Halogen microregulation in metal-organic frameworks for enhanced adsorption performance of ReO4-/TcO4.

Effective and selective removal of 99TcO4-, one of the most nuisance radionuclides in nuclear waste, is highly desirable but remains a significant challenge. Herein, two isostructural MOFs, NCU-3-X (X = Cl, Br) were constructed by ZnX2 coordinated to nitrogen-containing neutral ligand tri(4-(1H-imidazole-1-l) phenyl) amine for efficient adsorption ReO4-/TcO4-. Owning to the twofold interpenetrating structure, both of them exhibit strong alkaline resistance. Consequently, NCU-3-Br exhibited superior adsorption performances with a maximum capacity as high as 483 mg/g, which is 2.23 times larger than that of NCU-3-Cl. The primary reasons accounting for the enhanced adsorption performances of NCU-3-Br are that compared to chlorine atoms, the smaller electronegativity of bromine atoms as halogen bonds donor can facilitate the formation of σ-holes, enhance positively charged skeleton, and reduce the adsorption energy associated with ReO4-/TcO4-. In addition, the one-dimensional hydrophobic channels in the NCU-3-Br framework enable NCU-3-Br to have highly selective toward ReO4-, which has a low relative charge density against interfering ions. The SRS simulation removal experiment further confirmed the excellent adsorption capacity of NCU-3-Br to ReO4-/TcO4-. This work illustrated that the halogenated new strategy incorporated different halogen atoms into MOF skeletons can dramatically modulate the adsorption performances for ReO4-/TcO4-.

[1]  Fenglei Liu,et al.  Immobilizing nZVI particles on MBenes to enhance the removal of U(VI) and Cr(VI) by adsorption-reduction synergistic effect , 2022, Chemical Engineering Journal.

[2]  Q. Hu,et al.  Synthesis of cationic polymer decorated with halogen for highly efficient trapping 99TcO4-/ReO4. , 2022, Journal of hazardous materials.

[3]  L. Lei,et al.  Fast Room‐Temperature Synthesis of an Extremely Alkaline‐Resistant Cationic Metal–Organic Framework for Sequestering TcO4− with Exceptional Selectivity , 2022, Advanced Functional Materials.

[4]  Jiuqiang Li,et al.  Superhydrophobic Phosphonium Modified Robust 3D Covalent Organic Framework for Preferential Trapping of Charge Dispersed Oxoanionic Pollutants , 2022, Advanced Functional Materials.

[5]  Jianding Qiu,et al.  An alkali-resistant metal–organic framework as halogen bond donor for efficient and selective removing of ReO4−/TcO4− , 2022, Environmental Science and Pollution Research.

[6]  Xiangke Wang,et al.  Biochar for the removal of contaminants from soil and water: a review , 2022, Biochar.

[7]  Fenglei Liu,et al.  Insight into the performance and mechanism of persimmon tannin functionalized waste paper for U(VI) and Cr(VI) removal. , 2021, Chemosphere.

[8]  P. Sun,et al.  Halogen-halogen bonds enable improved long-term operational stability of mixed-halide perovskite photovoltaics , 2021, Chem.

[9]  Z. Chai,et al.  Task-Specific Tailored Cationic Polymeric Network with High Base-Resistance for Unprecedented 99TcO4– Cleanup from Alkaline Nuclear Waste , 2021, ACS central science.

[10]  Mengnan Huang,et al.  Immersion grinding and in-situ polymerization synthesis of poly(ionic liquid)s incorporation into MOF composites as radioactive TcO4- scavenger. , 2021, Journal of hazardous materials.

[11]  Xiangke Wang,et al.  Review of organic and inorganic pollutants removal by biochar and biochar-based composites , 2021, Biochar.

[12]  G. Hall,et al.  Ultrastable Zirconium-Based Cationic Metal-Organic Frameworks for Perrhenate Removal from Wastewater. , 2021, Inorganic chemistry.

[13]  Jianding Qiu,et al.  Synthesis of Imidazolium-Based Cationic Organic Polymer for Highly Efficient and Selective Removal of ReO4–/TcO4– , 2021 .

[14]  Jing Chen,et al.  Optimizing Strategy for Enhancing the Stability and 99TcO4– Sequestration of Poly(ionic liquids)@MOFs Composites , 2020, ACS central science.

[15]  R. Zhou,et al.  99TcO4− removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework , 2020, Nature Communications.

[16]  Long Zhao,et al.  Quaternary phosphonium modified cellulose microsphere adsorbent for 99Tc decontamination with ultra-high selectivity. , 2020, Journal of hazardous materials.

[17]  Hao Zhang,et al.  Effective decontamination of 99TcO4−/ReO4− from Hanford low-activity waste by functionalized graphene oxide–chitosan sponges , 2020, Environmental Chemistry Letters.

[18]  H. Mo,et al.  Evidence for Halogen Bonding in Amorphous Solid Dispersions , 2020 .

[19]  Hang Zhou,et al.  A Highly Efficient Coordination Polymer for Selective Trapping and Sensing Perrhenate/Pertechnetate. , 2020, ACS applied materials & interfaces.

[20]  B. Grambow,et al.  Adsorption mechanism of ReO4− on Ni–Zn layered hydroxide salt and its application to removal of ReO4− as a surrogate of TcO4− , 2019 .

[21]  Tian Wang,et al.  Synthesis of ZnO nanoparticle-anchored biochar composites for the selective removal of perrhenate, a surrogate for pertechnetate, from radioactive effluents. , 2019, Journal of hazardous materials.

[22]  S. Scheiner.  On the capability of metal–halogen groups to participate in halogen bonds , 2019, CrystEngComm.

[23]  J. Chen,et al.  Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption , 2019, Nature Communications.

[24]  Jing Chen,et al.  Anion-adaptive crystalline cationic material for 99TcO4− trapping , 2019, Nature Communications.

[25]  R. Zhou,et al.  Successful Decontamination of 99 TcO4 - in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets. , 2019, Angewandte Chemie.

[26]  Z. Chai,et al.  Effective Removal of Anionic Re(VII) by Surface-Modified Ti2CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration. , 2019, Environmental science & technology.

[27]  Qi Chen,et al.  Ultra-highly selective trapping of perrhenate/pertechnetate by a flexible cationic coordination framework. , 2019, Chemical communications.

[28]  Prabhat K. Singh,et al.  Ratiometric fluorescence turn-on sensing of perrhenate anion, a non-radioactive surrogate of hazardous pertechnetate, in aqueous solution , 2018, Sensors and Actuators B: Chemical.

[29]  V. Khrustalev,et al.  Finding a receptor design for selective recognition of perrhenate and pertechnetate: hydrogen vs. halogen bonding. , 2018, Chemical communications.

[30]  T. Hayat,et al.  Metal-organic framework-based materials: superior adsorbents for the capture of toxic and radioactive metal ions. , 2018, Chemical Society reviews.

[31]  Z. Chai,et al.  Efficient uptake of perrhenate/pertechnenate from aqueous solutions by the bifunctional anion-exchange resin , 2018 .

[32]  Itamar Willner,et al.  Stimuli‐Responsive Nucleic Acid‐Based Polyacrylamide Hydrogel‐Coated Metal–Organic Framework Nanoparticles for Controlled Drug Release , 2018 .

[33]  Riki J. Drout,et al.  Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs , 2018 .

[34]  O. Farha,et al.  Identifying the Recognition Site for Selective Trapping of 99TcO4- in a Hydrolytically Stable and Radiation Resistant Cationic Metal-Organic Framework. , 2017, Journal of the American Chemical Society.

[35]  M. Engelhard,et al.  Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation. , 2017, Environmental science & technology.

[36]  R. Zhou,et al.  Exceptional Perrhenate/Pertechnetate Uptake and Subsequent Immobilization by a Low-Dimensional Cationic Coordination Polymer: Overcoming the Hofmeister Bias Selectivity , 2017 .

[37]  P. Beer,et al.  Selective perrhenate recognition in pure water by halogen bonding and hydrogen bonding alpha-cyclodextrin based receptors. , 2017, Chemical communications.

[38]  T. Hayat,et al.  Interaction Mechanism of Re(VII) with Zirconium Dioxide Nanoparticles Archored onto Reduced Graphene Oxides , 2017 .

[39]  Z. Nie,et al.  Zirconium-Based Metal-Organic Framework for Removal of Perrhenate from Water. , 2016, Inorganic chemistry.

[40]  P. Beer,et al.  Halogen bonding anion recognition. , 2016, Chemical communications.

[41]  Pierangelo Metrangolo,et al.  The Halogen Bond , 2016, Chemical reviews.

[42]  P. Beer,et al.  Anion recognition in water by a rotaxane containing a secondary rim functionalised cyclodextrin stoppered axle. , 2015, Chemical communications.

[43]  P. Beer,et al.  Halogen bonding in water results in enhanced anion recognition in acyclic and rotaxane hosts. , 2014, Nature chemistry.

[44]  Paul G Tratnyek,et al.  Reductive sequestration of pertechnetate (⁹⁹TcO₄⁻) by nano zerovalent iron (nZVI) transformed by abiotic sulfide. , 2013, Environmental science & technology.

[45]  P. Thallapally,et al.  Switching Kr/Xe selectivity with temperature in a metal-organic framework. , 2012, Journal of the American Chemical Society.

[46]  Edward J. Mausolf,et al.  Tetraphenylpyridinium pertechnetate: a promising salt for the immobilization of technetium , 2012 .

[47]  M. Sonavane,et al.  Analysis of 99Tc in the radioactive liquid waste after extraction into suitable solvent , 2012, Journal of Radioanalytical and Nuclear Chemistry.

[48]  Steven C. Smith,et al.  Immobilization of 99-technetium (VII) by Fe(II)-goethite and limited reoxidation. , 2011, Environmental science & technology.

[49]  David L. Rogow,et al.  Reversible anion exchange and catalytic properties of two cationic metal-organic frameworks based on Cu(I) and Ag(I). , 2010, Journal of the American Chemical Society.

[50]  S. Oliver.  Cationic inorganic materials for anionic pollutant trapping and catalysis. , 2009, Chemical Society reviews.

[51]  C. Xiong,et al.  Adsorption of rhenium(VII) on 4-amino-1,2,4-triazole resin , 2008 .

[52]  Jianwei Xu,et al.  Trimeric supramolecular liquid crystals induced by halogen bonds , 2006 .

[53]  Yifeng Wang,et al.  Compositional and structural control on anion sorption capability of layered double hydroxides (LDHs). , 2006, Journal of colloid and interface science.

[54]  John G. Darab,et al.  Chemistry of Technetium and Rhenium Species during Low-Level Radioactive Waste Vitrification , 1996 .

[55]  Yanlong Wang,et al.  Efficient sequestration of radioactive 99TcO4- by a rare 3-fold interlocking cationic metal-organic framework: A combined batch experiments, pair distribution function, and crystallographic investigation , 2022 .