二氧化碲在250℃时在水蒸气中的溶解度

Jonathan Reed Adams, N. Hurtig, A. Gysi, A. Migdissov
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引用次数: 0

摘要

碲是一种在绿色能源技术中日益重要的关键矿物。利用以前的热力学数据进行的数值模拟预测,以h2te (g)为主要蒸汽种的超低温蒸汽中高达~0.1 ppm[1]。然而,流体包裹体研究表明,在低温热液矿床的蒸汽包裹体中,Te含量高达数百ppm[2]。本研究通过实验测量了碲在水热蒸汽中的溶解度,以确定水合碲在水蒸气中的形态。水合作用是水蒸气分子与金属结合的作用,大大增加了金属的溶解度[3]。实验在间歇式Ti Parr反应器中进行,温度为250°C,水蒸汽压(ph2o)范围内,使用几种不同的氧气缓冲液(例如MoO 2 -MoO 3, wo2 - wo3和Ni-NiO)。在250°C和20 bar以及不同的氧化还原条件下进行了1-25天的动力学实验。在氧化条件下,溶解Te为1.33±0.01 ppm,约10天后达到平衡状态,而在氮气脱气实验中,溶解Te为0.669±0.004 ppm,约22天后达到平衡状态,表明在较低的氧化还原条件下反应动力学较慢,溶解度降低。在250°C和-24 (MoO 2 -MoO 3缓冲液)的log O 2下的实验表明,随着ph2o的增加,Te的溶解度从15-25 bar之间的1-3 ppm增加到35 bar时的12.27±0.01 ppm Te。moo2 - moo3缓冲实验的浓度与氧化条件下动力学系列的结果重叠。在250°C和-39.37 (wo2 - wo3缓冲液)的对数o2下的实验表明,在15-35 bar之间,Te的溶解度从14.51 ppm增加到15.45±0.01 ppm。先前的实验工作表明,由于TeO 2 * x h2o与x = 1和2形成[1,4-5],TeO 2在水蒸气中的溶解度增强,而在本研究中,Te表现出与其他金属相似的更高的水化数[3]。基于wo2 - wo3缓冲实验的结果,我们的研究结果证明了ph2o对低密度流体中tesolbility的重要作用,以及对氧化还原的强控制。所得实验数据可应用于热液体系中碲迁移率的热力学模型。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The solubility of tellurium dioxide in water vapor at 250°C
Tellurium is a critical mineral of increasing importance in green energy technologies. Numerical simulations using previous thermodynamic data predict up to ~0.1 ppm in epithermal vapor with H 2 Te(g) as the dominant vapor species [1]. However, fluid inclusion studies show up to hundreds of ppm Te in vapor inclusions from epithermal ore deposits [2]. In this study, we measured experimentally the solubility of tellurium in hydrothermal vapors to determine the hydrated tellurium speciation in water vapor. Hydration is the effect of water vapor molecules binding to a metal, greatly increasing its solubility [3]. Experiments were conducted in batch-type Ti Parr reactors at 250°C and a range of water vapor pressures (P H2O ) using several different oxygen buffers (e.g., MoO 2 -MoO 3 , WO 2 -WO 3 and Ni-NiO). Kinetic experiments were conducted between 1-25 days at 250°C and 20 bar and at different redox conditions. At oxidizing conditions, equilibrium conditions were reached after ~10 days with 1.33 ±0.01 ppm dissolved Te, whereas in N 2 -degassed experiments equilibrium was reached after ~22 days with 0.669 ±0.004 ppm dissolved Te, indicating slower reaction kinetics and reduced solubility at lower redox conditions. Experiments at 250°C and log f O 2 of -24 (MoO 2 -MoO 3 buffer), show increasing Te solubility with increasing P H2O ranging from 1-3 ppm between 15-25 bar to 12.27±0.01 ppm Te at 35 bar. The MoO 2 -MoO 3 buffered experiments overlap in concentrations with results from the kinetic series at oxidizing conditions. Experiments at 250°C and log f O 2 of -39.37 (WO 2 -WO 3 buffer), show an increase in Te solubility between 15-35 bar from 14.51 ppm up to 15.45±0.01 ppm. Previous experimental work has shown enhanced solubility of TeO 2 in water vapor due to the formation of TeO 2 * x H 2 O with x = 1 and 2 [1,4-5], whereas in this study Te shows higher hydration numbers similar to other metals [3]. Our results demonstrate the significant role of P H2O on Tesolubility in low density fluids as wellas a strong redox control based on results from the WO 2 -WO 3 buffered experiment. The experimental data generated can be applied in thermodynamic models to discern tellurium mobility in hydrothermal systems.
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