CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhiang Hou,Jiangfeng Chu,Cong Liu,Jinnan Wang,Aimin Li,Tong Lin,Corvini Philippe François-Xavier
Photocatalytic denitrification has attracted great attention owing to its high efficiency and environmentally friendly features. However, selectively photocatalytic reduction of high concentration nitrate to N 2 is still a challenging problem due to the competition of photons between nitrate and photocatalysts. Herein, the Ag/SiO 2 core encapsulated in the crystalline TiO 2 shell (Ag/SiO 2 @ c TiO 2 ) was constructed for improvement of photocatalytic denitrification. Finite difference time domain (FDTD) simulation demonstrated that strong light scattering improved light harvesting via optical confinement. Meanwhile, surface plasmon resonance and electron sink effect of Ag not only enhanced the photogenerated electrons density but also promoted charge carriers separation of Ag/SiO 2 @ c TiO 2 . More importantly, e cb − of TiO 2 -shell could be immediately transferred to Ag to keep the balance between Ag 0 and Ag + , which contributed to the good stability of Ag/SiO 2 @ c TiO 2 . 95.8% nitrate ( C 0 = 2000 mg/L) was removed by 5 wt%Ag/SiO 2 @ c TiO 2 with N 2 selectivity of 93.6% within 4 h. Even after five cycles, 5 wt%Ag/SiO 2 @ c TiO 2 still remained high photocatalytic denitrification efficiency (92.2%). Notably, since TiO 2 -shell prevented the reaction between Ag and Cl − , more than 92% nitrate could be removed within 5.3 h in the presence of high concentration Cl − .
研究领域:
环境科学
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材料科学
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化学工程
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催化
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
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2020
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IF 14.588
Feng Ma,Yangyang Wan,Xiaoming Wang,Xinchao Wang,Jiashun Liang,Zhengpei Miao,Tanyuan Wang,Cheng Ma,Gang Lu,Jiantao Han,Yunhui Huang,Qing Li
The sluggish kinetics of lithium polysulfides (LiPS) transformation is recognized as the main obstacle against the practical applications of the lithium–sulfur (Li–S) battery. Inspired by molybdoenzymes in biological catalysis with stable Mo–S bonds, porous Mo–N–C nanosheets with atomically dispersed Mo–N2/C sites are developed as a S cathode to boost the LiPS adsorption and conversion for Li–S batteries. Thanks to its high intrinsic activity and the Mo–N2/C coordination structure, the rate capability and cycling stability of S/Mo–N–C are greatly improved compared with S/N–C due to the accelerated kinetics and suppressed shuttle effect. The S/Mo–N–C delivers a high reversible capacity of 743.9 mAh g–1 at 5 C rate and an extremely low capacity decay rate of 0.018% per cycle after 550 cycles at 2 C rate, outperforming most of the reported cathode materials. Density functional theory calculations suggest that the Mo–N2/C sites can bifunctionally lower the activation energy for Li2S4 to Li2S conversion and the decomposition barrier of Li2S, accounting for its inherently high activity toward LiPS transformation.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
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2025
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IF 9.8
Cong Jiang,Zong Meng
The development of green and efficient catalytic systems is crucial for sustainable chemical processes. This study engineered shellac nanoparticle-lipase conjugates for biphasic biocatalysis. Taking advantage of the inherent amphiphilicity and pH-triggered interfacial behavior of the shellac, the conjugates exhibited dual functionality as intelligent Pickering emulsifiers and interfacial biocatalysts. The covalent conjugation strategy achieved a protein loading capacity of 107.97 ± 5.24 mg/g under optimized conditions while preserving interfacial responsiveness. Reversible emulsification/breaking transitions were precisely regulated at least 30 times through pH adjustment or alternating CO₂/N₂ treatments, enabling convenient catalyst recovery. When applied to the esterification of phytosterols with oleic acid, the conjugates exhibited a higher esterification rate (78.93 %, 1.5-fold enhancement compared with the free lipase), retained 85.0 % initial catalytic activity after six consecutive cycles. The responsive Pickering system combined exceptional recyclability and enhanced catalytic performance, providing an innovative pathway for the development of Pickering interfacial catalysis.
研究领域:
绿色化学
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生物催化
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纳米技术
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胶体与界面科学
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酶工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Hucheng Zhang,Jianji Wang
In recent years, metal–organic frameworks (MOFs) have been explored as emulsifiers for the fabrication of Pickering emulsions and then used for hybrid material synthesis and interface catalysis. Nevertheless, stimuli-responsive Pickering emulsions stabilized by MOFs have been rarely reported so far, although they are of great importance for fundamental research studies and practical applications. Herein, for the first time, triethylenetetramine (TETA)-functionalized MOFs (ZIF-90/TETA) have been designed, synthesized, and used for fabricating CO2-/N2-response Pickering emulsions. It is shown that even at the ZIF-90/TETA content of 0.25 wt %, the functional MOF can still efficiently emulsify n-hexane and water to form a high internal phase Pickering emulsion. Importantly, the Pickering emulsion can be easily and reversibly switched between emulsification and demulsification by bubbling of CO2 and N2 alternatively at atmospheric pressure. The possible mechanism of the CO2/N2 switchable emulsion is investigated by zeta potential, water contact angle, interfacial tension, 13C NMR spectroscopy, and an optical microscope. It is found that the acid–base reaction of CO2 with TETA anchored on the surface of ZIF-90 leads to the production of hydrophilic ammonium bicarbonate and carbamate, which results in the emulsification of the Pickering emulsion. However, when N2 is bubbled to remove CO2, the reverse reaction takes place to cause the demulsification of the Pickering emulsion. Moreover, the CO2/N2 switchable Pickering emulsion has been successfully used as a microreactor for Knoevenagel reactions to demonstrate a highly efficient integration of chemical reaction, product separation, and ZIF-90/TETA recycling for a sustainable chemical process.
研究领域:
化学
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材料科学
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胶体科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sustainable Materials and Technologies
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2024
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IF 8.6
Lei Guo,Yan-He Chen,Li-Mei Xu,Xiao-Lu Chen,Jin-Qiu Shen,Jian-Yong Zhang,Zhen-Jiang Liu
Herein, a fern-like p-n heterojunction by anchoring Ni 3 Fe-LDH nanoplates onto Co 3 O 4 nanoneedles have been optionally constructed. Essentially, p-n heterojunction ensured to induce strong built-in electric field, and inherit interfacial electron redistribution. Based on their compatible and well-matched electronic band structures, a staggered type-II photo-generated electron/holes transfer pathway have been elaborated by density functional theory calculation (DFT), in situ irradiation X-ray photoelectron spectroscopy (XPS), and fluorescent decay. This band bending and charge migrating module conferred the architecture with strong redox ability, sufficient exciton dissociation, and admirable optoelectronic characteristics. Moreover, the heterostructure acquired broad absorption spectrum to exhibit outperforming photocatalytic effect. Totally, this electron redistribution at the hierarchical interface, a type-II scheme charge-transfer pathway and the oxygen defects would lead to high efficiency in solar light assisted N 2 reduction. Typically, Co@Ni 3 Fe-2 catalyst exhibited the highest NH 3 production rate of 16.15 μg h −1 mg cat. −1 and Faraday efficiency (FE) of 31.57% at −0.6 V vs. RHE in 0.1 M Na 2 SO 4 solution. Fortunately, with light exposure, the NH 3 production rate and FE could increase by 27.9% and 18.1% than that under dark. This work would provide a plausible attitude towards the design of high efficient photocatalyst for artificial photosynthesis with multi-functionalized coupling effect.
研究领域:
材料科学
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催化
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光化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
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2025
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IF 4.5
Shuang Wang,Dudu Li,Zelong Xu,Fan Zhou,Zhihua Qiao,Zibo Yang,Zhi Wang
Coordination polymer (CP) glasses offer high processability and permanent accessible pores, having promising potential in gas separation. However, their low porosity makes it difficult to prepare high-performance gas separation membranes. In this work, we combined the advantages of CP glasses and inorganic fillers, and selected ag Zn-P-dmbIm as the continuous phase and hydroxylated multi-walled carbon nanotubes (HMWCNTs) as the dispersed phase to prepare HMWCNTs/ ag Zn-P-dmbIm mixed matrix membranes (MMMs). The very favorable interfacial compatibility and excellent CO 2 /N 2 gas separation performance of the MMM-2 membrane were demonstrated by a series of characterizations. The test results revealed that the CO 2 permeability and ideal CO 2 /N 2 selectivity of MMM-2 membrane were 9776.8 Barrer and 31.1, respectively, which exceeded the Robeson 2019 upper bound. In addition, the well-defined long-term stability of the MMM-2 membrane lays the foundation for realizing gas separation membranes for industrial applications in practice. This provides a strategy for the subsequent preparation of CP glasses-based MMMs.
研究领域:
材料科学
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膜技术
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气体分离
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高分子化学
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纳米复合材料
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
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IF 7.2
Hui Zhang,Qiang Fu,Hongyun Qin,Xia Chen,Qicheng Zhang,Zixu Dong,Haoyuan Li,Shoudong Wang,Ming Wang
Hydrogen recovery from ammonia purge gas is a desirable method to relieve the pressure of increasing demand for hydrogen. Metal-organic frameworks (MOFs) are promising adsorbents for the separation of the H 2 –N 2 mixture. However, the separation of the H 2 –N 2 mixture using MOFs remains challenging due to the lack of adsorptive mechanism. Herein, the adsorption mechanism of the H 2 –N 2 mixture in SIFSIX-2-Cu-i has been systematically investigated with the method of a combination of excess adsorption experiments, molecular simulations , and DFT calculations. In the Grand Canonical Monte Carlo (GCMC) simulations, the polarizable force field was first applied to the adsorption of pure H 2 or N 2 and H 2 –N 2 mixture in SIFSIX-2-Cu-i. Ab Initio Molecular Dynamics (AIMD) was performed to investigate the distribution of the guest molecules in the pores of SIFSIX-2-Cu-i. Finally, Density functional theory (DFT) calculations were performed to predict the transfer of charge between MOF and guest molecules. Results revealed two binding sites of H 2 or N 2 in SIFSIX-2-Cu-i. A relatively high thermodynamic adsorption selectivity for N 2 over H 2 has been observed in SIFSIX-2-Cu-i. Furthermore, SIFSIX-2-Cu-i also exhibits a greater affinity with N 2 than with H 2 , which is probably because of the stronger induction interactions between F2 atoms and N 2 molecules. These findings are of significance to guide the design of the new highly selective adsorbents for the separation of H 2 /N 2 .
研究领域:
化学工程
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材料科学
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Healthcare Materials
·
2024
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IF 10
Wenxiao Shi,Yu Feng,Jincheng Tang,Yichang Xu,Wang Wei,Lichen Zhang,Xinzhao Jiang,Zhouye Ding,Kun Xi,Liang Chen,Yong Gu
The innate immune response is crucial to the inflammation, but how neutrophils and macrophages act in bone repair and tissue engineering treatment strategies await clarification. In this study, we found N2 neutrophils release stronger “eat me” signals to induce macrophage phagocytosis which then polarize into the M2c anti-inflammatory phenotype. This is beneficial for bone repair. Guided by this biological mechanism, we filled a mesoporous bioactive glass scaffold (MBG) with HAMA hydrogel loaded with TGFβ1 adenovirus (Ad@H), constructing a genetically engineered composite scaffold (Ad@H/M). The scaffold not only has good hydrophilicity and biocompatibility, but also provides mechanical stress support for bone repair. Adenovirus infection quickly induces N2 neutrophils, upregulating NF-κB and MAPK signaling pathways through Toll-like receptor 4 (TLR4) to promote the inflammatory response and macrophage phagocytosis. Macrophages perform phagocytosis and polarize towards the M2 phenotype, mediating the inflammatory response by inhibiting the PI3K-AKT-NF-κB pathway, maintaining homeostasis of the osteogenic microenvironment. The role of Ad@H/M scaffold in regulating early inflammation and promoting long-term bone regeneration was further validated in vivo. In brief, this study focuses on the cascade of reactions between neutrophils and macrophage subtypes, and reports a composite scaffold that coordinates the innate immune response to promote bone repair. This article is protected by copyright. All rights reserved
研究领域:
生物医学工程
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免疫学
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组织工程
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骨再生
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADSORPTION SCIENCE & TECHNOLOGY
·
2017
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IF 0.754
Weichao Du,Xiaolin Pu,Jinsheng Sun,Xiao Luo,Yanna Zhang,Lu Li
A novel monomeric amine sodium montmorillonite swelling inhibitor: N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide was obtained from diethanolamine, 1-bromotetradecane, and 1, 2-dibromoethane. N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide was characterized by means of Fourier transform infrared, 1H NMR spectroscopy, elemental analysis, linear swelling tests, particle size distribution tests, X-ray diffraction, and thermogravimetric. Linear swelling tests showed that the swelling height of sodium montmorillonite in 1.0 wt% N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide solution was only 2.0 mm after 16 h (fresh water was 5.0 mm). Particle size distribution tests exhibited that the median diameter and mean particle size of sodium montmorillonite in 1.0 wt% N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide solution obviously increased to 16.1 and 85.4 µm, respectively (fresh water was 8.1 and 21.8 µm). In thermogravimetric tests, in comparison with pure sodium montmorillonite, the decrease of water content in sodium montmorillonite/N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide indicated N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide expelled the water molecules out of the interlayer, which was beneficial to wellbore stability. Fourier transform infrared spectra of certain concentration N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide/sodium montmorillonite indicated the successful physical adsorption and interaction between N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide with sodium montmorillonite. In addition, the results of X-ray diffraction tests showed the obtained 1.0 wt% N1,N2-ditetradecy-N1, N1, N2, N2-tetrakis (2-hydroxyethyl) ethane-1,2-diaminium bromide solution could remarkably reduce the interlayer distance of wet sodium montmorillonite (from 1.94 to 1.37 nm).
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Niu Liu,Jun Cheng,Wen Hou,Xiao Yang,Junhu Zhou
In order to form strengthened active sites for superior CO 2 adsorption on core shell ZIF-8@ZIF-67 nanocomposites , graphene oxide (GO) with oxygen-containing functional groups was used as support to synthesize hybrid adsorbents with unsaturated Zn–N 2 –O active sites. The results of XPS O 1s and FTIR analysis revealed that the Me–O functional group content in the 0.5 wt% graphene oxide (GO)-supported core shell ZIF-8@ZIF-67 nanocomposite (38.9 at.%) was much higher than that in the 0.5 wt% reduced graphene oxide (RGO)-supported nanocomposite (19.4 at.%). This was because hydroxyl functional groups in the GO formed coordination bonds with zinc atoms in core shell ZIF-8@ZIF-67. XPS N 1s spectra indicated that the incorporation of oxygen-containing functional groups in GO resulted in the transition of binding form from Me–N 4 to Me–N 2 . The CO 2 adsorption capacity of GO-supported core shell ZIF-8@ZIF-67 gradually decreased from 2.15 to 1.30 mmol/g as GO weight percentage increased from 0.5 to 4 wt%, which was consistent with the decrease in BET surface area from 1378 to 585 m 2 /g and increase in peak pore diameter from 7.7 to 8.2 Å. Density functional theory (DFT) calculations demonstrated that unsaturated Zn–N 2 –O active sites in GO-supported core shell ZIF-8@ZIF-67 nanocomposites resulted in a decreased O C⋯Zn interaction distance from 4.65 (Zn–N 4 sites in core shell ZIF-8@ZIF-67) to 3.46 Å and an increased binding energy from 34.02 to 38.87 kJ/mol. Therefore, 0.5 wt% GO-supported core shell ZIF-8@ZIF-67 nanocomposites exhibited the highest CO 2 adsorption capacity of 2.15 mmol/g (at 273 K and 1 bar), 1.34 times higher than that of core-shell ZIF-8@ZIF-67.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
研究领域:
电化学
·
催化
·
材料科学
·
环境化学
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2025
·
IF 1.6
Zhiqing Liang,Zhongying Liu,Xiuyuan Wei,Hui Wu,Chanjuan Liu,Xiaohua Huang
Bifunctionalized NH2-UiO-66-CF3 nanofillers were successfully prepared by grafting - CF3 on NH2-UiO-66 via aldehyde-amine condensation reaction and applied to the preparation of 6FDA-ODA/NH2-UiO-66-CF3 mixed matrix membranes (MMMs). The successful introduction of -NH2 and -CF3 groups was verified by FT-IR, XRD, and XPS characterization, and the integrity of the crystal structure was ensured. Due to the presence of hydrogen bonding, NH2-UiO-66-CF3 showed good interfacial compatibility with the polymer matrix. Due to the introduction of the - CF3 group, the MMMs exhibited excellent thermal stability (T10% > 500°C, Tg = 300°C–305°C), hydrophobicity (contact angle of 92.96–97.71), and mechanical properties (tensile strength of 74–85 MPa). The gas separation performance tests showed that the MMMs exhibited significantly improved gas permeability and selectivity compared to the pure 6FDA-ODA membranes, which was attributed to the fact that the -NH2 and -CF3 groups provided more adsorption sites for gases. In particular, the PI/NUF(10) MMMs showed the best performance, with permeabilities of 42.71, 9.22, and 92.79 Barrer for CO2, O2, and He, respectively, which were 248%, 213%, and 173% higher than those of the pure membranes. Meanwhile, the selectivities of CO2/N2, O2/N2 and He/N2 were improved by 37%, 24%, and 8%, respectively. Close to the Robeson upper limit, demonstrating excellent gas separation potential.
研究领域:
材料科学
·
化学工程
·
膜技术
·
气体分离
·
纳米技术
✓ 已验证
DOI
高影响因子