JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ke Chen,Xin Guo,Linhan Ni,Junwen Qi,Jiansheng Li
Rational design and construction of fillers and polymers are crucial for the development of high-performance mixed matrix membranes (MMMs). In this work, amino-functionalized metal-organic frameworks KAUST-7 (KAUST-7-NH 2 ) with square-shaped sheet morphology were utilized as fillers to fabricate MMMs by physical blending with the polymer of intrinsic microporosity (PIM-1). The square-shaped KAUST-7-NH 2 sheets, prepared via in situ replacement of 2-aminopyrazine into the KAUST-7 framework, exhibited superior separation performance compared to the mono-ligand KAUST-7. Benefiting from the strong CO 2 affinity, high porosity and optimal pore sizes of KAUST-7-NH 2 , the outstanding CO 2 /CH 4 separation performance of the composite membrane was observed. The integration of square-shaped KAUST-7-NH 2 sheets provides a 2.5-fold improvement in CO 2 /CH 4 selectivity together with acceptable gas permeability as compared to the original PIM-1 membrane. Furthermore, a 100-h continuous permeation test validated the stability of the fabricated MMMs. Remarkably, the resulting MMM retained 92% of their initial CO 2 permeability after 150 days (drop of only 249 Barrer), indicating that the reduction in CO 2 permeability was approximately 10-fold lower than that of the pristine PIM-1 membrane. The prepared MMMs exhibit enhanced CO 2 /CH 4 selectivity and long-term stability, making it a highly promising candidate for practical application.
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
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Ke Chen,Linhan Ni,Hao Zhang,Chengming Xiao,Li Li,Xin Guo,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li
Rational design of fillers and polymers is of great importance to fabricate mixed matrix membranes (MMMs) with high performance. In this work, fluorinated metal-organic frameworks (KAUST-7 (also referred as NbOFFIVE-1-Ni)) were adopted as nanofillers to prepare MMMs through physically blending into the polymer of intrinsic microporosity (PIM-1). Benefiting from the features of porous KAUST-7, including well CO 2 affinity, distinctive pore characteristics (size, shape, and functionality) and strong intermolecular interactions with PIM-1, the achieved MMMs demonstrated increased CO 2 /CH 4 separation performance and improved anti-physical aging property. Specifically, with the assistance of KAUST-7, the CO 2 permeability and CO 2 /CH 4 (30:70 vol%) selectivity of the optimized MMMs increased up to 5928 Barrer and 23.5, corresponding to improvements of 50% of and 88% of the permeability and selectivity compared with the pristine membranes, respectively. Importantly, 100-h continuous separation test results confirmed the satisfying long-term stability of the prepared MMMs. Notably, the MMMs maintained 91% of the initial CO 2 permeability after 150 days (decreased only 539 Barrer), implying that the CO 2 permeability decrement is about 5-fold lower than that of the control PIM-1 membrane. These results suggest that the fabricated MMMs are promising candidates for CO 2 separation in practical applications.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Deli Jiang,Yimeng Zhou,Qianxiao Zhang,Qi Song,Changjian Zhou,Xiangli Shi,Di Li
Photocatalytic reduction of CO2 toward eight-electron CH4 product with simultaneously high conversion efficiency and selectivity remains great challenging owing to the sluggish charge separation and transfer kinetics and lack of active sites for the adsorption and activation of reactants. Herein, a defective TiO2 nanosheet photocatalyst simultaneously equipped with AuCu alloy co-catalyst and oxygen vacancies (AuCu-TiO2–x NSs) was rationally designed and fabricated for the selective conversion of CO2 into CH4. The experimental results demonstrated that the AuCu alloy co-catalyst not only effectively promotes the separation of photogenerated electron–hole pairs but also acts as synergistic active sites for the reduction of CO2. The oxygen vacancies in TiO2 contribute to the separation of charge carriers and, more importantly, promote the oxidation of H2O, thus providing rich protons to promote the deep reduction of CO2 to CH4. Consequently, the optimal AuCu-TiO2–x nanosheets (NSs) photocatalyst achieves a CO2 reduction selectivity toward CH4 up to 90.55%, significantly higher than those of TiO2–x NSs (31.82%), Au-TiO2–x NSs (38.74%), and Cu-TiO2–x NSs (66.11%). Furthermore, the CH4 evolution rate over the AuCu-TiO2–x NSs reaches 22.47 μmol·g–1·h–1, which is nearly twice that of AuCu-TiO2 NSs (12.10 μmol·g–1·h–1). This research presents a unique insight into the design and synthesis of photocatalyst with oxygen vacancies and alloy metals as the co-catalyst for the highly selective deep reduction of CO2.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
Small
·
2024
·
IF 13
Shuhan Fan,Qu Yang,Guilin Yin,Xiaosi Qi,Yuyu Feng,Junfei Ding,Qiong Peng,Yunpeng Qu,Qinglong Wang,Yan Shen,Mingkui Wang,Xiu Gong
Developing efficient and stable halide perovskite-based photocatalysts for highly selectivity reduction CO 2 to valuable fuels remains a significant challenge due to their intrinsic instability. Herein, a novel heterostructure featuring 2D Cs 3 Sb 2 I 9 nanosheets on a 3D flower-like mesoporous NiTiO 3 framework using a top-down stepwise membrane fabrication technique is constructed. The unique bilayer heterostructure formed on the 3D mesoporous framework endowed NiTiO 3 /Cs 3 Sb 2 I 9 with sufficient and close interface contact, minimizing charge transport distance, and effectively promoting the charge transfer at the interface, thus improving the reaction efficiency of the catalyst surface. As revealed by characterization and calculation, the coupling of Cs 3 Sb 2 I 9 with NiTiO 3 facilitates the hydrogenation process during catalytic, directing reaction intermediates toward highly selective CH 4 production. Furthermore, the van der Waals forces inherent in the 3D/2D heterostructure with face-to-face contact provide superior stability, ensuring the efficient realization of photocatalytic CO 2 reduction to CH 4 . Consequently, the optimized 3D/2D NiTiO 3 /Cs 3 Sb 2 I 9 heterostructure demonstrates an impressive CH 4 yield of 43.4 µmol g −1 h −1 with a selectivity of up to 88.6%, surpassing most reported perovskite-based photocatalysts to date. This investigation contributes to overcoming the challenges of commercializing perovskite-based photocatalysts and paves the way for the development of sustainable and efficient CO 2 conversion technologies.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Yunzhe Jiang,Chuanyao Liu,Jürgen Caro,Aisheng Huang
A new UiO-66-NH 2 based MOF named UiO-66-NH 2 @ICA has been prepared by grafting imidazole-2-carbaldehyde (ICA) to UiO-66-NH 2 through a post-synthesis reaction via amine condensation. FESEM , XRD , 1 H NMR, FT-IR and N 2 adsorption were used to characterize the morphology and structure of UiO-66-NH 2 @ICA. The grafted ICA mainly reduces the pore volume of UiO-66-NH 2 but increases the number of nitrogen atom as binding site of CO 2 . The UiO-66-NH 2 @ICA showed less BET surface area but a higher CO 2 /CH 4 adsorption selectivity in comparison with UiO-66-NH 2 . UiO-66-NH 2 @ICA and UiO-66-NH 2 crystals were dispersed in Matrimid ® 5218 to form mixed-matrix membranes (MMMs). Single gas permeation and mixed gas separation was carried out to investigate the effects of filler loading and feed gas pressure on the separation performances of the MMMs. The UiO-66-NH 2 @ICA/Matrimid ® MMM with 10 wt % filler showed a high CO 2 /CH 4 selectivity with a separation factor of 64.7, which is an increase by 40% in comparison with UiO-66-NH 2 /Matrimid ® MMM.
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
·
2024
·
IF 8.1
Xue Yang,Yuxuan Wang,Jingxian Hua,Rujing Hou,Jinfeng Chen,Qihan Gong,Chongqing Wang,Yichang Pan
Plate-like or sheet-like porous materials with nanometer thickness have been considered as the preferred fillers to improve mixed-matrix membranes (mmms)-based separation. Herein, hexagonal Co-fa (HG-Co-fa) nanoplates were simply synthesized without the addition of any modifier and used as fillers to construct 6FDA-DAM-based MMMs for efficient CO 2 /CH 4 separation. HG-Co-fa nanoplates exhibit high dispersion and interface compatibility in 6FDA-DAM matrix. The results demonstrated that the CO 2 /CH 4 separation performance of 6FDA-DAM was obviously improved after the incorporation of HG-Co-fa nanoplates. The resultant MMMs with nanoplate loading of 10 wt% showed CO 2 /CH 4 selectivity of 27 and CO 2 permeability of 1419 Barrer at 25 ℃ and 0.2 MPa, surpassing 2008 Robeson upper bound. Meanwhile, the high lattice integrity and structural stability of HG-Co-fa nanoplates contribute to the excellent thermal and mechanical stability of MMMs, contributing to their anti-plasticization property up to 14 bar and long-term stability up to 240 h, indicating their potential for natural gas separation.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2025
·
IF 2.3
Xiaoli Ding,Qiankun Zhang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang
Two series of mixed matrix membranes (MMMs) have been synthesized via in situ UV polymerization for the removal of N2 from CH4. MIL-100(Cr) particles activated at different temperatures were used as fillers. MIL-100(Cr) activated at 150°C with CH4-selective adsorption was incorporated with poly(ethylene oxide)-based polymer to improve the CH4/N2 separation performance, and that activated at 250°C with N2-selective adsorption and diffusion was incorporated with fluoropolymer to improve the N2/CH4 separation performance. The effects of the filler loadings on the gas permeation and separation performances were investigated. The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 150°C exhibited a 70% increased CH4/N2 permselectivity of 5.0 with a 37% increased CH4 permeability of 11.2 Barrer (tested at 0.2 MPa and 35°C). The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 250°C exhibited a 106% increased N2 permeability of 71.5 Barrer with an 89% increased N2/CH4 permselectivity of 1.9.
研究领域:
化学工程
·
材料科学
·
膜技术
·
气体分离
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Meidi Wang,Kaidong Quan,Xiaohong Zheng,Yu Cao,Xiangyu Cui,Ming Xue,Fusheng Pan
Two-dimensional (2D) covalent organic nanosheets (CONs) present versatile 2D materials, which hold great promise in mixed matrix membranes. The facile synthesis of CONs for the fabrication of mixed matrix membranes represents the development trend. Herein, mixed matrix membranes with facilitated transport ability were prepared based on self-exfoliated covalent organic nanosheets (CONs) and poly(ether-block-amide) (Pebax® MH 1657) matrix. The self-exfoliated TpDT CONs were facilely synthesized via Schiff base condensation reaction between 1,3,5-Triformylphloroglucinol (Tp) and 3, 5-diamino-1,2,4-triazole (DT). Abundant amine groups on TpDT CONs skeleton served as facilitated transport carriers to promote the transport of CO 2 by reversible nucleophilic addition reactions. And the highly ordered channels of TpDT CONs allowed the rapid transportation of CO 2 molecules to reach the facilitated transport carriers. Moreover, the incorporated TpDT CONs disturbed the packing of the Pebax chains by the intervention effects and increased the chain mobility. The facilitated transport carriers from TpDT CONs and the optimized structure endowed the as-prepared membranes with elevated permeance and selectivity. Specially, the Pebax-TpDT/PVDF membranes with 1 wt% TpDT CONs achieved an optimum CO 2 /CH 4 separation performance with a separation factor of 36.0 and a CO 2 permeance of 142.3 GPU, which were increased by 68% and 131%, respectively, compared with the pristine Pebax membrane.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Tongguo Huo,Kai Cao,Jianxin Zheng,Dan Zhu,Yuan Lin,Yu Dai,Jian Wu
The mechanism of β-SiC preparation via chemical vapor deposition (CVD) of the SiCl4–CH4–H2–N2 system remains unclear. Consequently, the change of molar Gibbs free energy of the CVD β-SiC chemical reaction in the SiCl4–CH4–H2–N2 system has been studied by the Helsinki Software Corporation (HSC) Chemistry code for the first time. The role of nitrogen in the reaction was confirmed. Seven potential reaction pathways of CVD β-SiC were presented, and the thermodynamic equilibrium components of each reaction were calculated systematically. The most viable reaction pathway and corresponding optimal temperature range for CVD β-SiC were determined. In addition, a kinetic study of CVD β-SiC was conducted. The microscopic morphology and crystal structure of β-SiC coatings prepared on the graphite surface at different temperatures were charactered by scanning electron microscopy (SEM), X-ray diffraction (XRD), Raman, etc. Ultimately, through SEM, XRD, and Raman observation, uniform and dense β-SiC coatings with fine grains and high crystallinity were successfully obtained. Furthermore, large β-SiC-coated graphite trays with diameters of 230 and 465 mm were prepared by CVD using the SiCl4–CH4–H2–N2 system, and the average thickness of β-SiC was about 100.6 μm. This study provides a theoretical basis and technical recommendations for the fabrication of SiC-coated graphite trays used in metal–organic chemical vapor deposition (MOCVD) equipment.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Materials Interfaces
·
2023
·Vol. 10
·期 12
·2202524
·
IF 5.4
Lei Wang,Xianying Bai,Yawei Gu,Xinxin Shi,Shilong Wang,Jingxian Hua,Rujing Hou,Chongqing Wang,Yichang Pan
2D metal–organic frameworks are attractive filler in mixed matrix membranes (MMMs) due to the high aspect ratio and contact opportunity at the filler–polymer interface. However, their alignment in polymer matrix remains a challenge to fully play their functions. Herein, to our best knowledge, for the first time, the facile synthesis of KAUST-7-NH 2 (KAUST, King University of Science and Technology) nanoplate is reported with 1D channels with an aspect ratio greater than 30. The nanoplates are incorporated and aligned in the 4,4′-(hexafluoroisopropylidene) diphthalic anhydride-2,4-diaminomesitylene (6FDA-DAM) polymer matrix under the shear force with a filler loading up to 50 wt%. The large difference in adsorption abilities between CO 2 and CH 4 from the (001)-oriented KAUST-7-NH 2 nanoplate-based MMMs and the favorable interaction at the filler–polymer interface contribute to the excellent CO 2 /CH 4 separation performance. The resultant membranes show CO 2 /CH 4 selectivity with 66.2% enhancement (surpassed 2008 Robeson upper bound), antiplasticization up to 17 bar, and long-term stability up to 240 h indicating its good potential for natural gas treatment.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2024
·
IF 3.8
An Sufeng,Wang Peng,Wang Kuanling,Wang Xuehai,Li Baozhong,Guo Xinwen
The M/SSZ-39 catalysts (M = In, Co, Cu, Fe) with different metal species and metal loadings were synthesized using the wet impregnation method on a small-pore SSZ-39 molecular sieve. X-ray diffraction (XRD), transmission electron microscopy (TEM), nitrogen adsorption-dehydrogenation and hydrogen temperature program reduction (H2-TPR) were employed to characterize the effects of various metal components and metal loadings on the performance of CH4 selective catalytic reduction of NO reaction (CH4-SCR). The characterization results showed that the In/SSZ-39 catalyst exhibited significantly higher catalytic activity compared to the Cu-, Co-, and Fe/SSZ-39 catalysts, suggesting that indium (In) is a more suitable active ingredient for the CH4-SCR reaction. The xIn/SSZ-39 (x = 1, 2, 3, x represents the In loadings of 1.0 wt%, 2.0 wt% and 3.0 wt%) catalysts, with different In loadings, all present excellent CH4-SCR performance. By varying the In loadings, the type of In species present in the catalyst can be regulated, thus enhancing DeNOx activity and CH4 selectivity in the CH4-SCR reaction. At a low temperature of 400 °C and a low CH4/NO feed ratio (CH4/NO = 1), the 3In/SSZ-39 catalyst, featuring highly active InOx clusters, achieves the best low-temperature CH4-SCR performance, with a high NO conversion rate of up to 90% and a CH4 selectivity of up to 74.2%.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Jun Ma,Jiahe Zhang,Ye Yuan,Yunqi Zhou,Shenzhen Cong,Guangyu Xing,Jixiao Wang,Zhi Wang
N 2 /CH 4 separation membranes based on N 2 preferential permeation can effectively reduce the recompression cost of CH 4 gas and show promising application prospects in the field of natural gas purification. However, the performance of N 2 /CH 4 separation membranes still needs to be improved. Here, we report a kind of mixed matrix membranes (MMMs) for N 2 /CH 4 separation via using HOF-21 as nanofiller and 6FDA-DAM polyimide as polymer matrix . In this work, the effects of HOF-21 loading, feed side pressure and temperature based on membrane performance were explored, and finally performance variation of the MMMs with operation time was tested. The incorporated HOF-21 nanoparticles with the most probable pore size of about 3.6 Å can significantly increase the diffusion rate of smaller N 2 molecules and enhance the N 2 /CH 4 diffusivity selectivity of the membrane. In addition, compared with polyimide, HOF-21 exhibits almost the same dynamic adsorption of N 2 and CH 4 , which can weaken the solubility of CH 4 and enhance the N 2 /CH 4 solubility selectivity of the membrane. When feed gas pressure was 0.2 MPa, the optimum membrane performance was achieved at the HOF-21 loading of 7 wt%, with N 2 permeance of 5.13 GPU and N 2 /CH 4 (50/50, vol%) selectivity of 20.52 at 298.15 K. Compared with N 2 permeation and N 2 /CH 4 selectivity of the 6FDA-DAM/PAN membrane, the MMMs increased by 67% and 54%, respectively, possessing potential applications in the field of N 2 removal in CH 4 purification.
研究领域:
材料科学
·
化学工程
·
天然气净化技术
✓ 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）