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Effect of temperature on the thermodynamic and spectroscopic properties of Np(V) complexes with picolinate

机译：温度对吡啶酸盐的NP（V）配合物热力学和光谱性能的影响

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摘要

Picolinate is a well-known chelating agent and is present in contaminated lands and nuclear wastes. Thermodynamic parameters of the complexation of picolinate with Np(V) at elevated temperatures are needed to help predict the migration behavior of Np(V) in nuclear waste repositories where the temperature could be high. In this work, the equilibrium constants of picolinate protonation and its complexation with Np(V) were determined at T = 283-343 K and I = 1.0 mol dm(-3) NaClO4 by potentiometry and spectrophotometry, respectively. Both the protonation and the complexation constants decrease with the increase of temperature, indicating the reactions are exothermic. The enthalpies of protonation and complexation were both found to be negative and moderately large at T = 298 K and I = 1.0 mol dm(-3) NaClO4 by titration calorimetry. The effect of temperature on the spectroscopic features of Np(V) is interpreted in terms of thermal expansion of the complex coordinates that results in blue shifts of the Np(V) absorption band at higher temperatures.
机译：普罗华酸盐是一个着名的螯合剂，存在于污染的土地和核废物中。需要在高温下与NP（V）络合的热力学参数，以帮助预测温度可能高的核废料储存库中NP（v）的迁移行为。在这项工作中，通过电位测定和分光光度法分别在T = 283-343k和I = 1.0mol dm（-3）NaClO 4处测定吡啶酸盐质子化的平衡常数及其与NP（V）的络合。质子化和络合常数均随温度的增加而降低，表明反应是放热的。通过滴定量热法发现质子化和络合的焓和络合焓在T = 298K和I = 1.0mol DM（-3）NaClO4中是阴性和中等的。在络合坐标的热膨胀方面解释了温度对NP（V）的光谱特征的影响，该坐标的热膨胀导致NP（V）吸收带在较高温度下的蓝色偏移。

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  • 来源
    《RSC Advances》 |2015年第92期|共8页
  • 作者

    Zhang Zhicheng; Yang Yanqiu; Liu Guokui; Luo Shunzhong; Rao Linfeng;

  • 作者单位

    Univ Calif Berkeley Lawrence Berkeley Natl Lab Div Chem Sci Berkeley CA 94720 USA;

    Univ Calif Berkeley Lawrence Berkeley Natl Lab Div Chem Sci Berkeley CA 94720 USA;

    Argonne Natl Lab Chem Sci &

    Engn Div Argonne IL 60439 USA;

    China Acad Engn Phys Inst Nucl Phys &

    Chem Mianyang 621900 Sichuan Peoples R China;

    Univ Calif Berkeley Lawrence Berkeley Natl Lab Div Chem Sci Berkeley CA 94720 USA;

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  • 正文语种 eng
  • 中图分类 化学;
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