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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Removal of trace radioactive Cs+ by zirconium titanium phosphate: From bench-scale to pilot-scale

Yongchuan Wu,Jitao Chen,Zhongmin Liu,Ping Na,Zhibin Zhang

Removing trace radioactive 137 Cs from aquatic system is still a challenge. Herein, Zirconium Titanium Phosphate (ZTP) was prepared and utilized for Cs removal from seawater. The structure and morphology of ZTP were systematically characterized. ZTP exhibited typical feature of tetravalent metal acid, and the surface was pocked with abundant hydroxyl groups which can reacted with H 2 O to form exchangeable protons. Bench-scale to pilot-scale adsorption was carried out to assess Cs removal capacity and rate. ZTP showed a good adsorption performance for Cs + especially at trace concentration (500 ppb) and the removal rate in deionized water and seawater were 98.8 % and 83.9 %, respectively. Radioactive experiments were conducted to test the selective removal of 137 Cs + and the removal rates reached 98.3 %. Slurry-bed adsorption device was designed and used as the pilot-scale equipment. The removal rate was as high as 92.7 % after 12 cycles, indicated that ZTP is one of the promising adsorbents in industrial application. Pyridine adsorption IR spectra indicated that surface of ZTP was riddled with Brønsted and Lewis acid sites, and the protons at the Brønsted acid site exchanged with Cs + . This work will provide reference for the treatment of large-scale Cs-contaminated wastewater.

研究领域: 环境科学 · 放射化学
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JOURNAL OF CHEMICAL THERMODYNAMICS · 2021 · IF 3.178

Volumetric properties of the ternary system (CsCl + Cs2SO4 + H2O) and its subsystems from 283.15 to 363.15 K and atmospheric pressure: Experimental and thermodynamic model

Kangrui Sun,Ziwei Bi,Yanqin Meng,Yafei Guo,Lingzong Meng,Tianlong Deng

The salt-water interactions on single salt aqueous solutions of cesium sulfate and cesium chloride, as well as their mixing solutions, have been investigated by a combination of density measurements by an Anton Paar Digital vibrating-tube densimeter and the correction of the Pitzer model of electrolyte. The volumetric properties including apparent molar volume ( V ϕ ) and the coefficient of thermal expansion of the solution ( α ) of the binary systems (CsCl + H 2 O), (Cs 2 SO 4  + H 2 O) and the ternary system (CsCl +  Cs 2 SO 4  + H 2 O) from 283.15 to 363.15 K at 5 K intervals and atmospheric pressure were derived. Variation trends of these volumetric properties against temperature and molality were revealed minutely. The Pitzer single salt parameters ( β MX 0 v , β MX 1 v and C MX v , MX = CsCl and Cs 2 SO 4 ), mixing ion-interaction parameters ( θ Cl , S O 4 v and ψ Cs , Cl , S O 4 v ) as well as the correlation coefficient a i in the temperature-dependence equation ( F ( i, p, j ) =  a 1  +  a 2 ln( T /298.15) +  a 3 ( T -298.15) +  a 4 /(620- T ) +  a 5 /( T -227)) have been obtained according to Pitzer ion-interaction model of electrolytes. These results are helpful to understanding the ion-interaction of aqueous solutions.

研究领域: 物理化学 · 热力学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2025 · IF 1.6

Coal fly ash as raw materials for stable solidification of radioactive cesium via microwave sintering: mechanism and chemical durability

Mai Yuzhen,Chen Jie,Jiang Fuliang,Zhang Junfeng,Xie Yupeng

Radioactive cesium represents a substantial risk to both human health and environmental safety due to its persistent and hazardous nature. Simultaneously, large quantities of coal fly ash (CFA) are produced annually without sufficient resource utilization. In this study, a combination of microwave sintering technology and CFA was utilized to fabricate pollucite [CsAlSi 2 O 6 ] ceramic designed to immobilize radioactive cesium. The CsAlSi 2 O 6 ceramic derive from CFA with > 98% cesium retention was achieved via microwave sintering at 850 °C for 30 min, which was ~ 300 °C lower and ~ 11% cesium retention rate higher that those of reported Cs-bearing hollandite. The influence of Cs 2 CO 3 content and sintering temperature on the phase evolution of the sintered samples were systematically examined. The chemical durability of the sintered forms was further assessed. The results indicated that the Cs(I) elements were uniformly distributed within the sintered matrix. Furthermore, the maximum solid solubility of Cs 2 CO 3 in the sintered forms was found to be 39 wt% at 850 °C. Notably, the solidified samples exhibited exceptional chemical durability, with normalized leaching rate of Cs + ions (LR Cs ) maintaining consistently low (~ 1.0 × 10 –6  g m −2  d −1 ) after 42 days. This study provides a valuable reference for the potential resource utilization of CFA in the stable solidification of radioactive cesium via microwave sintering, offering a promising strategy for future application.

CAS / MDL: 534-17-8
研究领域: 核废物管理 · 材料科学 · 环境修复 · 微波处理技术 · 陶瓷材料
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Stability studies of [CsxBay][(Al3+,Ti3+)2y+xTi4+8-2y-x]O16 ceramics for radioactive caesium immobilization

Yushan Yang,Xiaofen Wang,Shunzhong Luo,Xiaoyong Yang,Jiang Ma

[Cs x Ba y ][(Al 3+ ,Ti 3+ ) 2 y + x Ti 4+ 8-2 y - x ]O 16 (0.4 ≤  x ,  y  ≤ 0.8) ceramics were synthesized to investigate the substitution effects of Ba 2+ for Cs + on the stability of hollandite-ceramic waste forms. It was found that the substitution of Ba 2+ for Cs + in the (Cs,Ba)-hollandite system does not cause substantial variation in the crystallographic phase and microstructure. The normalized release rates of Cs and Ba at 90 °C in deionized water were < 0.005 g m −2 d −1 after 28 days. These results indicate that hollandite ceramics are an ideal host for permanent radioactive caesium disposal.

研究领域: 材料科学 · 核废料管理
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2016 · IF 2.567

Effects of Cesium Ions and Cesium Oxide in Side-Chain Alkylation of Toluene with Methanol over Cesium-Modified Zeolite X

He Han,Min Liu,Fanshu Ding,Yiren Wang,Xinwen Guo,Chunshan Song

The side-chain alkylation of toluene with methanol was studied on cesium-modified zeolite X prepared by ion-exchange and impregnation with different cesium precursors. The catalyst was characterized by X-ray diffraction, scanning electron microscopy, X-ray fluorescence spectroscopy, Ar physical adsorption–desorption, NH3 temperature-programmed desorption (TPD), CO2-TPD, thermogravimetric/differential thermal analysis, ultraviolet-Raman spectroscopy, energy-dispersive spectrometry, and X-ray photoelectron spectroscopy. Cesium hydroxide was found to be the most effective precursor for modifying zeolite X. Cesium ions bonded on the framework and cesium oxide formed in the pore were found to take different roles in this reaction. Cesium ions could adsorb and activate toluene or modify the basicity of framework oxygen, whereas cesium oxide could ensure the effective conversion of methanol to formaldehyde and inhibit the process of coke deposition. A possible reaction pathway for this reaction over cesium-modified samples was described. The synergistic effect of cesium ions and cesium oxide was proven to be important for the formation of styrene and ethylbenzene.

研究领域: 催化化学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Highly ordered macroporous silica dioxide framework embedded with supramolecular as robust recognition agent for removal of cesium

Ying Dai,Riwen Lv,Jiali Fan,Hong Peng,Zhibin Zhang,Xiaohong Cao,Yunhai Liu

Owning to highly mechanical strength and non-interference effectivity, silica dioxide is often explored as a stable supporter commonly with mesopore. It is known that a macroporous framework has larger mass transfer channel, possibly beneficial to adsorption process. Herein highly ordered macroporous silica dioxide framework (homogeneous pore size of 194.20 nm) was synthesized and embedded with supramolecular (CC/OMS). Cs cation adsorption onto CC/OMS was explored under different pH (presence or absence of humic acid), initial cesium concentration, shaking time, competing ions. The robust cesium uptake capacity demonstrated by a theory adsorption amount of 150.01 mg/g highlighted unique CC/OMS properties combining large mass transfer channel and superior complex capacity of supramolecular. The adsorption was well fit with Langmuir and pseudo-second-order model. Sodium and potassium at a lower concentration showed little influence on cesium adsorption. The results demonstrated that CC/OMS was an alternative material for cesium capture from acidic aqueous solution.

研究领域: 材料科学 · 环境科学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-10 · IF 14.7

“Ion-imprinting” strategy towards metal sulfide scavenger enables the highly selective capture of radiocesium

Tang Jun-Hao,Jia Shao-Qing,Liu Jia-Ting,Yang Lu,Sun Hai-Yan,Feng Mei-Ling,Huang Xiao-Ying

Highly selective capture of radiocesium is an urgent need for environmental radioactive contamination remediation and spent fuel disposal. Herein, a strategy is proposed for construction of “inorganic ion-imprinted adsorbents” with ion recognition-separation capabilities, and a metal sulfide Cs 2.33 Ga 2.33 Sn 1.67 S 8 ·H 2 O (FJSM-CGTS) with “imprinting effect” on Cs + is prepared. We show that the K + activation product of FJSM-CGTS, Cs 0.51 K 1.82 Ga 2.33 Sn 1.67 S 8 ·H 2 O (FJMS-KCGTS), can reach adsorption equilibrium for Cs + within 5 min, with a maximum adsorption capacity of 246.65 mg·g −1 . FJMS-KCGTS overcomes the hindrance of Cs + adsorption by competing ions and realizes highly selective capture of Cs + in complex environments. It shows successful cleanup for actual 137 Cs-liquid-wastes generated during industrial production with removal rates of over 99%. Ion-exchange column filled with FJMS-KCGTS can efficiently treat 540 mL Cs + -containing solutions (31.995 mg·L −1 ) and generates only 0.12 mL of solid waste, which enables waste solution volume reduction. Single-crystal structural analysis and density functional theory calculations are used to visualize the “ion-imprinting” process and confirm that the “imprinting effect” originates from the spatially confined effect of the framework. This work clearly reveals radiocesium capture mechanism and structure-function relationships that could inspire the development of efficient inorganic adsorbents for selective recognition and separation of key radionuclides.

CAS / MDL: 7803-57-8
研究领域: 环境科学 · 材料科学 · 核化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-10 · IF 14.7

Boosting selective Cs+ uptake through the modulation of stacking modes in layered niobate-based perovskites

Sun Hai-Yan,Chen Zhi-Hua,Hu Bing,Tang Jun-Hao,Yang Lu,Guo Yan-Ling,Yao Yue-Xin,Feng Mei-Ling,Huang Xiao-Ying

Selective separation of 137 Cs is significant for the sustainable development of nuclear energy and environmental protection, due to its strong radioactivity and long half-life. However, selective capture of 137 Cs + from radioactive liquid waste is challenging due to strong coulomb interactions between the adsorbents and high-valency metal ions. Herein, we propose a strategy to resolve this issue and achieve specific Cs + ion recognition and separation by modulating the stacking modes of layered perovskites. We demonstrate that among niobate-based perovskites, A LaNb 2 O 7 ( A  = Cs, H, K, and Li), HLaNb 2 O 7 shows an outstanding selectivity for Cs + even in the presence of a large amount of competing M n+ ions ( M n+  = K + , Ca 2+ , Mg 2+ , Sr 2+ , Eu 3+ , and Zr 4+ ) owing to its suitable void fraction and space shape, brought by the stacking mode of layers. The Cs + capture mechanism is directly elucidated at molecular level by single-crystal structural analyses and density functional theory calculations. This work not only provides key insights in the design and property optimization of perovskite-type materials for radiocesium separation, but also paves the way for the development of efficient inorganic materials for radionuclides remediation.

CAS / MDL: 534-17-8
研究领域: 材料科学 · 环境科学 · 核能技术
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Separations · 2023 ·Vol. 10 ·期 1 ·42 · IF 2.6

Separation of Cesium and Rubidium from Solution with High Concentrations of Potassium and Sodium

Junjie Xie,Kang Li,Zhuonan Shi,Changli Min,Shina Li,Zichen Yin,Ruixin Ma

Solvent extraction with 4-tert-butyl-2-(α-methylbenzyl) phenol (t-BAMBP) is an effective method for the separation and purification of rubidium and cesium. A solution containing a high K+concentration (exceeding 80 g/L), which was ultra-salty, with about 200 g/L alkali metal ions, was used to extract Rb+and Cs+. The effects of the process parameters on the separation of cesium and rubidium were systematically studied. The optimum conditions were as follows: NaOH concentration of 0.5 mol/L, t-BAMBP concentration of 1 mol/L (in sulfonated kerosene), organic/aqueous volume ratio (O/A ratio) of 3:1, and contact time of 1 min. The extraction rates of cesium and rubidium were 99.81 and 98.09%, respectively, and 19.31% of potassium was co-extracted in the organic phase after five-stage countercurrent extraction. About 99.32% of K+in the organic phase could be removed after five-stage countercurrent scrubbing with deionized water at an O/A ratio of 2:1 for 2 min. When 0.5 mol/L hydrochloric acid solution was used as detergent, almost all of the cesium and rubidium (>99%) could be recovered by two-stage countercurrent stripping at an O/A ratio of 3:1 for 2 min. A solid compound was found and collected from the organic phase during multi-stage solvent extraction. Its composition and structure were determined by XRD, infrared Fourier-transform, and ICP-MS.Keywords:t-BAMBP;rubidium;cesium;potassium;extraction complex

CAS / MDL: 1310-73-2 7647-01-0
研究领域: 化学工程 · 分析化学
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CHEMISTRY OF MATERIALS · 2016 · IF 9.407

Highly Selective and Rapid Uptake of Radionuclide Cesium Based on Robust Zeolitic Chalcogenide via Stepwise Ion-Exchange Strategy

Huajun Yang,Min Luo,Li Luo,Hongxiang Wang,Dandan Hu,Jian Lin,Xiang Wang,Yanlong Wang,Shuao Wang,Xianhui Bu,Pingyun Feng,Tao Wu

The safe use of nuclear energy requires the development of advanced adsorbent technology to address environment damage from nuclear waste or accidental release of radionuclides. Recently developed amine-directed chalcogenide frameworks have intrinsic advantages as ion-exchange materials to capture radionuclides, because their exceptionally negative framework charge can lead to high cation-uptake capacity and their 3-D multidimensional intersecting channel promotes rapid ion diffusion and offer a unique kinetic advantage. Prior to this work, however, such advantages could not be realized because organic cations in the as-synthesized materials are sluggish during ion exchange. Here we report an ingenious approach on the activation of amine-directed zeolitic chalcogenides through a stepwise ion-exchange strategy and their use in cesium adsorption. The activated porous chalcogenide exhibits highly enhanced cesium uptake compared to the pristine form and is comparable to the best metal chalcogenide sorbents so far. Further ion-exchange experiments in the presence of competing ions confirm the high selectivity for cesium ions. Excellent removal performance has also been observed in real water samples, highlighting the importance of stepwise ion exchange strategy to activate amine-directed chalcogenide framework for 137Cs+ removal.

CAS / MDL: 7440-36-0
研究领域: 核科学 · 材料科学 · 环境科学
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DALTON TRANSACTIONS · 2021 ·Vol. 51 ·期 4 ·1481-1488 · IF 4.39

A6Mo2P4O19 (A = Rb, Cs) and Rb2MoP2O9: new molybdophosphates with distinct polyanionic configurations

Maierhaba Abudoureheman,Juanjuan Zheng,Peng Wang,Bo Wei,Zhiyong Guo,Zhaohui Chen,Yanna Chen

The exploration of A–Mo–P–O (A = Rb, Cs) systems has allowed several new Mo(V) phosphates, Rb2MoP2O9, Rb6Mo2P4O19 and Cs6Mo2P4O19, to be synthesized through the spontaneous nucleation method. Single-crystal X-ray diffraction analysis reveals that the identical stoichiometry compounds Rb2MoP2O9 and Cs2MoP2O9 belong to different space groups C2/c and Pbca, respectively. Both compounds consist of dissimilar 1D [Mo–O–P]∞ chains with different repeated building units, while monovalent cations fill in spaces to form 3D structures. However, Rb6Mo2P4O19 and Cs6Mo2P4O19 are isostructural and crystallize in the same space group of P21/c. They exhibit a 3D framework structure with 0D Mo2O5O6P4O8 groups, which are separated by Rb/Cs atoms. Interestingly, structural relationships between the different monophosphates of the A–Mo–P–O (A = Rb, Cs) systems are presented in which distinct polyanionic configurations appear owing to the A/P ratios, as well as the size of the univalent cations. Further, detailed structural comparisons, optical properties and theoretical calculations are also discussed.

研究领域: 材料科学 · 化学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Novel Zr-Doped Thiostannate Spinning Fiber (Fiber-KZrTS) for Highly Efficient and Renewable Recovery of Cesium and Strontium from Geothermal Water

Chi Ma,Chenyu Qi,Dingbo Wei,Zhenzhen Jiang,Yafei Guo,Nelson Belzile,Tianlong Deng

The efficient and renewable recovery of cesium and strontium by absorption from a new type of geothermal water liquid mineral resource is highly desirable but still challenging. In this work, a new Zr-doped layered potassium thiostannate adsorbent (KZrTS) was first synthesized and used for Cs+ and Sr2+ green and efficient adsorption. It was found that KZrTS had very fast adsorption kinetics toward both Cs+ and Sr2+ with an equilibrium reached within 1 min, and the theoretical maximum adsorption capacities for Cs+ and Sr2+ were 402.84 and 84.88 mg/g, respectively. Moreover, to solve the loss problem of the engineering application of the powdered adsorbent KZrTS, KZrTS was uniformly coated with polysulfone by wet spinning technology to form micrometer-level filament-like absorbents (Fiber-KZrTS), whose adsorption equilibrium rates and capacities toward Cs+ and Sr2+ are almost the same as that of powder. Furthermore, Fiber-KZrTS showed excellent reusability, and the adsorption performance remained virtually unchanged after 20 cycles. Therefore, Fiber-KZrTS has potential application for green and efficient cesium and strontium recovery from geothermal water.

研究领域: 材料科学 · 环境科学
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