Yantasee Wassana, Fryxell Glen E, Addleman R Shane, Wiacek Robert J, Koonsiripaiboon View, Pattamakomsan Kanda, Sukwarotwat Vichaya, Xu Jide, Raymond Kenneth N
Pacific Northwest National Laboratory (PNNL), Richland, WA 99352, United States.
J Hazard Mater. 2009 Sep 15;168(2-3):1233-8. doi: 10.1016/j.jhazmat.2009.03.004. Epub 2009 Mar 13.
The increased demand for the lanthanides in commercial products result in increased production of lanthanide containing ores, which increases public exposure to the lanthanides, both from various commercial products and from production wastes/effluents. This work investigates lanthanide (La, Ce, Pr, Nd, Eu, Gd and Lu) binding properties of self-assembled monolayers on mesoporous silica supports (SAMMS), that were functionalized with diphosphonic acid (DiPhos), acetamide phosphonic acid (AcPhos), propionamide phosphonic acid (Prop-Phos), and 1-hydroxy-2-pyridinone (1,2-HOPO), from natural waters (river, ground and sea waters), acid solutions (to mimic certain industrial process streams), and dialysate. The affinity, capacity, and kinetics of the lanthanide sorption, as well as regenerability of SAMMS materials were investigated. Going from the acid side over to the alkaline side, the AcPhos- and DiPhos-SAMMS maintain their outstanding affinity for lanthanides, which enable the use of the materials in the systems where the pH may fluctuate. In acid solutions, Prop-Phos- and 1,2-HOPO-SAMMS have differing affinity along the lanthanide series, suggesting their use in chromatographic lanthanide separation. Over 95% of 100 microg/L of Gd in dialysate was removed by the Prop-Phos-SAMMS after 1 min and 99% over 10 min. SAMMS can be regenerated with an acid wash (0.5M HCl) without losing the binding properties. Thus, they have a great potential to be used as in large-scale treatment of lanthanides, lanthanide separation prior to analytical instruments, and in sorbent dialyzers for treatment of acute lanthanide poisoning.
商业产品中对镧系元素需求的增加导致含镧系元素矿石产量上升,这使得公众接触镧系元素的机会增加,无论是通过各种商业产品还是生产废物/废水。本研究调查了介孔二氧化硅载体上自组装单分子层(SAMMS)对镧系元素(La、Ce、Pr、Nd、Eu、Gd和Lu)的结合特性,这些单分子层用二膦酸(DiPhos)、乙酰胺膦酸(AcPhos)、丙酰胺膦酸(Prop-Phos)和1-羟基-2-吡啶酮(1,2-HOPO)进行了功能化修饰,研究对象包括天然水(河水、地下水和海水)、酸性溶液(模拟某些工业生产流程)和透析液。研究了镧系元素吸附的亲和力、容量和动力学,以及SAMMS材料的可再生性。从酸性体系到碱性体系,AcPhos-和DiPhos-SAMMS对镧系元素保持着出色的亲和力,这使得这些材料能够用于pH值可能波动的体系。在酸性溶液中,Prop-Phos-和1,2-HOPO-SAMMS在镧系元素系列中具有不同的亲和力,表明它们可用于镧系元素的色谱分离。Prop-Phos-SAMMS在1分钟后可去除透析液中100μg/L的Gd的95%以上,并在10分钟内去除99%。SAMMS可用酸洗(0.5M HCl)再生,且不会丧失结合特性。因此,它们在大规模处理镧系元素、分析仪器之前的镧系元素分离以及用于治疗急性镧系元素中毒的吸附性透析器方面具有巨大的应用潜力。