Tang Qilong, Liu Shuang, Hao Huaixin, Dong Xue, Guo Yuxiao, Lu Yuexiang, Wang Zhipeng, Xu Chao
Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China.
Nuclear Research Institute for Future Technology and Policy, Seoul National University, Seoul 08826, Republic of Korea.
Chem Bio Eng. 2025 Apr 30;2(7):431-436. doi: 10.1021/cbe.5c00008. eCollection 2025 Jul 24.
Efficient decontamination and recovery of neptunium (Np) are some of the most challenging tasks in nuclear waste management due to the unique redox nature of Np. A feasible path to fulfill this task is converting inextractable Np-(V) to extractable Np-(IV) or Np-(VI), yet it has not been satisfactorily solved, owing to the inefficient valence conversion. Herein, we report the design and synthesis of a novel redoxable deep eutectic solvent (DES) to realize the in situ reduction of Np-(V) in a biphasic extraction system. With the synergistic effects of complexation by a diglycolamide ligand (hydrogen-bonding acceptor) and reduction by phenol (hydrogen-bonding donor), Np-(V) in the aqueous phase can be effectively reduced to Np-(IV) and extracted into the organic phase, affording a 1000-fold increase in distribution ratios. Meanwhile, the DES is well reusable in a wide range of acidic environments, showing potential in real applications.
由于镎（Np）独特的氧化还原性质，高效净化和回收镎是核废料管理中最具挑战性的任务之一。完成这项任务的一条可行途径是将不可萃取的Np-(V)转化为可萃取的Np-(IV)或Np-(VI)，然而由于价态转化效率低下，这一问题尚未得到令人满意的解决。在此，我们报告了一种新型可氧化还原的深共熔溶剂（DES）的设计与合成，以实现双相萃取体系中Np-(V)的原位还原。在二甘醇酰胺配体（氢键受体）的络合作用和苯酚（氢键供体）的还原作用的协同效应下，水相中的Np-(V)可有效还原为Np-(IV)并萃取到有机相中，分配比提高了1000倍。同时，该DES在广泛的酸性环境中具有良好的可重复使用性，显示出实际应用潜力。
