纳米结晶低硅 X 沸石作为高效离子交换剂实现快速放射性锶捕获

IF 4.3 3区 工程技术 Q2 ENGINEERING, CHEMICAL Frontiers of Chemical Science and Engineering Pub Date : 2024-07-10 DOI:10.1007/s11705-024-2449-6
Hyungmin Jeon, Susung Lee, Jeong-Chul Kim, Minkee Choi
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摘要

NaA 沸石(Si/Al = 1.00)具有较高的表面电荷密度,可有效稳定多价阳离子,因此已被商业应用于捕获放射性 90Sr2+。然而,由于其微孔开口窄(4.0 Å)、微米级结晶大、水合 Sr2+ 体积大,因此 Sr2+ 与 NaA 的交换一直受到非常缓慢的动力学限制。在本研究中,我们通过尽量减少合成凝胶中的含水量,并利用甲基纤维素水凝胶作为晶体生长抑制剂,合成了纳米结晶低硅 X。所得到的沸石具有高结晶度和富铝框架(Si/Al 约为 1.00),且只存在四面体 Al 位点,这些位点具有较高的 Sr2+ 吸收能力和离子选择性。同时,与 NaA 相比,具有 FAU 拓扑结构的沸石具有更大的微孔开口尺寸(7.4 Å)和更小的晶粒尺寸(∼340 nm),从而显著增强了离子交换动力学。与传统 NaA 相比,纳米晶低硅 X 在批量实验中表现出明显提高的 Sr2+ 交换动力学(速率常数提高了 18 倍)。虽然在平衡条件下,纳米低硅石 X 和 NaA 的 Sr2+ 容量相当,但在动态条件下,前者的突破体积比 NaA 大 5.5 倍,这归因于其明显更快的 Sr2+ 交换动力学。
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Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture

NaA zeolite (Si/Al = 1.00) has been commercially applied for capturing radioactive 90Sr2+ because of its high surface charge density, effectively stabilizing the multivalent cation. However, owing to its narrow micropore opening (4.0 Å), large micron-sized crystallites, and bulkiness of hydrated Sr2+, the Sr2+ exchange over NaA has been limited by very slow kinetics. In this study, we synthesized nanocrystalline low-silica X by minimizing a water content in a synthesis gel and utilizing a methyl cellulose hydrogel as a crystal growth inhibitor. The resulting zeolite exhibited high crystallinity and Al-rich framework (Si/Al of approximately 1.00) with the sole presence of tetrahedral Al sites, which are capable of high Sr2+ uptake and ion selectivity. Meanwhile, the zeolite with a FAU topology has a much larger micropore opening size (7.4 Å) and a much smaller crystallite size (∼340 nm) than NaA, which enable significantly enhanced ionexchange kinetics. Compared to conventional NaA, the nanocrystalline low-silica X exhibited remarkably increased Sr2+-exchange kinetics (> 18-fold larger rate constant) in batch experiments. Although both the nanocrystalline low-silica X and NaA exhibited comparable Sr2+ capacities under equilibrated conditions, the former demonstrated a 5.5-fold larger breakthrough volume than NaA under dynamic conditions, attributed to its significantly faster Sr2+-exchange kinetics.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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