Preparation and characterization of a novel macroporous silica-bipyridine asymmetric multidentate functional adsorbent and its application for heavy metal palladium removal.
Preparation and characterization of a novel macroporous silica-bipyridine asymmetric multidentate functional adsorbent and its application for heavy metal palladium removal.
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DOI：
10.1016/j.jhazmat.2017.04.038
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发表时间：
2017-09
影响因子：
13.6
通讯作者：
Lei Xu;A. Zhang;Fengmei Zhang;Jiyong Liu
中科院分区：
文献类型：
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作者：
Lei Xu;A. Zhang;Fengmei Zhang;Jiyong Liu
从高活性废液中有效去除重金属107Pd(II)对于减少其对公众健康和环境的危害和风险是非常有价值的。为此，通过在大孔SiO_2-P载体上真空注入一种新的不对称N-供体配体CA-MTBP(联吡啶衍生物)，合成了一种新型的SiO_2-联吡啶多齿功能吸附剂。采用扫描电子显微镜、氮气吸附-脱附等温线、热重分析、X射线衍射、红外光谱、29Si固体核磁共振和XPS光谱等手段系统地表征了该吸附剂的物理化学性质。表征结果表明，CA-MTBP通过分子间相互作用成功地固定在SiO_2-P的孔道上。通过配体的单晶结构和~(29)Si核磁共振确定的强氢键相互作用可能在实现这种固定化中起到关键作用。TGA和TOC研究表明，CA-MTBP/SiO_2-P具有良好的热稳定性和较高的抗HNO_3性能。EDS和XPS研究为Pd(II)选择性吸附在吸附剂上提供了直接证据。在硝酸介质中，该吸附剂对Pd(II)具有较好的吸附能力、较快的吸附动力学和较高的选择性。
The effective removal of heavy metal107Pd(II) from highly active liquid waste (HLW) is very valuable for reducing its hazardous and risk to public health and environment. For this purpose, a novel silica-bipyridine multidentate functional adsorbent was synthesized by vacuum infusing a new asymmetric N-donor ligand CA-MTBP (bipyridine derivative) into the macroporous SiO2-P support. SEM, N2adsorption–desorption isotherms, TGA, XRD, FT-IR,29Si solid-state NMR and XPS spectroscopy were utilized to systematically characterize the physicochemical properties of the adsorbent. The characterization results indicated that CA-MTBP was successfully immobilized onto the pores of SiO2-P by intermolecular interaction. Strong hydrogen-bonding interactions identified by single crystal structure of the ligand and29Si NMR may play a key role in achieving this immobilization. TGA and TOC studies showed that CA-MTBP/SiO2-P had excellent thermal stability and highly HNO3resistance. EDS and XPS investigations provided directly evidences for Pd(II) being selectively adsorbed onto the adsorbent. The adsorbent had excellent adsorption capability, fast adsorption kinetics and high selectivity for Pd(II) over other typical tested metals in HNO3media.