Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 34141, Republic of Korea.
J Hazard Mater. 2023 Jun 5;451:131136. doi: 10.1016/j.jhazmat.2023.131136. Epub 2023 Mar 5.
Al-rich zeolites such as NaA (Si/Al = 1.00) have been widely applied to remove radioactive Sr because of their high surface charge density enabling efficient ion-exchange of multivalent cations. However, due to the small micropore diameters of zeolites and large molecular size of strongly hydrated Sr, Sr-exchange with zeolites suffers from very slow kinetics. In principle, mesoporous aluminosilicates with low Si/Al ratios close to unity and tetrahedrally coordinated Al sites can exhibit both high capacity and fast kinetics in Sr-exchange. Nonetheless, the synthesis of such materials has not been realized yet. In this study, we demonstrate the first successful synthesis of an Al-rich mesoporous silicate (ARMS) using a cationic organosilane surfactant as an efficient mesoporogen. The material exhibited a wormhole-like mesoporous structure with a high surface area (851 m g) and pore volume (0.77 cm g), and an Al-rich framework (Si/Al = 1.08) with most Al sites tetrahedrally coordinated. Compared to commercially applied NaA, ARMS exhibited a dramatically improved Sr-exchange kinetics (>33-fold larger rate constant) in batch adsorption while showing similarly high Sr capture capacity and selectivity. Due to the fast Sr-exchange kinetics, the material also exhibited 3.3-fold larger breakthrough volume than NaA in fixed-bed continuous adsorption.
富铝沸石,如 NaA(Si/Al=1.00),由于其高表面电荷密度,能够有效进行多价阳离子的离子交换,因此被广泛应用于去除放射性 Sr。然而,由于沸石的微孔直径较小,以及强水合 Sr 的分子尺寸较大,Sr 与沸石的交换动力学非常缓慢。原则上,硅铝比接近 1.0 的低 Si/Al 比值的中孔铝硅酸盐和四面配位的 Al 位可以在 Sr 交换中表现出高容量和快速动力学。尽管如此,这些材料的合成尚未实现。在本研究中,我们首次成功地使用阳离子有机硅烷表面活性剂作为有效的介孔生成剂合成了富铝中孔硅酸盐(ARMS)。该材料具有蠕虫状介孔结构,比表面积(851 m g)和孔体积(0.77 cm g)高,富铝骨架(Si/Al=1.08)中大多数 Al 位为四面配位。与商业应用的 NaA 相比,ARMS 在批量吸附中表现出显著改善的 Sr 交换动力学(速率常数大 33 倍),同时表现出相似的 Sr 捕获容量和选择性。由于 Sr 交换动力学较快,该材料在固定床连续吸附中的穿透体积也比 NaA 大 3.3 倍。