Materials Advances
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2022
·Vol. 3
·期 12
·4870-4877
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IF 0
Xupeng Zhi,Xiaomin Li,Fangfei Dong,Yiwei Huang,Suliang Yang,Taihong Yan,Yinglin Shen
Traditional anion exchangers for TcO4− usually have low selectivity and adsorption capacity due to the lack of functional groups that interact strongly with TcO4−. Here, we report a three-dimensional imidazolium network IMI-P that exhibits high adsorption capacity, fast kinetics, and outstanding selectivity for ReO4−/TcO4− at pH 2–13. It can remove 90% of ReO4− in 30 s and 99% ReO4− in 10 min, which is significantly faster than most commercial materials. Besides, the maximum sorption capacity of IMI-P (792 mg ReO4−/g) is also higher than that of most commercial materials. IMI-P shows good TcO4− removal efficiencies for simulated wastewater, which can reach 91.5% and 98.4% at the solid–liquid ratio of 10 g L−1 and 50 g L−1, respectively. Compared with other Tc-adsorption polymers, IMI-P with a larger particle size (10–30 μm) is more suitable for column chromatography separation. Therefore, IMI-P has important application potential in wastewater treatment in the nuclear industry. The adsorption mechanism of IMI-P and the interaction mode with ReO4− were also studied by IR, EDS, and XPS.
研究领域:
化学
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环境科学
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材料科学
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产品关联
DOI
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2021
·Vol. 330
·期 3
·1165-1176
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IF 1.371
Xu Yuwei,Tian Yin,Chen Bo,Yan Zijun,Ding Jie,Huang Yalin,Kang Jinyang,Chen Shanyong,Jin Yongdong,Xia Chuanqin
In this paper, porphyrin-based cationic conjugated network (PCCN) nanosheets were synthesized, and its adsorption for TcO 4 − /ReO 4 − was investigated. This material was stacked with AB dislocation, with an aperture of 1.2 nm. The Re(VII)/Tc(VII) adsorption kinetics of PCCN is extremely fast, and the adsorption capacity is relatively large, the selective order is ReO 4 − > NO 3 − > Cl − . XPS and DFT revealed that the exchange of Cl − on PCCN with ReO 4 − , while the hydrophobic pore of PCCN are the keys to improve adsorption selectivity. It could be used to remove Tc from groundwater around nuclear facilities. Graphic abstract
研究领域:
材料科学
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环境科学
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放射化学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yawen Cai,Jinghua Feng,Xiaoli Tan,Xin Wang,Zhimin Lv,Weiwei Chen,Ming Fang,Haining Liu,Xiangke Wang
The efficient decontamination of pertechnetate ( 99 TcO 4 − ) is an essential task for managing radioactive 99 Tc in nuclear wastes . Perrhenate, (ReO 4 − ), as a nonradioactive analog, exhibits almost identical physicochemical properties as 99 TcO 4 − . Herein, a novel magnetic amine-functionalized MIL-101(Cr) (NH 2 -MIL-101(Cr)@Fe 3 O 4 ) was prepared and used to efficiently remove ReO 4 − from solution for the facile magnetic separation. A series of environmental parameters were considered to investigate the adsorption performance of NH 2 -MIL-101(Cr)@Fe 3 O 4 . Experimental results suggested that NH 2 -MIL-101(Cr)@Fe 3 O 4 has reached a satisfied adsorption capacity (~401 mg/g) and a very fast adsorption kinetics at pH 7.0. The selectivity for ReO 4 − was maintained even in the presence of interfering anions with relatively high concentrations. ReO 4 − were mainly captured by N-donor sites of the surface-decorated amine via complexation and were trapped in the cavities of modified MIL-101(Cr). NH 2 -MIL-101(Cr)@Fe 3 O 4 exhibits satisfactory adsorption performance for ReO 4 − and can be conveniently separated from wastewaters after adsorption.
研究领域:
环境科学
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材料科学
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放射化学
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Yanqin Hu,Ben Qin,Xiaoyan Li,Fan Yang,Chuan-Pin Lee,Meiying Xie,Liyan Xue
With the development of nuclear energy, the reprocessing of 99TcO4–/ReO4– has become a very difficult problem due to environmental issues such as high output, long life, and easy leakage. In this study, three extraction systems containing carbamic acid were introduced into the reprocessing of 99TcO4–/ReO4– for the first time. The results involving one of the three results show that N-[N,N-di(2-ethylhexyl) aminocarbonylmethyl] glycine (D2EHAG) has ultrahigh selectivity for removal to 99TcO4–/ReO4–. When the extreme concentration ratio of SO42– and Cl– to ReO4– of D2EHAG is 10,000:1, the distribution coefficient of ReO4– still reaches 12.73 and 2.67, respectively. Additionally, the most hydrophilic NO3–, when the extreme concentration ratio of NO3– and ReO4– is 1000:1, still has a distribution coefficient close to 2.33, which is more than the most reported MOF adsorption materials. Moreover, the reaction kinetics, stripping rate, and reuse rate were studied. After five cycles, the removal rate is still 98.12%, with a decrease of less than 0.7%. The system containing carbamic acid is a potential extraction removal system to remove 99TcO4–/ReO4– from nuclear radioactive wastewater.
研究领域:
环境科学
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核化学
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放射性废物管理
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产品关联
DOI
PubMed
高影响因子
Toxics
·
2022
·Vol. 10
·期 10
·630
·
IF 4.472
Ben Qin,Yanqin Hu,Meiying Xie,Liyan Xue,Chunfa Liao,Fan Yang
The treatment of radioactive wastewater is one of the major problems in the current research. With the development of nuclear energy, the efficient removal of99TcO4−in radioactive wastewater has attracted the attention of countries all over the world. In this study, a novel functional polyamide polymer p-(Amide)-PAM was synthesized by the two-step method. The experimental results show that p-(Amide)-PAM has good adsorptive properties for99TcO4−/ReO4−and has good selectivity in the nitric acid system. The kinetics of the reaction of p-(Amide)-PAM with99TcO4−/ReO4−was studied. The results show that p-(Amide)-PAM has a fast adsorption rate for99TcO4−/ReO4−, the saturated adsorption capacity reaches 346.02 mg/g, and the material has good reusability. This new polyamide-functionalized polyacrylamide polymer material has good application prospects in the removal of99TcO4−from radioactive wastewater.Keywords:polyacrylamide;polyamidation;99TcO4−/ReO4−removal;polymer adsorption material
研究领域:
环境科学
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核化学与放射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RADIATION PHYSICS AND CHEMISTRY
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2023
·
IF 2.9
Nan Wang,Manman Zhang,Zhen Dong,Lifang Peng,Maolin Zhai,Long Zhao
In this study, two different alkylated nano-silicas were synthesized from in-situ growth and post-modification method respectively, and the 1-vinyl-3-ethylimidazolium bromide ([C 2 VIm]Br) was grafted onto them by radiation-induced grafting technique to fabricate nano-silica based adsorbents for ReO 4 − /TcO 4 − removal. The charged imidazolium moieties were controllably immobilized onto the nano-size substates by adjusting the radiation dose and monomer concentration, and the resulting adsorbents (S(P)–Si-MPTS-IL) were characterized by FTIR, SEM , EA and TGA. Subsequently, their adsorption properties for ReO 4 − were systematically studied in batch adsorption experiments. Combining the advantages of both nano-silica and ionic liquid, the prepared adsorbents exhibited ultrafast uptake (within 1min), high selectivity , and good cyclic stability (5 cycles, 95% retention) against ReO 4 − . Besides, they showed excellent radiation resistance and the adsorption properties were basically unchanged after 1200 kGy. Finally, FTIR and XPS analysis confirmed that the mechanism of adsorption process was ion exchange. This study laid a foundation for the synthesis and application of novel nano-silica adsorbent for ReO 4 − /TcO 4 − .
研究领域:
环境科学
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放射化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
·
IF 8.5
Xindi He,Kairuo Zhu,Ziying Jiang,Yang Yu,Sai Zhang,Xiaoling Dong,Ling-Ping Xiao,Shangru Zhai
Herein, an emerging vertically oriented alginate aerogel composites (QLHC@A aerogel) was constructed by combining the mild ionic crosslinking technique with directed freeze-casting to achieve adsorptive removal of ReO 4 − (the chemical analogue of TcO 4 − ). The lignin hydrochar in aerogel composites served as a bridge connecting quaternary ammonium groups to fabricate functional addition, among the PDDA-modified lignin hydrochar investigated, QLHC 100 exhibited the best adsorption performance, up to 212.95 mg/g, while the regular lamellar structure and good hydrophilic property of alginate-based aerogel allowed rapid diffusion of ReO 4 − anion in water. When the usage amount of QLHC 100 powder became 0.8 g, the optimal ReO 4 − removal efficiency of QLHC@A aerogel reached 188.90 mg/g at pH 4, 0.1 g/L and 303 K. Batch adsorption experiments also validate that the ReO 4 − adsorption process was mightily pH-dependent behavior, and adsorption behavior fitted both the pseudo-second-order kinetic model and the Langmuir isothermal model well. Meanwhile, QLHC@A aerogel had a high adsorption selectivity, excellent chemical tolerance, and good reuse performance. Based on various characterization techniques and DFT calculation result, the adsorption mechanism of ReO 4 − on QLHC@A aerogel is mainly dominated by electrostatic adsorption and strong affinity between quaternary ammonium groups and ReO 4 − . Significantly, this strategy can be expanded to include high-performance aerogel composites for the remediation of nuclear effluent contaminated with TcO 4 − .
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Long Li,Xuanhao Huang,Xiaoyang Hu,Xingyue Liu,Rui Li,Hang Zhou,Fengfeng Li,Fangxiang Luo,Qingjiang Pan,Songdong Ding
Efficient and selective extraction of pertechnetate (TcO 4 − ) from nitric acid medium has become a significant challenge, especially in the presence of a large excess of interfering anions. By employing a combined strategy involving H-bonding and electrostatic interaction, a highly selective extraction of TcO 4 − can be achieved. The present work reports three homologous amine-diamide ligands with different alkyl chain lengths on the amine N atom of 2,2′-(metylimino)bis( N , N -dioctylacetamide) (MIDOA), 2,2′-(butylimino)bis( N , N -dioctylacetamide) (BIDOA) and 2,2′-(octylimino)bis( N , N -dioctylacetamide) (OIDOA), and their extraction behaviors for TcO 4 − /ReO 4 − in HNO 3 solution are also investigated by using n -dodecane as a diluent. It has been shown that all of them exhibit excellent extractability and high selectivity to TcO 4 − /ReO 4 − . Their extractability and phase disengagement follow the order of OIDOA > BIDOA > MIDOA, revealing a greater extractability and rapider phase disengagement for the amine-diamide ligand with longer chain substituents on the amine N atom. Both slope analysis and loading capacity test indicate the formation of 1:1 metal/ligand extracted complex, which is also confirmed by the analyses of single-crystal X-ray diffraction (SC-XRD), electrospray ionization mass (ESI-MS), Fourier transform infrared (FT-IR), and X-ray photoelectron spectroscopy (XPS). The extraction of TcO 4 − /ReO 4 − by the amine-diamide ligand follows the anion exchange extraction model and is a spontaneous and endothermic process. Furthermore, a competing extraction test was also conducted and demonstrates excellent extractability and high selectivity to TcO 4 − /ReO 4 − .
研究领域:
化学
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核化学与放射化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 17
·7659-7670
·
IF 3.591
Kangjun Xie,Zhen Dong,Nan Wang,Wei Qi,Long Zhao
The selective elimination of radioactive TcO4− from radioactive waste is becoming increasingly critical for environmental security. In this work, a series of novel adsorbents (Si-IL-X, X = NO3, Cl, BF4, NTf2) modified with ionic liquids containing different anions (X) were synthesized via radiation grafting of 1-vinyl-3-ethylimidazolium tetrafluoroborate onto silanized silica and subsequent anion replacement. The surface and structural properties of the prepared adsorbents were characterized by FT-IR spectroscopy, TGA, XPS, and SEM-EDS. Subsequently, their adsorption properties for ReO4− (a nonradioactive surrogate of TcO4−) were studied in detail via batch and column experiments. The batch experiments indicated that the Si-IL-X showed high ReO4− removal efficiency over a broad pH range of 3–10, and their maximum adsorption capacities were in the range of 147.93–289.02 mg g−1 against ReO4−. It was found that the adsorption ability of Si-IL-X was related to the anion structure of the ionic liquid, and the order was Si-IL-NO3 > Si-IL-Cl > Si-IL-BF4 > Si-IL-NTf2, which was mainly determined by the hydrophilicity and ionic radius of the anions. Besides, their adsorption capacities barely decreased after electron beam radiation of 800 kGy. In column experiments, the adsorbents exhibited excellent selectivity and could capture ReO4− efficiently from simulated radioactive wastewater containing a large number of coexisting ions. In addition, the XPS and FT-IR spectroscopic analyses indicated that adsorption was carried out by an ion-exchange process. The results suggested that Si-IL-X showed excellent application prospect for efficient capture of TcO4− from Hanford waste and other common acidic radioactive wastes.
研究领域:
环境科学
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核化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Ning-xiao Wei,Yu-xing Wang,Hua-li Chen,Li-guang Wu,Ting Wang
In an effort to explore the potential application prospects of membrane separation technology in treating nuclear-contaminated wastewater, a TFN nanofiltration membrane incorporating the ZIF-8@Ti 3 C 2 T x nanocomposite was successfully synthesized using the interfacial polymerization method. This involved doping the microemulsion of ZIF-8@Ti 3 C 2 T x into the aqueous (organic) phase. The morphology and structure of ZIF-8@MXene nanocomposites and TFN nanofiltration membranes were characterized. The selective removal of ReO 4 - from simulated radioactive wastewater using the TFN nanofiltration membrane was evaluated. The results indicated that the ZIF-8@Ti 3 C 2 T x composite, uniformly dispersed in the polymer, effectively enhanced the pore structure and polarity of the nanofiltration membrane, thereby improving its permeability. The electronegativity of ZIF-8@Ti 3 C 2 T x also enhanced the negative charge on the surface of the polymer membrane, significantly improving the membrane’s performance in rejecting ReO 4 - while maintaining a low retention rate for Na + . This design facilitates the efficient selection of ReO 4 - from high-salinity wastewater. In addition, the layer spacing of Ti 3 C 2 T x further improved the screening of ReO 4 - and Na + . However, when 0.75 g·L −1 of microemulsion was added, it became challenging to disperse the microemulsion completely in the organic phase. This led to the agglomeration of composites in the nanofiltration membrane, weakening both flux and selectivity. Optimal performance was achieved with a microemulsion doping amount of 0.5 g·L −1 , resulting in the nanofiltration membrane M-O-1 exhibiting the best performance (Jp = 41.92 L·m 2 ·h −1 and R(ReO 4 - ) = 65.81%). Even at a high salt concentration (20 g·L −1 ), the M-O-1 membrane retained approximately 55% of pollutants after continuous operation for 5 h, indicating that the TFN nanofiltration membrane containing ZIF-8@Ti 3 C 2 T x holds significant promise for selectively extracting 99 Tc from wastewater with a high salt content.
研究领域:
环境科学
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材料科学
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水处理
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纳米技术
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膜技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 28
·期 14
·17752-17762
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IF 4.223
Xie Kangjun,Dong Zhen,Zhao Long
The decontamination of radioactive TcO 4 − from nuclear wastes is becoming increasingly crucial for spent nuclear fuel reprocessing and environmental remediation. In this work, a series of ionic liquid–immobilized silica-based adsorbents (SVIL-Cn, n = 1, 4, 8) were newly synthesized using the radiation-induced grafting of 4-vinylbenzyl chloride onto silanized silica and subsequent functionalization with 1-methylimidazole, 1-butylimidazole, or 1-octylimidazole. The synthesis conditions such as the solvent, absorbed dose, and monomer concentration were investigated in detail, and the resulting adsorbents were characterized by elemental analysis, FT-IR, SEM, and TGA. In batch experiments, the adsorbents exhibited a high ReO 4 − (a nonradioactive surrogate of TcO 4 − ) removal efficiency over a wide pH range (3 ~ 8), and SVIL-C1 showed a maximum adsorption capacity of 70.62 mg g −1 towards ReO 4 − . In addition, their adsorption performance barely changed after 800 kGy radiation. The column experiments for treating simulated radioactive wastewater showed that the SVIL-Cn adsorbents could selectively separate TcO 4 − /ReO 4 − from a variety of fission products, and they could be recycled four times with negligible capacity loss. Lastly, XPS and FT-IR analysis confirmed that the adsorption proceeded via an ion-exchange mechanism. The results showed that these adsorbents are suitable for the efficient removal of TcO 4 − /ReO 4 − from radioactive wastewater with complex compositions. Graphical abstract
研究领域:
核化学
·
环境科学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Kangjun Xie,Zhen Dong,Maolin Zhai,Weiqun Shi,Long Zhao
As a radioactive fission product, 99 Tc always existed in the combined extreme conditions of super acidity, high ionic strength, and strong radiation field, which made the efficient removal of Tc a challenge. Herein, for the first time, a series of n-alkyl-imidazolium ionic liquids were grafted onto silanized silica using radiation technique. The surface and structure properties of prepared adsorbents (SiO 2 -MPTS-[C n VIm]Br) were characterized by FT-IR, TGA, XPS, BET, and SEM-EDS. Subsequently, their adsorption properties for ReO 4 − (a nonradioactive surrogate of TcO 4 − ) were studied in detail. These adsorbents exhibited an adsorption capacity of approximately 190 mg g −1 for ReO 4 − . It was found that adsorbents with longer alkyl chains showed better selectivity against ReO 4 − under the conditions of strong acids and a large excess of competitive ions. Column experiments indicated that these adsorbents could be recycled 10 times with negligible capacity loss. In addition, their adsorption performance remained unchanged after 800 kGy radiation. The column experiments of treating simulated radioactive wastewater proved that SiO 2 -MPTS-[C n VIm]Br was promising for selective separation of TcO 4 − /ReO 4 − from a variety of fission products. Lastly, XPS and FT-IR analysis confirmed that the adsorption mechanism was based on ion-exchange.
研究领域:
核化学
·
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）