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鲜寒,黄家齐,刘金香,王国华,刘迎九,姜培烜.改性介孔托贝莫来石吸附水中U(VI)的性能及机理研究[J].南华大学学报(自然科学版),2024,(5):9~16.[XIAN Han,HUANG Jiaqi,LIU Jinxiang,WANG Guohua,LIU Yingjiu,JIANG Peixuan.Performance and Mechanism of Modified Mesoporous Tobermorite for U(VI) Adsorption in Water[J].Journal of University of South China(Science and Technology),2024,(5):9~16.]

改性介孔托贝莫来石吸附水中U(VI)的性能及机理研究

Performance and Mechanism of Modified Mesoporous Tobermorite for U(VI) Adsorption in Water

投稿时间：2024-03-21

DOI：

中文关键词: 托贝莫来石 U(VI) 改性

英文关键词:tobermorite U(VI) modification

基金项目:国家自然科学基金项目(51904155);湖南省自然科学基金项目(2020JJ5492);湖南省教育厅基金项目(21B0432)

作者	单位
鲜寒	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001
黄家齐	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001
刘金香	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001
王国华	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001
刘迎九	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001
姜培烜	南华大学污染控制与资源技术湖南省重点实验室,湖南衡阳 421001 南华大学土木工程学院,湖南衡阳 421001

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中文摘要:

以废弃粉煤灰和电石渣为原料,利用水热法制备了托贝莫来石(tobermorite,TOB),经热活化和酸化制得改性托贝莫来石(modify tobermorite,STOB)。实验结果表明,改性后,TOB的钙氧八面体晶体结构受到破坏,形成了更多的微孔和介孔,因此STOB的比表面积和孔容显著增加。在pH为5、温度为303 K、反应时间为60 min时,STOB对U(VI)的吸附率为91.72%,比TOB的吸附率提高了22.27%。干扰离子对STOB吸附U(VI)的影响最显著,这是由于STOB缺少与铀相关的特异性官能团,导致其他重金属离子与U(VI)争夺材料的吸附点位。此外,pH也对实验结果有一些影响,酸性越高,STOB吸附性能越差。STOB对U(VI)的吸附等温线与Dubinin-Radushkevich和Langmuir等温模型相吻合,且STOB对U(VI)的吸附行为符合准二阶动力学模型,表明吸附主要发生在表面,并且是以单层为主的化学反应。热力学参数揭示,U(VI)的吸附是一个吸热的自发过程,其吸附量和去除率随着吸附温度的增加而提高。在经过5次循环使用后,U(VI)的去除效率仍能保持在64.65%以上。

英文摘要:

Tobermorite (TOB) was prepared from waste fly ash and calcium carbide slag by hydrothermal method, and modified tobermorite (STOB) was produced by thermal activation and acidification, and the experimental results showed that, after the modification, the crystal structure of calcium-oxygen octahedron of TOB was damaged, and more microporous and mesoporous pores were formed, so the specific surface area and pore volume of STOB increased significantly. At pH 5, temperature 303 K, reaction time 60 min, the adsorption rate of U(VI) by STOB was 91.72%, which was 22.27% higher than that of TOB. The most significant effect of interfering ions on the adsorption of U(VI) by STOB was attributed to the lack of specific functional groups associated with uranium in STOB, which led to other heavy metal ions competing with U(VI) for the adsorption sites of the material. In addition, pH also has some effects on the experiments, and the higher the acidity, the worse the adsorption performance of STOB. The adsorption isotherms of STOB on U(VI) coincide with the Dubinin-Radushkevich and Langmuir isothermal models, and the adsorption behavior of STOB on U(VI) is consistent with the quasi-second-order kinetic model, indicating that the adsorption mainly occurs on the surface and is a monolayer dominated chemical reaction. The thermodynamic parameters revealed that the adsorption of U(VI) was a heat-absorbing spontaneous process, and its adsorption amount and removal rate increased with the increase of adsorption temperature. The removal efficiency of U(VI) was maintained above 64.65% after five cycles of use.

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