The removal of aqueous uranium by SBA-15 modified with phosphoramide: a combined experimental and DFT study
The removal of aqueous uranium by SBA-15 modified with phosphoramide: a combined experimental and DFT study
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磷酰胺修饰的 SBA-15 去除含水铀：实验和 DFT 相结合的研究
DOI：
10.1039/c6ra12269h
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发表时间：
2016-07
期刊：
影响因子：
3.9
通讯作者：
Chuipeng Kong
中科院分区：
文献类型：
--
作者：
Yiming Ren;Ruizhu Yang;Lang Shao;Hao Tang;Shaofei Wang;Jianlong Zhao;Jingrong Zhong;Chuipeng Kong
磷酰胺改性有序介孔二氧化硅 (SBA-DEPA) 材料通过两步过程制备，包括：(1) 通过磷酰氯与伯胺的酰胺化合成磷酰胺，以及 (2) 将磷酰胺修饰到 SBA-15 上。 FT-IR和NMR光谱证实了制备的成功。 ICP-AES和XRF分析结果表明，磷酰胺基团的接枝率高达12.5%。形貌信息和N2吸附-脱附技术分别证明了该材料的高度有序结构和大比表面积。铀吸附性能优异，最大负载量为 311.6 mg g−1，相对于未改性的 SBA-15 有显着提升。强烈的 pH 值和 CO2 依赖性表明接近中性的条件有利于最大的铀吸附。令我们惊讶的是，吸附只需要 5 分钟即可达到 90% 的容量，20 分钟即可达到平衡，与许多其他吸附剂材料相比，这是非凡的。离子强度部分影响吸附，这表明外球和内球吸附都在此过程中发挥作用。超过原始吸附容量的 90% 表明 SBA-DEPA 具有出色的重现性。基于簇模型的 DFT 计算表明铀酰表面结合位点具有“三齿状”结构，这可以解释该材料优异的吸附能力。
Phosphoramide-modified ordered mesoporous silica (SBA-DEPA) materials were prepared via a two-step process involving: (1) the synthesis of phosphoramide via amidation of phosphoryl chloride with a primary amine and (2) modification of the phosphoramide onto SBA-15. The successful preparation was confirmed by FT-IR and NMR spectroscopy. As indicated by the ICP-AES and XRF analysis results, the phosphoramide group has a grafting ratio as high as 12.5%. The morphological information and N2 adsorption–desorption technique proved the highly ordered structure and large specific area of the material, respectively. An excellent performance for uranium sorption was found with a loading maximum of 311.6 mg g−1, a marked promotion relative to unmodified SBA-15. A strong pH and CO2 dependence suggested that near neutral conditions favored the maximum uranium sorption. To our surprise, the sorption took only 5 min to reach a 90% capacity and 20 min for equilibrium, which is extraordinary when compared to many other sorbent materials. The ionic strength partially influences the sorption, which indicates outer and inner sphere sorption both play parts in the process. A sorption capacity of over 90% of the original indicates the excellent reproducibility of SBA-DEPA. DFT calculations based on cluster models suggested a ‘tri-dentate-like’ structure for the uranyl-surface binding site, which may explain the excellent sorption ability of this material.
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DOI：
10.1002/chin.199203329
发表时间：
1991-07
期刊：
ChemInform
影响因子：
--
作者：
T. Ziegler
通讯作者：
T. Ziegler
影响因子：
9.9
作者：
Liming Zhou;C. Shang;Zhi-rong Liu;Guolin Huang;A. Adesina
通讯作者：
Liming Zhou;C. Shang;Zhi-rong Liu;Guolin Huang;A. Adesina
影响因子：
3.9
作者：
Hongsen Zhang;Qi Liu;Jun Wang;Jingyuan Liu;Huijun Yan;X. Jing;Bin Zhang
通讯作者：
Hongsen Zhang;Qi Liu;Jun Wang;Jingyuan Liu;Huijun Yan;X. Jing;Bin Zhang
影响因子：
4
作者：
Yulong Wang;L. Song;Lu Zhu;Bo-Long Guo;Suwen Chen;Wang-suo Wu
通讯作者：
Yulong Wang;L. Song;Lu Zhu;Bo-Long Guo;Suwen Chen;Wang-suo Wu
DOI：
10.1016/j.colsurfa.2015.04.016
发表时间：
2015-10-05
影响因子：
5.2
作者：
Dudarko, Oksana A.;Gunathilake, Chamila;Jaroniec, Mietek
通讯作者：
Jaroniec, Mietek