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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Hydrothermal transformation of geopolymers to bulk zeolite structures for efficient hazardous elements adsorption

Peigang He,Qikun Wang,Shuai Fu,Meiling Wang,Shengjian Zhao,Xuzhao Liu,Yuqi Jiang,Dechang Jia,Yu Zhou

This paper reports a facile route to prepare bulk zeolites with tunable phase compositions and microstructures by combining hydrothermal treatment and geopolymer precursor technique. Amorphous Na-based geopolymer (NaGP) is transformed into crystalline analcime following hydrothermal treatments. By systematically investigating the effects of hydrothermal conditions on the phase compositions and microstructures of the products, the optimal hydrothermal procedure is screened as treating NaGP in 1 M NaOH solution at 160 °C for 6 h. Furthermore, we achieve control over phase compositions of the resulting bulk zeolites by tailoring the initial Na/K ratio of geopolymer precursors. For instance, treating the geopolymer precursor with a Na/K ratio of 9: 1 under the optimal hydrothermal procedure leads to the formation of zeolite consisting of analcime and zeolite-P. The as-prepared adsorbents exhibit outstanding adsorption performance for the hazardous elements, among which analcime-zeolite-P shows an adsorption efficiency of 93.3% for Cs + , and NaGP exhibits an adsorption efficiency of 99.6% for Sr 2+ . Moreover, we reveal the mechanisms underlying the adsorption of Cs + and Sr 2+ in the adsorbents to be chemisorption . Meanwhile, ion exchanges also occur in NaGP and analcime-zeolite-P during Cs + adsorption. These results render geopolymers and their derived bulk zeolites promising for hazardous elements adsorption.

研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2014 · IF 3.552

Efficient removal of cesium from aqueous solution with vermiculite of enhanced adsorption property through surface modification by ethylamine

Hang Long,Pingxiao Wu,Lin Yang,Zhujian Huang,Nengwu Zhu,Zhixian Hu

Ethylamine modified vermiculite (Ethyl-VER) with high specific surface area and excellent pore structure was prepared to remove cesium from aqueous solution. The physic-chemical properties of the pristine and modified vermiculite were analyzed by X-ray diffraction (XRD), Fourier-transform infrared (FTIR), specific surface area (BET) and scanning electron microscopy/energy disperse spectroscopy (SEM/EDS). The corroding effect of ethylamine increased the specific surface area of vermiculite from 4.35 to 15.59   m 2   g −1 , and the average pore diameter decreased from 6.8 to 5.34   nm. Batch adsorption experiments were conducted as a function of pH, initial Cs + concentration, contact time, coexisting cations (K + , Na + , Ca 2+ ) and low-molecular-weight organic acids (acetic acid, oxalic acid, citric acid) to illustrate the adsorption behavior. The study found that the adsorption capacity of cesium in aqueous solution was improved from 56.92 to 78.17   mg   g −1 after modification. The formation of micropores and mesopores and the increased surface area played a critical role in the enhancement of cesium adsorption. Kinetic experiments indicated that the adsorption process can be simulated well with a pseudo-second-order model. The presence of cations or low-molecular-weight organic acids inhibited cesium adsorption in different degrees. On the basis of our results, Ethyl-VER with good surface characteristics and high adsorption capacity is a suitable adsorbent for cesium removal from aqueous solution.

CAS / MDL: 7647-17-8 75-04-7
研究领域: 环境科学 · 材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Adsorptive Removal of Radioactive Cesium from Model Nuclear Wastewater over Hydroxyl-Functionalized Mxene Ti3C2Tx

Yujing Chi,Yuan Xu,Chenxiang Xu,Jiming Tian,Ying Li,Boxiang Gu,Haiyan Song,Han Zhang

Selective removal of 137Cs from nuclear wastewater is still a challenge due to the issues of efficient adsorbent exploitation and high concentrations of competitive ions. In this study, two-dimensional-layered Mxene Ti3C2Tx achieved the surface alkaline modification with KOH to be used as an efficient adsorbent for Cs+ removal from model wastewater. Hydroxyl-modified Ti3C2Tx obtained improved the delamination morphology and surface structure compared with the pristine Ti3C2Tx. In addition, the F species in Ti3C2Tx were efficiently removed and the hydroxyl groups were increased after modification. The adsorption efficiency of Cs+ over the hydroxyl-modified Ti3C2Tx was significantly enhanced, being attributed to the improvements in morphology, structure, and properties. 0.05 g of an optimal adsorbent achieved 90% removal of Cs+ with 5 mg·L–1 initial concentration in 50 mL of model wastewater within 5 min at ambient temperature and neutral conditions. Hydroxyl-modified Ti3C2Tx also exhibited high adsorption selectivity for Cs+ in the presence of competitive metal ions such as K+, Na+, Mg2+, and Ca2+. The mechanism study revealed that the ion exchange between [Ti–O]−H+/Cs+ mainly contributed to Cs+ adsorption, and the complexation between the oxygen-containing groups [Ti–O] in modified Ti3C2Tx and Cs was also involved. The hydroxyl-modified Ti3C2Tx was easy to regenerate and exhibited good recyclability for Cs+ adsorption.

研究领域: 环境科学 · 材料科学
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Journal of Water Process Engineering · 2023 · IF 7

Tannic acid-assisted prussian blue anchoring on membranes for rapid and recyclable removal of cesium

Jiayu Qin,Linxue Yan,Senjian Han,Xiaonan Yang,Yafei Guo,Long Li,Tianlong Deng

As an effective adsorbent, prussian blue (PB) has been used to selectively eliminate radioactive cesium from the complex and change wastewater. Multiple attempts were introduced to refrain from the recovery difficulty of direct application of PB. This study designed a novel strategy of tannic acid (TA) assisted multilayer PB immobilization on a commercial substrate for cesium adsorption. As an effective binder, TA-Fe was successfully applied to immobilize and disperse PB to increase the number of active particles. The resulting composite membrane (M TA-PB ) showed excellent cesium selectivity with a high K d value of 8986 mL/g in geothermal water and maintained its cesium adsorption ability after 5 cycles. Compared with the reported PB powder, the loaded PB gave full play to the adsorption performance. The convenient fabrication method and effective removal of Cs from complex solutions demonstrated that the M TA-PB has excellent potential for practical application in low wastewater concentrations.

CAS / MDL: 1401-55-4
研究领域: 环境科学 · 材料科学
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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 Environmental Chemical Engineering · 2024 · IF 7.4

Highly selective capture of cesium using an electrochemically renewable molybdenum-based crystalline adsorbent

Yangyang Bian,Yi Qiu,Jianfeng Zhang,Qiyu Meng,Li Wang,Shan Ni,Huizhou Liu,Liangrong Yang

The development of highly efficient adsorbents for the capture of 133 Cs and the removal of radioactive isotope 137 Cs from complex aqueous solutions is crucial for the chemical production and environmental remediation. Herein, Mo-based crystalline adsorbent with sub-nanometer (5.76 Å) channels was successfully prepared and used in electrochemically controlled Cs + separation process. Crystalline structures of MoIC (HNO 3 ) before and after adsorption of Cs + were clearly elucidated using powder X-ray diffractometer (PXRD). A more environmentally friendly electrochemical method was employed to achieve easy release and recapture of Cs + . Adsorption comparison experiments revealed that our material clearly outperforms the reported adsorbents for the removal or recovery of trace amount of Cs + (< 10 mg L −1 ). Furthermore, MoIC (HNO 3 ) also exhibited excellent selectivity for low concentration of Cs + over highly excess of competitive cations, such as Mg 2+ , Ca 2+ and K + , which are commonly distributed in brines. The maximum separation factors of Cs + /Mg 2+ , Cs + /Ca 2+ and Cs + /K + are 1.2 × 10 5 , 1.3 × 10 4 and 66, respectively. The remarkable selectivity can be attributed to the outstanding ion-sieving ability of sub-nanometer channels based on the differences in ionic radius and hydration energy of these cations. A real brine was introduced to further prove that one complete cycle of electrochemical adsorption and desorption can dramatically reduce the competing ions concentrations up to 980 times. We anticipate that our findings may give the prospect of opening up new path for the efficient separation of Cs + from brines using molybdenum-based adsorbent via electrochemically controlled process as a green and sustainable way.

CAS / MDL: 68-12-2
研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2022 · IF 11.072

Novel layered iron antimony thiostannate adsorbent of K1.61Fe0.04Sb0.03Sn3.1S7 for cesium green recovery from geothermal water

Zhenzhen Jiang,Chi Ma,Yanqing He,Mingli Li,Gaoling Liu,Yafei Guo,Duo Ji,Tianlong Deng

To develop a green and efficient cesium adsorbent with high adsorption capacity , rapid kinetics, and good regeneration performance is a tremendous challenge. In this work, potassium iron antimony thiostannate (PIATS) synthesized by the hydrothermal method was utilized for green recovery cesium from geothermal water for the first time. PIATS showed a high adsorption capacity of 401.23 mg/g, which was much higher than other types of adsorbents at present. Meanwhile, PIATS showed rapid ion exchange kinetics (within 3 min) and broad pH resistance (4–12). More importantly, PIATS still showed excellent selectivity to cesium even in geothermal water containing many other coexisted ions ( K d  = 1.96 × 10 4  mL/g), and the separation factors between Cs + and the coexisted competing ions were ranged from 462.77 to 963.76. Subsequently, the cesium-laden PIATS could be easily eluted with 0.50 mol/L NaNO 3 to achieve rapid desorption (within 10 min). The concentration of Cs + in the elution was enriched more than 11 times higher than that in the original solution. Furthermore, no organic solvents or other toxic reagents were involved during the whole process. Therefore, the adsorption advantages, excellent enrichment ability, and structural stability of PIATS make it a potential recyclable candidate for green cesium recovery from geothermal water.

研究领域: 环境科学 · 材料科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2023 ·Vol. 332 ·期 4 ·1263-1275 · IF 1.6

Systematic effect of different external metals of hexacyanoferrates on cesium adsorption behavior and mechanism

Nong Caiyong,Li Xiaodong,Xu Junhua

This study aims to investigate Cs removal by different external metals hexacyanoferrates M II –Fe PBA (M II : Co, Ni and Cu). Three PBAs were synthesized, characterized and followed by batch experiment testing and model fitting. Among the three PBAs, Cu–Fe PBA possessed the highest capacity 234.28 mg g −1 , the highest K d 2.8 × 10 6  mL g −1 and the fastest adsorption kinetics on Cs removal. Moreover, Cu–Fe PBA and Ni–Fe PBA were the more selective sorbents in coexisting ions study. Finally, the adsorption mechanism was proposed. This study provides new insights into the vacancies effect of the PBA structure and Cs adsorption application.

CAS / MDL: 7647-17-8 10026-22-9
研究领域: 环境科学 · 材料科学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2024 · IF 6.9

Enhanced cesium removal from wastewater using a potassium hexacyanoferrate/gelatin aerogel composite

Dongjun Chen,Juan Liu,Zhen Qian,Yunpeng Xiao,Yifan Liu,Yuancai Lv,Xiaoxia Ye,Chunxiang Lin

In the wake of the 2011 Fukushima nuclear disaster, the presence of radioactive cesium ( 137 Cs) in nuclear wastewater has posed a critical and enduring health risk. Addressing this challenge, we have synthesized a gelatin aerogel, denoted as KCuFC/GA, immobilized with potassium cupric ferrocyanide (KCuFC) through an in situ approach, aiming for the efficient extraction of 137 Cs from aqueous environments. This novel aerogel's rich porous structure enhances the accessibility of adsorption sites, thereby significantly promoting the capture of Cs + . The adsorption of cesium onto KCuFC/GA was investigated under various experimental conditions, including initial solution pH, contact time, initial cesium concentration, and the presence of coexisting ions (K + , Na + , Ca 2+ , Mg 2+ , Sr 2+ ). The results indicated that the adsorption performance was largely independent of pH, achieving a high cesium removal rate of 93.4 % within the first 5 minutes. The cesium adsorption data were well-described by the Langmuir adsorption model, indicating a maximum adsorption capacity of 222.22 mg·L −1 . Furthermore, in the presence of various competing ions, KCuFC/GA has demonstrated unparalleled selectivity for Cs + , with a partition coefficient ( K d ) of 2.49 × 10 5 mL·g −1 , and has sustained its adsorptive properties across five cycles of use. Through systematic investigation, including X-ray photoelectron spectroscopy (XPS) analysis, we have elucidated the adsorption mechanism, highlighting the pivotal role of ion exchange between lattice K + and Cs + . The straightforward fabrication process and the aerogel's robust cesium removal capabilities from complex solutions indicate that KCuFC/GA is a promising candidate for real-world applications in the treatment of radioactive wastewater.

研究领域: 环境科学 · 材料科学 · 核能工程
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2016 ·Vol. 311 ·期 3 ·1577-1591 · IF 0.983

Preparation of a novel microsphere adsorbent of prussian blue capsulated in carboxymethyl cellulose sodium for Cs(I) removal from contaminated water

Zong Youli,Zhang Yongde,Lin Xiaoyan,Ye Dong,Luo Xuegang,Wang Jing

A novel microsphere adsorbent based upon carboxymethyl cellulose sodium/prussian blue composite loaded with Lanthanum(III) (CMC/PB-La) was successfully synthesized via electrostatic ejection device for removal of cesium from contaminated water, and characterized by FT-IR, SEM, EDX and XPS. Influencing factors to adsorption cesium were investigated, including solution pH, adsorbent dosage, contact time, initial concentration, temperature and competing ions. Linear Freundlich isotherm was fitted satisfactorily to the adsorption data, and the adsorption kinetic data was fitted well with pseudo-second-order model. Moreover, the results of γ-irradiation experiments indicate that CMC/PB-La has good radiation stability.

CAS / MDL: 9004-32-4
研究领域: 环境科学 · 材料科学
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Journal of Water Process Engineering · 2022 · IF 7.34

Highly selective and easily regenerated novel porous polyacrylonitrile-ammonium phosphomolybdate beads for cesium removal from geothermal water

Qi Liu,Haojie Ge,Can Liu,Ningluo Zhang,Yafei Guo,Tianlong Deng

A novel porogen-added ammonium phosphomolybdate-polyacrylonitrile (AMP-PAN-N20) was prepared to remove Cs + from geothermal water. Compared with traditional AMP-PAN, porous AMP-PAN-N20 beads have a smaller particle size, larger adsorption capacity and faster adsorption rate. The adsorption batch experiments were carried out with the research objects' adsorbent contact time, dosage, pH value, initial Cs + concentration, temperature and competing ions. The results showed that AMP-PAN-N20 could effectively adsorb Cs + in a wide pH range and high concentration of competing ions. Remarkably, the adsorption performance hardly decreased after ten cycles of adsorption. In addition, the column adsorption tests were obtained using Cs-containing geothermal water. The results showed that the adsorption breakthrough time could be as long as 60 h (flow rate Q  = 2 mL·min −1 , bed height H  = 8 cm), and the maximum dynamic adsorption capacity was 25.62 mg·g −1 under the Thomas model. In addition, the AMP-PAN-N20 maintained good stability after a long time of adsorption.

研究领域: 环境科学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2024 · IF 2.7

Preparation of a copper-substituted Prussian blue analogue-immobilized membrane suitable for efficient Cs removal in complex geothermal water

Hengxi Wang,Xiaonan Yang,Lijun Meng,Senjian Han,Shiqiang Wang,Yafei Guo,Tianlong Deng

Prussian blue analogue (PBA) membranes for efficient Cs removal via in situ synthesis have attracted much interest. Herein, copper-substituted PBA was developed and optimized on the surface of a substrate with the aid of tannic acid (TA). The fabricated Cu-PBA-TA membrane was systematically investigated for its Cs adsorption property in static and dynamic experiments. The as-prepared membrane showed a maximum adsorption capacity of 265.0 mg g−1, which was the highest when compared to that of previously reported PBA membranes. Applied in geothermal water, the Cu-PBA-TA membrane showed favorable selectivity (Kd, 8680 mL g−1) and the removal rate of Cs+ was about 90%. Its fast adsorption rate that reached equilibrium within 40 min and the benign reusability in the dynamic treatment of geothermal water confirmed the potential of the membrane for large-scale application.

研究领域: 环境科学 · 材料科学
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