Th（Ⅳ）在白云母和钠长石上的吸附
摘要
Th(Ⅳ)在放射性废物处置库围岩上的吸附行为是深入研究钍在处置库介质中迁移规律不可缺少的内容,也是研究四价锕系元素在处置库围岩介质上吸附的主要方法之一,研究Th(IV)在处置库围岩组分上的吸附对放射性废物处置库的选址建造和安全影响评价具有重要意义。本文对花岗岩质处置库围岩成分白云母和钠长石的化学组成和结构组成进行了表征,采用实验室静态批式法研究了环境中Th(Ⅳ)在花岗岩的重要组分白云母和钠长石上的吸附规律。探讨了接触时间、吸附剂粒径、固液比、体系酸碱度、初始浓度、温度、不同价态阴离子、离子强度以及腐殖酸类物质对Th(Ⅳ)吸附行为的影响,探讨了白云母和钠长石吸附Th(Ⅳ)的机制。结果表明：
接触时间、固液比、吸附剂粒径大小、初始Th(Ⅳ)浓度、温度和HA对Th(Ⅳ)在白云母上的吸附有强烈的影响,离子强度对吸附没有明显影响。
Th(Ⅳ)在白云母上的吸附随固液比、体系pH的增大,温度的升高以及HA的存在而增大,NaCl04对Th(Ⅳ)在白云母上的吸附不产生影响,Th(Ⅳ)在白云母上的吸附受pH强烈影响以及不受离子强度的影响表明：在低pH范围内Th(Ⅳ)在白云母上的吸附机理为表面络合和化学吸附,而在高pH时以表面沉淀和络合为主。
升高温度促进Th(Ⅳ)在白云母上的吸附量,温度有利于白云母对Th(Ⅳ)的吸附,Th(Ⅳ)的吸附是自发吸热过程。
与白云母对Th(Ⅳ)的吸附规律类似,钠长石对Th(Ⅳ)的吸附受吸附剂浓度、吸附质初始浓度、共存阴离子、溶液pH、腐殖酸物质Hu-s的影响显著,吸附剂浓度的增大、pH升高、初始吸附质浓度的降低、腐殖酸物质的存在均增加Th(I V)在钠长石上的吸附百分数。
二价阴离子影响Th(IV)在钠长石上的吸附,研究发现：二价8O42-对吸附起抑制作用,相比之下三价阴离子P043-对Th(Ⅳ)吸附的促进作用显著。
在高离子强度溶液中,Th(I V)在钠长石上的吸附量随离子强度的增大而增大,高离子强度对Th(Ⅳ)吸附量的促进作用以及Th(IV)吸附对pH的强烈依赖性表明,在Th(Ⅳ)未发生沉淀前,Th(I V)在钠长石上吸附机理为内层络合,在有沉淀的情况下兼有沉淀和表面络合双重作用。
Sorption of Th(Ⅳ) on Muscovite and Albite,which are two important components of Granite existing extensively in earth crust, is of great significance for study of Th(Ⅳ) transportation in either host rock or near field environment, particularly for similar chemical behavior and steady valence state Th(Ⅳ) is generally regarded as analogy of actinides and therefore normally employed to research such tetra valence actinide as Pu.
In this paper, Muscovite and Albite were characterized respectively by XRD、SEM and FTIR for their structure、appearance and configuration with/without presence of Th(IV) due to its sorption, The sorption of Th(Ⅳ) on Muscovite and Albite were investigated by batch technique as a function of contact time, solid-liquid ratio、pH、initial total concentration、coexist anions、 temperature and Hu-s under atmosphere condition. The results were demonstrated as follows:
Sorption of Th(Ⅳ) on Muscovite was strongly dependent on contact time, solid content, pH, particle size, and temperature, an increase in solid content, pH, particle size mesh as well as HA gave rise to distinct change in sorption curves and was responded by corresponding increase in sorption percentage. Moreover the sorption was free from ion strength while temperature acted an positive role in sorption capacity, suggesting temperature was favorable to Th(Ⅳ) sorption on Muscovite and sorption reaction was an spontaneous endothermic process.
Based on the sorption effect that Th(Ⅳ) sorption on Muscovite was not affected by ion strength while extremely sensitive to pH, it was found the sorption mechanism was inner-complex under low pH whereas an combination of inner-complex with surface precipitation worked at high pH.
Like sorption of Th(Ⅳ) on Muscovite, sorption of Th(Ⅳ) on Albite beared similar phenomena with Muscovite, Sorption was significantly influenced and enhanced by such factors as higher adsorbent concentration, lower adsorbate concentration, high pH and HA/FA.
Furthermore, Sorption of Th(Ⅳ) on Albite was related to foreign anions, it was found PO43+contributed to positive sorption effect of Th(Ⅳ) percentage in contrast with negative sorption effect of SO42-.
Finally, instead of failure in obvious effect of Th(Ⅳ) sorption on Muscovite, there was an increase in sorption percentage of Th(Ⅳ) on Albite with increasing ion strength, from～0to1.2M NaClO4range Th(Ⅳ) sorption percentage rised rapidly by a margin about30%. This showed inner-complex was the main sorption mechanism at low pH values along with intense pH reliance.
接触时间、固液比、吸附剂粒径大小、初始Th(Ⅳ)浓度、温度和HA对Th(Ⅳ)在白云母上的吸附有强烈的影响,离子强度对吸附没有明显影响。
Th(Ⅳ)在白云母上的吸附随固液比、体系pH的增大,温度的升高以及HA的存在而增大,NaCl04对Th(Ⅳ)在白云母上的吸附不产生影响,Th(Ⅳ)在白云母上的吸附受pH强烈影响以及不受离子强度的影响表明：在低pH范围内Th(Ⅳ)在白云母上的吸附机理为表面络合和化学吸附,而在高pH时以表面沉淀和络合为主。
升高温度促进Th(Ⅳ)在白云母上的吸附量,温度有利于白云母对Th(Ⅳ)的吸附,Th(Ⅳ)的吸附是自发吸热过程。
与白云母对Th(Ⅳ)的吸附规律类似,钠长石对Th(Ⅳ)的吸附受吸附剂浓度、吸附质初始浓度、共存阴离子、溶液pH、腐殖酸物质Hu-s的影响显著,吸附剂浓度的增大、pH升高、初始吸附质浓度的降低、腐殖酸物质的存在均增加Th(I V)在钠长石上的吸附百分数。
二价阴离子影响Th(IV)在钠长石上的吸附,研究发现：二价8O42-对吸附起抑制作用,相比之下三价阴离子P043-对Th(Ⅳ)吸附的促进作用显著。
在高离子强度溶液中,Th(I V)在钠长石上的吸附量随离子强度的增大而增大,高离子强度对Th(Ⅳ)吸附量的促进作用以及Th(IV)吸附对pH的强烈依赖性表明,在Th(Ⅳ)未发生沉淀前,Th(I V)在钠长石上吸附机理为内层络合,在有沉淀的情况下兼有沉淀和表面络合双重作用。
Sorption of Th(Ⅳ) on Muscovite and Albite,which are two important components of Granite existing extensively in earth crust, is of great significance for study of Th(Ⅳ) transportation in either host rock or near field environment, particularly for similar chemical behavior and steady valence state Th(Ⅳ) is generally regarded as analogy of actinides and therefore normally employed to research such tetra valence actinide as Pu.
In this paper, Muscovite and Albite were characterized respectively by XRD、SEM and FTIR for their structure、appearance and configuration with/without presence of Th(IV) due to its sorption, The sorption of Th(Ⅳ) on Muscovite and Albite were investigated by batch technique as a function of contact time, solid-liquid ratio、pH、initial total concentration、coexist anions、 temperature and Hu-s under atmosphere condition. The results were demonstrated as follows:
Sorption of Th(Ⅳ) on Muscovite was strongly dependent on contact time, solid content, pH, particle size, and temperature, an increase in solid content, pH, particle size mesh as well as HA gave rise to distinct change in sorption curves and was responded by corresponding increase in sorption percentage. Moreover the sorption was free from ion strength while temperature acted an positive role in sorption capacity, suggesting temperature was favorable to Th(Ⅳ) sorption on Muscovite and sorption reaction was an spontaneous endothermic process.
Based on the sorption effect that Th(Ⅳ) sorption on Muscovite was not affected by ion strength while extremely sensitive to pH, it was found the sorption mechanism was inner-complex under low pH whereas an combination of inner-complex with surface precipitation worked at high pH.
Like sorption of Th(Ⅳ) on Muscovite, sorption of Th(Ⅳ) on Albite beared similar phenomena with Muscovite, Sorption was significantly influenced and enhanced by such factors as higher adsorbent concentration, lower adsorbate concentration, high pH and HA/FA.
Furthermore, Sorption of Th(Ⅳ) on Albite was related to foreign anions, it was found PO43+contributed to positive sorption effect of Th(Ⅳ) percentage in contrast with negative sorption effect of SO42-.
Finally, instead of failure in obvious effect of Th(Ⅳ) sorption on Muscovite, there was an increase in sorption percentage of Th(Ⅳ) on Albite with increasing ion strength, from～0to1.2M NaClO4range Th(Ⅳ) sorption percentage rised rapidly by a margin about30%. This showed inner-complex was the main sorption mechanism at low pH values along with intense pH reliance.
引文
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