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HYDROMETALLURGY · 2023 · IF 4.7

Highly efficient and selective adsorption of palladium(II) from simulated nuclear waste solution using Amberlite XAD-7 resin impregnated with a phenanthroline-derived diamide

Qian Xiao,Xueyu Wang,Lianjun Song,Fengfeng Li,Qiuju Li,Lanlan He,Zhen Shen,Fangxiang Luo,Songdong Ding

The increasing demand and limited natural resources for rare precious metal palladium render its separation and recovery from secondary sources such as acidic nuclear liquid waste greatly interesting. Herein, a novel Et-Tol-DAPhen extraction resin was prepared by impregnating Amberlite XAD-7 resin with a phenanthroline-derived diamide extractant N , N ′-diethyl- N , N ′-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen), and the adsorption behavior of this new extraction resin towards Pd 2+ in HNO 3 solution was investigated through the batch and column experiments. The Et-Tol-DAPhen extraction resin exhibited strong adsorbability, high adsorption capacity, excellent selectivity and good reusability for Pd 2+ in highly acidic HNO 3 solution. In addition, the pseudo-second-order and Langmuir models were applied to understand the adsorption process of Pd 2+ on Et-Tol-DAPhen extraction resin, respectively. It demonstrated the characteristics of a uniform single-layer chemisorption . The maximum uptake capacity could reach as high as 74.6 mg g − 1 for Pd 2+ in 3.0 mol/L HNO 3 solution which is much higher than most adsorbent materials of palladium reported before. Furthermore, Et-Tol-DAPhen extraction resin could selectively uptake Pd 2+ from a simulated acidic nuclear waste solution containing 20 different kinds of ions with the separation factor SF Pd/M values as high as 100 to 10,000. Moreover, although the adsorption efficiency had a slight decrease after 5 times of adsorption-desorption process, it still remained at a high level. This new extraction resin displayed a potential application prospect in the field of separation and recovery of Pd 2+ from acidic nuclear liquid waste .

研究领域: 化学工程 · 环境科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 · IF 1.5

Synthesis of P204 polystyrene resin adsorbents for efficient and selective removal of uranium

Jiang Xuan,Dai Bingyu,Zhou Yun,Chang Beijia,Li Yifan,Du Chen,Liu Tonghuan

Uranium wastewater is produced in many aspects of the nuclear fuel cycle, so the separation and analysis of uranium in Uranium wastewater is becoming increasingly important. In this work, we engineered and synthesized a novel uranium-targeted material P204 (di(2-ethylhexyl) phosphate) resin, The maximum adsorption capacity of P204 resin for uranium reached 101.11 mg/g at 303 K. Moreover, it maintained excellent selectivity, maintaining high performance even after 65 h of immersion in high concentrations of HNO 3 . Most prominently, the P204 resin has demonstrated significant potential in the treatment of actual uranium mine wastewater.

研究领域: 环境科学 · 材料科学
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RADIOCHIMICA ACTA · 2022 ·Vol. 110 ·期 5 ·311-322 · IF 2.083

Efficient enrichment of U(VI) by two-dimensional layered transition metal carbide composite

Yun Zhou,Huai-Xin Hao,Tian-Hao Dong,Xu-Feng Ni,Yi-Chen Hu,Jia-Ju Ma,Jun-Qiang Yang,Ke-Liang Shi,Guo-Jian Duan,Tong-Huan Liu

With the rapid development of nuclear energy, how to safely and efficiently dispose of radioactive waste solution has become an urgent environmental problem of public concern. It is of great significance to construct a new type of high-efficiency adsorbent material to recover uranium from nuclear waste solution. In this work, the Ti 3 C 2 T x material (an emerging two-dimensional inorganic layered material) with a stable layered structure was used as the matrix, and the amidoxime functionalized MXene composite material (PAO/Ti 3 C 2 T x ) was synthesized by in-situ polymerization. The amidoxime-functionalized Ti 3 C 2 T x showed excellent capacity to capture U(VI), with a maximum adsorption capacity of 98.04 mg/g at 25 °C, which was significantly better than that of Ti 3 C 2 T x , and the adsorption selectivity for U(VI) was greatly improved. The adsorption was conformed to Langmuir isotherm model and pseudo-second-order kinetic model. In addition, the adsorbed UO22+ could be effectively desorbed by 0.1 M HNO3, and the adsorption performance of PAO/Ti 3 C 2 T x did not decrease significantly after 5 adsorption/desorption cycles. The results of ionic strength experiment, FT-IR, SEM, and XPS jointly indicated that adsorption mechanism of U(VI) on PAO/Ti 3 C 2 T x was the combined effect of the amidoxime group and -O and -OH active groups on the surface of Ti 3 C 2 T x , mainly inner complexation. These advantages make PAO/Ti 3 C 2 T x composite a highly potential U(VI) adsorbent with great application prospects.

研究领域: 环境科学 · 材料科学
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INORGANIC CHEMISTRY · 2023 · IF 4.6

Ultraselective Extraction Reprocessing of 99TcO4–/ReO4– with a Promising Carbamic Acid Extractant System

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 · 核化学 · 放射性废物管理
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2021 ·Vol. 330 ·期 3 ·1271-1280 · IF 1.371

Hydrothermal synthesis of honey/bayberry microsphere for uranium removal from aqueous solution

Zhu Hui,Zhou Jian,Ding Pingping,Liao Hui,Jin Yifan,Ding Weicheng

In this work, a novel honey/bayberry (HSHB) microsphere was prepared via a simple and green hydrothermal method to investigate the UO 2 2+ adsorption behavior in simulated nuclear effluent. The results showed that spherical HSHB (about 40 nm) had the maximum adsorption capacity of 271.00 mg/g at 328.15 K and displayed a desirable selectivity for the UO 2 2+ . Furthermore, combined with the characterization analysis and adsorption experimental results, the phenolic hydroxyl group of HSHB could be combined with UO 2 2+ through chelation. Therefore, these facts indicate that HSHB could be used as a low-cost and environmentally friendly adsorbent for UO 2 2+ removal from nuclear effluent.

研究领域: 环境科学 · 材料科学
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Nanoscale · 2020 ·Vol. 12 ·期 47 ·24044-24053 · IF 6.895

Construction of covalent organic framework with unique double-ring pore for size-matching adsorption of uranium

Jie Zhang,Lihong Zhou,Zhimin Jia,Xiaofeng Li,Yue Qi,Chuting Yang,Xinghua Guo,Shanyong Chen,Honghan Long,Lijian Ma

The separation and recovery of key nuclides such as uranium and plutonium from effluents related to nuclear industry is of great significance for alleviating the shortage of nuclear energy resources and protecting the environment and human health. However, the high temperature, strong acidity and radioactivity of the nuclear effluents pose a severe challenge to the separation materials used in such conditions. The diversity of structure, flexibility of design, and excellent physicochemical stability of covalent organic framework materials (COFs) provide the possibility for the directional design and preparation of adsorbents for use under harsh conditions. Herein, three COFs with similar structure, different pore sizes and connecting modules were synthesized. The ingenious structure predesign enables Dp-COF to have three carboxyl groups oriented toward the pore center and laid out in appropriate spatial positions, which builds hydrogen-bonding bridges between carboxycarbonyl and hydroxyl groups, and thus constructs for the first time a unique COF material with a double-ring pore. The inner pore size of the “double-ring” is slightly larger than the diameter of uranyl hydrate, which leads to a size-matching adsorption of uranium by Dp-COF, thus greatly reducing the effect of protonation. Even in the simulated spent fuel reprocessing liquid with pH = 1.0, the adsorption capacity of Dp-COF for uranium can reach 66.3 mg g−1, and the adsorption capacity reaches 317.3 mg g−1 at pH = 4.5, which is very rare among the reported COFs. More excitingly, the removal rate for uranium reaches up to an unprecedented 99.8% due to the size-matching effect, more than any analogous adsorbents. This study not only proposes new ideas for the design and regulation of the microscopic configuration of COF materials, but also provides an alternative approach for the preparation of efficient uranium adsorbents.

研究领域: 材料科学 · 环境科学 · 核能工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Highly selective uranium adsorption on 2-phosphonobutane-1,2,4-tricarboxylic acid-decorated chitosan-coated magnetic silica nanoparticles

Yaoyao Huang,Huaili Zheng,Hong Li,Chun Zhao,Rui Zhao,Siqi Li

The separation and recovery of uranium resources from nuclear waste solutions is important for achieving uranium reuse and environmental protection. In this study, a novel adsorbent, 2-phosphonobutane-1,2,4-tricarboxylic acid (PBTCA)-decorated chitosan-coated magnetic silica nanoparticles, was fabricated and applied to the highly selective adsorption of uranium from aqueous solution. Selective sorption in a multi-ion solution (pH 4.0) containing 14 coexisting cations resulted in CoFe 2 O 4 @SiO 2 @CS-PBTCA showing an excellent uranium adsorption capacity of up to 83.16 mg g −1 , which was much higher than that of ungrafted CoFe 2 O 4 @SiO 2 @CS (29.99 mg g −1 ). The adsorbent also exhibited higher acid resistance than uncoated silica adsorbent under pH 1.0 conditions, with CoFe 2 O 4 @SiO 2 @CS-PBTCA showing barely any iron and cobalt leaching, while CoFe 2 O 4 @CS-PBTCA showed iron and cobalt leaching amounts of 2.97 and 0.93 mg L −1 , respectively. The desorption experiment used 0.2 M PBTCA (pH 1.0) as eluent, with the results showing that uranium ions were readily and rapidly desorbed. Furthermore, CoFe 2 O 4 @SiO 2 @CS-PBTCA maintained outstanding stability and adsorption performance after five reuse cycles. The mechanism for U(VI) removal was investigated by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy, with the results suggesting that the adsorbent binds to uranium mainly though oxygen atoms of carboxyl groups and phosphonic groups in PBTCA. This strategy shows strong potential for developing a variety of novel, highly active, acid resistance, and reusable immobilized functional magnetic materials for effective separation of uranium from a multi-ion solution.

CAS / MDL: 25952-53-8 6066-82-6
研究领域: 环境科学 · 材料科学 · 核工程 · 化学工程
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