 and an enthalpy of reaction Δ H=0.54 (kcal mol −1). The temperature dependence of the silica-rich surface complex formation constant, K T, was estimated from the van't Hoff equation and yielded K T=4.49 to 5.61 from 30 to 130 °C. Elevated CO 2(aq) concentrations enhance mineral dissolution indirectly by acidifying solution pH. At temperatures below 100 °C, labradorite dissolves incongruently with preferential dissolution of Na, Ca, and Al over Si.
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