JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Zhiying Li,Zhiwei Li,Ning Zhang,Junjiang Bao,Xiaopeng Zhang,Gaohong He,Cong Chen,Yongchen Song
Ultrathin and defect-free MOF membranes are actively pursued to realize high-performance hydrogen purification and carbon capture, which are of great significance for energy conservation and environmental sustainability. Zeolitic imidazolate framework-67 (ZIF-67) possesses exceptional pore apertures for sieving hydrogen from other larger gases. However, the preferential heterogeneous nucleation and growth of ZIF-67 crystals greatly challenge the synthesis of ZIF-67 membranes. In this work, a tunable-reaction-zone contra-diffusion synthesis is proposed to effectively assemble ZIF-67 nanocrystals into ultrathin GO laminates. The contra-diffusion-match growth of ZIF-67 constructs a compact ZIF-67@GO hybrid structure with superior H 2 /CO 2 separation factor of 140.8 and H 2 permeance of 1.7 × 10 −7 mol m −2 s −1 Pa −1 , transcending the state-of-art upper bounds. The excellent separation performance is attributed to the collaborative effect of the size-sieving and the selective attraction of the ZIF-67@GO hybrid structure. Long-term operation also reveals the superior stability of the ZIF-67@GO hybrid membrane for H 2 /CO 2 separation. The rational-design approach grants a novel way to fabricate ultrathin and defect-free ZIF-67 crystalline membranes for high-performance gas separation.
研究领域:
材料科学
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环境科学
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能源工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Chenyang Zhao,Yujia Liu,Hongwei Zhu,Junjie Feng,Huiyun Jiang,Fei An,Yan Jin,Wei Xu,Zhe Yang,Bing Sun
The ability to selectively remove H 2 from the product has made palladium (Pd) membrane reactor a good choice for steam reforming reaction. However, carbonaceous deposited on the surface of Pd membrane during reaction hindered its industrial application. In order to protect Pd membrane from being poisoned by water and light alcohols, a TS-1/Pd composite membrane was prepared by a facile one-step hydrothermal method combined with silane coupling treatment. The zeolite layer acted as a protective armor by keeping poisonous species away from the Pd bulk, and the silanization process increased the hydrophobicity by reducing the hydroxyl density on the surface of TS-1/Pd composite membrane. After 100 h’s exposure in the steam reforming condition, the percentage of carbon content was only 0.95% for the TS-1/Pd membrane, compared with 13.20% for the pure Pd membrane. The H 2 permeability and H 2 /N 2 selectivity of the TS-1/Pd remained constant, while that for pure Pd membrane fell by 50% and 80%, respectively. The significantly improved resistance to carbon deposition provides possibility for the large-scale application of Pd membrane reactor in hydrogen production via steam reforming.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Changdie Cao,Yurun Dai,Zhihao Liu,Zong Lu,Mide Luo,Yanying Wei,Haihui Wang
Two-dimensional (2D) nanosheet membranes presented excellent gas separation performance, which has attracted increasing attention. The electrophoretic deposition (EPD) method provides a fast and scalable route for the preparation of 2D nanosheet membranes aimed at future industrial applications. However, the formation of bubbles via water electrolysis during EPD would damage the membrane structure, and the expansion of interlayer spacing would hinder its utilization. Herein, the solvent-mediated structural regulation strategy for MXene membrane preparation via EPD is proposed for H 2 purification. The effect of various organic solvents on the EPD-prepared MXene membrane structure and gas separation performance has been investigated. Notably, the MXene membranes deposited using acetone as solvent exhibit outstanding gas separation performance, boasting an H 2 /CO 2 selectivity of 374 with a H 2 permeance of 748 GPU for at least 450 h. This work offers a novel approach to fast fabricating 2D nanosheet membranes with outstanding gas separation performance
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Shan Li,Huixia Li,Taotao Huang,Xuebo Chen
The development of efficient Cu–Ce catalysts for selective CO oxidation in hydrogen streams (CO-PROX) remains a critical challenge for hydrogen purification technologies. Herein, we report an acid-modified Cu–Ce/γ-Al2O3 catalyst synthesized through HCl-assisted wet impregnation and thermal aging, demonstrating exceptional low-temperature CO-PROX performance. The optimized CuCe0.8(Cl)0.2/γ-Al2O3 catalyst achieves superior CO conversion below 160 °C and maintains stable activity for 50 h at 160 °C. Mechanistic studies reveal that HCl modification induces dual enhancement effects: (1) increased Cu+ species density enhances CO adsorption capacity; (2) elevated Ce3+ concentration promotes oxygen vacancy formation for efficient O2 activation. Complementary characterization demonstrates that the acid treatment optimizes the active species dispersion and creates hierarchical pore structures in the γ-Al2O3 support, which facilitates reactant accessibility and stabilizes catalytic intermediates. The reaction mechanism involves synergistic cooperation between Cu+-mediated CO adsorption, oxygen vacancy-assisted O2 activation, and hydroxyl-assisted bicarbonate intermediate formation on the alumina support. This work establishes an effective acid-modification strategy for designing durable CO-PROX catalysts, advancing the development of a practical hydrogen purification system.
研究领域:
催化化学
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材料科学
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环境科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Heyu Li,Zhe Sun,Shaochen Shang,Yan Cao
The development of cost-effective and reactive oxygen carriers and the fast and complete conversion of solid fuels are two critical issues in the solid fuel chemical looping technology. Red mud, a solid waste from the alumina industry, was found to be an economic oxygen carrier candidate simultaneously realizing the use of solid wastes and the CO 2 abatement after comparing with other two different iron-based materials (pure Fe 2 O 3 and hematite). This study validated red mud as an excellent oxygen carrier to achieve the almost complete conversion of char in solid fuels (SFs) (99.4%) and meanwhile the hydrogen production with high-purity (97% H 2 purity) and higher H 2 yield (around 500 mL/g), in the optimized pyrolysis procedure of solid fuels with proper gasification agent and rationalized reaction temperatures (1000 °C) and residence time (10mins). Characterizations of red mud using SEM-EDS and XRD revealed that the unique microscopic crystalline structures of both Fe 2 O 3 and Ca 2 Al 2 SiO 7 particles nested on Na 4 Al 2 Si 2 O 9 molten substrate, implying that the existence of Na-containing component of the red mud OC likely accounts for its higher reactivity and stability in multiple redox cycles.
研究领域:
能源科学
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材料科学
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环境工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Zhou Yisa,Wu Ying,Wu Haoyu,Xue Jian,Ding Li,Wang Rui,Wang Haihui
Two-dimensional graphitic carbon nitride (g-C 3 N 4 ) nanosheets are ideal candidates for membranes because of their intrinsic in-plane nanopores. However, non-selective defects formed by traditional top-down preparation and the unfavorable re-stacking hinder the application of these nanosheets in gas separation. Herein, we report lamellar g-C 3 N 4 nanosheets as gas separation membranes with a disordered layer-stacking structure based on high quality g-C 3 N 4 nanosheets through bottom-up synthesis. Thanks to fast and highly selective transport through the high-density sieving channels and the interlayer paths, the membranes, superior to state-of-the-art ones, exhibit high H 2 permeance of 1.3 × 10 −6 mol m −2 s −1 Pa −1 with excellent selectivity for multiple gas mixtures. Notably, these membranes show excellent stability under harsh practice-relevant environments, such as temperature swings, wet atmosphere and long-term operation of more than 200 days. Therefore, such lamellar membranes with high quality g-C 3 N 4 nanosheets hold great promise for gas separation applications.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
AICHE JOURNAL
·
2020
·Vol. 66
·期 10
·e16543
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IF 3.519
Shanshan He,Xu Jiang,Songwei Li,Feitian Ran,Jun Long,Lu Shao
The high fractional free volume (FFV) endowed polymers of intrinsic microporosity (PIMs) with high gas permeability but low selectivity. Herein, an intermediate temperature range was deliberately utilized to tune PIM-1 membrane microstructure in nitrogen atmosphere to enhance gas separation performance. During intermediate thermal manipulation, the synergistic effects of thermal-induced cross-linking and decomposition on PIM-1 membranes have optimized the micropores for significantly increasing membrane molecular-sieving ability with the boosted selectivity of 350 (H 2 /N 2 ), 1,472 (H 2 /CH 4 ), 3,774 (H 2 /C 3 H 8 ), and 197 (CO 2 /CH 4 ) respectively, with the H 2 permeability of 234 Barrer, correspondingly, surpassing the “Robeson's Upper Bound”. The facile strategy simultaneously utilizing the thermal-induced cross-linking and decomposition, might provide a new platform to develop the high-performance membranes for highly-efficient hydrogen purification and CO 2 separations.
研究领域:
材料科学
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高分子科学
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化学工程
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膜技术
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气体分离
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
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IF 4.084
Feng Chen,Songlin Dong,Zhi Wang,Jiayou Xu,Rui Xu,Jixiao Wang
The incompatibility between nanofillers and polymer, caused by the agglomeration of nanoparticles and their weak interaction with each other, is still a challenge to develop mixed matrix composite membrane . Herein, we introduced the ZIF-8-TA nanoparticles synthesized by in situ hydrophilic modification into the hydrophilic poly(vinylamine) (PVAm) matrix to prepare composite membranes for H 2 purification. The dispersion of ZIF-8 in water was improved by tannic acid modification, and the compatibility between ZIF-8 particles and PVAm matrix was enhanced by chemical crosslinking between the quinone groups in oxidized tannic acid (TA) and the amino groups in PVAm. Moreover, the compatibility between hydrophobic polydimethylsiloxane (PDMS) gutter layer and hydrophilic separation layer was achieved by the adhesion of TA-Fe 3+ complex to the surface of PDMS layer during membrane preparation. The interlayer hydrophilic modification and the formation of separation layer were accomplished in one step, which simplified the preparation process. The experimental results indicated that when the TA addition used for modification was 0.5 g and the ZIF-8-TA 0.5 content in membrane was 12 wt%, the prepared membrane showed the best separation performance with the CO 2 permeance of 987 GPU and the CO 2 /H 2 selectivity of 31, under the feed gas pressure of 0.12 MPa.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Guang Miao,Pengxian Ye,Junyang Wang,Jiawu Huang,Jing Xiao,Chunshan Song
The development of cost-effective, high-performance sorbents for CO2 capture in hydrogen purification remains a critical challenge, particularly under industrial conditions of ultralow CO2 concentrations and ambient temperatures. This study systematically investigates polyethylenimine (PEI)-impregnated SiO2 and SBA-15 sorbents, with a focus on enhancing CO2 uptake and kinetics through polyethylene glycol (PEG) incorporation. Although PEI-SBA-15 sorbents showed higher static and dynamic CO2 uptakes compared to PEI-SiO2 sorbents, its diffusion barrier lowers the adsorption rate in the flow system. The poly(ethylene glycol) (PEG) polymers were introduced to PEI-SiO2 to improve the mass transfer of CO2 in PEI clusters. The low PEI loading was found to be beneficial to CO2 adsorption on SiO2, resulting in superior CO2 uptakes and a lower diffusion barrier than PEI-SBA-15 sorbents. The characterization was conducted to uncover physical and chemical properties. The breakthrough experiments of PEI-30-SiO2 with PEG derivates confirmed that the O in the skeleton of PEG played an important role in the interaction between PEI and PEG rather than terminal OH groups. This work also demonstrated the CO2 desorption and stability of PEG-modified PEI-SiO2 sorbents in H2.
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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能源技术
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吸附分离
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功能高分子材料
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Fengting Yao,Ziheng Li,Yan Dai,Xuehua Ruan,Xiaohang Yang,Xiaobin Jiang,Wenji Zheng,Gaohong He
Metal organic frameworks (MOFs)-based mixed matrix membranes (MMMs) exhibit great prospects for H 2 purification. However, their further development is hindered by interfacial incompatibility and framework flexibility-induced selectivity loss. Inspired by the “like compatible like” principle, a fluorinated engineering strategy is developed by introducing isoelectronic −CF 3 groups into ZIF-9 (FZIF-9), achieving dual regulation of MOF-polyimide (6FDA-TFMB) interfaces and molecular sieving architecture. The −CF 3 functionalization synergistically enhances interfacial compatibility through dipole interactions (C═O···F−C), optimizes pore size (3.67 Å) to achieve size-exclusive H 2 /CH 4 separation. Meanwhile, it suppresses the dissolution and adsorption of CH 4 molecules by reducing the CH 4 adsorption capacity on FZIF-9 by 40% compared with ZIF-9. The FZIF-9/PI-20 wt.% MMM exhibits excellent improvements of 22.1% and 133.1% in H 2 permeability (159 Barrer) and H 2 /CH 4 selectivity (295) over ZIF-9/PI-20 wt.% MMM. Importantly, its selectivity is superior to state-of-the-art MOFs/6FDA-based MMMs, approaching the 2015 Robeson upper bound. This work establishes fluorine-mediated interface engineering as a universal strategy for advanced gas-separation membranes, particularly in H 2 /CH 4 separation.
研究领域:
化学工程
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材料科学
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膜技术
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气体分离
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yiyang Zeng,Shuai Yang,Mao Yang,Yu Gong,Xingrui Tang,Xiaolong Fu,Junyan Wang,Guangming Ran,Chengjian Xiao
Hydrogen separation and purification play a crucial role in the chemical industry. High-temperature electrochemical hydrogen pump (HT-EHP) technology based on polybenzimidazole (PBI) membranes has great potential for hydrogen purification, the key to this application lies in the design of PBI membranes with high proton conductivity. To achieve this, we optimized the spatial conformation of polymer chains by coordinating metal ions (Zn 2+ /Co 2+ ) with the imidazole groups in PBI, forming continuous coordination cavities. Molecular dynamics (MD) simulations revealed that the coordination between metal ions and imidazole induces polymer chain distortion, creating sub-nanometer coordination cavities (∼8 Å). Wide-angle X-ray scattering (WAXS) and wide-angle X-ray diffraction (WAXD) confirmed the existence of these coordination cavities. After the removal of metal ions, the residual cavities were filled with phosphoric acid (PA), constructing long-range ordered proton conduction pathways in the high-performance PBI membranes ( o -PBI-Zn and o -PBI-Co). Scanning electron microscopy (SEM) analysis showed that the continuous porous network within the polymer chains resembles a root-like structure, facilitating efficient three-dimensional proton transport. The resulting membranes exhibited excellent mechanical properties (tensile strength of 45 MPa) and outstanding proton conductivity (0.126 S/cm at 160 °C). When assembled into a HT-EHP, the membranes achieved a hydrogen purification rate of 9.22 mL (cm 2 ·min) −1 at 180 °C, with an energy consumption as low as 0.1 kWh/L(H 2 ). This study presents an innovative strategy for designing high-proton-conductivity PBI membranes, significantly enhancing their potential for HT-EHP applications, offering a promising alternative for hydrogen purification technologies.
研究领域:
材料科学
·
化学工程
·
膜技术
·
能源技术
·
电化学
✓ 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）