RSC Advances
·
2023
·Vol. 13
·期 10
·6346-6355
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IF 3.9
Lina Wu,Huiping Wang,Xiangqian Kong,Haibo Wei,Sheng Chen,Lisheng Chi
Effective removal of strontium isotopes in radioactive waste streams has important implications for the environment and the sustainable development of nuclear energy. In this work, a zirconium phosphate/18-crown-ether-6 (ZrP/18C6) composite was prepared using the intercalation method by loading crown ether into zirconium phosphate. The composite was structurally and morphologically characterized by XRD, FT-IR, XPS, and SEM. The adsorption experiments of Sr2+ onto the ZrP/18C6 composite were conducted as a function of temperature, pH, Sr2+ concentration and competing ions. The results indicate ZrP/18C6 can adsorb 98.6% of Sr2+ within 30 minutes at an Sr2+ concentration of 100 mg L−1 and maintain a high removal rate with a distribution coefficient of 7 × 105 mL g−1 when Sr2+ is at a low level of 4.28 mg L−1. The ZrP/18C6 composite reached a maximum adsorption capacity of 195.74 mg g−1 at an Sr2+ concentration of 380 mg L−1, which is significantly higher than the 43.03 mg g−1 of α-ZrP. The adsorption performance of Sr2+ onto ZrP/18C6 is not significantly affected by temperature, pH and competing ions. Furthermore, the adsorption kinetics and thermodynamics were analyzed based on the adsorption data obtained in the present work. It is shown that the adsorption of Sr2+ onto ZrP/18C6 follows the pseudo-second-order model and the Langmuir monolayer model, respectively. Additionally, the adsorption mechanism of Sr2+ by ZrP/18C6 is discussed.
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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DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 12
·2908
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IF 4.2
Yudong Xie,Xiaowei Wang,Jinfeng Men,Min Zhu,Chengqiang Liang,Hao Ding,Zhihui Du,Ping Bao,Zhilin Hu
The efficient segregation of radioactive nuclides from low-level radioactive liquid waste (LLRW) is paramount for nuclear emergency protocols and waste minimization. Here, we synthesized Na3FePO4CO3(NFPC) via a one-pot hydrothermal method and applied it for the first time to the selective separation of Sr2+from simulated LLRW. Static adsorption experimental results indicated that the distribution coefficientKdremained above 5000 mL·g−1, even when the concentration of interfering ions was more than 40 times that of Sr2+. Furthermore, the removal efficiency of Sr2+showed no significant change within the pH range of 4 to 9. The adsorption of Sr2+fitted the pseudo-second-order kinetic model and the Langmuir isotherm model, with an equilibrium time of 36 min and a maximum adsorption capacity of 99.6 mg·g−1. Notably, the adsorption capacity was observed to increment marginally with an elevation in temperature. Characterization analyses and density functional theory (DFT) calculations elucidated the adsorption mechanism, demonstrating that Sr2+initially engaged in an ion exchange reaction with Na+. Subsequently, Sr2+coordinated with four oxygen atoms on the NFPC (100) facet, establishing a robust Sr-O bond via orbital hybridization.
研究领域:
环境科学
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核化学
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理论化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
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IF 5.774
Sen Yang,Meiyun Xu,Jia Yin,Tongxin Zhao,Chengqi Li,Daoben Hua
Recovery of uranium from highly saline radioactive effluents is strategically important both for environmental concerns and sustainable development of nuclear energy. However, high-efficiency extraction of uranium from highly saline low-level liquid wastes (SLLWs) remains challenges of slow rate, poor selectivity and complicated regeneration. In this work, we report a strategy for highly selective separation and facile recovery for uranium from SLLWs by thermal-responsive uranyl ion-imprinted magnetic microspheres (UIMM). The adsorbent showed better selectivity for uranium against other cations compared with non-imprinted magnetic microspheres (NIMM), and the adsorbent has good salt resistance. Moreover, the adsorption equilibrium of UIMM could be achieved within 10 min, and the maximum uptake capacities are 122.7 mg/g and 231.5 mg/g at 298.15 K and 305.15 K, respectively. Importantly, highly efficient elution can be attained facilely via changing the temperature of elution, which can avoid secondary pollutants caused by the use of a large number of eluents. And the magnetic separation of the adsorbent can greatly improve its practical performance. XPS spectra indicate that uranium(VI) is partly reduced to a lower uranium(IV) state by Fe 2+ on the Fe 3 O 4 surface besides being adsorbed on the materials by phosphonic acid and N -isopropylacrylamide.
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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产品关联
DOI
高影响因子
Nanomaterials
·
2025
·Vol. 15
·期 10
·714
·
IF 4.3
Junli Wang,Chen Luo,Wentao Wang,Hui Wang,Yao Liu,Jianwei Li,Taihong Yan
The separation of palladium from radioactive waste streams represents a critical aspect of the secure handling and disposal of such hazardous materials. Palladium, in addition to its radioactive nature, holds intrinsic value as a resource. Despite the urgency, prevailing adsorbents fall short in their ability to effectively separate palladium under highly acidic environments. To surmount this challenge, our research has pioneered the development of 1,3,5-tris(4-aminophenyl)benzene-2,5-Bis(methylthio)terephthalaldehyde COF (TAPB-BMTTPA-COF), a novel material distinguished by its remarkable stability and an abundance of sulfur-containing functional groups. Leveraging the pronounced affinity of the soft ligands’ nitrogen and sulfur within its molecular architecture, TAPB-BMTTPA-COF demonstrates an exceptional capability for the selective adsorption of palladium. Empirical evidence underscores the material’s swift adsorption kinetics, with equilibrium achieved in as little as ten minutes, and its broad tolerance to varying acidity levels ranging from 0.1 to 3 M HNO3. Furthermore, TAPB-BMTTPA-COF boasts an impressive adsorption capacity, peaking at 343.6 mg/g, coupled with high selectivity in 13 interfering ions’ environment and the ability to be regenerated, making it a sustainable solution. Comprehensive analyses, including Fourier Transform Infrared Spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS), alongside Density Functional Theory (DFT) calculations, have corroborated the pivotal role played by densely packed nitrogen and sulfur active sites within the framework. These sites exhibit a robust affinity for Pd(II), which is the cornerstone of the material’s outstanding adsorption efficacy. The outcomes of this research underscore the immense potential of COFs endowed with resilient linkers and precisely engineered functional groups. Such COFs can adeptly capture metal ions with high selectivity, even in the face of severe environmental conditions, thereby paving the way for the more effective and environmentally responsible management of radioactive waste.
研究领域:
化学工程
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环境科学
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核能技术
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 48
·27320-27331
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IF 12.732
Pengcheng Wu,Hui Liu,Mengqi Sun,Yaxin Zeng,Jiawei Ye,Song Qin,Yimin Cai,Wen Feng,Lihua Yuan
Efficient palladium recovery from high level liquid wastes (HLLW) is of increasing priority for sustainable development and addressing issues in radioactive waste treatment. However, searching for robust materials for palladium sorption, in the presence of large amounts of competing ions even at rather high acidity still poses a great challenge. Herein we present two novel cationic covalent triazine frameworks (denoted as CTF-S and CTF-L) created by polymerization of monomers IL-S and IL-L for palladium recovery. The resultant CTF-S and CTF-L with respective surface areas of 212.9 m2 g−1 and 342.5 m2 g−1 exhibit excellent sorption ability toward palladium at high acidity. This has been demonstrated by a maximum sorption capacity of 333 mg g−1, which is the highest at 3 M HNO3 among all porous adsorbents reported so far. More importantly, these materials reveal remarkable selectivity toward palladium over other metal ions that are co-existing in simulated HLLW. In addition, thanks to the relatively large π-conjugated structures, no obvious decrease in sorption capability was observed after being exposed to 1000 kGy γ irradiation. Desorption could be easily achieved by a single contact with a mixed solution of 1 M thiourea and 1 M HCl and the sorption performance still remains at the initial level without conspicuous loss after five cycles. The XPS results, anion competitive experiments, and DFT calculations propose a sorption mechanism in which the anion exchange between anionic Pd complexes and chloride, and the chemical coordination between triazine N and Pd(II) work coorperatively to enhance the sorption capacity. This work not only provides a new kind of excellent adsorbent for selective palladium recovery, but also demonstrates a promising approach for constructing robust materials for nuclear waste remediation.
研究领域:
材料科学
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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
Journal of Water Process Engineering
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2023
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IF 7
Fuqiu Ma,Wenmin Zhu,Wanting Cheng,Jiaqi Chen,Jianzhang Gao,Yun Xue,Yongde Yan
In this study, the electrosorption property of potassium hydroxide modified activated carbon fiber felt (ACFF-KOH) to Co 2+ in simulated radioactive effluent was evaluated. Factors influencing the electrosorption such as applied voltage, initial concentration, pH, cyclic flow rate, competitive ions and cycle numbers on Co 2+ removal rate were investigated. Kinetic models and isotherm models were used to evaluate the electrosorption performance of ACFF-KOH. The results showed that the voltage enhanced the removal capacity of Co 2+ , which raised from 5.92 to 14.80 mg·g −1 when the applied voltage increased from 0 to 1.6 V. Higher initial concentration of the solution induced larger electrosorption capacity. In addition, the optimal adsorption pH of the electrosorption was around 5. When competing ions exist, the removal rate of Co 2+ decreased. Furthermore, ACFF-KOH had excellent cycling performance, and the removal rate remained above 85 % after 6 cycles. The pseudo-first-order (PFO) model fitted the data better than the pseudo-second-order (PSO) model, indicating that physisorption was the rate-limiting step during the eletrosorption process. A s the Langmuir isotherm had a higher regression coefficient (0.9983) than the Freundlich isotherm, monolayer adsorption was the main adsorption mechanism for Co 2+ on the ACFF-KOH electrode. The BET results showed that KOH modification improved the pore parameters of ACFF. According to the XPS and XRD results, Co(OH) 2 precipitates were generated on the electrode surface after electrosorption. The above results indicated that ACFF-KOH had excellent electrosorption and regeneration performance for Co 2+ in aqueous solution, thus it has great application value in the treatment of cobalt-containing radioactive effluent.
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
Advanced Science
·
2021
·Vol. 8
·期 7
·2002717
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IF 16.806
Tong Wu,Zhe Wang,Yuexiang Lu,Shuang Liu,Hongpeng Li,Gang Ye,Jing Chen
Graphene oxide (GO) membranes with unique nanolayer structure have demonstrated excellent separation capability based on their size-selective effect, but there are few reports on achieving ion–ion separation, because it is difficult to inhibit the swelling effect of GO nano sheets as well as to precisely control the interlayer spacing d to a specific value between the sizes of different metal ions. Here, selective separation of uranium from acidic radioactive waste containing multication is achieved through a precise dual-adjustment strategy on d . It is found that GO swelling is greatly restricted in highly acidic solution due to protonation effect. Then the interlayer spacing is further precisely reduced to below the diameter of uranyl ion by increasing the oxidation degree of GO. Sieving uranyl ions from other nuclide ions is successfully realized in pH =3–3 mol L −1 nitric acid solutions.
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
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Zeqian Zhang,Pengcheng Wu,Jiayi Liu,Qing Li,Liancheng Hu,Yida Wu,Qiongying Kong,Xiangyang Yuan,Xiaowei Li,Yimin Cai,Lihua Yuan,Wen Feng
Palladium (Pd) capture from high-level liquid waste for subsequent photocatalytic applications is desirable for the development of nuclear energy and the reutilization of valuable resources. Herein, we approach our design with a unique porous organic polymer containing thiazolo[5,4-d]thiazole units (denoted as TzPOP–OH). It possesses two potential soft–hard (N–O and S–O) combined coordination sites for Pd(II) coordination and features strong donor–acceptor repeating units and high planarity of linkage enforced by hydrogen bonds for subsequent photocatalysis. Accordingly, TzPOP–OH with three hydroxyl groups on the linkage exhibits a high Pd(II) capacity of 369 mg g–1 at 3 M HNO3, considerably surpassing those of the controlled polymer TzPOP without hydroxyl groups and most other reported materials. Additionally, TzPOP–OH boasts other merits, including outstanding acid tolerance, extraordinary radiation stability, good reusability, and remarkable selectivity. After palladium adsorption, Pd@TzPOP–OH demonstrates impressive photodegradation efficiency to reduce the concentration of rhodamine B in contaminated urban water from 10 to less than 0.1 ppm. This work provides a feasible approach to designing materials with both suitable coordination microenvironments and semiconductor properties for metal separation and photocatalysis.
研究领域:
材料科学
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环境科学
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核能技术
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 19
·8660-8666
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IF 2.7
Deyan Yu,Baole Li,Zhi Cao,Qi Chen,Chen Zuo,Tiansheng He,Taihong Yan,Weifang Zheng
The 5 wt% Ru/AC catalysts were prepared using the impregnation method. The catalysts were characterized by N2 physical adsorption, XRD, SEM, EDX, TEM and ICP-AES. The catalytic activity and stability of the catalysts in decomposing hydroxylamine nitrate (HAN) and hydrazine nitrate (HN) in nitric acid were evaluated. The results demonstrated that the Ru/AC catalyst effectively decomposed HAN and HN with complete conversion under moderate reaction conditions (60–90 °C). When used for an extended duration of 1580 hours in radioactive nitric acid waste liquid, this catalyst displayed a remarkable processing capacity of 6.32 kilograms per gram of catalyst. Due to its environmentally friendly nature resulting from harmless gas product formation along with its simple device structure design, this protocol offers practicality and economic attractiveness.
研究领域:
环境科学
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化学工程
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核能技术
✓ 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）