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    Pu(OH)4(am)与碳酸根的配位行为研究

    Complex Formation of Pu(OH)4(am) With Carbonate

      摘要
    • 摘要: 为了解在惰气环境Pu(OH)4(am)与碳酸盐溶液中HCO-3，CO2-3的配位行为，考察了放置时间对Pu总浓度的影响；同时也考察了pH值、碳酸根总浓度变化对碳酸盐溶液中Pu的主要存在形态及溶解总浓度的影响。实验结果表明，HCO-3离子与Pu(OH)4(am)生成Pu(OH)4(HCO3)22-（lg K=-2.61±0.18, lgβ=54.25±0.18）或Pu(OH)2(CO3)22-（lgK=-2.61±0.18, lgβ=46.91±0.18）；CO2-3离子与Pu(OH)4(am）生成Pu(OH)4(CO3)24-（lgK=-3.52±0.11, lgβ=53.33±0.11）。可能的配位反应方程式为：
      Pu(OH)4(am)+2HCO-3 = Pu(OH)4(HCO3)22-,
      Pu(OH)4(am)+2HCO-3 =Pu(OH)2(CO3)22-+2H2O,
      Pu(OH)4(am)+2CO2-3=Pu(OH)4(CO3)24-。

       

      Abstract: The complex formation of Pu(OH)4(am) with carbonate is studied with the variation of pH(8.92~13.08), and the total carbonate concentration range of 10-4~10-2 mol/L. The effect of pH value and total carbonate concentration on the dissolved total concentration of Pu(OH)4(am) and species of Pu in solution are discussed. All experiments were performed in a anaerobic glove box which contained high purity Ar(99.99%), with an oxygen content of less than 5×10-6mol/mol. The experimental results show that 1∶2 complex of Pu(OH)4(am) with bicarbonate is obtained and the complex formation constants determined in the experiments.
      Pu(OH)4(am)+2HCO-3=Pu(OH)4(HCO3)22-， K=10(-2.61±0.18)
      Pu(OH)4(am)+2HCO-3=Pu(OH)2(CO3)22-+2H2O， K=10(-2.61±0.18)
      
      At high pHs （10.28~13.08） where carbonate ion is dominant, 1∶2 complex of Pu(OH)4(am) with carbonate ion is obtained:
      Pu(OH)4(am)+2CO2-3=Pu(OH)4(CO3)24-， K=10(-3.52±0.11).

       

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