Toxics
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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
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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
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DOI
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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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
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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DOI
高影响因子
Environmental Chemistry Letters
·
2020
·Vol. 18
·期 4
·1379-1388
·
IF 5.922
Zhang Hao,Yang Fan,Lu Chuan,Du Chang,Bai Ruixi,Zeng Xian,Zhao Zhigang,Cai Chunqing,Li Jianguo
Treatment and recycling of radioactive waste are major challenges for the nuclear energy sector. Pertechnetate anions, 99 TcO 4 − , occur in nuclear waste and are formed mainly during nuclear fission. 99 TcO 4 − is a very hazardous contaminant due to its long half-life and high solubility and mobility in water. The effective capture of 99 Tc contamination at legacy nuclear sites remains a serious and unsolved environmental issue. In this work, 99 TcO 4 − /ReO 4 − was adsorbed by compressible graphene–chitosan sponges with grafted tertiary amine groups. Moreover, the hydrophobic branched chains strongly reduced the interference of competitive anions during adsorption. Results show that 99 TcO 4 − /ReO 4 − can be effectively removed even under highly acidic conditions and in the presence of competing anions. More than 98% of 99 TcO 4 − /ReO 4 − was removed using simulated nuclear wastes.
研究领域:
环境科学
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核能工程
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材料科学
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DOI
高影响因子
DESALINATION
·
2026
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IF 9.9
Xiangjun Liao,Huining Zhang,Yuxiao Tian,Guangtai Zheng,Shijian Pan,Jing Chen,Yuri A. Ustynyuk,Valentin G. Nenajdenko,Yuan Liao,Cheng-peng Li
The sustainable and efficient treatment of high-salinity radioactive wastewater containing 99 TcO 4 − represents a critical challenge, driven by the severe environmental risks of 99 TcO 4 − and the inadequacy of existing treatment technologies. Here, we introduced membrane distillation (MD) as a novel approach for such wastewater and developed a robust superhydrophobic membrane (# PVDF-PN ) that simultaneously resisted wetting and scaling while overcoming the conventional selectivity-permeability trade-off. The # PVDF-PN was fabricated through in situ hydrolysis and polymerization of trichloromethylsilane (TCMS) on hydroxylated polyvinylidene fluoride (PVDF), yielding a surface densely covered with low-surface-energy polysiloxane nanofilaments. This unique nanofilament architecture significantly enhanced the gas-liquid interfacial area for vapor evaporation, without compromising pore integrity or permeability due to surface modification. When tested with challenging feeds containing surfactants or supersaturated gypsum, # PVDF-PN maintained a stable flux of ∼33.0 kg·m −2 ·h −1 and near-complete salt rejection (>99.99%), outperforming both unmodified # PVDF and fluorinated silica-coated # PVDF-FS . Its exceptional performance was attributed to a high liquid entry pressure, an elevated energy barrier for crystal nucleation, and reduced liquid-solid contact area and interaction time. Importantly, in long-term MD treatment of simulated 99 TcO 4 − /ReO 4 − -laden high-salinity wastewater, # PVDF-PN achieved non-detectable effluent concentrations of target oxyanions, demonstrating its potential as a reliable and efficient solution for radioactive wastewater management and emergency response.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2025
·
IF 3.7
Tangzheng Lu,Jiayi Feng,Yong Kang
The design of highly stable and efficient porous materials is crucial for physisorption-based separation of radioactive species ( 99 TcO 4 - /ReO 4 - ), serving as an alternative to current concentrate-storage-solidification treatment technologies. Herein, employing a covalent-ionic dual-crosslinking strategy with economical ionic compounds as reactive monomers, a novel cationic organic polymer (TJU-COP-1) was synthesized for the first time via facile radical polymerization for 99 TcO 4 - /ReO 4 - sequestration. TJU-COP-1 demonstrates exceptional adsorption capacity, kinetics and selectivity ( K d ) for 99 TcO 4 - /ReO 4 - (861.87 mg·g –1 , K d = 5.0 × 10 5 ml·g -1 ), achieving adsorption equilibrium within merely 1 min. Notably, TJU-COP-1 maintains adsorption efficiency as high as 96.25% after five adsorption-desorption cycles. The TJU-COP-1 showed high stability after acid (3 mol·L –1 HNO 3 ), alkali (3 mol·L –1 NaOH) and radiation (200 kGy 60 Co γ) treatment. More significantly, TJU-COP-1 demonstrated robust and promising removal performance in complex solution, achieving 98.55% efficiency for 99 TcO 4 - /ReO 4 - amid high concentrations of competing anions and an excellent 72.11% removal in simulated Hanford LAW waste solution. Combined experimental characterization and density functional theory theoretical validation confirmed that the adsorption mechanism involves a synergistic combination of electrostatic interactions and anion exchange. This study illustrates that TJU-COP-1 has great potential for practical application in the capture of 99 TcO 4 - /ReO 4 - , and provides a new approach to the design of high-performance adsorbents for the treatment of nuclear wastewater.
研究领域:
环境科学
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材料化学
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核化学
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吸附技术
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聚合物化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Xiaoyong Xia,Jiaqing Huang,Qimeng Sun,Jinkai Qiu,Parada Weaoseng,Chanat Chokejaroenrat,Cheng Lian,Qingfeng Xu,Jianmei Lu
A cage-like multi-imidazolium sorbent is designed for 99 TcO 4 − /ReO 4 − capture. • Cooperative clamping in confined spaces enables ultrafast adsorption kinetics. • The sorbent exhibits a high ReO 4 − uptake capacity of 730 mg g −1 . • Excellent selectivity is achieved in highly competitive nuclear waste media. • Composite beads allow efficient fixed-bed removal with good regenerability. The efficient and selective removal of pertechnetate ( 99 TcO 4 − ) from water remains a significant challenge due to its high solubility, low charge density, and competition from coexisting anions. Herein, we report tetraphenylethene (TPE)-based, imidazolium-functionalized nanomicrospheres for pertechnetate ( 99 TcO 4 − )/perrhenate (ReO 4 − ) capture with high efficiency. The nonplanar, propeller-like TPE core stereospecifically arranges multiple imidazolium sites in a semi-encapsulating/polyhedral fashion, generating size-complementary pockets. Hierarchically confined nano-spaces enable cooperative multi-imidazolium clamping, where hydrophobic effects, electrostatic attraction, ion exchange, multipoint C–H···O hydrogen bonding, and geometric confinement act in concert to afford precise recognition and strong binding. Using ReO 4 − as a nonradioactive surrogate for 99 TcO 4 − , the sorbent delivers ultrafast kinetics (11.23 g mg −1 min −1 ), high capacity (730 mg g −1 ), and 86.5% removal from Hanford low-activity waste (LAW) stream. The powder is readily formed into mechanically robust granules and shows excellent regenerability in fixed-bed tests, retaining >95% efficiency after multiple cycles. This work demonstrates that cooperative multi-imidazolium clamping within confined nano-spaces amplifies multimechanism synergy, providing a general strategy for precise recognition and strong binding of weakly coordinating anions. Propeller-like TPE-based cage-like microspheres spatially organize multiple imidazolium sites into confined binding pockets, enabling cooperative multi-site clamping for rapid and selective ReO 4 − / 99 TcO 4 − capture through hydrogen bonding, electrostatic attraction, ion exchange, and hydrophobic confinement. Download: Download high-res image (184KB) Download: Download full-size image
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高影响因子
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