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Selenium(IV) Sorption Onto γ-Al2O3: A Consistent Description of the Surface Speciation by Spectroscopy and Thermodynamic Modeling
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2018-01-05 00:00:00 , DOI: 10.1021/acs.est.7b04546 Natalia Mayordomo 1 , Harald Foerstendorf 2 , Johannes Lützenkirchen 3 , Karsten Heim 2 , Stephan Weiss 2 , Ursula Alonso 1 , Tiziana Missana 1 , Katja Schmeide 2 , Norbert Jordan 2
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2018-01-05 00:00:00 , DOI: 10.1021/acs.est.7b04546 Natalia Mayordomo 1 , Harald Foerstendorf 2 , Johannes Lützenkirchen 3 , Karsten Heim 2 , Stephan Weiss 2 , Ursula Alonso 1 , Tiziana Missana 1 , Katja Schmeide 2 , Norbert Jordan 2
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The sorption processes of Se(IV) onto γ-Al2O3 were studied by in situ Infrared spectroscopy, batch sorption studies, zeta potential measurements and surface complexation modeling (SCM) in the pH range from 5 to 10. In situ attenuated total reflection fourier-transform infrared (ATR FT-IR) spectroscopy revealed the predominant formation of a single inner-sphere surface species at the alumina surface, supporting previously reported EXAFS results, irrespective of the presence or absence of atmospherically derived carbonate. The adsorption of Se(IV) decreased with increasing pH, and no impact of the ionic strength was observed in the range from 0.01 to 0.1 mol L–1 NaCl. Inner-sphere surface complexation was also suggested from the shift of the isoelectric point of γ-Al2O3 observed during zeta potential measurements when Se(IV) concentration was 10–4 mol L–1. Based on these qualitative findings, the acid–base surface properties of γ-Al2O3 and the Se(IV) adsorption edges were successfully described using a 1-pK CD-MUSIC model, considering one bidentate surface complex based on previous EXAFS results. The results of competitive sorption experiments suggested that the surface affinity of Se(IV) toward γ-Al2O3 is higher than that of dissolved inorganic carbon (DIC). Nevertheless, from the in situ experiments, we suggest that the presence of DIC might transiently impact the migration of Se(IV) by reducing the number of available sorption sites on mineral surfaces. Consequently, this should be taken into account in predicting the environmental fate of Se(IV).
中文翻译：
硒（IV）吸附在γ-Al系2 ö 3：通过光谱学和热力学模型表面形态的一个一致的说明
在5〜10的pH范围内，通过原位红外光谱，批吸附研究，ζ电位测量和表面络合建模（SCM）研究了Se（IV）在γ-Al 2 O 3上的吸附过程。反射傅立叶变换红外光谱（ATR FT-IR）揭示了氧化铝表面主要形成单个内球表面物质，支持先前报道的EXAFS结果，而与是否存在大气衍生的碳酸盐无关。随着pH的升高，Se（IV）的吸附降低，在0.01至0.1 mol L –1的范围内未观察到离子强度的影响氯化钠 内球表面络合也从的等电点的移位建议的γ-Al 2 ö 3期间zeta电位测量观察到当硒（IV）的浓度为10 -4摩尔大号-1。基于这些定性结果，的酸-碱的表面特性的γ-Al 2 ö 3以及Se的使用一个1-p的成功（IV）所述的吸附边缘ķ CD-MUSIC模型，考虑一个二齿表面复杂的基于先前的EXAFS结果。竞争吸附实验的结果表明，硒（IV）朝向的表面亲和力的γ-Al 2 ö 3高于溶解的无机碳（DIC）。然而，从原位实验中，我们建议DIC的存在可能会通过减少矿物表面上可用的吸附位点的数量而短暂地影响Se（IV）的迁移。因此，在预测Se（IV）的环境命运时应考虑到这一点。
更新日期：2018-01-06
中文翻译：
硒（IV）吸附在γ-Al系2 ö 3：通过光谱学和热力学模型表面形态的一个一致的说明
在5〜10的pH范围内，通过原位红外光谱，批吸附研究，ζ电位测量和表面络合建模（SCM）研究了Se（IV）在γ-Al 2 O 3上的吸附过程。反射傅立叶变换红外光谱（ATR FT-IR）揭示了氧化铝表面主要形成单个内球表面物质，支持先前报道的EXAFS结果，而与是否存在大气衍生的碳酸盐无关。随着pH的升高，Se（IV）的吸附降低，在0.01至0.1 mol L –1的范围内未观察到离子强度的影响氯化钠 内球表面络合也从的等电点的移位建议的γ-Al 2 ö 3期间zeta电位测量观察到当硒（IV）的浓度为10 -4摩尔大号-1。基于这些定性结果，的酸-碱的表面特性的γ-Al 2 ö 3以及Se的使用一个1-p的成功（IV）所述的吸附边缘ķ CD-MUSIC模型，考虑一个二齿表面复杂的基于先前的EXAFS结果。竞争吸附实验的结果表明，硒（IV）朝向的表面亲和力的γ-Al 2 ö 3高于溶解的无机碳（DIC）。然而，从原位实验中，我们建议DIC的存在可能会通过减少矿物表面上可用的吸附位点的数量而短暂地影响Se（IV）的迁移。因此，在预测Se（IV）的环境命运时应考虑到这一点。
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