SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Guodong Li,Guoxun Ji,Xia Wang,Wei Liu,Duo Zhang,Lanhua Chen,Linwei He,Suzhuocheng Liang,Xihai Li,Fuyin Ma,Shuao Wang
Efficient capture and separation of xenon (Xe) and krypton (Kr) from nuclear fuel reprocessing plants is of great significance for the control of discharge of gaseous radioisotopes into the environment. However, due to the similar size and chemically inert spherical properties of Xe/Kr, the discovery of an adsorbent with both high adsorption capacity and high selectivity remains a challenge. Here, we report a microporous MOF (Ni-MOF, [Ni 2 II Ni III (μ 3 -OH)(bdc) 3 (tpt)]·guest) featuring two different cavities with an appropriate triangular hole window size. One is composed of parallel aromatic rings with spacings of approximately 4.3 Å comparable to the kinetic diameter of Xe (4.047 Å), affording excellent binding affinity for Xe while the larger one with narrow pore window provides sufficient space for gas adsorption. The Ni-MOF material exhibits an exceptionally high Xe uptake of 5.43 mmol/g and Xe/Kr selectivity of 7.66 at 298 K and 1 bar. The adsorption capacity is the highest among all MOFs without open-metal-sites. Furthermore, the sorption selectivity of Xe over Kr within Ni-MOF originates from a special sandwiched π-Xe-π interaction revealed by Van der Waals interaction calculations.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Huiyan Li,Gaimei Wang,Kok-Giap Haw,Jialu Li,Huazhen Rong,Hao Ren,Yongyan Deng,Ye Yuan,Guangshan Zhu,Xiaoqin Zou
Xenon is found a wide range of applications in our modern life, and its purification and separation is of paramount importance in industry. For this goal, we have synthesized several porous organic frameworks (POFs) from the perspective of pore chemistry. The prepared materials (CTF-0, PAF-45, PAF-67) show almost identical pore size of ~5.0 Å, appreciable surface areas (528.4–1158.5 m 2 g −1 ), substantial micropore volumes (0.158–0.3 cm 3 g −1 ) and high stabilities (400–600 °C). Adsorption measurements demonstrate that the prepared materials have xenon uptakes in the range of 25.2–62.8 cm 3 g −1 at 1.0 bar and 298 K, and Henry predictions reveal that they are selective for separating xenon from krypton with selectivities of 5.2–8.1. As a representative material, PAF-45 has been tested for xenon separation by the breakthrough experiment, and selectivity of 12.3 for xenon over krypton and xenon capacity of 92.4 mmol kg −1 are obtained.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yu Luo,Zijun Yan,Fenglei Wang,Zining Wang,Min Zhou,Yongdong Jin,Yuanhua Wang,Chuanqin Xia
The reduction of environmental pollution and the exploration of economic values require the efficient separation and purification of xenon (Xe) and krypton (Kr) from radioactive gases generated during nuclear fission processes. To address this issue, we have synthesized three thieno[3,2-b]thiophene-based porous organic polymers (POP-ch-ET, POP-ch-SP and POP-ch-ME) via high yield C–H direct arylation reaction, all of which exhibited excellent thermal and acid-base stability. Notably, the three-dimensional (3D) structures of POP-ch-SP and POP-ch-ME allowed higher Xe capacity compared to the two-dimensional (2D) structure of POP-ch-ET. Density functional theory (DFT) calculations confirmed that thieno[3,2-b]thiophene moieties contributed to a more negative adsorption energy for Xe than benzene. Among them, POP-ch-SP with fixed group showed superior Xe capacity (2.37 mmol/g) at 298 K and 1.0 bar and the highest ideal adsorption solution theory (IAST) selectivity (11.5). This superior performance is attributed to its 3D ultra-micropore structure, which enables closer proximity between aromatic rings, thereby enhancing Xe interaction. The DFT calculation further revealed that the adsorption energy of Xe in POP-ch-SP was more negative compared to other POPs , indicating a stronger interaction. In addition, POP-ch-SP exhibited the largest ΔQ st (14.2 kJ/mol) between Xe and Kr , highlighting a marked affinity difference. In dynamic breakthrough experiments, POP-ch-SP demonstrated robust Xe/Kr separation efficiency under both low (400 ppm Xe and 40 ppm Kr in dry air) and high concentration scenarios (Xe/Kr, v/v, 20/80), underscoring its promising potential for practical applications in radioactive gas management.
研究领域:
材料科学
·
环境科学
·
放射性气体管理
✓ 已验证
产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
Zhaotong Yan,Youjin Gong,Chu-Ting Yang,Xiaonan Wu,Boyu Liu,Qiang Liu,Shunshun Xiong,Shuming Peng
The design and construction of radioactive stable metal–organic frameworks (MOFs) are highly desirable for noble gases (Xe and Kr) separation from off-gas steams during used nuclear fuel reprocessing under radiation environments. Al-based MOFs are promising for realistic applications of Xe/Kr separation due to their high hydrothermal and chemical stability and comparatively easy and massive preparation by nonpoisonous, abundant, and cheap metal. Herein, we report on two isoreticular microporous Al-MOFs Al-Fum (Al-fumarate, Basolite A520) and Al-Fum-Me (Al-methyl-fumarate) with high radioactive stability for Xe/Kr separation. Appending methyl groups on the framework provides an effective approach to reduce and fine-tune the pore size of Al-Fum-Me to match well with the Xe atom and remarkably improve the framework-Xe affinity. Al-Fum-Me exhibits significantly enhanced Xe/Kr separation performance compared to Al-Fum, demonstrated by adsorption isotherms and breakthrough experiments. Gamma-ray irradiation experiments also identified the high radioactive stability of Al-Fum-Me, suggesting its great potential for practical application on Xe/Kr separation.
研究领域:
材料科学
·
核能工程
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2020
·
IF 2.369
Peixin Zhang,Yao Zhong,Qing Yao,Xing Liu,Yan Zhang,Jun Wang,Qiang Deng,Zheling Zeng,Shuguang Deng
Separation of a gas mixture achieved by the vacuum swing adsorption (VSA) technology is considered as an efficient and energy-saving method for Xe/Kr mixtures, but developing efficient and stable adsorbents remains challenging. Herein, we report an ultramicroporous metal–organic framework, namely, MIL-120 with a suitable pore size (5.4 Å × 4.7 Å), rich hydroxyl-decorated sites, and ultrahigh stability, which is capable of highly selective adsorption of xenon from krypton. Specifically, MIL-120 exhibits an excellent adsorption capacity of Xe up to 1.15 and 1.99 mmol g–1 at 298 K under 0.1 bar and 1 bar, respectively, and outstanding ideal adsorbed solution theory selectivity of 9.6 for the Xe/Kr mixture, which is comparable to those of benchmark porous materials. The isosteric heat of adsorption (Qst) and density functional theory calculations further confirm the stronger interaction of the adsorbent toward Xe than Kr. Furthermore, the cycling breakthrough experiments, hydrothermal and acid-based stability tests, and VSA assessment comprehensively demonstrate that the MIL-120 is an efficient and potent adsorbent for Xe/Kr separation under industrial conditions.
研究领域:
材料科学
·
气体分离技术
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2019
·
IF 3.771
Yi Xi Song,Min Zhi Rong,Ming Qiu Zhang
As an ideal smart wearable natural material, α-keratin type mammalian hairs have proved to exhibit multiple-responsive shape memory effects under water, wet, xenon and redox stimuli, in which the inherent disulfide bonds played the roles of either netpoints or switching units. Accordingly, here in this work, we proposed to increase the content of disulfide bonds of representative mammalian hairs - wool fibers , which are widely used in daily life, by means of three chemical methods so as to improve their multiple-responsive shape memory effects. On the basis of systematic researches, it was found that the treatment with cystamine gave the highest efficiency of introducing disulfide bonds due to full use of the free functional groups of wool, while the valuable crystalline phases of wool were nearly not affected. As a result, the cystamine modified wool fibers possessed greater shape recovery ratio under water and heat conditions, and larger shape fixation ratio under xenon and redox conditions , in comparison with the untreated version. The mechanisms involved were carefully analyzed. The application scope of the on-demand programmed wool in intelligent fabrics and textiles would thus be broadened.
研究领域:
材料科学
·
纺织工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zijun Yan,Yu Luo,Bo Chen,Fenglei Wang,Lang Chen,Zining Wang,Pengwei Zhao,Jinyang Kang,Zhihai Fu,Yongdong Jin,Yuanhua Wang,Chuanqin Xia
Radioactive isotopes of krypton (Kr) and xenon (Xe) are produced from the fission reaction of nuclear reactors. The separation of Xe/Kr from the nuclear off-gas is important for the spent fuel reprocessing. Compared with the industrial method of cryogenic distillation, physical adsorption is a simple and energy-saving method for Xe/Kr separation. Here, three rigid conjugated micropore polymers, including thiophene containing CMP-PY-BTP, TBTP and fluorine-containing CMP-PY-TFB, were prepared in high yield through direct C H arylation reaction, and their structure–function relationship with Xe/Kr separation was described. CMP-PY-TFB, BTP, and TBTP all possessed rigid micropores with Brunauer-Emmett-Teller specific surface areas of 786.25, 141.64 and 488.30 m 2 /g, respectively. Among three polymers, CMP-PY-TBTP exhibited the highest Xe/Kr selectivity (11.9 for ideal adsorption solution theory selectivity and 9.3 for Henry selectivity), owing to the combined effect of stronger polarization of its thiophene structural unit and micropore confinement (5.4 Å). The density functional theory (DFT) calculation revealed that Xe was more strongly adsorbed in thiophene-containing units than that of fluorine-containing unit which verified the stronger interaction caused by thiophene group’s polarization. Though having weaker polarization to Xe, fluorine-containing CMP-PY-TFB exhibited the highest Xe uptake of 43.59 cm 3 g −1 due to its largest specific surface area (786.25 m 2 /g).
研究领域:
材料科学
·
核能工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2025
·
IF 19.6
Guodong Li,Guoxun Ji,Shunshun Xiong,Zhen Jiang,Mengjia Yuan,Fuwan Zhai,Shujing Lin,Lixi Chen,Chunyi Yu,Mingrui Zuo,Xia Wang,Zhiyong Peng,Benxian Huang,Nannan Shen,Lanhua Chen,Yanlong Wang,Xihai Li,Xuanjun Wang,Xiaofeng Fang,Congwei Wu,Hui Zhang,Wei Liu,Xiaolin Wang,Lifeng Ding,Fuyin Ma,Zhifang Chai,Shuao Wang
The disposal of radioactive xenon and krypton generated by nuclear fission is essential for the zero emission of nuclear energy, while their efficient capture at low concentrations remains a daunting challenge. We present here a design philosophy for noble gas uptake by introducing the concept of the confinement-intensified multi-heavy-atom effect derived from the Lennard-Jones 12–6 potential, which is achieved by the construction of a previously unnoticed structural unit of a tetrahedral halogen cage arranged in a metal-organic framework (Cu(idc-I)). Record-high adsorption capacities of 128.58 and 20.83 cm 3 cm −3 for Xe and Kr, respectively, were achieved at 0.1 bar and ambient temperature, along with the highest Kr Henry coefficient (10.19 mmol cm −3 bar −1 ). The dense tandem-arrayed tetrahedral iodine cages, as powerful binding sites have been visualized by in situ single-crystal X-ray diffraction studies and theoretical simulations, endowing Cu(idc-I) with the ability to effectively capture trace Xe and Kr from mimic nuclear reprocessing off-gas.
研究领域:
核化学
·
材料科学
·
环境科学
·
无机化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）