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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Efficient extraction of U(VI) from uranium enrichment process wastewater by amine-aminophosphonate-modified polyacrylonitrile fibers

Xiaoqin Nie,Yujing Zhang,Yating Jiang,Ning Pan,Chang Liu,Junling Wang,Chunyan Ma,Xue Xia,Mingxue Liu,Hongping Zhang,Xiaoan Li,Faqin Dong

The enrichment and recovery of U(VI) from low-level radioactive wastewater in the process of uranium enrichment is important for the sustainable development of nuclear energy and environmental protection. Herein, a novel amine-aminophosphonate bifunctionalized polyacrylonitrile fiber (AAP-PAN), was prepared for the extraction of U(VI) from simulated and real uranium-containing process wastewater. The AAP-PAN fiber demonstrated a maximum adsorption capacity of 313.6 mg g −1 at pH = 6.0 and 318 K in the batch experiments. During the dynamic column experiment, over 99.99% removal of U(VI) could be achieved by the fiber using multi-ion simulated solution and real wastewater with an excellent saturation adsorption capacity of 132.0 mg g −1 and 72.5 mg g −1 , respectively. It also exhibited an outstanding reusability for at least 5 cycles of adsorption process. The mechanism for U(VI) removal was studied by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy analysis in the assist of simulation calculation. It suggested that the amine and aminophosphonate groups can easily bind uranyl ions due to U(VI) is more likely to combine with oxygen atoms of C O and P O, respectively.

研究领域: 环境科学 · 核能工程 · 材料科学
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Polymer Chemistry · 2015 ·Vol. 6 ·期 12 ·2283-2289 · IF 5.52

A novel methacrylate with a bisphosphonate group: RAFT polymerization and flame retardant property of the resultant polymers

Tianchi Xu,Lifen Zhang,Zhenping Cheng,Xiulin Zhu

A number of phosphorus-based monomers have been evaluated by free radical polymerization or photopolymerization, but fewer examples have been involved in the “living”/controlled radical polymerization (LRP) of such type of monomers, whereas LRP techniques allow the synthesis of well-defined polymers with designable structures, compositions and properties. In this work, a novel methacrylate based monomer with a bisphosphonate group 4-(bis(diethoxyphosphoryl)methyl)phenyl methacrylate (BPMA) was synthesized first and then polymerized by reversible addition-fragmentation chain transfer (RAFT) polymerization. The polymerization showed typical “living” features such as the polymerization, which indicates first order kinetics with respect to monomer concentration, and the molecular weights of the resultant polymers increase with monomer conversion. Furthermore, the resultant polymers demonstrated better thermal and flame-retardant properties. According to the thermal gravimetric analyzer (TGA) test, the amount of residual carbonaceous mass (char) increased with the molecular weight of the resultant polymers. Furthermore, the micro-scale combustion calorimetry (MCC) test also confirmed its superior flame-retardant performance.

CAS / MDL: 920-46-7
研究领域: 高分子化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Selective lead (II) sorption using aminophosphonate-based sorbents: Effect of amine linker, characterization and sorption performance

Rana R. Neiber,Ahmed A. Galhoum,Ibrahim El-Tantawy El Sayed,Eric Guibal,Jiayu Xin,Xingmei Lu

A one-pot synthesis procedure is designed for preparing two α-aminophosphonate-based-sorbents (DA and TA sorbents). The reaction takes place between amine precursors (two different aliphatic amines with different chain lengths and amino group content; i.e., ethylenediamine (DA) or diethylenetriamine (TA), respectively) and both salicylaldehyde and diphenyl phosphite. Ionic liquid may be used under controlled conditions as an alternative to TiCl 4 catalyst. These materials are first characterized by SEM-EDX, AFM, BET, XRD, FTIR, 1 H-, 13 C-, and 31 P NMR, XPS, TGA, elemental analysis (CHNP), and titration (PZC). Combined with the study of pH effect on Pb(II) sorption, FTIR and XPS analyses are used for exploring the mechanisms involved in metal binding. In a second step, the sorption properties are compared for Pb(II) recovery at pH ≈5. Maximum sorption is influenced by the length of the chain: DA (0.694 mmol Pb g −1 ) > TA (0.494 mmol Pb g −1 ). The sorption isotherms are modelled by the Sips equation for DA (and the Langmuir Dual Site equation) and by the Langmuir equation for TA. Thermodynamic parameters (ΔG°, ΔH° and ΔS°) indicate the spontaneous, endothermic nature and randomness increases during the sorption process. The uptake kinetics (equilibrium reached ≈120 min) is almost equally fitted by the pseudo-first-order rate equation and the pseudo-second-order rate equation. The sorbents show selective Pb(II) sorption against heavy base metals in multi-component solutions. QSAR tools (quantitative activity structure–activity relationships) are used for evaluating the correlation between their intrinsic metal characteristics and their affinities for sorbents. The sorbents are efficiently recycled for at least 5 cycles using 0.2 M HCl as the eluent (loss in sorption and desorption performances ≈10-14% at the fifth cycle, compared with the first cycle).

研究领域: 化学工程 · 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Precisely modulating the branching functional groups of MIL-53(Al) for highly efficient sequestration of uranium

Shuya Liu,Xinjie Ma,Yuxin Liu,Weiwei Chen,Yuejie Ai,Kexin Li,Xiushen Ye,Ming Fang,Xiaoli Tan

To fully utilize the customizable characteristics of metal-organic framework (MOF) materials in environmental applications, it is important to precisely modulate the branching groups of MOFs for improved performance. In this work, MIL-53(Al) was modulated by different numbers of nitrogen atoms and carboxyl groups/phosphite groups (MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 , and MOF-N 2 -(PO(OH) 2 ) 3 ) via a post-synthesis modification method, and the influence of functional groups and chain length on adsorption and the mechanism of modified groups on the adsorption of uranium (U) are demonstrated. Batch experiments suggest the removal of U(VI) reaches 37%, 27%, and 90% for MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 and MOF-N 2 -(PO(OH) 2 ) 3 , respectively (pH = 4.0, T = 25 ℃, I = 0.01 M NaNO 3 ). The surface complexation between UO 2 2+ and the surface of functional groups on the modulated MOF dominates the adsorption. Nevertheless, the steric hindrance in MOF porous structure can explain the inferiority of U(VI) adsorption on MOF-N 3 -(COOH) 4 (27%) to MOF-N 2 -(COOH) 3 (37%). MOF-N 2 -(PO(OH) 2 ) 3 is more conducive to uranyl adsorption than MOF-N 2 -(COOH) 3 or MOF-N 3 -(COOH) 4 , which is due to better affinity of U(VI) to phosphate group than the carboxyl group by density functional theory (DFT) calculation. Moreover, the excellent regeneration performance and U(VI) adsorption of MOF-N 2 -(PO(OH) 2 ) 3 in natural water or wastewater further confirmed the practical application of modulated MOFs in practical application.

CAS / MDL: 75-05-8 7784-27-2
研究领域: 环境科学 · 材料科学 · 化学
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SOLID STATE IONICS · 2018 · IF 2.751

Astonishing synergetic effect of proton conducting between phosphonic acid groups and triazolyl groups tethered simultaneously on poly(ether sulfone) backbone

Guangbo Zeng,Baohua Yue,Xuejiao Li,Liuming Yan

A novel phosphonic acid and triazolyl functionalized poly(ether sulfone) (PES-TriPA) containing simultaneously phosphonic acid and triazolyl side groups is synthesized. The PES-TriPA is prepared by polycondensation of phosphonated bisphenol (PBP) and 3,3′-diethynyl-4,4′-difluorodiphenylsulfone, followed by click reaction to introduce triazolyl groups and hydrolysis to free phosphonic acid groups. Phosphonic acid functionalized poly(ether sulfone) (PES-PA) and triazolyl functionalized poly(ether sulfone) (PES-Tri) are also synthesized for comparison with PES-TriPA. The proton conducting polymers are hot-pressed into proton exchange membranes , and the membrane morphologies, proton conductivities , oxidation and thermal stabilities, water uptakes and methanol permeabilities are characterized. PES-TriPA exhibits more excellent comprehensive properties in comparison with PES-PA and PES-Tri. At 100 °C and 90% relative humidity (RH), the proton conductivity of PES-TriPA reaches 113.0 mS cm −1 , in comparison with 55.7 mS cm −1 for PES-PA and 4.3 mS cm −1 for PES-Tri. PES-TriPA also shows better oxidation stability with 95.7% weight left after Fenton's test at 80 °C for 120 h, while only 68.7% left for PES-PA and 75.7% left for PES-Tri. In addition, PES-TriPA exhibits favorable thermal stability and water uptake compared with PES-PA and PES-Tri. Moreover, the methanol permeability of PES-TriPA is only 0.24 × 10 −8  cm 2  s −1 , which is lower than these of PES-PA and PES-Tri with 0.77 × 10 −8  cm 2  s −1 and 1.20 × 10 −8  cm 2  s −1 , respectively. These superior characteristics are attributed to the synergetic effect between the phosphonic acid groups and triazolyl groups caused by the intermolecular hydrogen bonding interaction throughout the PES-TriPA acid-base amphoteric polymer.

研究领域: 高分子科学 · 材料科学 · 电化学
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