Materials Advances
·
2022
·Vol. 3
·期 12
·4870-4877
·
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
·
环境科学
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材料科学
✓ 已验证
产品关联
DOI
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2021
·Vol. 330
·期 3
·1165-1176
·
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
·
环境科学
·
放射化学
✓ 已验证
产品关联
DOI
高影响因子
RADIATION PHYSICS AND CHEMISTRY
·
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
·
放射化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Xueyu Wang,Songdong Ding,Zhipeng Wang,Lianjun Song,Xiuying Yang,Qian Xiao,Haowei Xu,Junli Wang,Zhen Shen,Hui Wang
Effective and selective separation of technetium from acidic nuclear liquid waste is highly desirable for partitioning and transmutation but is of significant challenge. Highly efficient extraction of pertechnetate can be achieved by taking H-bonding and electrostatic interaction combined strategy. Base on this strategy, an amine–amide ligand NTAamide(n-Oct) was employed to extract TcO4– in HNO3 solution. Using n-dodecane as a diluent, NTAamide(n-Oct) demonstrated excellent extractability and good selectivity toward TcO4– with a rapid extraction equilibrium that could be reached in less than 1 min. Its maximal loading capacity for TcO4– was almost 100 times as much as that of traditional amine extractant Aliquat-336 nitrate. Meanwhile, TcO4– could be efficiently stripped from the loaded organic phase by (NH4)2CO3 solution. Slope analysis indicated the formation of a 1:1 complex of NTAamide(n-Oct) with TcO4–. The extraction conformed to the anion exchange extraction model, as confirmed by analyses of single-crystal X-ray diffraction, 1H NMR titration, FTIR, and ESI-MS.
研究领域:
核化学
·
放射性废物处理
·
配位化学
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 28
·期 14
·17752-17762
·
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
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环境科学
·
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 2
·673-681
·
IF 1.754
Xie Kangjun,Hua Rong,Dong Zhen,Wang Nan,Zhang Manman,Qi Wei,Zhai Maolin,Yang Jun,Zhao Long
Selective adsorption of TcO 4 − from radioactive waste is important for the nuclear industry. In this work, three 1-vinyl-3 benzylimidazole chloride modified mesoporous silica bearing different pore volumes and specific surface areas were synthesized using radiation grafting. The effect of pore structure on the adsorption properties of the three adsorbents were studied. The adsorbents with bigger specific surface area and pore volume were conducive to ReO 4 − adsorption in terms of both adsorption rate and capacity. The prepared adsorbents displayed good radiation resistance under gamma rays in dry or wet conditions, and they could selectively remove ReO 4 − from simulated Hanford wastewater in column experiments.
研究领域:
核化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 6
·1869-1881
·
IF 1.6
Zhang Na,Yang Miao,Zhang Manman,Du Jifu,Bao Qiburi,Zhao Long,Dong Zhen
Amphiphilic double poly(imidazole ionic liquid) grafted silica (SMIL-n) was prepared by radiation grafting of hydrophilic 1-vinyl-3-ethylimidazolium bromide and hydrophobic 1-vinyl-3-octylimidazolium bromide at different ratio onto silica. The adsorption behavior of SMIL-n was investigated. The adsorption equilibrium could reach less than 45 min, and their adsorption capacity were 152–171 mg/g obtained from Langmuir model. The selectivity of SMIL-n to ReO 4 − increased with the increasing content of hydrophobic ionic liquid. SMIL-n displayed good reusability, excellent acid resistance and irradiation resistance. Particularly, SMIL-n showed promising for ReO 4 − uptake from simulated contaminated Beishan groundwater and radioactive wastewater.
研究领域:
材料科学
·
环境科学
·
核化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 18
·8809-8819
·
IF 3.3
Zhen Dong,Na Zhang,Manman Zhang,Miao Yang,Qiburi Bao,Long Zhao
Pertechnetate (TcO4−) poses long-term potential radioactive hazards to the ecological environment, so it is an urgent challenge to selectively separate TcO4− from radioactive wastewater. In this work, we firstly developed a series of binary ionic liquid functionalized silica (SiO2-g-PC2-CnvimBr) by simultaneous radiation grafting of the hydrophilic ionic liquid 1-vinyl-3-ethylimidazole bromide ([C2VIm]Br) and hydrophobic ionic liquid 1-vinyl-3-alkylimidazolium ([CnVIm]Br, n = 4, 6, 8, and 12) onto silica for the removal of ReO4− as an analogue of TcO4−; single ionic liquid functionalized silica (SiO2-g-PC2vimBr) was also synthesized for comparison. The effects of absorbed dose and RAFT agent content on grafting yield were investigated. The grafting yield (GY) increased with increasing absorbed dose and decreasing RAFT agent content. SiO2-g-PC2-CnvimBr showed excellent acid and irradiation resistance; the adsorption efficiency was still more than 90% after soaking in acid solution for 3 months or after being irradiated at 1000 kGy. SiO2-g-PC2-CnvimBr presented superior selectivity for ReO4− over SiO2-g-PC2vimBr. Furthermore, the continuous uptake of ReO4− using SiO2-g-PC2-CnvimBr with varying alkyl chain lengths of hydrophobic imidazolium was investigated and compared in the simulated radioactive wastewater. It was found that the relative column adsorption capacity and selectivity increased with increasing alkyl chain length of hydrophobic imidazolium. In addition, SiO2-g-PC2-C8vimBr displayed excellent reusability; the adsorption capacity did not change and the desorption efficiency could reach 97% in the flow-through column cycle experiment. On the basis of experimental results, SiO2-g-PC2-CnvimBr was deemed to be promising for continuous separation of TcO4−/ReO4− in the practical treatment of radioactive wastewater and TcO4− contaminated groundwater.
研究领域:
材料科学
·
环境工程
·
核化学
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
HYDROMETALLURGY
·
2019
·
IF 3.465
Zhenning Lou,Mengnan Huang,Junshuo Cui,Shuyao Wu,Shanshan Xing,Peng Zhou,Weijun Shan,Ying Xiong
Technetium ( 99 Tc), a radionuclide generated from uranium fission in nuclear reactors, has posed a major threat to humans due to its long half-life and radioactivity. Therefore, it is urgent to develop a strategy of selectively and efficiently capturing of 99 Tc. In this work, a series of solid copolymers (denoted as DVB-[C x ClVim][Cl]) were synthesized for efficient adsorption of perrhenate (ReO 4 − , a surrogate for TcO 4 − ) from mixed ions solution. The adsorbents with vinylimidazolium-based ionic liquid as functional group and divinylbenzene (DVB) as the basic framework exhibited stable structure and good ReO 4 − adsorption performance. The influences of the linear n-alkyl chain length on the morphology and adsorption property of the copolymers were discussed in detail. The maximum uptake of Re(VII) on DVB-[C 4 ClVim][Cl] was 517.61 mg·g −1 . Rhenium could be separated from molybdenum in the presence of co-anions and co-cations by DVB-[C 6 ClVim][Cl], which demonstrated its good adsorption selectivity . The kinetic studies showed that pseudo-second-order model was more suitable for describing the behavior of Re(VII) adsorption. The adsorption mechanism was ion-exchange between Cl − and ReO 4 − confirmed by FI-IR, IC and XPS analysis. Additionally, DVB-[C x ClVim][Cl] remained effective Re(VII) capture ability after eight adsorption/elution cycles, demonstrating their good reusability.
研究领域:
环境科学
·
材料科学
·
放射化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Mengnan Huang,Lixin Kan,Wenyan Zhao,Yuejiao Wang,Ying Xiong,Weijun Shan,Zhenning Lou
99 Technetium ( 99 Tc) is one of the most dangerous radioactive isotopes in the legacy nuclear waste, and harmful to the environment and human health. Effectively removing it remains a long-term challenge. Herein a resin-like imidazolium-based ionic liquid polymer (DVB-2C 8 VEIMBr) was prepared for selective adsorption of TcO 4 − (ReO 4 − as an alternative for laboratory operation). It is manifested that DVB-2C 8 VEIMBr integrates high adsorption capacity (313.28 mg·g −1 ) and selectivity (90.68% in 6000 times excess of SO 4 2− ions). A real-scenario experiment exhibits DVB-2C 8 VEIMBr can remove up to 93% of TcO 4 − from the simulated Hanford LAW scrubber solution. More importantly, DVB-2C 8 VEIMBr displays super acid and alkaline resistance and stability after immersing for 8 months under extreme conditions of 3 M HCl and 2 M NaOH. It can also effectively separate rhenium from molybdenum solution in the range of 3 M HCl - pH 2. Additionally, it still showed perfect regeneration performance after 10 cycles. In particular, this work demonstrates the feasibility of imidazolium-based ionic liquid adsorbents in the TcO 4 − or ReO 4 − immobilization process, which can be applied to capture these radioactive oxygen anions under high acid and high alkali conditions.
研究领域:
环境科学
·
放射化学
·
材料科学
✓ 已验证
DOI
高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Li Jie,Zhao Yuting,Li Baoyu,Chen Lixi,Guo Qi,Song Wanrong,He Linwei,Chen Long,Zhang Mingxing,Chai Zhifang,Wang Shuao
Efficient segregation of TcO 4 − from high-level radioactive wastes (HLW) is critical for robust nuclear waste management and environmental protection. However, achieving deep decontamination is especially challenging in complex conditions of strong basicity, high radiation, and excessively competitive anions. Herein, we addressed the long-term challenge by modifying the imidazolium core with phenyl, trimethylphenyl, and benzyl groups in a flexible polymer chain, which constructs a precisely targeted microenvironment for selective TcO 4 − capture. This custom-engineered material (SCU-CPN-7) exhibits fast kinetics, high adsorption capacity (314.7 mg/g), excellent distribution coefficient (1.3 × 10 7 mL/g), and remarkable efficiency in TcO 4 − uptake under the combining extreme conditions of strong alkalinity (1 M NaOH) and high radioactivity. More importantly, owing to the synergistic effects of the hydrophobic effect, electrostatic affinity, and p- π interactions, SCU-CPN-7 demonstrates exceptional selectivity, capable of almost quantificationally removing TcO 4 − in the coexistence of a large excess of NO 3 − and SO 4 2− , leading to an unparalleled uptake performance of TcO 4 − from simulated HLW in both batch and dynamic column separation tests.
研究领域:
环境科学
·
核化学与放射化学
✓ 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）