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用于螯合镧系阳离子的纳米多孔二氧化硅上的羟基吡啶酮功能化自组装单分子层

Hydroxypyridinone functionalized self-assembled monolayers on nanoporous silica for sequestering lanthanide cations.

作者信息

Yantasee Wassana, Fryxell Glen E, Lin Yuehe, Wu Hong, Raymond Kenneth N, Xu Jide

机构信息

Pacific Northwest National Laboratory, Richland, Washington 99352, USA.

出版信息

J Nanosci Nanotechnol. 2005 Apr;5(4):527-9. doi: 10.1166/jnn.2005.096.

Abstract

1,2-Hydroxypyridinone (1,2-HOPO) ligands were installed as self-assembled monolayers on nanoporous silica (MCM-41) to create a superior class of sorbent materials for lanthanide cations. Lanthanides were used as a model system for the radioactive, expensive, and highly hazardous actinides in preliminary screening studies. The ligand properties of the 1,2-HOPO ligand field and the extremely large surface area of MCM-41, coupled with the dense monolayer coating, contribute to the extremely high lanthanide binding capacity of the 1,2-HOPO nanoporous sorbent. At pH 4-5.9, the mass-weighted partition coefficients (Kd) for La, Nd, Eu, and Lu were 354,000, 344,000, 210,800, and 419,800, respectively. The rigid, open pore structure of the silica also allows for very rapid sorption. Being silica-based, the sorbent is compatible with vitrification processing into a final glasseous waste form, for subsequent disposition in a deep geological repository.

摘要

1,2-羟基吡啶酮(1,2-HOPO)配体以自组装单分子层的形式安装在纳米多孔二氧化硅(MCM-41)上,以制备一类用于镧系阳离子的优质吸附剂材料。在初步筛选研究中,镧系元素被用作放射性、昂贵且极具危害性的锕系元素的模型体系。1,2-HOPO配体场的配体性质以及MCM-41极大的表面积,再加上致密的单分子层涂层,使得1,2-HOPO纳米多孔吸附剂对镧系元素具有极高的结合能力。在pH值为4 - 5.9时,镧、钕、铕和镥的质量加权分配系数(Kd)分别为354,000、344,000、210,800和419,800。二氧化硅的刚性开孔结构也使得吸附速度非常快。这种基于二氧化硅的吸附剂与玻璃化处理兼容,可制成最终的玻璃质废料形式,以便随后处置于深部地质处置库中。

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