首页> 外文期刊>Chemistry of Materials: A Publication of the American Chemistry Society >Topotactic Transformations of Metal-Organic Frameworks to Highly Porous and Stable Inorganic Sorbents for Efficient Radionuclide Sequestration
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Topotactic Transformations of Metal-Organic Frameworks to Highly Porous and Stable Inorganic Sorbents for Efficient Radionuclide Sequestration

机译:从金属有机骨架到高多孔性和稳定的无机吸收剂的高效放射性核素螯合的定势转变

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摘要

Innovative solid-phase sorbent technologies are needed to extract radionuclides from harsh media for environmental remediation and in order to close the nuclear fuel cycle. Highly porous inorganic materials with remarkable sorptive properties have been prepared by topotactic transformations of metal-organic frameworks (MOFs) using both basic and acidic solutions. Treatment of Ti and Zr nanoMOFs with NaOH, Na3PO4, and H3PO4 yields Ti and Zr oxides, oxyphosphates, and phosphates via sacrificial removal of the organic hgands. This controlled ligand extraction process results in porous inorganic materials, which preserve the original MOF morphologies and impart useful surface functionalities, but are devoid of organic linkers. Structural investigation by X-ray absorption spectroscopy reveals preservation of the coordination environment of the scattering metal. Changing the MOF template introduces different metal and structural possibilities, while application of different digest solutions allows preparation of metal oxides, metal oxyphosphates, and metal phosphates. The high stability and porosity of these novel materials makes them ideally suited as nanosorbents in severe environments. Their potential for several radionuclide separations is demonstrated, including decontamination of high level nuclear waste, extraction of lanthanides, and remediation of radionuclide-contaminated seawater.
机译:需要创新的固相吸附剂技术从恶劣的介质中提取放射性核素,以进行环境修复,并关闭核燃料循环。通过使用碱性溶液和酸性溶液对金属有机骨架(MOF)进行定势转变,已经制备了具有显着吸附性能的高度多孔无机材料。用NaOH,Na3PO4和H3PO4处理Ti和Zr纳米MOF可以通过牺牲性去除有机配体产生Ti和Zr氧化物,氧磷酸盐和磷酸盐。这种受控的配体萃取过程产生了多孔无机材料,该材料保留了原始的MOF形态并赋予了有用的表面功能,但缺少有机连接基。通过X射线吸收光谱进行的结构研究表明,保留了散射金属的配位环境。更改MOF模板会引入不同的金属和结构可能性,而应用不同的消化液则可以制备金属氧化物,金属氧磷酸盐和金属磷酸盐。这些新型材料的高稳定性和孔隙率使其非常适合在恶劣环境中用作纳米吸附剂。证明了它们在几种放射性核素分离中的潜力,包括对高水平核废料的净化,镧系元素的提取以及对放射性核素污染的海水的修复。

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