CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Guangyuan Chen,Linzhen Wu,Zeru Wang,Ruixi Liu,Chuan Tan,Yi Tan,Yawen Liu,Miaomiao He,Hao Zhang,Yikun Huang,Jiongzhi Zhu,Tao Duan,Lin Zhu
The capture of radioactive gaseous iodine is essential for the sustainable development of nuclear energy and the long-term safe supply of nuclear fuel. However, the presence of nitrogen oxides in the exhaust gas generated during spent fuel reprocessing poses significant challenges to the stability of iodine adsorbents. It is crucial to consider the impact of NOx on the structure and adsorption performance of the materials. We report here the development of an aluminum-based metal–organic framework (MOF), CAU-1, engineered for efficient iodine capture. Synthesized through a cost-effective and straightforward method, CAU-1 exhibits excellent structural stability and robust adsorption performance, with a maximum iodine vapor adsorption capacity of 1277.18 mg/g at 130 °C and methyl iodide adsorption capacity of 533.10 mg/g, highlighting its potential for efficient iodine vapor removal. Notably, CAU-1 retains its structural integrity and iodine adsorption performance even in the presence of 5 % NO 2 , maintaining high adsorption capacities for I 2 (1129.41 mg/g) and CH 3 I (436.79 mg/g). Mechanistic analysis revealed the key role of the –NH 2 group in the iodine adsorption process. Additionally, co-adsorption studies with I 2 and NO 2 showed that CAU-1 can still capture iodine in the form of both I 2 and I 3 - in the presence of NO 2 . This study illustrates the potential of CAU-1 as an effective industrial adsorbent for removing iodine from NO 2 -containing gas streams.
研究领域:
材料科学
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核能工程
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Han Dong,Pu Zhou,Fan Yang,Enhao Zhang,Yifan Liu,Yefei Tian,Hongye Yuan
The development of metal–organic framework (MOF)-based adsorbents with high uptake capacity and mild regeneration conditions represents a promising avenue for addressing environment-based issues. In this study, we present the successful synthesis of temperature-responsive composite aerogels comprising MOF-808 and poly(N-isopropylacrylamide) (PNIPAM), which forms interpenetrated networks with acrylamide (AM). The resulting thermally responsive PNIPAM/MOF-808 composite aerogels achieved an impressive maximum water capture exceeding 2267 wt % at room temperature, with reversible release observed above 32 °C due to the hydrophilicity–hydrophobicity transition of PNIPAM. Interestingly, the aerogels also exhibit an iodine (I2) capacity of 234 wt % based on the charge transfer mechanism. This study provides a novel strategy for the preparation of efficient and reusable porous adsorbent materials, and it also demonstrates broad application prospects in areas such as water resource management and waste reduction.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2019
·Vol. 55
·期 4
·1854-1864
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IF 3.442
Zhang Zhizhong,Li Liang,An Duo,Li Hanxue,Zhang Xinghua
Novel triazine-based covalent organic polycalix[4]arenes, CalCOPs, were synthesized via the copolymerization of calix[4]arene derivatives and 2,4,6-trichloro-1,3,5-triazine (TCT) or 2,4-dichloro-1,3,5-triazine (DCT). The resulting CalCOPs have permanent pores that can be regulated by the variation of the alkyl chain lengths of the calixarene backbones and the reaction sites. With the alkyl chain length at the low rim in calixarene units increasing from ethyl to butyl during the reaction, the Brunauer–Emmett–Teller surface areas decrease with surface areas of 280, 31.5, 18.4 and 1.6 m 2 g −1 obtained for CalCOP1, CalCOP2, CalCOP3 and CalCOP4, respectively. Among these CalCOPs, CalCOP1 shows ultrahigh absorption for iodine capture in a water solution with an uptake of up to 232 wt%. Furthermore, the adsorption and release efficiency of iodine were obtained by using the UV–Vis spectroscopy. In addition, these polymers can be recycled at least five times while maintaining high removal capacity, suggesting that CalCOPs are ideal absorbent materials for reversible iodine capture in the mitigation of environmental issues.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Zengming Tang,Dong Xie,Suzhe Li,Xiaomin Yang
Finding an inexpensive and efficient porous adsorbent to capture the gaseous radioiodine generated during spent fuel reprocessing has been challenging. Herein, we present a design philosophy for waste control to develop porous carbon for gaseous iodine capture from sewage sludge waste. Among them, the novel in situ etching of polytetrafluoroethylene was employed to improve pore accessibility. The hazards of the conventional preparation of sludge-derived carbon using highly corrosive NaOH and HF solutions were overcome. Polytetrafluoroethylene etched porous carbon with large specific surface area (1103 m 2 /g), interconnected hierarchical porous structure, and excellent hydrophobicity (water contact angle 126.52°), providing efficient adsorption of gaseous iodine in hot (30–150 °C) and humid (50–96% relative humidity [RH]) environments. The iodine adsorption of hierarchical porous carbon was tested under static and dynamic conditions, and high records have been achieved. Notably, due to the structural advantage of hydrophobicity, a considerable dynamic adsorption capacity (1746.77 mg/g) was also maintained in a mixed iodine gas stream containing water vapor in a humid (50% RH) hot (75 °C) condition. This study is the first to use an in situ etching strategy for polytetrafluoroethylene, which opens a new avenue for converting sludge waste into low-cost porous carbon and provides an attractive option for capturing iodine in hot and humid environments.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
INORGANICA CHIMICA ACTA
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2024
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IF 2.7
Guang-Li Zhou,Bo-Wen Liu,Guang-Yu Cui,Wei Zhang,Ji-Min Yang
Radioactive iodine waste from the nuclear industry poses a critical threat to human health, and its effective capture has become an important research topic. In this study, modified UiO-66-X adsorbents (where X is ATA, BTA, or STA) were used to investigate the effects of the free functional groups in the UiO-66 skeleton on iodine capture in the vapor and solution states. The adsorption behavior revealed that the capture efficiency of UiO-66-ATA was substantially higher than that of UiO-66-BTA and UiO-66-STA because the electron-donating amino groups could enhance the I − I···π halogen bond interactions compared with the electron-withdrawing carboxyl and sulfonic acid groups. In addition, the pore volume of UiO-66-ATA was significantly higher than those of UiO-66-BTA and UiO-66-STA. In particular, the removal uptakes of UiO-66-ATA were 1108.1 mg/g (vapor phase) and 3601.9 mg/g (aqueous solution). This study is the first to investigate the effects of functional groups on the adsorption uptake of UiO-66 toward iodine. This efficient functional group modification strategy holds significant promise for the development of novel metal–organic framework adsorbents.
研究领域:
材料科学
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环境科学
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核能工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Qian Zhao,Xin Li,Guangyuan Chen,Zeru Wang,Chuan Tan,Cheng Liu,Hao Zou,Jing Ma,Lin Zhu,Tao Duan
Effective capture of radioactive iodine from nuclear fuel reprocessing is of great importance for public safety as well as the secure utility of nuclear energy. In this work, a hydrophobic nanosheet silicalite-1 (NSL-1) zeolite with an adjustable size was developed for efficient iodine (I 2 ) and methyl iodide (CH 3 I) adsorption. The optimized all-silica zeolite NSL-1 exhibits an excellent I 2 uptake capacity of 553 mg/g within 45 min and a CH 3 I uptake capacity of 262 mg/g within 1 h. Benefiting from the reduced thickness and enhanced porosity, microporous NSL-1 possesses enhanced iodine adsorption capacity and fast adsorption kinetics , which is a considerable high value among inorganic materials . Unexpectedly, the remarkable characters of high hydrophobicity , acid-resistance and anti-oxidation endow it a higher iodine uptake capacity than traditional aluminosilicate zeolites. More importantly, the high uptake selectivity toward I 2 possessed by NSL-1 owing to its hydrophobic skeleton under simulated dynamic conditions. The low cost, facile and scalable synthesis of NSL-1 further highlights great prospects for applications in the nuclear industry. This work provides useful insights for designing efficient adsorbents for iodine capture .
研究领域:
材料科学
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核能工程
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环境科学
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DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Xiaoping Li,Xinpeng Wang,Lei Dong,Qing Zou,Chunlin He,Yanqiu Zhu,Toyohisa Fujita,Changzhong Liao,Cheng-Wei Kao,Ying-Rui Lu
As the main fission products of nuclear power plants, radioactive iodine isotopes are of great concern because of their great harm to public safety. In this work, a nanocomposite of bismuth sulfide coated with the electrospinning SiO2 nanofibers with a diameter of about 280 nm nanostructure-based membranes (Bi2S3@SiO2) was successfully prepared to dispose of gaseous iodine. Results showed that the adsorption capacity of Bi2S3@SiO2 for iodine can be up to 1180 mg g–1, which is higher than the commercial silver-exchanged zeolite (AgZ) and other bismuth-based adsorbents. Chemisorption is the major adsorption behavior of iodine capture. Thermogravimetric analysis results demonstrated that the Bi2S3@SiO2 nanocomposites were stable up to 300 °C before and after capturing iodine. X-ray diffraction results revealed that BiSI was initially formed and then transformed to BiI3. Scanning electron microscopy revealed that the sulfur element remains in the samples after interacting with iodine, and X-ray absorption near-edge spectra further confirmed that its oxidation states are a mixture of S0, S3+, and S6+. The oxidation states of bismuth and iodine are Bi3+ and I–, respectively, revealed by X-ray photoelectron spectroscopy. The reactions between Bi2S3@SiO2 nanocomposites and I2 vapor are as follows: I2 was reduced to be I– and the BiI3 crystalline phase is the final form; S2– in Bi2S3 was oxidized to higher valences (S0, S3+, and S6+), and amorphous phases are their final forms. The research results demonstrated that the nanostructure-based membranes prepared by this work would be a promising candidate nanomaterial for capturing iodine in the plant off-gas streams.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Zengming Tang,Dong Xie,Suzhe Li
Activated carbon fibers (ACF) are widely used to remove gaseous radioiodine produced during spent fuel reprocessing owing to their excellent adsorption properties. However, ACF's strong affinity for moisture tends to dominate, significantly reducing its ability to capture iodine in humid environments. The study used a one-step facile modification method of spray-deposited poly(divinylbenzene) (PDVB) nanoparticles on ACF to prepare hydrophobic activated carbon fiber (ACF-PDVB1.5). Compared to the initial ACF, the ACF-PDVB1.5 enhances the specific surface area to 1571 m 2 /g while maintaining abundant active sites, overcoming the disadvantage of pore reduction caused by traditional modification methods. More importantly, they also have excellent acid and alkali resistance and hydrophobicity (water contact angle 131.1°), with a preference for I 2 pores (97 % microporosity). The iodine capture capacity of ACF PDVB 1.5 showed a significant increase compared to the initial ACF, as indicated by both static and dynamic adsorption tests. Notably, the dynamic iodine adsorption capacity of ACF-PDVB1.5 in a mixed iodine-water vapor stream at actual temperature (75 °C) and humid (50 % RH) conditions was 1847.69 mg/g, an increase of 55.47 % over the capacity of initial ACF (1188.71 mg/g). This work improves the overall I 2 adsorption performance through hydrophobicity and pore size coordination.
研究领域:
材料科学
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环境工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ya-Nan Yu,Wei-Min Ma,Jia-Xin Wu,Qian Zhang,Jie Zhou,Ke-Ke Jiang,Dan-Dan Wang,Yong-Kang Li,Yang-Min Ma,Zheng Yin
The radioactive iodine as highly harmful fission waste from nuclear power production features fifteen-million years radiation period and easy diffusion, yet its efficient treatment and sensing is greatly challenged by the operation concentration as low as several ppm in gaseous and aqueous medium. A (3,12)-connected and [Pb 6 ( µ 4 -O) 2 (COO) 8 ] based MOFs of [Pb 6 ( μ 4 -O) 2 (pia) 4 ]·4DMF ( 1 ) was rationally constructed as a multifunctional materials for iodine capture and sensing, which possesses the highest void fraction of 34.4 % among all known cluster based Pb-MOFs. Microwave-assistant solvothermal reaction facilitates gram-scale synthesis of 1 with yield of 82 % within 4 h. The 1D round channels sized at 1.0 nm coupled with high structure stability of the MOFs contribute to accommodate iodine. 1 can rapidly capture iodine vapor at 70 °C in 6 h with fully utilized nanopores, resulting in a high iodine packing density of 3.52 g cm −3 closely matching that of iodine single crystal. Particularly, the MOFs of 1 exhibits long-lasting adsorption to iodine vapor at extremely low concentration of 120 ppm, as well as efficient capture of I 2 in 1.0 × 10 -4 M aqueous solution with removal percentages of 67.1 % in only 20 min, driven by synergistic host–guest interactions. The MOFs is further discovered as a single-phase white-emitting phosphor with quite broad fluorescence spectrum covering the entire visible region, benefited from the multiple Pb···Pb interactions and change-transfer between the metal and ligand. White light emitting diodes can be created by coating commercial blue LEDs with phosphor 1 , generating pure white chromaticity coordinates of (0.313, 0.338), a near daylight color temperature of 6420 K, a high color rendering index of 85 and light maintenance up to 120 °C. The migration of iodine into the channels of 1 led to obvious fluorescence quenching. As the combined result, 1 presents a rare and instructive multifunctional MOFs that exhibiting efficient capture to low-concentration iodine in gaseous/aqueous condition and fluorescent detection to iodine.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Alemtsehay Tesfay Reda,Dongxiang Zhang,Xiyan Xu
The search for efficient material to capture iodine from off-gas streams continues. Herein, a novel composite of lithium aluminate and melamine , abbreviated as LiAlO 2 -Mel, was synthesized and exhibited high vapor iodine capture capacity accompanied by good regeneration ability. The LiAlO 2 -Mel showed an enormous capture capacity of 1281 mg/g within 4 h towards I 2 (g) at 150 °C. The kinetics study showed that the dominant process (at 150 °C) was chemisorption via N∙∙∙I and C–NH∙∙∙I bonding mechanisms. Additionally, LiAlO 2 -Mel has a low surface area (14.6157 m 2 /g) yet produced high capacity, suggesting chemisorption played a critical role. However, physisorption was the dominant process at lower temperature values, as proved by kinetics fittings and activation energy (E a = 23.19 KJ/mol) studies. The kinetics models were validated by statistical error validity models (sum of square error, Chi-square test, and normalized standard deviation). Thermogravimetric analysis and adsorption-desorption experiments showed that the LiAlO 2 -Mel can be recovered by heat treatment (25–800 °C) in N 2 atmosphere and ethanol washout (24 h, 25 °C) of the LiAlO 2 -Mel-I. The high capture capacity, along with eco-friendly and cost-effectiveness, highlights the promising potential of LiAlO 2 -Mel for iodine capture.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
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IF 4.551
Jian Wang,Congcong Wang,Hongchao Wang,Bo Jin,Peiping Zhang,Lina Li,Shiding Miao
The effective capture of radioactive volatile iodine ( 131 I and 129 I) from nuclear waste stream is of vital significance. In this work three kinds of porous organic frameworks (POFs) knitting with N -containing building units were constructed via cost-effective and maneuverable Scholl reaction. The obtained PAFs exhibited moderate porosity and satisfying thermal stability. With coexistence of open porous structure, the electron-rich amino group featured with π-π interactions was found to improve the affinity to iodine, and the iodine uptake capacities were 408 wt%, 335 wt% and 268 wt% when the prepared POFs of P-DPDA, P-TPB and P-PC were employed for the adsorption experiments. The results were superior to most of the porous adsorbents including zeolite , metal-organic frameworks (MOFs) and porous organic polymers (POPs). Iodine adsorption capacities of 289.50 mg g −1 (for P-DPDA), 194.63 mg g −1 (for P-TPB) and 259.69 mg g −1 (for P-PC) in organic solution were achieved, and the adsorbed iodine molecules could be released to ethanol. Such promising and cost-effective materials can be envisaged for application in the field of nuclear waste management.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CELLULOSE
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2022
·Vol. 29
·期 4
·2553-2563
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IF 6.123
Luo Ruiqing,Liu Ruihua,Li Yongqiang,Li Yarong,He Chiyang
The main challenge in developing polymer/covalent organic framework (COF) hybrid matrix membrane is to find effective strategies for strongly attaching crystalline COF to the supporting surface as defect-free membrane layers. In this article, we demonstrated for the first time a method for the preparation of a chitosan (CS)/COF mixed matrix dual-layer membrane based on solvothermal synthesis method. A novel surface modification strategy was developed using p-phthalaldehyde as covalent linkers between COF and CS membrane substrate, and then the nitrogen-containing covalent organic framework (NCOF) membrane was further grown in situ on the modified CS membrane substrate utilizing solvothermal synthesis methods. The resultant CS/NCOF dual-layer membrane exhibited highly homogeneous texture due to the excellent compatibility between NCOF crystals and CS matrixes. The combination of NCOF and CS membrane formed a large number of channels in the nitrogen environment, enabling the CS/NCOF dual-layer membrane to have an enhanced iodine uptake capacity up to 3.15 g/g. Furthermore, the CS/NCOF dual-layer membrane could be recycled at least five times while maintaining 95% iodine capture capacity. These properties make the obtained CS/NCOF dual-layer membrane ideal absorbent material for reversible iodine capture. This ingenious dual-layer membrane preparation strategy provides a new avenue to customize synthesis of novel membrane materials for clean energy and environmental remediation. Graphical abstract
研究领域:
材料科学
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环境科学
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DOI
高影响因子