EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2023
·Vol. 26
·期 22
·e202300121
·
IF 2.3
Yixin Pan,Pengkun Zhang,Rui Huang,Jisheng Kou
Graphical A novel nanocomposite (TNTs-FeS) was developed for removal of U(VI) and Re(VII) from aqueous solutions. Experiment results revealed that TNTs as a stabilizer for FeS had good stability and prevention FeS agglomeration. The pseudo-second-order kinetic model was both able to adequately interpret the experimental rate data of U(VI) and Re(VII) removal. The U(VI) adsorption affected by the coexisting ions (Cd 2+ and Cu 2+ ) significantly due to competitive adsorption. A novel nanocomposite (TNTs-FeS) was developed by anchoring ferrous sulfide (FeS) nanoparticles immobilized on titanate nanotubes (TNTs) by hydrothermal method to remove U(VI) and Re(VII) from aqueous solution, and the removal mechanism and efficiency were examined. The experimental results showed that the TNTs can effectively improve the dispersibility and stability of FeS. The environmental conditions, including initial solution pH, initial concentration, equilibrium time, and dosage, played an important role in the remediation process, which can affect the immobilization efficiency significantly. The maximum quantity removal of U(VI) and Re(VII) was 291.67 and 226.23 mg/g at pH of 6.0 and 12.0. The adsorption kinetics and the equilibrium isotherms of U(VI) and Re(VII) all fitted well with the pseudo-second-order model ( R 2 >0.99) and the Freundlich model ( R 2 >0.99). The main mechanism of removal by TNTs-FeS was electrostatic attraction, chemical reduction, and surface complexation. Thus, TNTs-FeS composites exhibited a high potential to remove U(VI) and Re(VII) heavy metal ions from the surface and groundwater.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 5
·2311-2317
·
IF 1.754
Wu Tao,Geng Zilong,Feng Zhengye,Pan Guoxiang,Shen Qiang
The diffusion of Re(VII), Se(IV) and Cr(VI) in compacted Gaomiaozi bentonite was conducted by an integrated diffusion setup. The effective diffusion coefficient and the rock capacity factor of Re(VII), Se(IV) and Cr(VI) were measured. Re(VII) and Cr(VI) were excluded from the surface of bentonite particles with an accessible porosity of 0.40 and 0.23. The geometric factor decreased in a sequence of Cr(VI) < Se(IV) < Re(VII), indicating that Cr(IV) had a lower tortuosity, a larger diffusion pore diameter, and a stronger anionic exclusion effect from the surface of bentonite platelets.
研究领域:
环境科学
·
地球化学
·
材料科学
✓ 已验证
DOI
高影响因子
RADIOCHIMICA ACTA
·
2021
·Vol. 110
·期 2
·107-119
·
IF 1.44
Yuzhen Sun,Hui Zhang,Rong Hua,Mingbiao Luo,Chuan-Pin Lee,Zhifen Wang,Weigang Liu,Jie Kong,Yunfeng Shi
Tamusu area is the primary pre-selection site of clayrock disposal repository for high-level radioactive waste (HLW) in China. However, the research on the migration behavior of nuclides in Tamusu clayrock is still in its infancy. For the first time in laboratory, the diffusion behavior of Re(VII) in Tamusu clayrock core was studied by means of through-diffusion method. The effects of pH, ionic strength and humic acid on the diffusion behavior of Re(VII) in clayrock were studied. The effective diffusion coefficient, apparent diffusion coefficient and rock capacity factor value were obtained. All the experimental conditions of Re(VII) diffusion in Tamusu clayrock are compared with other geological samples under the same conditions in literature data. The diffusion mechanism of radionuclide in Tamusu clay is discussed, which can provide experimental data for site selection and safety assessment of high-level radioactive waste repository in China. The experimental results showed an effective application and reference for the countries disposed HLW in mudrocks or clayrocks, such as France, Belgium etc. in Europe. Moreover, this research can provide the original data support for the metallogenic regularity and prospecting prognosis of rare element rhenium in different geological environments.
研究领域:
环境科学
·
核废料管理
·
地质学
·
放射化学
✓ 已验证
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2017
·
IF 3.101
Tao Wu,Zhifen Wang,Hai Wang,Zhiqiang Zhang,Luc R. Van Loon
The through-diffusion method was employed to investigate the effect of the salt concentration on the diffusion behaviour of Re(VII) and Se(IV) in compacted bentonite . The accessible porosity , ε acc , of Re(VII) increased from 0.25 to 0.38 with an increase of the ionic strength from 0.1 to 1.0 mol/L. The dependency of the accessible porosity ε acc on the salt concentration could be described approximately by a first-order decay exponential function. The interlayer porosity of GMZ bentonite was 21% of the total porosity at a bulk dry density of 1600 kg/m 3 at 12 °C. The D e values of Re(VII) and Se(IV) increased from 2.6 × 10 − 11 to 6.1 × 10 − 11 m 2 /s and from 1.6 × 10 − 11 to 4.7 × 10 − 11 m 2 /s in GMZ bentonite with an increase of the ionic strength from 0.1 to 1.0 mol/L, respectively. In the case of Se(IV), the adsorption showed a different ionic strength dependency in GMZ bentonite and montmorillonite . The ionic strength has no significant effect on the adsorption (K d = 1.8 × 10 − 4 m 3 /kg) on GMZ bentonite, indicating the formation of inner-sphere surface complexes. In the case of synthetic montmorillonite, the K d values increased with increasing ionic strength. This can be explained by the fact that the electric potential of surface sites becomes less negative with increasing ionic strength resulting in an increase in the adsorption of Se(IV) at a pH above the point of zero salt effect (PZSE). The D e values of both Re(VII) and Se(IV) increased with increasing salt concentration. Both anions are totally excluded from the interlayer space and partially from the diffuse double layer. Ionic strength alters the effective diffusion coefficient of anions by controlling the thickness of the diffuse double layer. Anion diffusion data from the literature (effective and apparent diffusion coefficients) were satisfactorily evaluated by Archie's relation.
研究领域:
环境科学
·
地球化学
✓ 已验证
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2016
·
IF 2.586
Tao Wu,Zhifen Wang,Qingmei Li,Guoxiang Pan,Jinying Li,Luc R. Van Loon
In order to understand the diffusion properties of anionic radionuclides (RN) in bentonite in the presence of organic compounds with chelating and reducing properties, the effect of humic acid (HA), citrate, oxalate and formate on Re(VII) diffusion was investigated by a through-diffusion method under different pH (pH 7.0 and 10.0) and temperature conditions (10–65 °C). When the molar ratio of oxalate to Re(VII) was higher than 1:1, the accumulated mass and flux were observed to decrease drastically as a function of time. It can be explained by photocatalytic impact of Fe(III) on the reduction of Re(VII) to insoluble Re(IV) by oxalate. Thus, the diffusion of Re(VII) was also observed to decrease in the presence of minor citrate, oxalate and formate. Effective diffusion coefficient (D e ) values decreased from 8.7 × 10 − 11 m 2 /s to (5.1–5.9) × 10 − 11 m 2 /s. In contrast, HA had no significant impact on Re(VII) diffusion. The D e values of 1.54 × 10 − 11 and 6.5 × 10 − 12 m 2 /s were obtained at pH 7.0 and 10.0, respectively. HA thus neither has an effect on the speciation of Re(VII) nor does it change the charge of the surface. The latter is probably due to the fact that HA preferentially interacts with the aluminol sites of the montmorillonite edges without changing the zeta potential of the surface. The dependence of D e of Re(VII) on temperature in the absence and presence of citrate or formate was described by the Arrhenius equation . The activation energy, E a , was in the range of (20.7–25.1) kJ/mol, demonstrating that Re(VII) diffusion followed a pore water diffusion model .
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·Vol. 60
·期 33
·23438-23449
·
IF 12.2
She Jingye,Kang Mingliang,Jin Wujian,Weng Hanqin,Qin Danwen,Gu Zhixing
Reductive immobilization of 99 Tc(VII) to sparingly
soluble
TcO 2 -type phases is a key process limiting 99 Tc transport in the environment. However, the reactivity of natural
pyrite toward 99 Tc(VII) under conditions relevant to nuclear
waste repositories remains poorly understood. Here, we investigate
the interactions of 99 Tc(VII) and its nonradioactive congener
Re(VII) with natural pyrite under γ-irradiation (0–100
kGy; 0–100 Gy/min). In the absence of γ-irradiation,
natural pyrite exhibited limited reactivity toward 99 Tc(VII)
at circumneutral to alkaline pH over the investigated time scales.
Under γ-irradiation, however, pyrite-mediated reductive sequestration
of both Tc(VII) and Re(VII) was substantially enhanced, producing
a TcO 2 /TcO x -TcS x mixture and ReO 2 as dominant reduction
products. Mechanistic analyses indicate that radiolytically generated
hydrated electrons (e aq – ) and hydrogen
radicals (·H) directly reduce TcO 4 – and ReO 4 – , while pyrite and dissolved
Fe 2+ scavenge hydroxyl radicals (·OH) and sustain
a reducing interfacial environment. Under acidic conditions, protonation
of e aq – to ·H limits Tc(VII)/Re(VII)
reduction efficiency. At higher pH, OH – suppresses
intermediate disproportionation, promoting efficient stepwise reduction
via consecutive one-electron transfer from e aq – . These findings demonstrate that γ-irradiation fundamentally
alters the redox reactivity of natural pyrite and promotes radionuclide
immobilization under nuclear waste repository conditions, providing
critical constraints for predicting long-term radionuclide transport
in deep geological disposal systems.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zuzhuo Zhang,Zhongliang Li,Jian Wang,Xiaoli Wang,Jianrui Wu,Tong Wang,Haifeng Zou,Yanhua Song,Wenfu Yan
Efficient removal of pertechnetate ( 99 TcO 4 − ) from nuclear wastewater is crucial for environmental protection and long-term waste management. However, many existing adsorbents suffer from exhibiting limited selectivity and insufficient chemical or radiation stability under the harsh conditions typical of nuclear effluents. Here, we report a series of pyridinium and methylpyridium-functionalized anion exchange resins (PMCl-Py 0 , PMCl-Py 2 , and PMCl-Py 3 ) for the selective capture of ReO 4 − as a non-radioactive analogue of 99 TcO 4 − . These resins show high adsorption capacities for Re(VII) across a broad pH range (2−12) at 25 °C, reaching 701.92, 567.63, and 652.02 mg·g −1 for PMCl-Py 0 , PMCl-Py 2 , and PMCl-Py 3 , respectively. They also exhibit excellent chemical and radiation resistance, with negligible loss of Re(VII) uptake after exposure to 2 M HNO 3 , 5 M HCl, 5 M NaOH, 20% H 2 O 2 , or β/γ irradiation up to 200 kGy. Importantly, the resins present excellent selectivity. Even at ReO 4 − :NO 3 − or ReO 4 − :SO 4 2− molar ratios of 1:1000, PMCl-Py 3 retains high removal efficiencies of 63.48% and 97.81%, respectively, outperforming the commercial nuclear-grade resin ZGANR170. In simulated Hanford low-activity waste, PMCl-Py 3 achieves 95.87% removal of ReO 4 − . Dynamic adsorption experiments indicate that PMCl-Py 3 has a favorable industrial application prospect (dynamic adsorption capacity 545.94 mg·g −1 ). Spectroscopic analysis and DFT calculations indicate that the adsorption process is achieved through a synergistic mechanism of N + electrostatic attraction and C-H⋯O/Cl − hydrogen bonds. Owing to their outstanding adsorption performance, these pyridinium-based anion exchange resins are promising candidates for the practical remediation of 99 Tc-contaminated nuclear wastewater.
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2016
·Vol. 311
·期 1
·655-661
·
IF 0.983
Wang Zhifen,Zhang Jianying,Chen Jiang,Zhang Zhiqiang,Zheng Qing,Li Jinying,Wu Tao
A through-diffusion method was used to investigate the Re(VII) (as a surrogate to 99 Tc(VII)) diffusion in compacted illite-, hematite- and limonite-montmorillonite mixtures. The effective diffusion coefficient D
e values were in the range of (4.29–6.71) × 10 −11 m 2 /s at pH 3.0 and (3.44–5.72) × 10 −11 m 2 /s at pH 9.0, respectively. Compared to montmorillonite, both D
e and α values enhanced at least three-folds in montmorillonite mixtures, indicating that the impurities changed the diffusion path. Interestingly, the K
d values of (0.63–3.94) × 10 −4 kg/m 3 were found in montmorillonite mixtures. However, the change of D
a value was less than two-folds, indicating that the illitization and iron corrosion of a back-fill material had no obvious influence on Re(VII) diffusion velocity.
研究领域:
环境科学
·
放射性废物管理
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2020
·Vol. 326
·期 1
·445-454
·
IF 1.137
Liu Fuping,Hua Rong,Zhang Feng,Liu Heng,Lee Chuan-Pin,Liu Hesheng,Xu Bin
A new strong base anion exchange resin (LSL-1) was synthesized by grafting trimethylamine groups onto polystyrene-divinylbenzene microspheres and used for the selective recovery of Re(VII) from U(VI)-containing effluent. The morphology and structural properties of LSL-1 were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The adsorption mechanism is discussed. In both batch and column experiments, LSL-1 showed excellent enrichment capacity for Re(VII). This study demonstrates a new approach for the separation and recovery of Re(VII) from U(VI)-containing effluent by using amino-modified polystyrene-divinylbenzene microspheres.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·Vol. 333
·期 5
·2273-2280
·
IF 1.5
Zhang Hui,Wang Ju,Wu Wangsuo,Luo Mingbao,Hua Rong,Zhou Zhichao,Ling Hui
This paper presents the first laboratory-based, simultaneous diffusion experiments of Re(VII) and Se(IV) in Tamusu (TMS) clay, using the capillary method. We determined diffusion coefficients ( D a ) and adsorption values ( K d ) for these nuclides under varying clay compaction densities, solution pH values, ionic strengths, and in the presence of humic acid (HA). The results indicated rapid acquisition of diffusion data, the D a values predominantly ranging from 10 −9 m 2 /s to 10 −10 m 2 /s, and weak adsorption for both Re(VII) and Se(IV). While the presence of HA augmented the D a and K d values for Re(VII) and Se(IV) diffusion in clay, these values did not exhibit significant alterations in response to increasing HA concentrations.
研究领域:
环境科学
·
地质学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Chuanqi Tang,Yiming Zhang,Jiangang Han,Ziqi Tian,Liang Chen,Jianqiang Chen
Supported carbon quantum dots (CQDs), used as fluorescent sensors for the detection of metal ions , have rarely been used to remove heavy metals from water. Nitrogen-doped CQDs immobilized in hydrophilic silica hydrogels exhibited a more superior sensitivity and selectivity for the detection of Re(VII) and Cr(VI) than other metal ions, including Fe(III), Fe(II), Zn(II), Cu(II) and Mn(II). For the first time, low limits of detection (LOD) of 2.3 μM for Re(VII) detection and 65 nM for Cr(VI) detection were reported by a facile method. Based on the high selectivity of fluorescent silica hydrogels for Re(VII) and Cr(VI) detection, the removal of Re(VII) and Cr(VI) by graphene oxide (GO) in water was monitored with the hydrogels used as a turn-off fluorescent sensing platform. The consistent results of the sorption isotherms of each metal on GO, which were obtained from the fluorescence spectra and by UV absorption, further verified the possibility of monitoring metal removal by fluorescence detection. Remarkably, GO removed 1186 mg/g of Re(VII) but only 178 mg/g of Cr(VI). The density functional theory (DFT) calculations indicated that both Re(VII) and Cr(VI) formed stable bonds with silica hydrogels, confirming that the interactions between the metal ions and the substrate would promote the fluorescence quenching of the supported CQDs. On the other hand, Re(VII) interacted more strongly with the carboxyl groups of GO than Cr(VI). In addition, a real-time detection system was designed to alarm the service life of a GO filter used for Re(VII) removal.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Mu Ding,Lang Chen,Yuwei Xu,Bo Chen,Jie Ding,Rulei Wu,Chao Huang,Yi He,Yongdong Jin,Chuanqin Xia
99 Tc is a β-emitting radionuclide with high fission yield, long half-time and it is urgent to remove Tc from liquid radioactive waste due to its potential toxicity for human. Herein, we presented a viologen-based cationic organic polymer (VBCOP) as a novel adsorbent with cationic sites and functional groups for efficient capture of Re/Tc(VII, IV) from aqueous medium. The results showed that this material could rapidly remove TcO 4 − /ReO 4 − from aqueous solution within 5 min and the maximum sorption capacity for Re(VII) could reach up to 444 mg g −1 , and the distribution coefficient ( K d ) towards Re(VII) and Tc(VII) reached 4.0 × 10 5 and 7.2 × 10 5 mL g −1 , respectively. And more, the adsorption mechanism was also studied by X-ray photoelectron spectroscopy (XPS), Energy dispersive spectrometer (EDS) mapping and Ion chromatography (IC), the results suggested an ion-exchange process in which the Cl − in this material was replaced by ReO 4 − . Additionally, we investigated its adsorption mechanism towards low-valent Re which was prepared by reducing ReO 4 − with NaBH 4 , and the flexible tetraaza macrocycle introduced in the material chelated with Re(IV) was confirmed by X-ray photoelectron spectroscopy (XPS) and Extended X-ray absorption fine structure (EXAFS) analysis. In general, the research exhibits a new sorbent material that can remove both TcO 4 − /ReO 4 − and the low-valent Tc/Re, and provide a new strategy to treat radioactive waste containing Tc with different valences.
研究领域:
放射化学
·
环境科学
✓ 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）