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The effect of CO2 and salinity on olivine dissolution kinetics at 120 degrees C

机译:CO2和盐度对120摄氏度橄榄石溶解动力学的影响

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This paper reports the results of an experimental study on the dissolution kinetics of olivine (Mg1.82Fe0.18SiO4) at operating conditions relevant to the mineral carbonation process for the permanent storage Of CO2. In particular, we investigated the effects Of CO2 fugacity (f(CO2)) and of salinity on the kinetics of olivine dissolution, which is assumed to be the rate-limiting step of the overall carbonation process. Dissolution experiments were carried out at 120 degrees C in a stirred flow-through reactor. Different pH values (between 3 and 8) and solution compositions were investigated by varying f(CO2) and by dosing LiOH (for pH control), NaCl, and NaNO3. The specific dissolution rate values, r, were estimated from the experimental data using a population balance equation (PBE) model coupled with a mass balance equation. The logarithms of the obtained r values were regressed with a linear model as a function of pH and compared to the model reported earlier [Hanchen, M., Krevor, S., Mazzotti, M., Lackner, K.S., 2007. Validation of a population balance model for olivine dissolution. Chem. Eng. Sci. 62, 6412-6422] for experiments with neither CO2 nor salts. Our results confirm that, at a given temperature, olivine dissolution kinetics depends on pH only, and that f(CO2) and the concentrations of NaCl and NaNO3 affect it through their effect on pH.
机译:本文报道了在与矿物碳酸化过程有关的永久保存CO2的操作条件下,橄榄石(Mg1.82Fe0.18SiO4)溶解动力学的实验研究结果。特别是,我们研究了CO2逸度(f(CO2))和盐度对橄榄石溶解动力学的影响,这被认为是整个碳酸化过程的限速步骤。溶解实验在搅拌的流通式反应器中于120摄氏度进行。通过改变f(CO2)和添加LiOH(用于pH控制),NaCl和NaNO3,研究了不同的pH值(3至8)和溶液组成。使用群体平衡方程(PBE)模型和质量平衡方程从实验数据中估算出特定的溶出速率值r。用线性模型将获得的r值的对数作为pH的函数进行回归,并与先前报道的模型进行比较[Hanchen,M.,Krevor,S.,Mazzotti,M.,Lackner,KS,2007。橄榄石溶解的种群平衡模型。化学。科学62,6412-6422]既不使用CO2也不使用盐的实验。我们的结果证实,在给定温度下,橄榄石的溶解动力学仅取决于pH值,并且f(CO2)以及NaCl和NaNO3的浓度通过它们对pH的影响而对其产生影响。

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