Highly Selective and Rapid Uptake of Radionuclide Cesium Based on Robust Zeolitic Chalcogenide via Stepwise Ion-Exchange Strategy

Abstract

The safe use of nuclear energy requires the development of advanced adsorbent technology to address environment damage from nuclear waste or accidental release of radionuclides. Recently developed amine-directed chalcogenide frameworks have intrinsic advantages as ion-exchange materials to capture radionuclides, because their exceptionally negative framework charge can lead to high cation-uptake capacity and their 3-D multidimensional intersecting channel promotes rapid ion diffusion and offer a unique kinetic advantage. Prior to this work, however, such advantages could not be realized because organic cations in the as-synthesized materials are sluggish during ion exchange. Here we report an ingenious approach on the activation of amine-directed zeolitic chalcogenides through a stepwise ion-exchange strategy and their use in cesium adsorption. The activated porous chalcogenide exhibits highly enhanced cesium uptake compared to the pristine form and is comparable to the best metal chalcogenide sorbents so far. Further ion-exchange experiments in the presence of competing ions confirm the high selectivity for cesium ions. Excellent removal performance has also been observed in real water samples, highlighting the importance of stepwise ion exchange strategy to activate amine-directed chalcogenide framework for 137Cs+ removal.

Direct observation of charge transfer between molecular heterojunctions based on inorganic semiconductor clusters

“…Crystalline inorganic metal chalcogenides with supertetrahedral clusters (denoted as Tn, where n is the number of metal sites along the tetrahedron edge) serving as SBUs have been extensively investigated because of their fascinating architectures and the effective integration of porosity with semiconducting properties. [27][28][29][30][31][32] Recently, discrete clusters with uniform size and atomically precise crystal lattice structure have been successfully dispersed into cluster-based quantum-dotlike nanoparticles (also called supraclusters) in solvents, and correlations between the cluster structure and function (such as electrochemical, photocatalytic and photoelectric applications) have been established. [33][34][35][36][37] Although the roles of clusters in crystalline open frameworks remain unclear, the signicance of clusters in these frameworks seems to extend beyond the beauty of a symmetrical structure and apparent functionality as nodes for open framework construction.…”

Structural Expansion of Chalcogenido Tetrelates in Ionic Liquids by Incorporation of Sulfido Antimonate Units

“…Metal chalcogenide compounds possess av ariety of desirable properties, mostly based on their intrinsic semiconducting, photo-conducting or ion conducting properties. [1][2][3][4][5][6][7][8][9] However, beside the native features of corresponding binary M x E y compounds( M= d-block or p-block (semi)metal, E = O, S, Se, or Te ), the combinationo fd ifferent Mo rd ifferentEatoms, and the formation of chalcogenido( semi)metalates by (formal) incorporation of Cat 2 E( Cat = alkali metal or non-metal cation) can be used to additionally tune the corresponding structurala nd electronic properties. [10][11][12][13][14][15] In order to achieve at argeted synthesis of such compounds, variouss ynthetic methods have been applied.…”

Macrocyclic Pyridone Pentamers for Highly Selective High‐Capacity Removal of Caesium Ions from Radioactive High‐Salinity Waste

“…There has been widespread improvement of different extractive materials, mainly focusing on separation and isolation of Cs + from aquatic ecosystems. For instance, inorganic (crystalline silicotitanates, [7] metal thiophosphate, [8] sulfide clusters, [9] zeolitic [23–29] chalcogenides, [23] Prussian blue, [30] etc) and organic (phenolic resins, [31] polysaccharides, [32] resorcinol‐formaldehyde, [33] etc) ion exchangers are the major treatment methods for removal of Cs + from liquid waste. Additionally, organic extractants based on functionalised calixarenes, [3–5,22] cucurbit[n]urils, [12] uranyl organic framework, [14] isoguanosine tetramer [24] or pentamer, [25] and carbon nanotubes have been recently reported as suitable host molecules for selective binding with Cs + .…”