Xu Lei, Xu Chao, Bao Hongliang, Spanopoulos Ioannis, Ke Weijun, Dong Xue, Xiao Chengliang, Kanatzidis Mercouri G
College of Chemical and Biological Engineering, Zhejiang University, 38 Zheda Road, Hangzhou 310027, China.
Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China.
ACS Appl Mater Interfaces. 2021 Aug 11;13(31):37308-37315. doi: 10.1021/acsami.1c12004. Epub 2021 Jul 29.
Thorium as a potential nuclear fuel for the next-generation thorium-based molten salt reactors holds significant environmental and economic promise over the current uranium-based nuclear reactors. However, because thorium (Th) usually coexists with other rare earth elements, alkali or alkaline earth metals in minerals, or highly acidic radioactive waste, seeking acid-resistant sorbents with excellent selectivity, high capacity, and fast removal rate for Th is still a challenging task. In this work, we investigated a robust layered metal sulfide (KInSnS, KMS-5) for Th removal from strong acidic solutions. We report that KMS-5 could capture Th from a 0.1 M HNO solution with extremely high efficiency (∼99.9%), fast sorption kinetics (equilibrium time < 10 min), and large distribution coefficient (up to 1.5 × 10 mL/g). Furthermore, KMS-5 exhibited excellent sorption selectivity towards Th in the presence of large amounts of competitive metal ions like Eu, Na, and Ca. This extraordinary capture property for Th is attributed to the facile ion exchange of Th with K in the interlayers and subsequent formation of a stable coordination complex via Th-S bonds. These results indicate that KMS-5 is a promising functional sorbent for the effective capture of Th from highly acidic solutions.
钍作为下一代钍基熔盐反应堆的潜在核燃料,与当前的铀基核反应堆相比,具有重大的环境和经济前景。然而,由于钍(Th)通常与矿物中的其他稀土元素、碱金属或碱土金属共存,或者存在于高酸性放射性废物中,寻找对钍具有优异选择性、高容量和快速去除率的耐酸吸附剂仍然是一项具有挑战性的任务。在这项工作中,我们研究了一种用于从强酸性溶液中去除钍的坚固层状金属硫化物(KInSnS,KMS-5)。我们报告称,KMS-5能够以极高的效率(约99.9%)、快速的吸附动力学(平衡时间<10分钟)和较大的分配系数(高达1.5×10 mL/g)从0.1 M HNO溶液中捕获钍。此外,在存在大量竞争性金属离子如铕、钠和钙的情况下,KMS-5对钍表现出优异的吸附选择性。钍的这种非凡捕获特性归因于钍与层间钾的 facile离子交换以及随后通过Th-S键形成稳定的配位络合物。这些结果表明,KMS-5是一种从高酸性溶液中有效捕获钍的有前景 的功能性吸附剂。