Molecular and Crystal Structures of Uranyl Nitrate Coordination Polymers with Double-Headed 2-Pyrrolidone Derivatives

Abstract

Double-headed 2-pyrrolidone derivatives (DHNRPs) were designed and synthesized as bridging ligands for the efficient and selective separation of UO from a HNO solution by precipitation. The building blocks, UO(NO) and DHNRPs, were successfully connected to form an infinite 1D coordination polymer. The solubility of [UO(NO)(DHNRP)] is no longer correlated to the hydrophobicity of the ligand but is exclusively governed by the ligand symmetry and packing efficiency. The newly designed DHNRP family can be used to establish a new spent nuclear fuel reprocessing scheme.

Crystallization of colourless hexanitratoneptunate(iv) with anhydrous H+ countercations trapped in a hydrogen bonded polymer with diamide linkers

“…The diamide linker molecules (L1 and L2) were prepared through a method reported elsewhere. [19][20][21] The Np 4+ stock solution (50 mM, 50 mL) was layered with 3 M HNO 3 aq (30 mL) and 3 M HNO 3 solution of 0.50 M diamide (L1 or L2, 10 mL) in a f5 mm glass test tube. Slow diffusion of Np 4+ and L resulted in deposition of colourless crystals of (HL) 2 [Np(NO 3 ) 6 ] (L ¼ L1 (3), L2 (4)) in 88% and 91% yield, respectively.…”

“… 20,21. Nevertheless, L still plays another important role to construct the crystal structures of 3 and 4.…”

Coordination Chemistry of Actinide Nitrates with Cyclic Amide Derivatives for the Development of the Nuclear Fuel Materials Selective Precipitation (NUMAP) Reprocessing Method

“…In a similar manner to NRPs (Scheme ), DHNRPs are easily accessible. Scheme displays a general synthetic route to prepare DHNRP and the ligand structures we reported so far . Although these DHNRPs were white or opaque solid materials except for L27 (yellow oil), all of them are immediately dissolved upon contact with water.…”

“…General procedure to prepare DHNRPs (top) and ligand structures (bottom, L25 – L29 ) we reported so far …”

“…Molecular structures of [UO 2 (NO 3 ) 2 (DHNRP)] n one‐dimensional coordination polymers (DHNRP = L25 (a), L26 (b), L27 (c), L28 (d), L29 (e)) drawn at 50 % probability level , . Panels (a), (b), and (c) were reproduced from ref . (Copyright 2017, 2020) with permission from the American Chemical Society.…”