MOLECULES
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2023
·Vol. 28
·期 1
·449
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IF 4.6
Canran Wang,Shan Jiang,Wenyue Ma,Zhaoyang Liu,Leijing Liu,Yongcun Zou,Bin Xu,Wenjing Tian
Radioactive iodine-capturing materials are urgently needed for the emerging challenges in nuclear waste disposal. The various pore structures of covalent organic frameworks (COFs) render them promising candidates for efficient iodine adsorption. However, the detailed structure–property relationship of COFs in iodine adsorption remains elusive. Herein, two polymorphic COFs with significantly different crystalline structures are obtained based on the same building blocks with varied molecular ratios. The two COFs both have high crystallinity, high specific surface area, and excellent chemical and thermal stability. Compared with the [C4+C4] topology (PyT-2) with an AA stacking form, the [C4+C2] topology (PyT-1) with an AB stacking form has more twisted pore channels and complex ink-bottle pores. At ambient conditions, PyT-1 and PyT-2 both exhibit good adsorption properties for iodine capture either in a gaseous or liquid medium. Remarkably, PyT-1 presents an excellent maximum adsorption capacity (0.635 g g−1), and the adsorption limit of PyT-2 is 0.445 g g−1in ann-hexane solution with an iodine concentration of 400 mg L−1, which is highly comparable to the state-of-the-art iodine absorption performance. This study provides a guide for the future molecular design strategy toward novel iodine adsorbents.Keywords:covalent organic framework;polymorphism;iodine adsorption
研究领域:
材料科学
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化学工程
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-8
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IF 14.919
Lei Yuting,Zhang Guihua,Zhang Qinglan,Yu Ling,Li Hua,Yu Haili,He Yi
Zeolitic imidazolate frameworks (ZIFs) are very useful as high-capacity iodine (I 2 ) adsorbents. The adsorption performance is usually probed by measuring a statistical average property over an entire sample consisting of a large number of ZIF particles, leaving the interparticle heterogeneity information among individuals. Here we report a dark-field microscopy (DFM) method to visualize gaseous I 2 adsorption on single ZIF-90 particles in situ and in real time. The adsorption of I 2 is found to alter the scattering spectrum of ZIF-90 particles, inducing a distinct color change from bluewhite to yellow. According to correlating the adsorption amount of gaseous I 2 with the change of B value from DFM images, we quantitatively image the adsorption process and estimate the related kinetic parameters at the single particle level. Single particle measurements clarify the large particle-to-particle heterogeneity in adsorption reactivity and significant adsorption activity improvement of ZIF-90 after introduction of linker defects, which provides a microscopic understanding of the structure-activity relationship. We further demonstrate the capacity of this strategy for studying gaseous I 2 adsorption on single ZIF-91 particle as a derivative of ZIF-90 to illustrate the generality.
研究领域:
材料科学
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化学
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PubMed
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Chang Liu,Xiaowei An,Peifen Wang,Xuli Ma,Xingfa Li,Xin Chen,Yongguo Li,Xiaogang Hao,Xiaoxu Zhang,Abuliti Abudula,Guoqing Guan
In this study, a highly efficient and cost-effective adsorbent for gaseous iodine, nitrogen-doped KOH-activated coconut shell biochar (NKBC), is presented. A two-step pore expansion assisted by KOH activation process, enhanced by nitrogen doping, created a hierarchical porous structure with ultra-high specific surface area of 2977.90 m 2 /g, large total pore volume of 2.19 cm 3 /g and available micropore volume of 1.17 cm 3 /g, resulting in an iodine adsorption capacity of 6635 mg/g at 75℃ within 3 hours. The low desorption rate (12.93 % at room temperature) highlights the material's stability. Grey relational analysis identified specific surface area and pore structure as key determinants of adsorption capacity, while pore size distribution and nitrogen content significantly influenced desorption. DFT calculations confirmed the enhanced iodine adsorption by nitrogen functionalities and the effectiveness of micro- and narrow mesopores in iodine capture. This sustainable approach offers a significant advancement in developing high-capacity adsorbents for the effective remediation of radioactive iodine.
研究领域:
环境科学
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材料科学
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INORGANIC CHEMISTRY
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2021
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IF 5.165
Amir Said,Chang Gao,Caiyun Liu,Huihui Niu,Dexin Wang,Yanshu Liu,Lin Du,Chen-Ho Tung,Yifeng Wang
A three-dimensional (3D) mesoporous material with an atomically precise structure, Ti16Pb5O16(C6H5CO2)2(OCH3)40 (Ti16Pb5), comprised of a novel high-nuclearity Pb-doped titanium oxide cluster (TOC), was synthesized. Ti16Pb5 exhibited a surface area of 45 m2 g–1 and a pore diameter of 3.5 nm. It exhibited an uptake capacity of I2 of ≤2.2 g g–1 in vapor, and the performance was maintained after seven uptake–release cycles. Ti16Pb5 also showed a high adsorption ratio and capacity (93% and 3.1 g g–1) in hexane. The characterization data, including Fourier transform infrared, Raman, and powder X-ray diffraction, suggested the lattice structure of Ti16Pb5 was rigid and I2 was accommodated in the pores of Ti16Pb5. To the best of our knowledge, this is the first example of using a TOC in I2 adsorption. In addition, Ti16Pb5 showed excellent activity and recyclability in visible-light degradation of dye pollutants and photocurrent generation. Our structural analysis suggested the alkoxide ligands within the channels of Ti16Pb5 build up a confined polar environment and thereby facilitate I2 accommodation, and meanwhile, the improved performances and stabilities of Ti16Pb5 are correlated with its cluster-based, 3D hierarchical structure.
研究领域:
材料科学
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环境科学
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高影响因子
APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Xinqi Liu,Huiling Yuan,Qian Zheng,Bingyuan Huang,Fang Liao,Hejun Gao,Hongquan Fu,Juan Zhang,Yunwen Liao
The effective capture and storage of radioactive iodine is of great significance to the safe use of nuclear energy. In this study, nitrogen- and oxygen-doped carbon nanotubes acted as effective iodine capture agents in a low concentration of iodine solution of approximately 100 mg L −1 . The iodine uptake capacity is proportionate to hydroxy-functional groups as oxygen species and graphitic nitrogen as nitrogen species, respectively, rather than defects and the specific surface area of carbon nanotubes. The essential adsorption activity of oxygen-doped carbon nanotubes is more than 2.5 times that of nitrogen-doped carbon nanotubes, indicating oxygen-doped carbon nanotubes as a potential carbon material in practical applications for the adsorption of iodine. Theoretical study further deepened the understanding of the iodine adsorption sites on carbon nanotubes. This work provided a new method for the design and synthesis of high-performance radioactive iodine solid adsorbents in the future.
研究领域:
材料科学
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环境科学
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核能安全
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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
Linshuai Liu,Nannan Wang,Chunlin He,Yuezhou Wei,Jingjing Wang,Xinpeng Wang
Considering the unexpected nuclear power waste emission and potential nuclear leakage, the exploration of robust materials for the effective capture and storage of radioactive iodine is of great importance but still remains a challenge. In this work, we report the rational synthesis of functionalized NH 2 -UiO-66-on-ZIF-67 architecture to enhance the static adsorption and retention of volatile iodine. Such MOF-on-MOF heterostructures was fabricated through seeding ZIF-67 core on the surface of NH 2 -UiO-66 satellite via a facile polyvinylpyrrolidone (PVP) regulated internal extended growth strategies. NH 2 -UiO-66-on-ZIF-67 exhibited unique core-satellite structure, which significantly promotes the binding interactions with iodine through synergizing of the N-rich imidazole moieties and surface functionalized amino groups within the porosity channels. As a result, the as fabricated NH 2 -UiO-66-on-ZIF-67 achieves enhanced mass diffusion and high capture capacity of 3600 mg/g for iodine vapor under static sorption conditions. Moreover, water vapor in humid conditions (relative humidity of 18 %) has almost no effect on the static iodine adsorption performance of the material. This study sheds light on a reliable MOF-on-MOF hybrid strategy for effective radioiodine treatment to ensure the safety nuclear waste management.
研究领域:
材料科学
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环境科学
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高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Yunchao Ma,Shengnan Qi,Yuxin Yao,Chuanxue You,Chunbo Liu,Baixiang Ren
Covalent organic frameworks (COFs) are widely used for gaseous radioiodine capture through distinctive properties. Herein, 2D fluorinated imine COF (JLNU-316) was designed and constructed in this study. JLNU-316 exhibited large BET surface area of 596.25 mg 2 /g and pore size (2.74 and 3.78 nm), excellent thermal and chemical stability. The adsorption of iodine by JLNU-316 reached 4.08 g/g, which exceeded most of the current fluorine-containing porous iodine adsorption materials. Furthermore, the iodine adsorption capacity remains at 99 % after seven days of exposure to air conditions, and JLNU-316 maintains stable performance following ten cycles. The introduction of heteroatoms enhanced the stability of JLNU-316 and enriched the adsorption sites, thereby increasing the iodine adsorption capacity. This study guides for the design and preparation of novel iodine adsorbents.
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
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Shiyan Sun,Xuefeng Sha,Jie Liang,Guang Yang,Xin Hu,Ziyang He,Meiying Liu,Naigen Zhou,Xiaoyong Zhang,Yen Wei
The adsorption applications of MXene-based adsorbents have intensively investigated recently. However, the performance of MXene-based adsorbents has been largely limited owing to their lack of functional groups and adsorptive sites. Therefore, surface functionalization of MXene is an important route to achieve better performance for environmental adsorption. Herein, polyionic liquid functionalized MXene (named as MXene-PIL) was prepared through a multi-component reaction and adsorptive removal of iodine by MXene-PIL was also evaluated. The successful generation of PIL on MXene was confirmed by a series of characterization measurements. Furthermore, the effects of contact time, iodine concentration, environmental temperature and other factors on the adsorption performance of MXene-PIL were investigated. Adsorption kinetic analysis including pseudo-first-order dynamic model, pseudo-second-order dynamic model and Weber-Morris model, adsorption thermodynamic analysis such as Langmuir and Freundlich models and Van’t Hoff equation were used for further analysis the adsorption behavior of iodine by MXene-PIL. We demonstrated that the adsorption capacity could be as high as about 170 mg/g, which is obviously larger than the unmodified MXene and most of other reported adsorbents. Taken together, a simple strategy has been developed for in-situ generation of PIL on MXene and the resultant composites show potential application for adsorptive removal of iodine.
研究领域:
材料科学
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环境科学
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高影响因子
JOURNAL OF ENVIRONMENTAL RADIOACTIVITY
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2022
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IF 2.655
Sheng Liu,Yiyang Zeng,Ai Zhang,Yuxin Song,Yuran Ni,Jiamao Li,Fangting Chi,Chengjian Xiao
Due to the rapid diffusion of radioactive iodine, the demand for safe and efficient capture and storage of radioactive iodine is increasing worldwide. The use of porous carbon materials to capture iodine has aroused great interest. This work prepared porous carbon materials derived from polymetallic oxides of the zeolitic imidazolate framework (ZIF) by pyrolysis at 1000 °C. The carbon materials (CZIF-1000) have a high specific surface area of about 1110 m 2 /g and a total pore volume of 0.92 cm 3 /g. Adsorption studies have shown that the CZIF-1000 had significant adsorption performance for iodine, and the adsorption capacity can reach 790.8 mg/g at 8h. The potential mechanism of adsorption is that the carbonization causes the charge-transfer interaction and pore size distribution. Compared with the conventional adsorbents, the adsorbents showed faster kinetics and high extraction capacity for iodine. This experiment provides an effective method for designing a highly efficient adsorbent for iodine and broadens the ideas for developing new iodine extraction adsorbents.
研究领域:
材料科学
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环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Sheng Liu,Yiyang Zeng,Jun Liu,Jiamao Li,Hao Peng,Hui Xie,Hao Zou,Chengjian Xiao,Xiaohui Hua,Jingliang Bao,Liang Xian,Yuanli Li,Fangting Chi
The capturing and storage of iodine from nuclear waste through secure and advantageous techniques are significant. In this work, a novel bismuth-based porous carbon material referred to as Bi@MVF is elaborately synthesized employing a dipping-reduction technique to seize iodine-129 ( 129 I), in which bismuth particles are uniformly embedded and allotted on the porous carbon network as multiple active sites. Accordingly, Bi@MVF lets in a highly-efficient iodine absorption potential of up to 1560 mg/g after publicity to iodine at 120 ℃ for 4 h, superior to most standard iodine adsorbents. The excessive adsorption kinetics of these Bi@MVF adsorbents is typically attributed to the specific porous carbon substrates' full-size particular surface area and the adsorbent’s synergistic effect. An in-depth perception of the iodine adsorption mechanism exhibits that the chemical adsorption turns into a powerful mechanism via the reaction between bismuth and iodine to structure a steady section BiI 3 . Moreover, an easy post-treatment system for these Bi@MVF adsorbents is adopted to gain the greater corrosion-resistant iodine-binding segment Bi 5 O 7 I, attaining a nominal iodine leaching rate. Therefore, the designed Bi@MVF will be a tremendous 129 I stabilizer, and we will contribute a new approach for customizing new iodine adsorbents with excessive adsorption doses.
研究领域:
材料科学
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环境科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zhichun Shi,Haoyuan Tang,Liqiu Sun,Jianjun Wang,Jun Li,Dan Wang,Liying Qi,Liyan Wang,Guohua Dong,Ming Zhao
Designing and preparing of materials for highly efficient and reversible iodine adsorption remains a challenging task. In this study, a series of benzonquanmine-based hypercrosslinked polymers (BHCPs) with nitrogen-rich were designed and synthesized via Friedel-Crafts reaction. The obtained BHCPs showed the high specific surface and high thermal stability. Moreover, the BHCP-3 of BHCPs exhibits excellent iodine capture performance, including ultrahigh iodine vapor adsorption capacity of 619 wt%, the breakthrough iodine experiment of the adsorption capacity reached 2.29 g/g, which is the highest published capacity of HCP adsorbent. And the removal rate of iodine in aqueous solution also reached 92.5 %, and reached 87.4 % the first 10 min, demonstrating rapid adsorption effects. Additionally, the iodine adsorption process of BHCPs conformed to the pseudo-second-order kinetic models, and which were a multi-layer adsorption on non-homogeneous surfaces. Furthermore, the three adsorbents maintained more than 85 % of their iodine capture capacity after five cycles, demonstrating their good recyclability and potential for practical applications.
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
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2024
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IF 1.2
Min Li,Qing Li,Lijie Li,Zixuan Xu,Jie An,Gaohong He,Zhifang Wu,Sijin Li,Wenjun Zhang
Radioactive iodine waste generated from nuclear power and radioactive medical treatments has become a serious environmental issue, raising concerns about public health. Cross-linked chitosan adsorbed iodide anions through electrostatic attraction yet limit-efficiently. To achieve better adsorption performance, chitosan-coated cuprous oxide microspheres (Cu₂O@CM) was proposed via one-step in-situ liquid-phase method. Both Cu₂O@CM-e cross-linked with epichlorohydrin and Cu₂O@CM-g cross-linked with glutaraldehyde, performing rough and spherical morphology, exhibited rapid iodine removal capacities of 0.1843 mmol/g for Cu₂O@CM-e and 0.1819 mmol/g for Cu₂O@CM-g within just 10 min. The adsorption process occurred through a combination of physical multilayer adsorption and chemical monolayer adsorption, driven spontaneously and endothermically. After four regeneration cycles, Cu₂O@CM-e and Cu₂O@CM-g maintained almost identical adsorption efficiencies, highlighting their reusability. Considering the interference of Cl⁻ and CO₃²⁻, both adsorbents showed significant selectivity towards competing ions. Thus, both adsorbents showed promising potential for the removal of iodine waste
研究领域:
环境科学
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材料科学
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高影响因子
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