SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhenliang Zhu,Bei Li,Xing Liu,Peixin Zhang,Shixia Chen,Qiang Deng,Zheling Zeng,Jun Wang,Shuguang Deng
Adsorptive separation of xenon (Xe) from krypton (Kr) is challenging owing to their low concentrations and similar physical properties. Herein, we report two metal–organic frameworks (MOFs) assembled from the same aliphatic ligand ( trans -1, 4-cyclohexanedicarboxylic acid, H 2 CDC), but showing distinct pore shapes. The rhombus pores on Al-CDC show a narrower pore aperture of 4.5 Å × 6.0 Å, contracting to the pseudo-square pores (5.8 Å × 6.8 Å) on Cu-CDC. As a result, Al-CDC exhibits a high Xe adsorption capacity (2.45 mmol g −1 ) and Xe/Kr selectivity (10.7) at 298 K and 1.0 bar. The confined pore space and abundant saturated C-H groups provide stronger van der Waals interactions toward Xe, which is disclosed by the Grand Canonical Monte Carlo (GCMC) and Density Functional Theory (DFT) calculations. Dynamic breakthrough experiments further confirm their industrial application potential and stable reusability.
研究领域:
化学
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材料科学
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物理化学
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产品关联
DOI
高影响因子
Nanomaterials
·
2024
·Vol. 14
·期 20
·1629
·
IF 4.4
Penghui Lei,Qing Chang,Mingkun Xiao,Chao Ye,Pan Qi,Fangjie Shi,Yuhua Hang,Qianwu Li,Qing Peng
A new type of SiCf/TiC-Ti3SiC2composite was prepared by the Spark Plasma Sintering (SPS) method in this work. The phase transformation and interface cracking of this composite under ion irradiation (single Xe, Xe + He, and Xe + He + H ions) and subsequent annealing were analyzed using transmission electron microscopy (TEM), mainly focusing on the interface regions. Xe ion irradiation resulted in the formation of high-density stacking faults in the TiC coatings and the complete amorphization of SiC fibers. The implanted H ions exacerbated interface coarsening. After annealing at 900 °C for 2 h, the interface in the Xe + He + H ion-irradiated samples was seriously damaged, resulting in the formation of large bubbles and cracks. This damage occurred because the H atoms reduced the surface free energy, thereby promoting the nucleation and growth of bubbles. Due to the absorption effect of the SiCf/TiC interface on defects, the SiC fiber areas near the interface recovered back to the initial nano-polycrystalline structure after annealing.
研究领域:
材料科学
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核材料
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复合材料
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jiaoqin Liu,Chengjie Guo,Nannan Wu,Chenguang Li,Ruijuan Qu,Zunyao Wang,Riya Jin,Yina Qiao,Zengdi He,Jing Lu,Xingqiao Feng,Yufan Zhang,Anlong Wang,Jingshuai Gao
In this work, the kinetics and mechanisms of photocatalytic degradation of perfluorooctanoic acid (PFOA) by nitrogen-doped indium trioxide (N-doped In 2 O 3 or NH 4 NO 3 -In 2 O 3 ) under Xe lamp irradiation were systematically investigated. Nitrogen originating from various inorganic and organic nitrogen compounds was doped into In 2 O 3 to examine the catalytic effect. The NH 4 NO 3 -In 2 O 3 catalyst was characterized by SEM , TEM, FT-IR, UV-DRS, BET surface area, XPS, and XRD , and showed the best catalytic performance. After 18 h of irradiation, PFOA was almost completely degraded with addition of 5 mg catalyst, while it was hardly degraded by simulated sunlight alone. The low photocatalytic degradation efficiency of PFOA was observed in different natural waters, which was due to the inhibitory effect of high pH and common anions like SO 4 2− . The calculation results of Materials Studio showed that a shoulder-to-shoulder π system between nitrogen atom and oxygen atom (NO π*) was formed after nitrogen doping into interstitial sites of In 2 O 3 , therefore resulting in a reduction in band gap energy. Occupied NO π* states were responsible for the red shift, while unoccupied NO π* levels restrained the recombination of electrons (e − ) and holes (h + ). Nitrogen doping reduced the excitation energy for electronic transition, and thus accelerated the reaction. According to mass spectrometry analysis, decarboxylation and elimination were still the main photodegradation pathways of PFOA. To the best of our knowledge, this report is the first to explore the reaction mechanisms of PFOA in an N-doped In 2 O 3 /Xe lamp irradiation system.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Geng Chen,Mengying Wei,Mengjie Jing,Rui Zhang,Zhe Wang,Yifan Li,Yingsi Huo,Keliang Shi,Tonghuan Liu,Kang Kang
The separation of xenon (Xe) and krypton (Kr) from gaseous mixtures is a crucial yet challenging industrial process, primarily due to the inherent inertness and similar physicochemical properties. Herein, we report the synthesis of a novel pyrazole-based microporous organic polymer for efficient Xe/Kr separation. This porous organic polymer possesses abundant nitrogen sites and a concentrated microporous network with pore sizes predominantly centered within the 4–6 Å range. The material exhibited promising Xe adsorption capacity (2.22 mmol·g −1 ) and Xe/Kr Ideal Adsorbed Solution Theory (IAST) selectivity (13.74) at 298 K and 1.0 bar. Furthermore, taking advantage of the strong coordination interactions between the pyrazole groups and metal nanoparticles, silver nanoparticles were successfully introduced to form the composite MOP-PZ-Ag, thereby improving the Xe/Kr separation capability. Under dilute conditions, MOP-PZ-Ag exhibited significantly higher IAST selectivity and Henry's coefficient for Xe compared with MOP-PZ. In dynamic breakthrough experiments, MOP-PZ-Ag showed better separation performance toward Xe/Kr, with the Xe adsorption capacity increasing from 3.79 mmol·kg −1 to 4.91 mmol·kg −1 under low concentration (400 ppm Xe and 40 ppm Kr in dry air). Besides, the superior separation performance of MOP-PZ-Ag can be well maintained over at least five adsorption-desorption cycles. Such experiment results revealed the potential of MOP-PZ-Ag for Xe/Kr separation in used nuclear fuel (UNF) off-gas management.
研究领域:
材料科学
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吸附分离
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核化学
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多孔聚合物
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环境工程
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Shuwen Yu,Shichun Li,Huazhao Wang,Chunhua Zhu,Jingwei Hou,Sheng Cui,Xiaodong Shen,Yu Liu
The Kr/Xe separation based on membranes is of great significance for radioactive 85 Kr capture from nuclear fuel reprocessing plants and expensive Xe production, thus the membrane material that has both high separation performance and stability is highly sought after. Herein, the crosslinked polymeric micro-porous polyarylate (PAR) membrane was synthesized by interfacial polymerization, and its Kr/Xe separation performance and stability under various conditions including γ irradiation were investigated. The PAR membrane displays Kr permeance of 0.22 GPU and Kr/Xe selectivity of 3.6 tested with mixed gas at room temperature, which is better than other reported polymeric membranes and even better than the amorphous carbon membrane. After the γ irradiation, the PAR can preserve its chemical structures , while the physical ageing is accelerated, which leads to only 25% decrease in Kr/Xe selectivity after 20 kGy irradiation. This work demonstrates that the micro-porosity and the crosslinking structures play crucial roles in improving both separation performance and stability of polymeric membranes for radioactive Kr/Xe separation.
研究领域:
材料科学
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核能工程
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhiwei Zhao,Ke Wu,Yong Peng,Yi Liu,Zhenning Deng,Xinxin Han,Shixia Chen,Jingwen Chen,Shuguang Deng,Jun Wang
The direct adsorptive separations of xenon (Xe) and krypton (Kr) using granular porous carbons remain challenging yet industrially important. Herein, we report microporous carbon granules with narrow pore size distributions and rich oxygen functionalities for efficient Xe/Kr separation. The optimized granular carbon (GBC-900) breaks the trade-off effect by showing high Xe uptake capacity (4.71 mmol g −1 ) and Xe/Kr selectivity (18.3) at 298 K and 1.0 bar. Notably, the synergistic effect of oxygen-functionalities and uniform micropores renders the ultrahigh Xe uptake of 2.78 mmol g −1 at 0.2 bar. Furthermore, density functional theory calculations disclose the strong affinity between oxygen groups and Xe atoms. Dynamic breakthrough experiments confirm the practical Xe/Kr separation feasibility even from humid and low-concentration Xe/Kr gas-mixtures.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2026
·
IF 8.8
Jialin Wang,Wenxiao Qiao,Meng He,Xiangdong Ding,Weiqun Shi,Xue Liu
Interunit linkage flexibility regulates irradiation responses of ultrathin polymer membranes. • Diaryl ether linkages enable structural accommodation under γ irradiation. • PX-BPO membranes retain He and Kr/Xe separation after 50 kGy irradiation. • Crack formation causes nonselective transport pathways in rigid-linkage membranes. Efficient membrane separation of He/Kr/Xe noble gas mixtures is essential for He recycling and radioactive off-gas treatment in advanced nuclear reactors. Nevertheless, radiation induced structural degradation greatly limits the practical application of polymeric membranes in radioactive service conditions, especially for high-performance thin film composite membranes. Establishing valid molecular design strategies to suppress such nanoscale structural damage still poses a major obstacle to the development of radiation resistant separation membranes. Here, we show that ultrathin polyxanthene membranes containing different interunit linkages exhibit markedly different responses to γ irradiation. Three approximately 100 nm selective layers containing biphenyl (PX-BP), diaryl ether (PX-BPO), and hexafluoroisopropylidene (PX-HFP) linkages were evaluated for He/Kr/Xe separation after irradiation in air up to 50 kGy. At 50 kGy, PX-BP and PX-HFP developed severe cracking accompanied by substantial losses in selectivity, whereas PX-BPO underwent pronounced wrinkling while retaining selective-layer continuity and over 74% of its initial He/Kr and He/Xe separation factors. Structural characterization and molecular calculations further showed that PX-BPO underwent pronounced structural reorganization while retaining selective-layer continuity. Its diaryl ether linkage exhibited the lowest torsional barrier and a more distributed electronic and geometric response to one-electron ionization. These results identify linkage conformational flexibility as an important molecular factor associated with the distinct irradiation response of PX-BPO within this PX series. Download: Download high-res image (417KB) Download: Download full-size image
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Duo Yue,Rui-Ming Li,Le Yan,Xiao-Yan Zhu,Mihail Barboiu,Hai-Ping Wang,Zhang-Wen Wei,Cheng-Yong Su,Ji-Jun Jiang
Xenon (Xe) and krypton (Kr) have a variety of medical, industrial, and environmental applications, but their separation is difficult due to their chemical inertness and similar physical properties. This study presents a dual-functional modulation strategy for designing halogen-decorated pillar-layered MOFs (LIFM-DMOF-X 2 , X = F, Cl, Br) to improve the efficiency of Xe/Kr separation. The incorporation of halogenated terephthalate linkers (BDC-X 2 ) and DABCO pillars enabled the frameworks to synergistically control the pore geometry and surface polarity via the steric and electronic effects of the halogens. LIFM-DMOF-Cl 2 exhibited optimal performance with a Xe uptake of 3.58 mmol g −1 (298 K, 1.0 bar) due to its balance between pore size (6.14 Å) and high surface area (1259.8 m 2 g −1 ). Dynamic breakthrough experiments confirmed the practical efficacy of this MOF, which showed a Xe retention time of up to 21 min/g and reusability for five cycles. GCMC simulations revealed multidimensional Xe-binding sites, including halogen bonds and π-interactions, with brominated variants showing exceptional polarization effects ( Q st = 20.77 kJ mol −1 ). This work demonstrates the promise of halogen engineering in MOFs for nuclear off-gas treatment and noble gas capture.
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shuwen Yu,Ben Qin,Fan Yang,Meiying Xie,Liyan Xue,Zhigang Zhao,Kaixian Wang
Reduced graphene oxide (rGO) membranes have shown promising separation and purification in the fields of water treatment and gas capture due to their unique physicochemical characteristics. However, how to further reduce the transport resistance of rGO membranes and improve separation performance is still a thorny issue. In this work, the reported metal-crosslinked rGO membranes showed a reverse-selective separation behaviors for the adsorbed gas molecules at low pressure. The effect of metal ions on the membrane structure and the separation performance were investigated. Metal ions not only can improve the cross-linking structure and control interlamellar spacing of rGO membranes for the precise molecular sieve, but also can provide abundant metal sites to enhance the affinity, which led to a diffusion-controlled process for the targeted gas molecules. The resulting metal-crosslinked rGO membranes presented outstanding gas permeance and selectivity for gas pairs of the He/CO 2 , N 2 /CO 2 and Kr/Xe, with the highest selectivity of 21, 11.4 and 4.1, respectively. The work will provide a new avenue towards specific molecule capture for the development of rGO membranes in the fields of natural gas purification and radioactive gas recovery.
研究领域:
材料科学
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化学工程
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环境科学
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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
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）