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MOLECULES · 2024 ·Vol. 29 ·期 13 ·3126 · IF 4.2

Cs-Doped WO3 with Enhanced Conduction Band for Efficient Photocatalytic Oxygen Evolution Reaction Driven by Long-Wavelength Visible Light

Dong Li,Siyu Tian,Qiuhua Qian,Caiyun Gao,Hongfang Shen,Fei Han

Cesium doped WO3(Cs-WO3) photocatalyst with high and stable oxidation activity was successfully synthesized by a one-step hydrothermal method using Cs2CO3as the doped metal ion source and tungstic acid (H2WO4) as the tungsten source. A series of analytical characterization tools and oxygen precipitation activity tests were used to compare the effects of different additions of Cs2CO3on the crystal structure and microscopic morphologies. The UV–visible diffuse reflectance spectra (DRS) of Cs-doped material exhibited a significant red shift in the absorption edge with new shoulders appearing at 440–520 nm. The formation of an oxygen vacancy was confirmed in Cs-WO3by the EPR signal, which can effectively regulate the electronic structure of the catalyst surface and contribute to improving the activity of the oxygen evolution reaction (OER). The photocatalytic OER results showed that the Cs-WO3-0.1 exhibited the optimal oxygen precipitation activity, reaching 58.28 µmol at 6 h, which was greater than six times higher than that of WO3-0 (9.76 μmol). It can be attributed to the synergistic effect of the increase in the conduction band position of Cs-WO3-0.1 (0.11 V) and oxygen vacancies compared to WO3-0, which accelerate the electron conduction rate and slow down the rapid compounding of photogenerated electrons–holes, improving the water-catalytic oxygen precipitation activity of WO3.

研究领域: 材料科学 · 环境科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

CsBr-Triggered Reversible Phase Transition of Perovskite Nanocrystals for Advanced Information Encryption and Decryption

Qing Xu,Tianwei Zhang,Mengjia Liu,Min Wang,Kun Cao,Rong Chen

Luminescent perovskite nanocrystals (NCs), possessing the advantages of low cost, easy detection, and excellent luminescence, are becoming more and more significant in the fields of information encryption and decryption. Most hydrochromic perovskite NCs for information encryption have moderate reversibility and are easily passively decrypted by water in the moist air, limiting their practical applications. Herein, a lyochromic material is synthesized based on reversible phase transition between luminescent CsPbBr3–HBr (pretreating CsPbBr3 with HBr) and nonluminescent Cs4PbBr6, exhibiting excellent reversibility in 50 cycles triggered by CsBr solution. HBr treatment boosts the ion migration of NCs via diminishing surface ligands and passivating Br vacancy, assisting CsBr concentration acting as a crucial factor in dynamic ion exchange equilibrium between the trigger solution and CsPbBr3–HBr. By utilizing CsPbBr3–HBr as a safety ink, the CsBr-triggered photoluminescence switch has been demonstrated to be reproducible, stable, and reliable for information encryption and decryption.

研究领域: 材料科学 · 光学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 · IF 1.5

Enhanced decontamination of surface radioactive contamination using a hydrogel coating composited with Prussian blue

Yang Man,Li Zhanguo,Wang Yi,Lin Xiaoyan

In this study, a hydrogel-based strippable coating was expeditiously synthesised by employing hydrogen bonding between eco-compatible guar gum (GG), borax, and glycerol (Gly), thereby endowing the coating with excellent swelling capabilities and a high water retention capacity. This approach was specifically designed to navigate the intricate rheological management associated with strippable coating decontaminants. Through the incorporation of Prussian blue (PB), a material highly effective in adsorbing cesium (Cs), the solubility and diffusion of radionuclides within the hydrogel were significantly enhanced, thereby augmenting the decontamination efficacy of the hydrogel. The PB–GG–Gly composite demonstrated remarkable decontamination efficiencies, removing Cs from surfaces of glass, stainless steel, rubber, lacquer, and cement with percentages of 99.66%, 99.37%, 99.71%, 99.67%, and 83.83%, respectively.

研究领域: 材料科学 · 环境科学 · 放射性污染治理
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Surfaces and Interfaces · 2024 · IF 5.7

Reverse osmosis membrane with crown ethers decoration for enhanced radionuclides sieving

Yi Wang,Jianlong Wang,Li'an Hou

Reverse osmosis (RO) membranes have been widely applied in the increasingly discharged radioactive wastewater treatment . However, conventional RO membranes suffer from the issues of the limited nuclides rejections and the relatively low water permeance. In this work, a new type of RO membrane with decoration of crown ethers (15C5 and 18C6) was prepared via an interfacial polymerization process to remove the radionuclide-contaminated components. Due to the special hollow structure of crown ethers (CEs) and the hydrogen bonding within the amidogen, the obtained MPD@15C5-TMC and MPD@18C6-TMC membranes exhibited smoother surfaces and thinner polyamide active layers than the pristine MPD-TMC membrane. The optimized MPD@15C5-TMC and MPD@18C6-TMC RO membranes presented excellent pure water permeances up to 2.16 and 2.91 L m −2 h −1 bar −1 , and maintained high rejections towards Cs + , Sr 2+ and Co 2+ , respectively. Furthermore, the membrane possessed a remarkable operational stability and an excellent anti-fouling property. These results confirmed the possibility of adopting crown ethers for RO membrane fabrication and verified their great potential for the practical application in removing radioactive elements from wastewater.

CAS / MDL: 68131-04-4
研究领域: 环境科学 · 材料科学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2019 ·Vol. 95 ·期 4 ·1085-1092 · IF 2.659

The application of polyethylenimine grafting reverse osmosis membrane in treating boron-containing low-level radioactive wastewaters

Boxian Chen,Ding Chen,Xuan Zhao

BACKGROUND Reverse osmosis (RO), which is widely utilized in wastewater treatment, has been proven to be an effective tool for ion separation with high salts rejection. However, owing to the extremely low concentration of nuclides in boron-containing low-level radioactive wastewaters (LRWs), there is a significant reduction in rejection of nuclides by using commercial RO membranes. In this study, in order to obtain higher nuclides rejection under trace-level condition, novel polyamide RO membranes were fabricated by grafting polyethylenimine (PEI) with different molecular weights on commercial RO membrane surfaces. RESULTS The properties of PEI-modified membranes were analyzed, such as surface charge, morphology and hydrophilicity. The results showed that zeta potential at pH 7 increased from −22.89 mV to 20.19 mV, which indicated that surface charge altered from negative to positive. Meanwhile, hydrophilicity of membranes was improved since the contact angle decreased from 65° to 36°. The decontamination factor (DF) of cesium(I) increased from 11.69 to 114.23 and the DF of cobalt(II) increased from 28.62 to 3306.88. CONCLUSION The laboratory-scale experiments with cross-flow demonstrated the effective rejection of nuclides without obvious membrane flux loss of PEI-modified membranes. In addition, PEI-modified membranes offered a stable nuclides removal under high-level background boron and various pH conditions, which demonstrated a possible application in boron-containing LRW treatment. © 2019 Society of Chemical Industry

研究领域: 环境科学 · 材料科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2020 · IF 2.726

Investigations on the structural evolution and aqueous durability of [CsxBay][Fe3+2y+xTi4+8-2y-x]O16 ceramics for radioactive cesium storage

Xiaofen Wang,Jiang Ma,Xirui Lu,Zhiwei Fang,Lingshuang Li,Linyan Li,Yushan Yang

Hollandite ceramics are considered as a promising host matrix for cesium immobilization. In the paper, [Cs x Ba y ][Fe 3+ 2 y + x Ti 4+ 8-2 y - x ]O 16 (0.3 ​≤ ​ x , y  ​≤ ​0.75) ceramics were synthesized by solid-state reaction method using 133 Cs and 133 Ba as the substitutes for radioactive Cs and its daughter product Ba. It was found that the as-prepared (Cs,Ba)-hollandite solid solution shows a tetragonal structure ( I 4/m) with >90% crystallinity and good Cs retention at 1250 ​°C. Moreover, the normalized release rates of Cs and Ba are in the order of 10 −3  ​g ​m −2  ​d −1 for 28 days, exhibiting excellent aqueous durability.

研究领域: 材料科学 · 核废物管理
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JOURNAL OF MOLECULAR LIQUIDS · 2024 · IF 5.3

A mixed solvent system of amino crown ether and ionic liquids for a high-efficient extraction of cesium

Jintao He,Junyuan Hua,Xiaohua Ma,Ranil Wickramasinghe,Jianxin Li

Efficient extraction of Cs + from aqueous solution was investigated by liquid–liquid extraction based on ionic liquids (ILs). In this study, Di(aminobenzo)-18-crown-6 (DAB18C6) was used as the extractant and three ILs (1-butyl-3-methylimidazolium hexafluorophosphate ([C 4 mim][PF 6 ]), 1-hexyl-3-methylimidazolium hexafluorophosphate ([C 6 mim][PF 6 ]), and 1-butyl-3-methylimidazolium bis-trifluoromethyl sulfonamide ([C 4 mim][NTf 2 ])) were employed as co-extractants in the construction of a liquid–liquid extraction system for efficient and selective extraction of Cs + from aqueous solutions. It was demonstrated that the DAB18C6-[C 4 mim][NTf 2 ] mixed solvent system at 0.12 mol/L DAB18C6, a mass ratio of ILs/CHCl 3 of 1:4 and a volumetric ratio of O/A of 1:1 exhibited a high % extraction of Cs + up to 99.94 %, with a higher selectivity for Cs + relative to coexisting ions such as K + ( β Cs/K  = 1216.7) and Rb + ( β Cs/Rb  = 139.03). The high selectivity of the extraction system for Cs + was attributed to the lower hydration binding energy of Cs + (−366.51 kJ/mol) and the stronger interaction between DAB18C6 and Cs + , g(r) = 12.7. Further, the hydrogen bonding interaction between the amino crown ether and ionic liquid increases the viscosity and surface tension of the extraction system, thus enhancing the stability of the system. Noteworthy, the most stable structure formed by DAB18C6-Cs + -[NTF 2 ] − is attributed to cation exchange. In summary, this study demonstrates the great potential for efficient separation and extraction of cesium from aqueous solutions.

研究领域: 化学工程 · 环境科学
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Journal of Cleaner Production · 2019 · IF 6.395

Optimization analysis and mechanism exploration on the removal of cesium and the solidification of secondary residue wastes in electrokinetics

Fangzhu Xiao,Tao Huang,Shuwen Zhang,Longfei Liu,Cheng Wang,Guowen Peng,Shuya He

The fallout of the radioactive nuclide cesium (Cs) has posed its potential environmental threat to human health and ecosystem during the Fukushima accident. Thus, Cs decontamination from radioactive wastewater is strongly required for treating similar occurrences. In this work, a coupling method was applied to achieve Cs + removal and solidification in one conducting system. Ammonium molybdophosphate (AMP) was loaded to blast furnace slag (BFS) particles for the preparation of adsorbent (BFS-AMP) and binder. The maximum adsorption capacity of BFS-AMP for Cs + was 23.36 mg/g obtaining at the pH of 8 and the initial concentration of 500 mg/L in the equilibrium adsorption experiments. Cs + uptake confirmed to the pseudo-first-order kinetic model . Electrokinetics (EK) not only increased the adsorption capacity of BFS-AMP also enhanced the migration of Cs + ions from the anode to cathode in the electrolyzer . The transfer of Cs + ions from liquid to solid in the electrolyzer was controlled by both voltage gradients and flow rates. The solidification of EK-treated BFS-AMP mortar was mainly dominated by the mass ratios (wt.%) of alkali activator to adsorbent and the initial pH values. Cs + leaching from the solidified products of EK-treated BFS-AMP mortars ranged from approximately 1.18 × 10 −7 to 9.54 × 10 −6  g cm −2 ∙d −1 . The electromigration , geopolymer stabilization, and hydration encapsulation were concluded as the main incorporation mechanisms for Cs + ions transferring from the stock solution into the BFS-AMP-based solidification in the electrolyzer.

CAS / MDL: 7722-76-1 12054-85-2
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Interplay between storage temperature, medium and leaching kinetics of hazardous wastes in Metakaolin-based geopolymer

Peigang He,Jingyi Cui,Meiling Wang,Shuai Fu,Hualong Yang,Chengyue Sun,Xiaoming Duan,Zhihua Yang,Dechang Jia,Yu Zhou

Notwithstanding the success of carbon-free nuclear power in the new energy industry, an effective way to address nuclear contamination is still lacking. As a generally accepted method to date, immobilization of radioactive nuclear wastes with inexpensive and environment-friendly matrix such as geopolymer has attracted extensive attention. In this contribution, Na-based and K-based metakaolin geopolymer were prepared to encapsulate simulated radioactive Cs + and Sr 2+ under different temperatures and environments during long-term leaching tests. The temperature-dependent and environmental-dependent leaching kinetics as well as their dominant leaching mechanisms have been revealed. The results showed that Na-based and K-based geopolymer exhibited better immobilization performance than that of Portland cement, ceteris paribus. For the immobilization of Cs + , Na-based geopolymer showed lower leaching rate than K-based geopolymer under the same leaching conditions. Both higher temperature and salt solution accelerated the leaching behaviors of Sr + and Cs 2+ from the encapsulation matrix. This contribution sheds light on understanding the dominant leaching mechanisms of hazardous elements under different storage environments and highlights the significance of salt-tolerant matrix for the immobilization of nuclear wastes.

CAS / MDL: 7789-18-6 10042-76-9
研究领域: 环境科学 · 材料科学
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2017 ·Vol. 100 ·期 10 ·4412-4424 · IF 2.841

Effects of Na+ substitution Cs+ on the microstructure and thermal expansion behavior of ceramic derived from geopolymer

Jingkun Yuan,Peigang He,Dechang Jia,Jinsong You,Xuzhao Liu,Yao Zhang,Delong Cai,Zhihua Yang,Xiaoming Duan,Shengjin Wang,Yu Zhou

As part of a series of studies, effects of Na + substitution on the thermal evolution of cesium-based geopolymers on heating were studied. A series of sodium-substituted cesium-based geopolymers, Cs (1− x ) Na x GPs (where x =0, 0.1, 0.2, 0.3, and 0.4), were prepared and treated at 1300°C for 2 hours to obtain the corresponding ceramic products. The thermal evolution process was disclosed by virtue of a variety of technical, including TG-DTA, thermal shrinkage, XRD analysis, SEM, and TEM investigation. The results indicated that unheated Cs (1− x ) Na x GPs was not completely amorphous after the substitution of Na + and the crystallinity of Cs (1− x ) Na x GPs gradually increased with the rise of sodium content. Meanwhile, the average particle sizes of Cs (1− x ) Na x GPs also increased evidently with increases in sodium substitution. The final product after heat treatment mainly consisted of pollucite (CsAlSi 2 O 6 ) and amorphous glass phase. The particle size of pollucite grain gradually decreased as more Cs + were replaced maybe owing to the role of Na + in the nucleation process of pollucite. Two forms of Na + present in the final products: A small portion was present in the pollucite grains due to Na + partial occupied the crystallographic sites of Cs + ; and the rest were present in the amorphous glass phase among the pollucite grains. The average coefficient of thermal expansion (CTE) of resulting Cs (1− x ) Na x GPs ceramics increased from 4.80×10 -6 K −1 ( x =0) to 7.26×10 −6 K −1 ( x =0.4) with increases in sodium substitution, which could be due to the amorphous glass phase had a relatively higher CTE than that of pollucite.

CAS / MDL: 1310-73-2
研究领域: 材料科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Laser-induced breakdown spectroscopy for contamination analysis of Sr and Cs on 316L stainless steels in alkaline environment for spent nuclear fuel storage

Yupeng Xie,Jie Wang,Yaocheng Hu,Jing Zhang,Yong Gao,Haipeng Li,Sheng Wang

The contamination of fission products ( 90 Sr and 137 Cs) on the metallic material (316L stainless steel) of alkaline spent fuel storage pond threatens to decommission nuclear facilities. Compared with previous studies unable to detect Cs on the surface of contaminated steel by laser-induced breakdown spectroscopy (LIBS), this study selected the emission lines of Sr II 407.74 nm and Cs I 455.77 nm as the analytical spectral lines of LIBS, and for the first time satisfactorily measured and analyzed the accumulation of Sr and Cs on the surface of 316L stainless steel for 7, 14, 21, 30 and 60 days, respectively. It was found during the accumulation, the concentration of Sr and Cs on the surface reached their maximum after 21 days, and relatively stabilized 30 days later. In addition, combined with the physicochemical characterizations, the contamination mechanism of Sr and Cs on 316L stainless steel was proposed, with the contaminants gradually diffusing from the oxide layer dissolved and damaged in the alkaline corrosive environment to the matrix. Strontium had two forms on the steel surface: SrCrO 4 in the oxide layer and SrCO 3 in the matrix, but the contamination of Cs was more inclined to the surface than Sr.

研究领域: 材料科学 · 核能工程 · 表面分析
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OPTICS EXPRESS · 2023 ·Vol. 31 ·期 5 ·9123-9134 · IF 3.8

Optimization of deliquescence-proof perovskite-like Cs3ErF6 phosphor and dual-mode luminescent intensity ratio thermometry

Hanyu Xu,Zuoling Fu,Yanling Wei

The susceptibility of Cs-based fluorides to deliquescence has led to the fact that lanthanide-doped Cs-based fluorides and their related applications have hardly been reported. Herein, the method to solve the deliquescence of Cs3ErF6 and its excellent temperature measurement performance were discussed in this work. Initially, the soaking experiment of Cs3ErF6 found that water had irreversible damage to the crystallinity of Cs3ErF6. Subsequently, the luminescent intensity was ensured by the successful isolation of Cs3ErF6 from the deliquescence of vapor by the silicon rubber sheet encapsulation at room temperature. In addition, we also removed moisture by heating samples to obtain temperature-dependent spectra. According to spectral results, two luminescent intensity ratio (LIR) temperature sensing modes were designed. The LIR mode which can quickly respond to temperature parameters by monitoring single band Stark level emission named as “rapid mode”. The maximum sensitivity of 7.362%K-1 can be obtained in another “ultra-sensitive mode” thermometer based on the non-thermal coupling energy levels. This work will focus on the deliquescence effect of Cs3ErF6 and the feasibility of silicone rubber encapsulation. At the same time, a dual-mode LIR thermometer is designed for different situations.

CAS / MDL: 12061-16-4 1314-36-9
研究领域: 材料科学 · 光学
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