INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Rongzhen Xie,Nannan Shen,Xijian Chen,Jie Li,Yaxing Wang,Chao Zhang,Chengliang Xiao,Zhifang Chai,Shuao Wang
99Tc is one of the most abundant radiotoxic isotopes in used nuclear fuel with a high fission yield and a long half-life. Effective removal of pertechnetate (TcO4–) from an aqueous solution is important for nuclear waste separation and remediation. Herein, we report a series of facilely obtained benzene-linked guanidiniums that could precipitate TcO4– and its nonradioactive surrogate ReO4– from a high-concentration acidic solution through self-assembly crystallization. The resulting perrhenate and pertechnetate solids exhibit exceptionally low aqueous solubility. The benzene-linked guanidiniums hold one of the highest TcO4– removal capacities (1279 mg g–1) among previously reported materials and possess a removal percentage of 59% for ReO4– in the presence of Cl– over 50 times. The crystallization mechanism was clearly illustrated by the single-crystal structures and density functional theory calculations, indicating that TcO4– is captured through a charge-assisted hydrogen bonding interaction and stabilized by π–π stacking layers. In addition, the removal process is easily recycled and no toxic organic reagents are introduced. This work provides a green approach to preliminarily separate TcO4– from high-level nuclear wastes.
研究领域:
化学
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环境科学
·
核能工程
✓ 已验证
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yawen Cai,Jinghua Feng,Xiaoli Tan,Xin Wang,Zhimin Lv,Weiwei Chen,Ming Fang,Haining Liu,Xiangke Wang
The efficient decontamination of pertechnetate ( 99 TcO 4 − ) is an essential task for managing radioactive 99 Tc in nuclear wastes . Perrhenate, (ReO 4 − ), as a nonradioactive analog, exhibits almost identical physicochemical properties as 99 TcO 4 − . Herein, a novel magnetic amine-functionalized MIL-101(Cr) (NH 2 -MIL-101(Cr)@Fe 3 O 4 ) was prepared and used to efficiently remove ReO 4 − from solution for the facile magnetic separation. A series of environmental parameters were considered to investigate the adsorption performance of NH 2 -MIL-101(Cr)@Fe 3 O 4 . Experimental results suggested that NH 2 -MIL-101(Cr)@Fe 3 O 4 has reached a satisfied adsorption capacity (~401 mg/g) and a very fast adsorption kinetics at pH 7.0. The selectivity for ReO 4 − was maintained even in the presence of interfering anions with relatively high concentrations. ReO 4 − were mainly captured by N-donor sites of the surface-decorated amine via complexation and were trapped in the cavities of modified MIL-101(Cr). NH 2 -MIL-101(Cr)@Fe 3 O 4 exhibits satisfactory adsorption performance for ReO 4 − and can be conveniently separated from wastewaters after adsorption.
研究领域:
环境科学
·
材料科学
·
放射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xuemei Wei,Xiankui Cheng,Xinyu Zhang,Guodong Sheng,Huiting Xu
The utilization of biocompatible and inexpensive adsorbents for the effective scavenging of U(VI) and Eu(III) from wastewater is still an open challenge in nuclear waste management. Herein, three kinds of α-Fe 2 O 3 nanocrystals with different morphologies, i.e., α-Fe 2 O 3 nanospheres (HNSs), nanoplates (HNPs) and nanorods (HNRs), which were exposed (1 0 2), (0 0 1), and (1 1 0) facet, respectively, was used to scavenge U(VI) and Eu(III) from aqueous solutions via an adsorption procedure. Various techniques of N 2 adsorption–desorption, FT-IR, XRD, XPS, TEM, SEM and EDS were applied to characterize these adsorbents before or after adsorption. The results indicated that the adsorption capacity of U(VI) and Eu(III) was in the order of HNPs (0 0 1) > HNRs (1 1 0) > HNSs (1 0 2), namely, α-Fe 2 O 3 nanoplates was proved to be a good adsorbents, with removal capacity of 221 mg/g and 131 mg/g for U(VI) and Eu(III) scavenged on HNPs, respectively. The kinetics of U(VI) and Eu(III) scavenging agreed with the pseudo second order kinetic model, suggesting that chemical interaction is mainly responsible for U(VI) and Eu(III) scavenging on these materials. Furthermore, the Freundlich model fit the best for adsorption isotherms of U(VI) and Eu(III). The present study demonstrated that these α-Fe 2 O 3 nanocrystals are promising materials in nuclear waste management.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Linshuai Liu,Nannan Wang,Chunlin He,Yuezhou Wei,Jingjing Wang,Xinpeng Wang
Considering the unexpected nuclear power waste emission and potential nuclear leakage, the exploration of robust materials for the effective capture and storage of radioactive iodine is of great importance but still remains a challenge. In this work, we report the rational synthesis of functionalized NH 2 -UiO-66-on-ZIF-67 architecture to enhance the static adsorption and retention of volatile iodine. Such MOF-on-MOF heterostructures was fabricated through seeding ZIF-67 core on the surface of NH 2 -UiO-66 satellite via a facile polyvinylpyrrolidone (PVP) regulated internal extended growth strategies. NH 2 -UiO-66-on-ZIF-67 exhibited unique core-satellite structure, which significantly promotes the binding interactions with iodine through synergizing of the N-rich imidazole moieties and surface functionalized amino groups within the porosity channels. As a result, the as fabricated NH 2 -UiO-66-on-ZIF-67 achieves enhanced mass diffusion and high capture capacity of 3600 mg/g for iodine vapor under static sorption conditions. Moreover, water vapor in humid conditions (relative humidity of 18 %) has almost no effect on the static iodine adsorption performance of the material. This study sheds light on a reliable MOF-on-MOF hybrid strategy for effective radioiodine treatment to ensure the safety nuclear waste management.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiaoyang Liu,Na Zhang,Zhen Dong,Jifu Du,Lifang Peng,Long Zhao,Miao Yang
Technetium ( 99 Tc) is a main long-lived radionuclide of nuclear waste, which poses a great threat to the environment and human health. The reasonable disposal of 99 Tc is vital important. In this paper, a series of novel materials (SMILR m , m = 0, 1/500, 1/200, m is the molar ratio of IL to RAFT reagent) was synthesized by radiation-induced grafting combined with reversible addition-fragmentation chain transfer (RAFT) polymerization. The adsorption performance of SMILR m to 99 Tc were investigated. The graft polymerization process is controlled by the RAFT reagent, resulting in a restricted dispersion of SMILR m molecular weight. With the increase of RAFT reagent content, the grafting yield (GY) decreased. The addition of RAFT reagent increases the specific surface area of the adsorbent, accelerates the adsorption rate, increases the adsorption capacity, but reduces the adsorption selectivity. Especially, the adsorption of SMILR 0 was a single step adsorption and obeyed Langmuir adsorption model, while SMILR m (1/500, 1/200) showed a stepwise adsorption isotherm model. SMILR m exhibited excellent recyclability and could efficiently capture Re O 4 - from a simulated Beishan groundwater in dynamic experiments. Finally, XPS and FT-IR analysis confirmed that the adsorption was an ion exchange mechanism. The results showed that SMILR m are suitable for the effective removal of Re O 4 - / T c O 4 - from radioactive wastewater with complex composition.
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
JOURNAL OF NUCLEAR MATERIALS
·
2021
·
IF 2.936
Jing Wang,Chenchen Niu,Kaiwen Hu,Xiujian Zhao,Kai Xu
Rhenium (Re), a non-radioactive surrogate for technetium (Tc), was incorporated into the lattice of SnO 2 by reductive co-precipitation process at room temperature, and Re volatility from Re(SnO 2 ) under different conditions (in air and N 2 and with glass frit) at elevated temperatures was carefully investigated. Re began to evaporate from Re(SnO 2 ) both in air and N 2 at 400 °C, while Re exhibited a faster volatilization in air than in N 2 , as all Re was gone at 1200 °C in air, but ∼40% of Re still remained at 1200 °C in N 2 . Additionally, Re did not volatilize from Re(SnO 2 )-containing glass frit until 800 °C and only ∼15% of Re volatilized at 1200 °C, suggesting the loss of Re decreased by ∼30% points through incorporation of Re into SnO 2 before vitrification. The analysis of Re valence transition revealed that the reduced Re 4+ was easily oxidized to volatile Re 7+ in air, but in N 2 , Re 4+ disproportionated to form Re 7+ and the lower valence states of Re at temperatures from 600 °C to 1000 °C. In Re(SnO 2 )-containing glass frit, the formation of NaReO 4 during vitrification inhibited Re 7+ volatilization before 800 °C, while the presence of Re 4+ in the glass melt enhanced Re retention at temperature above 800 °C.
研究领域:
材料科学
·
核化学
·
环境科学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2015
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IF 2.605
Xirui Lu,Long Fan,Xiaoyan Shu,Sijin Su,Yi Ding,Facheng Yi
(Gd 1− x Nd x ) 2 (Zr 1− x Ce x ) 2 O 7 (0≤ x ≤1.0) ceramics were synthesized to investigate the co-doping effects on the phase evolution and chemical durability of Gd 2 Zr 2 O 7 based nuclear waste forms. The phase structures of these solid solutions were identified by X-ray diffraction and their chemical durability was evaluated by static leach test (Materials Characterization Center, MCC-1). The results show that the Gd 2 Zr 2 O 7 ceramic adopts a pyrochlore structure while the co-doped (Gd 1− x Nd x ) 2 (Zr 1− x Ce x ) 2 O 7 (0.2≤ x ≤1.0) compositions exhibit a defect fluorite structure. Moreover, the normalized release rates of each element in (Gd 1− x Nd x ) 2 (Zr 1− x Ce x ) 2 O 7 (0≤ x ≤1.0) waste forms increase with the growing temperature and converge to constant values with enhanced leaching time. In the discussed time range (42 days), all the considered elements show a normalized release rate lower than 10 −4 g m −2 d −1 . Gd shows the highest normalized release rate of all the involved elements, while Zr shows the best chemical durability.
研究领域:
材料科学
·
核能工程
✓ 已验证
DOI
高影响因子
RADIOCHIMICA ACTA
·
2022
·
IF 2.083
Lei Li,Ran Ma,Xuewei Liu,Tao Wen,Bo Wu,Mingtai Sun,Zheng Jiang,Suhua Wang,Xiangke Wang
Inorganic ion-exchange materials show potential application for toxic radioactive ions due to their remarkable high efficiency and selectivity features. Here, two type of carbon-supported titanate (C@TNFs and C@TNFs(H)) nanofibers have been synthesized by a cost-effective in suit growth method. The resulting C@TNFs and C@TNFs(H) microspheres present uniform flower-like morphology and large surface area. The interlayer Na + in the titanate shell provides docking sites for ion-exchange of radioactive ions (U(VI), Ba(II), and Sr(II)). Interestingly, the exceeding theoretical cation-exchange capacities (CECs) are achieved on C@TNFs for U(VI) ∼4.76 meq g −1 and Ba(II) ∼2.65 meq g −1 and C@TNFs(H) for Ba(II) ∼2.53 meq g −1 and Sr(II) ∼2.24 meq g −1 , respectively. The impressive adsorption performance is mainly attributed to the synergistic effects of ion-exchange and surface complexation. More significantly, C@TNFs and C@TNFs(H) maintain high distribution coefficients ( K
d
U ) of >104 mL g −1 over a wider pH range (pH = 3.5–9.0) and high adsorption rate with short equilibrium time within 50 min. Competitive ion-exchange investigation shows a selectivity order of U(VI) > Ba(II) > Sr(II) at individual 10 ppm concentration, pH = 6.0 and T = 298 K. The related spectroscopic studies reveal the intercalative mechanism of radionuclides in the deformed titanate structure, as a result of target ions firmly trapped in the interlayer of C@TNFs and C@TNFs(H). These advantageous features allow the C@TNFs and C@TNFs(H) to be promising candidates for the remediation of toxic radioactive ions polluted water.
研究领域:
材料科学
·
环境科学
·
放射化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xilin Gao,Anting Ding,Yuxin Li,Chuanying Liu,Chengliang Xiao
Efficient utilization of uranium resources and minimization of nuclear waste are critical challenges for the sustainable development of nuclear energy. The separation of actinides (An) from lanthanides (Ln) is essential to reduce the impact of neutron poisons and enhance the efficiency of Partitioning & Transmutation (P&T) processes. In this study, we propose the use of a concentrated AlCl 3 solution as a selective leaching agent to separate Ln from An in spent nuclear fuel (SNF). At a mass ratio of 1:15, the AlCl 3 solution effectively dissolves nearly 100 % of lanthanide oxides from simulated SNF at 75 °C, while the coexisting actinide oxides remain largely insoluble. The high separation factors between Ln 2 O 3 and AnO 2 (average of 1630 for Ln/U and 490 for Ln/Th) provide a novel and efficient approach for the selective separation of lanthanides from SNF. The lanthanides are subsequently recovered through oxalic acid precipitation and calcination to produce Ln 2 O 3 . Based on our characterization results, the primary driving force for the dissolution of Ln 2 O 3 is the acidity of the H 2 O-AlCl 3 system, with the lattice energies of oxides identified as the key factor affecting the differential dissolution of Ln(III) and U/Th with higher valent under identical conditions. This selective dissolution and separation process using AlCl 3 solution presents a highly efficient method for the removal of lanthanides from SNF and improves the utilization of nuclear fission products. With its mild operating conditions and reduced environmental impact, this method offers a promising approach for the recovery of rare earth elements from nuclear waste and other secondary resources.
研究领域:
核化学与放射化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Yonghao Wang,Biao Chi,Chengliang Xiao,Dagui Chen,Yongjing Wang,Minghua Liu
In this work, a layered nanocomposite with a superior adsorption ability has been designed and prepared for the preconcentration of Eu(III), a chemical analogue of trivalent lanthanides [Ln(III)] and actinides [An(III)] in nuclear waste. This nanocomposite was obtained by fabricating magnesium silicate (MgSi) of the Talc-phase Mg 3 Si 4 O 9 (OH) 10 on graphene oxide (GO) nanosheets, in which the GO matrix can effectively avoid the agglomeration of MgSi. A hierarchical structure of GO@MgSi with interwoven nano-sized MgSi lamellae dispersedly standing on the surface of GO was observed by scanning electron microscope (SEM) and transmission electron microscopy (TEM). Such a hierarchical structure effectively increases the surface area of MgSi, leading to up to date the highest adsorption capacity (344.82 mg·L −1 ) for enriching Eu(III). Powder X-ray diffraction pattern (PXRD) of Mg 3 Si 4 O 9 (OH) 10 shows that the (0 2 0) and (2 0 0) diffraction peaks disappear after the adsorption of Eu(III), indicating structural changes in MgSi lamellae after adsorption. The infrared absorption spectra (IR) and X-ray photoelectron spectroscopy (XPS) measurements confirm the structural transformations in the Si O tetrahedral and Mg OH octahedral sheet in MgSi, suggesting that MgSi lamella rather than GO sheet might play a dominant role during the adsorption process. The superior adsorption behaviors of GO@MgSi indicate that it is a highly promising and efficient candidate for Eu(III) preconcentration in aqueous solution.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2020
·
IF 4.495
Zhangyi Huang,Qiuyao Li,Yutong Zhang,Junjing Duan,Haomin Wang,Zhe Tang,Yao Yang,Jianqi Qi,Tiecheng Lu
A nitrate–citrate combustion method combined with microwave sintering was firstly employed for the rapid fabrication of the Gd 2 Zr 2 O 7 matrix immobilizing various amounts of simulated nuclear wastes . Phase evolutions, microstructure changes, element distributions, densification processes and mechanical properties of the as-prepared (1 – x )Gd 2 Zr 2 O 7 · x TRPO (0.0 ≤ x ≤ 0.6) at various temperatures were investigated. Compared to the reported studies, we have increased the immobilization amount of simulated TRPO waste within a crystal structure from 45 to 60 wt%. T d and T g (the threshold temperatures to trigger accelerated densification and grain growth, respectively) were employed to divide the densification process into three stages. the mechanical properties and the densification stages of the (1 – x )Gd 2 Zr 2 O 7 · x TRPO (0.0 ≤ x ≤ 0.6) ceramics sintered under microwave sintering at various temperatures were finally determined. Fine-grained (1 – x )Gd 2 Zr 2 O 7 · x TRPO (0.0 ≤ x ≤ 0.6) ceramic waste forms with average grain size less than 200 nm and relative density higher than 90% can be obtained by microwave sintering at sintering temperature less than 1400 °C.
研究领域:
材料科学
·
核废料管理
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Jian Wang,Congcong Wang,Hongchao Wang,Bo Jin,Peiping Zhang,Lina Li,Shiding Miao
The effective capture of radioactive volatile iodine ( 131 I and 129 I) from nuclear waste stream is of vital significance. In this work three kinds of porous organic frameworks (POFs) knitting with N -containing building units were constructed via cost-effective and maneuverable Scholl reaction. The obtained PAFs exhibited moderate porosity and satisfying thermal stability. With coexistence of open porous structure, the electron-rich amino group featured with π-π interactions was found to improve the affinity to iodine, and the iodine uptake capacities were 408 wt%, 335 wt% and 268 wt% when the prepared POFs of P-DPDA, P-TPB and P-PC were employed for the adsorption experiments. The results were superior to most of the porous adsorbents including zeolite , metal-organic frameworks (MOFs) and porous organic polymers (POPs). Iodine adsorption capacities of 289.50 mg g −1 (for P-DPDA), 194.63 mg g −1 (for P-TPB) and 259.69 mg g −1 (for P-PC) in organic solution were achieved, and the adsorbed iodine molecules could be released to ethanol. Such promising and cost-effective materials can be envisaged for application in the field of nuclear waste management.
研究领域:
材料科学
·
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）