JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2022
·Vol. 331
·期 2
·673-681
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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
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 6
·1869-1881
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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
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环境科学
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核化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 18
·8809-8819
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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
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环境工程
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核化学
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废水处理
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 5
·2604-2618
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IF 3.3
Fangfang Niu,Wan Xu,Gang Wu,Siyuan Lu,Xiaojian Ou,Zhenbin Chen,Xinyu Zhao,Yuan Sun,Yuanjun Song,Peng Zhang
Ion imprinted polymers (IPs) are very promising for separation processes because of their intended selectivity. However, the trade-off between their selectivity and desorption leads to difficulties in reusing them, which seriously hampers their development. Herein, we design ReO4− temperature sensitive ion-imprinted porous microspheres (ReO4−-TIIM) for the selective separation of ReO4− from aqueous solutions. The introduction of the temperature-sensitive block polymer PDEA-b-P(DEA-co-AM) allowed for a highly controlled blotting site in the ReO4−-TIIM matrix, maintaining a high balance of selectivity and desorption. Pickering emulsion polymerization was used to provide the ReO4−-TIIM with a porous and interoperable structure, thereby enhancing their mass transfer rate and adsorption performance. The adsorption properties of ReO4−-TIIM prepared under optimum process conditions were investigated by adsorption kinetics and adsorption thermodynamics. FTIR, SEM, and BET-specific surface area analyses fully characterized their structure and morphology. The design of the ReO4−-TIIM offers a new approach to the industrial precision separation of Re.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2024
·
IF 5.5
Jia-Qi Luo,Meng-Meng Lun,Qiang-Qiang Jia,Zhi-Jie Wang,Hai-Feng Lu,Yi Zhang,Da-Wei Fu
Comprehensive Summary Molecular ferroelastics with the natural features of mechanical flexibility and switchable spontaneous strain have attracted widespread attention in the scientific community due to their potential applications in tunable gratings, flexible memorizers, strain sensors, and intelligent actuators. However, most designs of molecular ferroelastics remain in the stage of blind exploration, posing a challenge to achieve a functional ferroelastic more effectively. Herein, we have successfully obtained a molecular ferroelastic, [Me 2 NH(CH 2 ) 2 NH 3 ](ReO 4 ) 2 (Me 2 NH(CH 2 ) 2 NH 3 = N , N -dimethylethylenediammonium), under the guidance of the mono-/double-protonation strategy. The double-protonated [Me 2 NH(CH 2 ) 2 NH 3 ](ReO 4 ) 2 undergoes a paraelastic-ferroelastic phase transition with the Aizu notation of 2/ m F at 322 K. Meanwhile, the theoretical calculation and experimental measurement simultaneously show that [Me 2 NH(CH 2 ) 2 NH 3 ](ReO 4 ) 2 possesses good mechanical flexibility, because its elastic modulus ( E ) of 8.26 GPa and hardness ( H ) of 0.45 GPa are smaller than the average values of organic crystals ( E of 12.05 GPa and H of 0.5 GPa), which makes it promising to apply in wearable pressure sensors, implantable medical sensors, high-precision tuners, etc . This work further enriches the molecular ferroelastic family and demonstrates that mono-/double-protonation is one of the effective molecular modification strategies for designing ferroelastics.
研究领域:
材料科学
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化学
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DOI
高影响因子
ACS Applied Nano Materials
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2019
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IF 0
Xia Jin,Guang-Qing Wang,Ding Ma,Shu-Qi Deng,Song-Liang Cai,Jun Fan,Wei-Guang Zhang,Sheng-Run Zheng
Oxo-anion pollutants pose a serious threat to natural water systems. It is highly necessary to develop cationic porous materials capable of removing oxo-anion from sewage. However, they are relatively rarely reported compared with anionic and neutral materials. Herein, two cationic amorphous metal–organic cage-based solids containing cages of different sizes, namely, aMOC-1 and aMOC-2, were constructed and use for removing oxo-anions from water. Because the cages in these materials have large cavities (with about 3.5 and 4.5 nm in diameter for aMOC-1 and aMOC-2, respectively) and high positive charges (positive +24 for both), both aMOC-1 and aMOC-2 exhibit rapid kinetics in carcinogenic chromate (CrO42– and Cr2O72–) and ReO4– (a surrogate anion of radioactive isotope TcO4–) adsorption. The adsorption equilibrium can be reached within only a few minutes. The adsorption capacities of aMOC-1 for CrO42–, Cr2O72–, and ReO4– are 157.4, 203.8, and 350 mg/g, respectively. Because aMOC-2 contains larger metal–organic cage, the corresponding adsorption capacities are 242.0, 407.0, and 583.9 mg/g, respectively. The capacity of aMOC-2 for Cr(VI) oxo-anion adsorption ranks the highest among all related materials ever reported. In addition, the oxo-anions can be released rapidly within several minutes from the oxo-anion-loaded aMOCs in 2 M NaNO3 solution, which allows these materials to exhibit good reusability. Finally, the aMOCs have a potential application in the removal of Cr(VI) from electroplating bath wastewater, in which the concentration changes from 10 to 0.17 ppm after treatment with aMOCs.
研究领域:
环境科学
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材料科学
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产品关联
DOI
ACS Applied Polymer Materials
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2024
·
IF 4.4
Jiang Liu,Zhaoheng Zhu,Yukun Huang,Long Wang,Kai Jia
There is a critical need to develop cost-effective and efficient adsorption materials for the removal of technetium-99 (99Tc) from contaminated water sources. This research presents the synthesis of amino-modified cellulose microspheres (CM-APTS) through the addition of 3-amino-propyl triethoxysilane (APTS) to regenerated cellulose microspheres (CM), followed by a subsequent reaction with ethylene dibromide (EDB) to produce halogen-modified amino cellulose microspheres (CM-APTS-EDB). These are engineered for the effective absorption of ReO4–, serving as a chemical surrogate for TcO4–. By altering the amount of ethylene dibromide used, two variations of bromine-modified cellulose microspheres, CM-APTS-EDBs and CM-APTS-EDBe, are synthesized. Among these, CM-APTS-EDBe exhibits robust adsorption capabilities for ReO4– across a pH spectrum of 2.5–10, attaining a peak capacity of 281 mg·g–1, and demonstrates selective adsorption of ReO4– even in the presence of competing anions such as NO3–, Cl–, and SO42–. Characterization through X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FTIR) indicates that the adsorption mechanism predominantly involves interactions between ReO4– and N+, hydrogen bonding with amino hydrogen, and σ-hole-anion interactions between Re–O and C–Br. After eight adsorption–desorption cycles, CM-APTS-EDBe retains notable stability and reusability. Additionally, the material efficiently captures ReO4– from simulated Hanford Low Activity Waste (LAW) wastewater, achieving an adsorption efficiency of 77.26% at a solid–liquid ratio of 40 g·L–1. This investigation underlines the potential of halogenated regenerated cellulose microspheres in designing advanced adsorbents for the removal of radioactive pollutants like TcO4–/ReO4–, offering a strategy for environmental remediation efforts.
研究领域:
环境科学
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放射化学
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材料科学
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产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2025
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IF 4.7
Ming Zhang,Yan Zhang,Xuede Li,Jie Li,Yufeng Liu
The efficient simultaneous extraction of radioactive metal cations and anions from radioactive waste is crucial for the proper disposal of spent fuel and environmental protection. Modifying metal-organic frameworks (MOFs) into multifunctional materials with tailored properties offers a promising strategy to enhance their practical applications. In this study, polyaniline (PANI)-modified MOF nanosheets (NM53P) are synthesized through a simple, low-cost method and employed to uptake uranium (UO 2 2+ ) and rhenium (ReO 4 - ) from aqueous solutions. The adsorption performance of NM53P-3 composites is evaluated by studying the effects of solution pH, contact time, initial UO 2 2+ /ReO 4 - concentrations, ionic strength, and interfering ions. The maximum adsorption amounts for UO 2 2+ and ReO 4 - are 293.91 and 526.32 mg/g, which surpass most reported adsorbents. Adsorption of UO 2 2+ /ReO 4 - is pH-dependent, spontaneous, and endothermic, and best fit the pseudo-second-order (PSO) kinetic model and Freundlich isotherm. Batch experiments and X-ray photoelectron spectroscopy (XPS) analysis confirm that adsorption is primarily influenced by the abundant amine functionalities and unsaturated metal sites in the NM53P-3 adsorbents. Furthermore, NM53P-3 demonstrates excellent recycling performance. This study highlights the potential of NM53P-3 composites for effectively extracting various radionuclides from aqueous solutions, paving the way for the development of new multifunctional materials for wastewater treatment.
研究领域:
环境科学
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核化学与放射化学
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DOI
高影响因子
HYDROMETALLURGY
·
2019
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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
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材料科学
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放射化学
✓ 已验证
DOI
高影响因子
TALANTA
·
2021
·
IF 6.057
Shengyuan Zhao,Runtian Wang,Xiaojian Ou,Jun Zhang,Hui Li,Chunli Liu,Zhengcan Chen,Xiaoyan Zhang,Ting Huo,Zhenbin Chen,Wenxia Cheng,Jinian Zhu,Sujun Lu,Peng Zhang
A new type of temperature-sensitive imprinted composite membranes(ICMs) was developed. Poly N,N-diethylacrylamide (DEA) blocks, as temperature-sensitive polymer, were grafted onto the substrate of the imprinted polymer separation layer to endow membranes with better adsorption effect. The comprehensive properties of the imprinted composite membranes were adequately tested and evaluated in detail. Results showed that ReO 4 − -ICMs (Re-ICMs) with temperature-sensitive recognition sites could adjust the structure of the imprinted holes at different temperatures, which presented excellent performance in the selective separation and purification of ReO 4 − . The prepared Re-ICMs exhibit the maximum adsorption capacity of 0.1639 mmol/g at 35 °C with the equilibrium adsorption time of 2 h. After ten adsorption/desorption cycles, Re-ICMs could still maintain 73.5% of the original adsorption capacity, the separation degree of ReO 4 − /MnO 4 − was only reduced from the initial 24.5 to 15.9, and the desorption ratio dropped from 80.4% to 68.4%, indicating that Re-ICMs have excellent adsorption and separation performance and reusability.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Minsi Shi,Dingyang Chen,Xinyue Zhao,Yuyang Tian,Rui Zhao
High-efficiency capture of 99 TcO 4 − from radioactive wastewater and natural aqueous environment is urgently in demand. In this study, nonporous cationic polymeric networks (CPN-n) were employed as the building units to construct the cationic porous aromatic frameworks (iPAF-10) through a molecular expansion strategy. This process was simple and efficient, in which iPAF-10 with fast mass transfer channels and high adsorption site utilization was achieved. In addition, this strategy could also improve the materials’ stability in highly acidic and alkaline conditions. Remarkably, compared with CPN-n, iPAF-10 exhibited rapid kinetics (3 min) and a high adsorption capacity of 1287 mg g −1 toward ReO 4 − (a safe alternative to 99 TcO 4 − ), ranking iPAF-10 among the top in existing advanced 99 TcO 4 − /ReO 4 − adsorbents. iPAF-10 also maintained the stable removal of ReO 4 − from excess competition anions (NO 3 − and SO 4 2− ), high acid/alkali (1 M HNO 3 and 2 M NaOH) and radiation condition (200 kGy). As a result, iPAF-10 showed satisfying ReO 4 − elimination performance from simulated Hanford and Savannah River Site waste streams. The anion exchange mechanism during adsorption and desorption processes was clearly elucidated through experimental and computational analysis. This work demonstrated the synthesis of new cationic porous aromatic frameworks, which showed great potential for 99 TcO 4 − /ReO 4 − removal from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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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
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放射化学
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材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）