Zhao Shilei, Feng Tiantian, Zhang Jiacheng, Cao Meng, Feng Lijuan, Ma Yue, Liu Tao, Yuan Yihui, Wang Ning
State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228, P. R. China.
Adv Sci (Weinh). 2024 Dec;11(48):e2408642. doi: 10.1002/advs.202408642. Epub 2024 Nov 4.
Highly efficient separation of dispersed uranium is important for the sustainable development of nuclear industry, and adsorption is the most recognized approach. However, there are many coexisting interfering metal ions that compete with uranyl ion for the chelating ligands in the adsorbents and lead to low separation selectivity and efficiency. Herein, a coordination-induced magnetism strategy is presented for the separation of uranium based on the conversion of diamagnetic cyanoferrocene (Fc-CN) nanocrystals to uranium-containing magnetic recoverable ferromagnetic aggregates. Different from previous adsorption strategies, this strategy combines the mechanisms of photocatalytic uranium enrichment and chemical uranium adsorption. Under light irradiation, electron of Fe(II) in Fc-CN is excited and transfers to uranyl ion via the cyano group to form tight coordination bond between N atom in cyano group and uranium. This phenomenon is unique for uranyl ion, and thus, a high uranium removal rate of 97.98% is achieved in simulated nuclear wastewater with the presence of tremendous interfering ions, proving its highly selective and efficient uranium separation performance. The ability to form highly stable magnetic aggregates via photoinduced interaction between Fc-CN and uranium enriches the understanding on the chemical properties of Fc-CN and uranium.
高效分离分散的铀对核工业的可持续发展至关重要,吸附是最受认可的方法。然而,存在许多共存的干扰金属离子,它们与铀酰离子竞争吸附剂中的螯合配体,导致分离选择性和效率较低。在此,提出了一种配位诱导磁性策略,用于基于抗磁性氰基二茂铁(Fc-CN)纳米晶体转化为含铀磁性可回收铁磁聚集体来分离铀。与以往的吸附策略不同,该策略结合了光催化铀富集和化学铀吸附的机制。在光照下,Fc-CN中Fe(II)的电子被激发,并通过氰基转移到铀酰离子上,在氰基中的N原子与铀之间形成紧密的配位键。这种现象对铀酰离子来说是独特的,因此,在存在大量干扰离子的模拟核废水中实现了97.98%的高铀去除率,证明了其对铀的高度选择性和高效分离性能。通过Fc-CN与铀之间的光诱导相互作用形成高度稳定的磁性聚集体的能力,丰富了对Fc-CN和铀化学性质的理解。