ACS Applied Polymer Materials
·
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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DOI
高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Xingsheng Liu,Shengyuan Zhao,Wan Xu,Huijuan Zhang,Siyuan Lu,Zhenbin Chen,Fangfang Niu,Gang Wu
With decreasing global rhenium resources, it has become important to separate and purify rhenium in secondary resources, so a preparation strategy for a chitosan-comodified surface-grafted thermosensitive ion-imprinted composite membrane (CS-Re-TIICM) was developed in this work. The key of this design was that the two ends of a poly(N,N-diethylacrylamide) (PDEA) chain were grafted onto the imprinted polymer separating the layer matrix and the surface of the membrane, respectively, which aimed to improve the selectivity and desorption ratio of this material simultaneously. The structure and morphology of this material were characterized by FTIR and SEM, respectively. In addition, CS-Re-TIICM was applied to the secondary leaching solution of the high-temperature alloy to test the actual separation effect, and results showed that CS-Re-TIICM, possessing thermoresponsive recognition sites, and the structure of the imprinting cavity could be adjusted by temperature, which helped this material achieve good selective separation and purification performance for ReO4–. The maximum adsorption capacity was 0.1071 mmol/g at 35 °C. CS-Re-TIICM not only showed an excellent selectivity (separation ReO4–/MnO4– of 3.90 in the presence of interfering ion MnO4–) but also presented an excellent desorption performance (desorption ratio of 68.94%) and good reusability (adsorption capacity of 0.0425 mmol/g, desorption ratio of 59.13%, and separation degree of 1.24). When CS-Re-TIICM was applied to the secondary leaching solution of high-temperature alloys, the purity of Re was increased from 35.41% to 65.10% after one adsorption/desorption cycle, which depicted a prospective application in the industrialized separation of ReO4– from a complex environment.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yanyan Chen,Hao Deng,Pengliang Liang,Heng Yang,Long Jiang,Jing Yin,Jia Liu,Shuying Shi,Huiqiang Liu,Yuxiang Li,Ying Xiong
Sustainable photocatalysis can effectively reduce the radioactive 99TcO4– to less soluble TcO2·nH2O(s), but the reduction efficiency is highly susceptible to coexisting nitrate (NO3–). Here, we quantitatively investigate photocatalytic remediation conditions for Tc-contaminated water stimulated by the analogue perrhenate (ReO4–) in the presence of NO3–, and we elucidate the influence mechanism of NO3– by in situ characterizations. The interfering NO3– can compete with Re(VII) for the carbonyl radical (·CO2–) produced by formic acid (HCOOH) oxidation to generate nitrogen-containing products such as NH4+, NO2–, and NOx, resulting in the decrease in the Re(VII) reduction ratio. Under the conditions of 4% (volume ratio) HCOOH and pH = 3, the yield of NOx is the lowest, and the selectivity of N2 reaches 93%, which makes the overall reaction more in line with the pollution-free concept. The X-ray absorption fine structure reveals that the redox product Re(IV) mainly exists in the form of ReO2·nH2O(s) and is accompanied by a decrease with the increase in NO3– concentration. Re(VII)/Tc(VII) reduction suffers from a serious interferential effect of NO3–, whereas the higher the concentration of NO3–, the more conducive to slowing down the reoxidation of the reduction products, which is advantageous for the subsequent sequestration or separation.
研究领域:
环境科学
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放射化学
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DOI
PubMed
高影响因子
Pigment & Resin Technology
·
2021
·Vol. 52
·期 1
·123-133
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IF 1.263
Jun Zhang,Xiaojian Ou,Lin Li,Qianqian Chen,Zifan Zhang,Ting Huo,Xiaoyu Lin,Fangfang Niu,Shengyuan Zhao,Fang We,Hui Li,Chunli Liu,Zhenbin Chen,Sujun Lu,Peng Zhang,Jinian Zhu
Purpose A novel grafted temperature-responsive ReO 4 − Imprinted composite membranes (Re-ICMs) was successfully prepared by using polyvinylidene fluoride (PVDF) resin membranes as substrates, this study aimed to separate and purify ReO effectively. Design/methodology/approach Re-ICMs were synthesized by PVDF resin membranes as the substrate, acrylic acid (AA), acrylamide (AM), ethylene glycol dimethacrylate (EGDMA) were functional monomers. The morphology and structure of Re-ICMs were characterized by scanning electron microscope and Fourier transform infrared spectroscopy. Findings The maximum adsorption capacity toward ReO 4 − was 0.1,163 mmol/g and the separation decree had relation to MnO 4 − was 19.3. The optimal operation conditions were studied detailedly and the results as follows: the molar ratios of AA, AM, EGDMA, ascorbic acid, NH4ReO 4 , were 0.8, 0.96, 0.02, 0.003 and 0.006. The optimal time and temperature were 20 h and 40°C, respectively. The Langmuir and pseudo-second-order models were fit these adsorption characteristics well. Practical implications Rhenium (Re) is mainly used to chemical petroleum and make superalloys for jet engine parts. This study was representing a technology in separate and purify of Re, which provided a method for the development of the petroleum and aviation industry. Originality/value This contribution provided a novel method to separate ReO 4 − from MnO 4 − . The maximum adsorption capacity was 0.1163 mmol/g at 35°C and the adsorption equilibrium time was within 2 h. Meanwhile, the adsorption selectivity rate ReO 4 − /MnO 4 − was 19.3 and the desorption rate was 78.3%. Controlling the adsorption experiment at 35°C and desorption experiment at 25°C in aqueous solution, it could remain 61.3% of the initial adsorption capacity with the adsorption selectivity rate of 13.3 by 10 adsorption/desorption cycles, a slight decrease, varied from 78.3% to 65.3%, in desorption rate was observed.
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
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2020
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IF 2.463
Xueyu Wang,Xiaoyang Hu,Lianjun Song,Xiuying Yang,Qian Xiao,Haowei Xu,Songdong Ding
The two DOTA-tetraamide ligands, DOTAM- n -butyl (1,4,7,10-tetrakis[( N - n -butyl; carbamoyl)methyl]-1,4,7,10-tetraazacyclododecane) and DOTAM-benzyl (1,4,7,10- tetrakis[( N -benzylcarbamoyl)methyl]-1,4,7,10-tetraazacyclododecane), were synthesized and characterized by MS, NMR and FTIR spectra. In acid solution, DOTAM- n -butyl was liable to be protonated. FTIR, 1 H NMR, ESI-MS spectra and X-ray diffraction analyses revealed that the nitrogen atoms of cyclen ring combined two protons to form a cation with two positive charges. The protonated DOTAM- n -butyl had strong extraction ability and good selectivity for ReO 4 − . It was extracted by means of the substitution of one ReO 4 − for one NO 3 − in the 1:2 complex of DOTAM- n -butyl with HNO 3 . The solvent extraction and X-ray crystallography demonstrated an anion-exchange extraction model. Meanwhile, X-ray crystal structure analyses of ligand complexes with HReO 4 or HNO 3 also indicated that ReO 4 − or NO 3 − ions were located in the gap between the upper and lower protonated ligands through multiple hydrogen bonds and electrostatic interactions.
研究领域:
化学
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放射化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2024
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IF 7.6
Miaomiao He,Yuxuan Chen,Guangyuan Chen,Wenhao Li,Mingxing Zhang,Chao Zhang,Hao Zhang,Xingyi Long,Kui Tang,Tao Duan,Lin Zhu
The extraction of 99 TcO 4 − from radioactive effluents is extremely crucial for the purposes of nuclear disposal and environmental remediation. Herein, utilizing a facile and low-cost synthesis method, we report a pyridinium-based cationic polymer network , CPP-Cl, with impressive adsorption performance and ultrafast adsorption kinetics towards ReO 4 − . The structure featuring highly density of charged pyridinium units was synthesized, making it an effective adsorbent for capturing ReO 4 − . The material showed fast ReO 4 − adsorption kinetics reaching adsorption equilibrium within 30 s, an excellent capture capability of 1069.7 mg/g, and exceptional separation efficiency of 94.3% for removing 1000 ppm ReO 4 − . Furthermore, it possessed excellent reusability in multiple sorption/desorption trials and good uptake capacity within a widely ranging pH values. It is noteworthy that the extraction efficiency of CPP-Cl for ReO 4 − from simulated nuclear waste can be up to 94.2%. The favorable performance of the material in multiple tests revealed that CPP-Cl has tremendous potential as a high-efficiency sorbent for capturing 99 TcO 4 − /ReO 4 − in complex nuclear associated environmental systems.
研究领域:
环境科学
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核化学
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材料科学
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产品关联
DOI
PubMed
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
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 42
·e56095
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IF 2.7
Xianhang Bu,Zhengcan Chen,Xiaoyu Lin,Wan Xu,Yuanjun Sun,Xiaojian Ou,Yuan Sun,Zhenbin Chen
In this study, we combined the imprinting technique, temperature-sensitive polymer, and Pickering emulsion polymerization to prepare a temperature-sensitive porous imprinted polymer. First, the temperature-sensitive block polymer PDEA-b-P (DEA-co-AM) was prepared by reversible-addition fragmentation chain transfer polymerization, and then a temperature-sensitive porous ReO 4 − imprinted polymer (ReO 4 − -TPIP) was prepared using the Pickering-like polymerization technique, which was introduced to the preparation of the imprinted polymer. The structure and morphology of the polymer were characterized by FTIR, SEM-EDS, and BET. The adsorption experiments showed that the maximum adsorption (Q), separation (R), and desorption (D) of ReO 4 − -TPIP were 0.1568 mmol/g, 3.41, and 85.22%, respectively, and the adsorption equilibrium could be reached after 120 min, which decreased to 0.1212 mmol/g, 1.23, and 70.01% after repeated use for 11 times. These results indicate that ReO 4 − -TPIP has good adsorption and reusability properties. The adsorption studies showed that ReO 4 − -TPIP conformed to the zero-level kinetic model in the pre-adsorption stage, the quasi-one-level kinetic model in the late stage, and the isothermal adsorption process conformed more to the Langmuir model. In addition, in the secondary leach solution of high-temperature alloys, the purity of rhenium in the solution increased from 35.4119% to 53.4812% after one adsorption/desorption cycle. The prepared ReO 4 − -TPIP provides a new material and strategy for the selective separation and purification of rhenium in complex rhenium-containing solutions for the industry.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
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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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2022
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IF 6.137
Pengwei Zhao,Xiaoyuan Zhou,Yalin Huang,Yuwei Xu,Shanyong Chen,Chengbin Zheng,Yongdong Jin,Chuanqin Xia
Removal of TcO 4 − from liquid radioactive waste is urgent due to its long half-life and high mobility. Herein, two guanidine-based cationic covalent organic polymers (TG-TPAL-H and TG-TPAL-OMe) were synthesized, and were used to research for the removal of ReO 4 − . TG-TPAL-H showed high removal efficiency, its sorption capacity got to 549 mg g −1 and distribution coefficient K d was 1.17 × 10 6 mL g −1 . What impressively, the TG-TPAL-H removed 80% of ReO 4 − even there was 1000 times of competing anions (Cl − , SO 4 2− , H 2 PO 4 − ). While TG-TPAL-OMe showed a poor performance on ReO 4 − with the capacity of 317 mg g −1 and K d of 6.9 × 10 4 mL g −1 . TG-TPAL-H can remove 87% ReO 4 − from simulated Hanford LAW stream sample, while TG-TPAL-OMe just can remove 35%. The difference between the two materials can be attributed to the electron donating group (Methoxy) in TG-TPAL-OMe reduced the positive charge density of guanidine, which was demonstrated by the ESP of density functional theory (DFT) calculation.
研究领域:
材料科学
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环境科学
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放射化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Dingyang Chen,Zhaoli Liu,Shuying Li,Xiaofei Jing,Yuyang Tian,Wei Hu,Fengchao Cui,Rui Zhao,Guangshan Zhu
Developing cationic adsorbents for efficient radioactive pertechnetate ( 99 TcO 4 − ) removal from water is of great significance in both nuclear fuel management and nuclear-related environmental treatment fields. However, tremendous efforts should be taken to improve the comprehensive performance of the adsorbent materials. Herein, novel cationic electrospun nanofibers were synthesized via the blending electrospinning from the branched polyethylenimine based solution and the following quaternization reaction by benzyl bromide. Consequently, abundant specific anion traps with hydrophobic microenvironment were constructed on the fibers. The obtained fiber adsorbents were systematically investigated to remove perrhenate (ReO 4 − ) ions (the nonradioactive surrogate for TcO 4 − ), which exhibit satisfying adsorption performance in several aspects: high adsorption capacity (943 mg g −1 ), fast kinetics (30 min), good removal depth (distribution coefficient = 1.1 × 10 6 mL g −1 ), large dynamic column adsorption volume (1540 bed volume), and excellent ReO 4 − capture from solution with high ionic strength or acidity/alkalinity. The adsorption performance surpassed all macroscopic shapeable adsorbents and many powdery advanced porous materials, owing to their abundant adsorption sites, tailored anion traps and macroscopic fibrous structures. Overall, this work gives a useful insight into designing novel adsorbents for effective TcO 4 − /ReO 4 − capture.
研究领域:
材料科学
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环境科学
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核能工程
✓ 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）