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Eu(Ⅲ)在蒙脱石上的吸附及碳酸根和磷酸根对其吸附的影响 被引量:1
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作者 常明凯 胡娜 +5 位作者 李遥 鲜东帆 周万强 王静一 时燕琳 刘春立 《物理化学学报》 SCIE CAS CSCD 北大核心 2022年第3期74-82,共9页
锕系核素在处置库围岩和缓冲回填材料中的吸附和迁移参数是处置库安全评价的重要数据模块之一,而Eu(Ⅲ)由于其与三价锕系元素An(Ⅲ)相似的离子半径和化学性质常被用于模拟三价锕系元素的化学行为。本文通过批式吸附实验研究了固液比、... 锕系核素在处置库围岩和缓冲回填材料中的吸附和迁移参数是处置库安全评价的重要数据模块之一,而Eu(Ⅲ)由于其与三价锕系元素An(Ⅲ)相似的离子半径和化学性质常被用于模拟三价锕系元素的化学行为。本文通过批式吸附实验研究了固液比、接触时间、离子强度、p H、碳酸根及磷酸根等对Eu(Ⅲ)在蒙脱石上吸附的影响,重点关注了吸附机理和表面种态。研究结果表明,低p H时Eu(Ⅲ)在蒙脱石上的吸附方式为外层配位吸附,近中性时为内层配位吸附,高p H时则以表面沉淀的方式被吸附。离子强度的增大对Eu(Ⅲ)在低p H时的吸附产生抑制作用。低p H时碳酸根对Eu(Ⅲ)吸附的影响不明显,但在高p H时其会改变Eu(Ⅲ)的表面吸附种态。尽管磷酸根本身的吸附非常弱,但磷酸根会显著增强Eu(Ⅲ)的吸附。X射线光电子能谱结果和磷酸根吸附实验说明Eu(Ⅲ)在蒙脱石表面上形成了Eu PO4沉淀。本工作研究了蒙脱石/Eu(Ⅲ)二元体系和蒙脱石/Eu(Ⅲ)/阴离子三元体系的吸附行为,并用光谱技术探究了其吸附种态,为理解三价锕系核素在蒙脱石上的吸附行为提供了重要参考。 展开更多
关键词 矿物-水界面 吸附 荧光 表面配位 沉淀
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CHEMSPEC模拟铀在塔木素地下水中的种态分布 被引量:3
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作者 徐雪雯 周万强 +3 位作者 董亮 谭昭怡 王祥云 刘春立 《中国科学:化学》 CAS CSCD 北大核心 2019年第10期1308-1314,共7页
本文使用CHEMSPEC软件模拟了铀在塔木素地下水中的种态分布,并讨论了pH、Eh、离子浓度以及温度对铀种态分布的影响.结果表明,铀在强酸性条件下,主要以UO2^2+(aq)的形式存在;在弱酸性、中性以及弱碱性条件下,主要以UO2(OH)2(aq)的形式存... 本文使用CHEMSPEC软件模拟了铀在塔木素地下水中的种态分布,并讨论了pH、Eh、离子浓度以及温度对铀种态分布的影响.结果表明,铀在强酸性条件下,主要以UO2^2+(aq)的形式存在;在弱酸性、中性以及弱碱性条件下,主要以UO2(OH)2(aq)的形式存在;在强碱性条件下,主要以UO2(OH)3^?的形式存在,可能会生成CaUO4沉淀.Eh<33 mV时,U(OH)4(aq)为优势种态;而Eh>33 mV时,U(VI)更为稳定.不同阴离子的引入对铀的种态分布影响的大小顺序为HCO3^?>F^?>SO4^2?>Cl^?.UO2^2+浓度的增加促进了CaUO2(CO3)32?和Ca2UO2(CO3)3(aq)的生成.温度升高使塔木素地下水中UO2OH+的浓度显著提高. 展开更多
关键词 CHEMSPEC 塔木素 种态分布 影响因素
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锶在黑云母上的吸附及影响因素研究 被引量:1
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作者 胡娜 牛玉清 +5 位作者 常明凯 鲜东帆 周万强 周根茂 杨小雨 刘春立 《中国科学:化学》 CAS CSCD 北大核心 2020年第4期498-506,共9页
本文通过静态批式吸附实验研究了离子强度、pH、温度以及共存离子等对Sr2+在黑云母上吸附的影响.结果表明,当pH在3.0~5.0之间时, Sr2+在黑云母上的吸附可忽略;当pH在5.0~10.0之间时,随着pH的增加, Sr2+在黑云母上的吸附百分比迅速上升.... 本文通过静态批式吸附实验研究了离子强度、pH、温度以及共存离子等对Sr2+在黑云母上吸附的影响.结果表明,当pH在3.0~5.0之间时, Sr2+在黑云母上的吸附可忽略;当pH在5.0~10.0之间时,随着pH的增加, Sr2+在黑云母上的吸附百分比迅速上升.随着离子强度的增大, Sr2+在黑云母上的吸附百分比逐渐降低. Sr2+在黑云母上的吸附动力学和吸附等温线分别符合准二级动力学模型和Freundlich等温吸附模型. X射线光电子能谱分析结果表明, Sr2+主要是与黑云母表面的铁羟基发生了配合作用. 展开更多
关键词 黑云母 吸附 环境放射化学
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Uranium sorption on oxyhydroxide minerals by surface complexation and precipitation 被引量:4
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作者 Jingyi Wang wanqiang zhou +4 位作者 Yanlin Shi Yao Li Dongfan Xian Ning Guo Chunli Liu 《Chinese Chemical Letters》 SCIE CAS CSCD 2022年第7期3461-3467,共7页
During the chemical weathering of the uranium mill tailings,released uranium could be immobilized by the newly formed secondary minerals such as oxyhydroxides.A deeper understanding of the interaction between uranium ... During the chemical weathering of the uranium mill tailings,released uranium could be immobilized by the newly formed secondary minerals such as oxyhydroxides.A deeper understanding of the interaction between uranium and common oxyhydroxides under environmental conditions is necessary.In this work,uranium sorption behaviors on Al-,Mn-and Fe-oxyhydroxide minerals(boehmite,manganite,goethite,and lepidocrocite)were investigated by batch experiments.Results showed that the uranium sorption on Al-oxyhydroxide behaved significantly differently from the other three minerals.The sorption edge of the Mn-and Fe-oxyhydroxides located around pH 5,while the sorption edge of boehmite shifted about 1.5 pH unit to near neutral.The sorption isotherms of uranium on manganite,goethite and lepidocrocite at pH 5.0 could be well fitted by the Langmuir model.Instead of surface complexation,sorption on boehmite happened mainly by uranium-bearing carbonates and hydroxides precipitation as illustrated by the characterization results.Both carbonate and phosphate strongly affected the uranium sorption behavior.The removal efficiency of uranium by boehmite exceeded 98%after three sorption-desorption cycles,indicating it may be a potential material for uranium removal and recovery. 展开更多
关键词 Uranium mill tailings Oxyhydroxides Uranium sorption Surface complexation Surface precipitation
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Influence of inherent iron and oxygen concentrations on selenite sorption process using bentonite
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作者 Jiangang He Xueling Qiao +4 位作者 Yanlin Shi Yao Li Xiaoyu Yang wanqiang zhou Chunli Liu 《Science China Chemistry》 SCIE EI CAS CSCD 2017年第9期1258-1264,共7页
The oxygen concentration and inherent Fe in bentonite have a significant influence on the Se(IV) sorption process. In this study, the sorption of selenite on natural bentonite was investigated using a batch experiment... The oxygen concentration and inherent Fe in bentonite have a significant influence on the Se(IV) sorption process. In this study, the sorption of selenite on natural bentonite was investigated using a batch experiment method, and the distribution coefficient (Kd) values were obtained in the pH range from 2.0 to 10.0 under oxic/anoxic conditions. The Kdvalues always reached a maximum value at a pH of 4 under oxic conditions and at a pH of 8 under anoxic conditions; meanwhile, the Kdvalue under anoxic conditions was larger than the value under oxic conditions, especially in regard to the maximum Kdvalues. The oxygen conditions have a significant influence on the ratio of redox-sensitive Fe2+/Fe3+, which was closely related to the difference in the Kdvalues under both oxic/anoxic conditions. Ferric selenite and green rust could be responsible for the maximum Kdvalues under oxic/anoxic conditions. In the leaching experiments, we found that the Fe2+in bentonite could replace Mg2+and Al3+in the octahedral sheet. Spectroscopy methods, such as Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) were used to characterize the surface properties of the samples after reaction. Overall, this study shows that the addition of Fe2+-containing materials into backfill/buffer materials under anoxic condition could enhance the sorption of79Se(IV). © 2017, Science China Press and Springer-Verlag GmbH Germany. 展开更多
关键词 BENTONITE OXYGEN SORPTION Spectroscopic analysis X ray absorption spectroscopy X ray diffraction
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