SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Fuhai Li,Yun Shang,Zuoming Ding,Hanqin Weng,Jiaxin Xiao,Mingzhang Lin
The extraction and separation of platinum group metals (PGMs) from HLLW is of great value for resource recycling and the running of reprocessing plants. In this paper, the photochemical method was proposed to extract and separate PGMs (Pd, Ru) from simulated high level liquid wastes (HLLW). Pd and Ru metal were extracted from aqueous solution by photoreduction with high efficiency (reduction ratio >90%) in the presence of alcohols, which was confirmed by UV–vis spectroscopy, XRD, XPS and TEM analysis. The effects of various parameters such as exposure wavelength, reducing agents, Cl − and pH value were investigated to optimize the photoreaction. The highly efficient extraction and separation of Pd or/and Ru metal from their mixture with lanthanide (Nd) by selective photoreduction was realized. The results suggest that the photochemical method is a promising method for the efficient extraction and separation of PGMs from HLLW.
研究领域:
化学
·
核能工程
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Hanqin Weng,Yi Wang,Fuhai Li,Yusa Muroya,Shinichi Yamashita,Sheng Cheng
Recovery of platinum group metals (PGMs) including palladium (Pd), rhodium (Rh), and ruthenium (Ru) from high-level radioactive liquid waste (HLLW) possesses enormous environmental and economic benefits. A non-contact photoreduction method was herein developed to selectively recover each PGM from HLLW. Soluble Pd(II), Rh(III), and Ru(III) ions were reduced to insoluble zero-valent metals and separated from simulated HLLW containing neodymium (Nd) as a representative for lanthanides , another main component in HLLW. Detailed investigation on the photoreduction of different PGMs revealed that Pd(II) could be reduced under 254- or 300-nm UV exposure using either ethanol or isopropanol as reductants. Only 300-nm UV light enabled the reduction of Rh(III) in the presence of ethanol or isopropanol. Ru(III) was the most difficult to reduce, which was only realized by 300-nm UV illumination in isopropanol solution. The effects of pH was also studied, suggesting that lower pH favored the separation of Rh(III) but hindered the reduction of Pd(II) and Ru(III). A delicate three-step process was accordingly designed to achieve the selective recovery of each PGM from simulated HLLW. Pd(II) was reduced by 254-nm UV light with the help of ethanol in the first step. Then Rh(III) was reduced by 300-UV light in the second step after the pH was adjusted to 0.5 to suppress the Ru(III) reduction. In the third step, Ru(III) was reduced by 300-nm UV light after isopropanol was added and the pH was adjusted to 3.2. The separation ratios of Pd, Rh, and Ru exceeded 99.8%, 99.9%, and 90.0%, respectively. Meanwhile, all Nd(III) still remained in the simulated HLLW. The separation coefficients between Pd/Rh and Rh/Ru exceeded 56,000 and 75,000, respectively. This work may provide an alternative method to recover PGMs from HLLW, which minimize the secondary radioactive wastes compared with other approaches.
研究领域:
环境科学
·
核化学与放射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Fuyin Ma,Zheng Li,Haogui Zhao,Yiyun Geng,Wei Zhou,Qingnuan Li,Lan Zhang
As a new carbon-based membrane material used for ionic and molecular sieving, the graphene oxide (GO) membrane also has potential application in radiochemical separation. In this work, the permeation performances of some typical metallic elements in high level-liquid waste (HLLW) through the ionic sieving 5-μm-thick GO membranes were investigated. It was found that the permeation rates of ions through GO membranes markedly decreased with the increase of hydrated ionic radii. Cs(I) and Sr(II) permeated through GO membranes quickly, whereas lanthanide ions and actinide ions infiltrated much more slowly, thus providing the feasibility of separation according to the difference of hydrated ionic radii. Moreover, the concentrations of initial metal ions and acidity in feed solutions also had influences on the permeation of ions through GO membranes, and higher initial metal ions and feed solution acidity were favorable to the removal of Cs(I) and Sr(II). The barrier separation test indicated that GO membranes had promising ability for the separation of Cs(I) and Sr(II) from lanthanide and actinide ions due to the difference of hydrated ion radius, and the separation factor of Cs(I)/U(VI) and Sr(II)/U(VI) would reach about 10 and 3 in single penetration. The presented results demonstrated that the membrane separation based on GO membrane would be a promising candidate for the removal of Cs(I) and Sr(II) from HLLW.
研究领域:
放射化学
·
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Haoran Dong,Shunyan Ning,Zengyuan Li,Sizhi Xu,Shichang Zhang,Xinpeng Wang,Youbin Wang,Lifeng Chen,Xiangbiao Yin,Toyohisa Fujita,Mohammed F. Hamza,Yuezhou Wei
Separation of palladium from high level liquid waste (HLLW) not only manages the dispose of HLLW, but could also aid in overcoming the shortage of palladium resources. Herein, three novel adsorbents, namely, 2-mercaptobenzimidazole (MBI)/XAD7HP, 2-mercaptobenzothiazole (MBT)/XAD7HP, 2-mercaptobenzoxazole (MBO)/XAD7HP were prepared by vacuum impregnation method using Amberlite XAD7HP resin (XAD7HP) as the carrier for the selective separation of Pd(II) from simulated HLLW. SEM-EDS (Scanning Electron Microscopy), BET (Brunauer-Emmett-Teller) and PXRD (Powder X-ray diffraction) analysis showed that the ligands were successfully impregnated into the carrier. The saturated adsorption capacities of MBI/XAD7HP, MBT/XAD7HP, MBO/XAD7HP in 0.5 M HNO 3 were 126.2 mg Pd/g, 137.6 mg Pd/g, 98.4 mg Pd/g, respectively, and excellent adsorption and separation performance towards Pd(II) ( SF Pd/other metals > 500 and K d > 10 4 mL/g from 0.1 to 4 M HNO 3 ) were also achieved. The adsorption kinetics and adsorption isotherms for Pd(II) matched well with pseudo-second-order kinetic model and Langmuir model, indicating that the adsorption for Pd(II) by three adsorbents were monolayer chemical adsorption . The adsorption mechanism was analyzed by FT-IR, XPS combined with DFT calculation. The extremely high selectivity of three adsorbents towards Pd(II) among 15 metal ions is due to the soft N and S donor atoms at ligands which have good affinity for Pd(II) in HNO 3 solution. As MBT/XAD7HP exhibited the best adsorption and separation properties, it is supposed to have more application potential for the separation of Pd(II) from HLLW.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NUCLEAR ENGINEERING AND DESIGN
·
2024
·
IF 1.9
Changfu Wang,Lin Li,Xu Liu,Bobo Shao,Yan Liu,Yun Wang,Shengheng Tan,Zhirong Liu,Shengdong Zhang
The two-step vitrification process involves converting high-level waste from a liquid to a solid state through calcination , followed by melting the calcines with glass matrix material to form glassy wasteforms. The calcination process is a critical stage in the vitrification process. This study investigated the thermal decomposition performance and phase evolution of power reactor simulated high-level waste during the calcination process. As the calcination temperature increased from 100 to 900 °C, the resultant waste calcines showed increasingly darker color and smaller general particle sizes. Below 600 °C, the waste experienced thermal decomposition of nitrate and formate compounds, leading to an approximate 40 wt% weight reduction. At 600 °C, the waste's weight remained constant, and crystalline phases such as Zr x M 1-x O 2 (M = Ce, Pr, Nd), BaMoO 4 , CeO 2 , and Gd x Ce 1-x O 2 were observed.
研究领域:
核化学与化工
·
放射性废物处理
✓ 已验证
产品关联
DOI
高影响因子
DESALINATION
·
2025
·
IF 9.8
Shunyan Ning,Sizhi Xu,Jiaxu Zheng,Shichang Zhang,Xiangbiao Yin,WenLong Li,Yuezhou Wei,Lifeng Chen
Spent fuel reprocessing typically produces high-level liquid waste (HLLW), where lots of palladium and other radioactive nuclides exist. Palladium recovery from HLLW contributes to not only increasing the palladium supply but also addressing the issue of furnace clogging during the vitrification of HLLW. To achieve this, several aminopyridine-functionalized silica-based resins (SiPAc-NH-Pys) were prepared in this study through in-situ polymerization and post-synthetic modification, and the adsorption behaviors and mechanisms toward palladium were systematically studied by batch experiment and spectroscopy. The results showed that aminopyridine-functionalized SiPAc-NH-Pys with porous structure and uniform shapes were successfully prepared. These SiPAc-NH-Pys exhibited high selectivity for palladium in simulative HLLW, with almost no affinity for lanthanides or alkaline metal ions. In addition, SiPAc-NH-Pys exhibited fast adsorption and desorption kinetics, with equilibrium reached within 10 min. The adsorption kinetics were fitted well by the pseudo-second-order kinetic model, and the adsorption isotherm was well described by the Langmuir model. Spectroscopy experiments suggested that the nitrogen atom in the pyridine ring was the main active site for palladium adsorption and that nitrate anions were involved in palladium coordination; thus, they were co-adsorbed. The direct and selective recovery of palladium from simulative HLLW was finally realized in column mode, with the recovery rate close to 100 %. Overall, this work provides excellent functional material candidates for the separation of rare metal palladium from HLLW, showing significant potential.
研究领域:
核化学与化工
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zhiliang Ma,Chao Xie,YueZhou Wei,Xiangbiao Yin,Caiwu Luo,Shunyan Ning,Qiang Wu,Tianjiao Jiang
The efficient separation and recovery of palladium (Pd) from high-level liquid waste (HLLW) are critical for promoting resource sustainability and advancing the nuclear fuel cycle. In this study, a novel silica-based sorbent (HT-paPBI@SiO 2 ) enriched with nitrogen adsorption sites was synthesized via a polymerization–vacuum impregnation–high-temperature optimization strategy to address the challenges of Pd(II) recovery in highly acidic and ionically complex environments. HT‑paPBI@SiO 2 was systematically characterized using SEM, EDS, TG‑DSC, BET, and FT‑IR analyses, which confirmed its rigid framework, abundant porosity, high loading efficiency, and excellent thermal stability. Static batch adsorption experiments demonstrated that HT‑paPBI@SiO 2 efficiently adsorbs Pd(II) over a broad acidity range (0.1–9 M HNO 3 ). In simulated HLLW at 6 M HNO 3 , the material exhibited outstanding selectivity ( SF Pd/other metal ions > 1.05 × 10 3 ) and a high saturation adsorption capacity of 128.2 ± 1.8 mg/g. Furthermore, the adsorption kinetics fit well with a pseudo‑second‑order model, while the equilibrium data conform to the Langmuir isotherm and van’t Hoff thermodynamic models, indicating a spontaneous, endothermic, monolayer chemical adsorption process. Furthermore, dynamic adsorption experiments successfully achieved the selective recovery of Pd(II) from simulated HLLW, highlighting the potential of HT-paPBI@SiO 2 for industrial-scale applications. Mechanistic investigations, supported by FT-IR, XPS, and DFT calculations, revealed that the benzene ring in paPBI was oxidized to a quinone structure under high-temperature treatment. The electron-rich regions resulting from the interaction of the C=O group in quinone with the C=N − C moiety in imidazole enhance the affinity for Pd(II). This interaction facilitates the coordination of nitrogen and oxygen atoms with Pd(II), while NO 3 − ions coordinate to balance the charge.
研究领域:
核化学与化工
·
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2020
·Vol. 326
·期 2
·1323-1331
·
IF 1.137
Wu Hao,Kubota Masahiko,Osawa Naoki,Kim Seong-Yun
Adsorption and separation performances of a microporous silica-based (DAMIA-EH + TOA)/SiO 2 -P adsorbent towards Pd(II) were systematically investigated under the effect of contact time, temperature, concentration of nitric acid, chromatography etc. in a simulated high-level liquid waste containing 14 kinds of representative co-existing metal ions. Successful recovery of around 97.95% Pd(II) was achieved under the elution with 0.01 M Tu (pH = 2) solution in column experiment.
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 Cleaner Production
·
2020
·
IF 7.246
Haogui Zhao,Jing Yang,Zheng Li,Yiyun Geng,Jie Li,Mumei Chen,Ruifen Li,Qingnuan Li,Lan Zhang
The drawbacks of current high-level liquid waste (HLLW) separation processes would bring some adverse effects on the sustainable and clean utilization of nuclear power. In this work, a novel separation method for HLLW treatment based on graphene oxide membranes (GOMs) was investigated. Effects of nitric acid concentration and membrane thickness on the permeation behaviors of typical ions through GOMs were systematically investigated. On the whole, the permeation rates were in the order: hydrogen ion , cesium ion > sodium ion > strontium ion > europium ion, uranyl ion > thorium ion, which could be well explained by size exclusion and chemical interaction. As the nitric acid concentration decreased, strong coordination cations were generally restrained from migrating through GOMs due to cations hydrolysis and deprotonation of graphene oxide sheets. Ions permeation was supposed to be a two-step process which included entrance to the membrane and intramembrane migration. Based on the favorable rejection of f-block elements, GOMs separation showed promising potential in HLLW treatment. Furthermore, a new technical route for HLLW separation was proposed which showed superiority of simplified process, low running cost, less secondary radioactive waste production.
研究领域:
核能工程
·
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zeqian Zhang,Hongshan Wu,Qiming Chen,Xiaowei Li,Yimin Cai,Lihua Yuan,Wen Feng
Efficient and selective palladium (Pd) recovery from high-level liquid waste (HLLW) constitutes a crucial task for both precious resource recovery and environmental remediation, but remains challenging to achieve high efficiency, sufficient selectivity, and fast kinetics. Herein, we report a new pyrazinamide ligand (denoted as PA) as the first example of employing pyrazine-based ligand for Pd 2 + separation with impressive efficiency. Using an ionic liquid C 8 mimNTf 2 as diluent, the developed pyrazinamide-ionic liquid (PA-IL) extraction system exhibited attractive merits for Pd 2+ separation such as a wide range of workable acidities from 0.2 M to 5 M HNO 3 , ultra-fast extraction kinetics with equilibrium time of 3 min, and good Pd 2+ selectivity over 16 ions coexisting in simulated HLLW and other non-metallic anions. Slope analysis indicated that the extraction mechanism involves the cation exchange of C 8 mim + and the coextraction of NO 3 - anions in the course of Pd 2+ extraction. Results from a set of spectroscopic investigations and single crystal X-ray diffraction analysis suggest the formation of complexes with stoichiometry of both 1:1 and 2:1 (PA/Pd 2+ ) in solution and in solid state, of which the formation of 2:1 complex is the most thermodynamically favored according to DFT theoretical calculations. This work provides a highly promising pyrazinamide-based extraction system for efficient and selective Pd 2+ separation from HLLW, and brings more understanding about the complexation and coordination behaviors between N-based ligands and Pd 2+ ions.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Zhe Su,Shunyan Ning,Zengyuan Li,Shichang Zhang
A silica-polymer-based adsorbent ( iso Pentyl-BTBP/SiO 2 -P) was prepared via a vacuum impregnation method for efficient and continuous separation of palladium from complex systems. The results revealed that the distribution coefficient ( K d ) value of iso Pentyl-BTBP/SiO 2 -P toward Pd in 3 M HNO 3 solution was 5226 mL/g, with a maximum adsorption capacity of 31.7 mg/g. Besides, iso Pentyl-BTBP/SiO 2 -P exhibited a superior adsorption selectivity toward Pd to the other 14 coexisting interfering fission product ions, with the separation factor SF Pd/M value over 433 in 0.1–6 M HNO 3 solution. Moreover, column experiments results demonstrated that iso Pentyl-BTBP/SiO 2 -P can efficiently separate Pd with approximately 100% recovery, from simulated high level liquid waste (HLLW) solutions with multiple competing ions. Finally, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy analysis results revealed strong interactions between nitrogen-containing functional groups (C-N C) and Pd throughout the adsorption process , wherein the NO 3 − acting as the counterions to balance the charge. In conclusion, iso Pentyl-BTBP/SiO 2 -P has shown promising applications for effectively separating Pd from multi-component and highly acidic environments.
研究领域:
化学工程
·
核化学与放射化学
✓ 已验证
DOI
高影响因子
PROGRESS IN NUCLEAR ENERGY
·
2015
·
IF 1.119
Junchuan Zhao,Xingeng Ding,Cheng Meng,Chunrong Ren,Huiqin Fu,Hui Yang
The novel SiO 2 –ZrO 2 -calcium alginate aerogels were prepared by Sol–Gel process with phase separation method for investigating the adsorption and immobilization performance of the plutonium and minor actinides from high-level liquid waste (HLLW). The materials contained porous network structure with high surface area (233.44–481.08 m 2 /g) and pore volume (0.50–1.26 m 3 /g). The aerogels were superior adsorbents for the removal of plutonium and minor actinides, the maximum adsorption capacity and adsorption rate (35 °C, 75 rpm) reached 231.5 mg/g and 99.2%. For all the waste forms, SiO 2 , ZrO 2 and Ca 2 SiO 4 phases were simultaneously observed in the matrix. Moreover, Ce entered into Ca sites of Ca 2 SiO 4 and Zr sites of ZrO 2 . The substitution of Ca and Zr by Ce in the Ca 2 SiO 4 and ZrO 2 implies a promising disposal measure of actinides.
研究领域:
材料科学
·
核化学与放射化学
·
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）