JOURNAL OF MEMBRANE SCIENCE
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2014
·
IF 4.908
Zhihua Qiao,Zhi Wang,Shuangjie Yuan,Jixiao Wang,Shichang Wang
Small molecular amines (SMAs) (ethanediamine (EDA), piperazine (PIP), monoethanolamine (MEA) and diethanol amine (DEA)) were separately used to modify the polyvinylamine (PVAm). ATR-FTIR, elemental analyzer, XRD and SEM were employed to characterize the SMA interacted PVAm. The PVAm–SMA/polysulfone (PS) membranes were developed by coating PVAm–SMA mixed solutions on the PS ultrafiltration membrane. CO 2 permeance and CO 2 /H 2 selectivity of the PVAm–SMA/PS membranes were investigated. Among different PVAm–SMA/PS membranes, the PVAm–MEA/PS membrane shows the highest CO 2 /H 2 separation performance. Moreover, the effect of the selective layer thickness on the CO 2 /H 2 separation performance of the PVAm–MEA/PS membrane was studied. With increasing the PVAm–MEA selective layer thickness, the CO 2 /H 2 separation performance of the membrane apparently decreases. Finally, the CO 2 /H 2 separation performance stability of the PVAm–MEA/PS membranes was investigated and no deterioration in the membrane permselectivity was observed.
研究领域:
材料科学
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化学工程
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2020
·
IF 7.183
Xiaochang Cao,Haoqing Xu,Songlin Dong,Jiayou Xu,Zhihua Qiao,Song Zhao,Jixiao Wang,Zhi Wang
In this work, we proposed a simple method to prepare high-performance and pressure-resistant mixed matrix membranes (MMMs) for CO 2 /H 2 separation. The groups or segments of poly-(vinylamine) (PVAm) were used to modify covalent organic frameworks (COFs), and COFs with similar frameworks but different surfaces were obtained. Then, modified COFs were mixed with PVAm matrix and used to coat the modified-polysulfone (mPSf) to prepare MMMs for CO 2 /H 2 separation. Modified COFs and the PVAm matrix were highly compatible because COF surfaces possessed the same groups or segments as PVAm. Meanwhile, in the coating solution, COF surfaces were found to induce penetration of PVAm molecules into COF pores, narrowing the pore size of the COFs and providing an amino environment for CO 2 preferential absorption and transport. The penetration degree was affected by the hydrogen bond between COF surfaces and the PVAm molecules. In addition, the incorporated COFs effectively restricted the mobility of the PVAm matrix, increasing the pressure resistance for MMMs under high pressure. In the gas permeation test, the optimal MMMs could achieve a CO 2 permeance of 957 GPU and a CO 2 /H 2 selectivity of 17.1 at 2.0 MPa because of the high compatibility and size of the channels (0.94 nm).
研究领域:
材料科学
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化学工程
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Meng Rong,Liangrong Yang,Chao Yang,Jiemiao Yu,Huizhou Liu
Herein, a new tetraphenyladamantane-cored triazine-based multiamine (TPADT) was designed and synthesized. Its bulky molecular volume, strong rigidity, and high amine functionality enable it easy to prop up the polymer backbone and form a high hypercrosslinking degree to obtain high microporosity. A series of highly microporous tetraphenyladamantane-based polyaminals (Ad-MALPs) were prepared through the catalyst-free copolymerization of TPADT and commercial aromatic aldehydes. By changing the strut length and functionality of aldehyde monomers , the resulting polymers exhibit tailored BET surface area (1541–1779 m 2 /g) and narrow ultramicropore size distribution (0.52–0.93 nm). Ad-MALP-2 with the largest microporosity possesses the highest CO 2 uptake (21.1 wt %, 273 K/1.0 bar) and CO 2 /N 2 adsorption selectivity (35.2). Interestingly, Ad-MALP-3 shows the highest H 2 uptake (2.26 wt%, 77 K/1.0 bar) due to larger total pore volume . In addition, highly microporous Ad-MALPs simultaneously contain aromatic and cycloaliphatic components, and thus show exceptionally large aromatic and cycloaliphatic organic vapor adsorption capacity under low pressure. At P/P 0 = 0.1, the benzene and cyclohexane vapor uptakes of Ad-MALPs are up to 44.8 wt% and 39.0 wt %, far exceeding that of most previously reported porous organic polymers . Considering that Ad-MALPs have outstanding gas adsorption performance, simple preparation, good stability, and cycle ability, they are expected to be promising adsorbent materials for CO 2 adsorption/separation, H 2 storage and low-concentration volatile organic vapors capture.
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Science Advances
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2026
·Vol. 12
·期 31
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IF 13.9
Kun Li,Yuan Peng,Wentai Hu,Xinyu Wang,Weishen Yang
Carbon capture is essential for producing blue hydrogen and syngas. However, designing a single membrane with dual CO 2 -selective and H 2 -selective separations has long been considered impractical because these modes rely on fundamentally different mechanisms. We report a stimuli-responsive membrane that overcomes this limitation by integrating two functional materials. A zirconium metal-organic polyhedron (Zr-MOP) polymerized hydrogel membrane was fabricated via a stepwise molecular-level blending and polymerization strategy, achieving excellent filler dispersion, strong interfacial compatibility, and good solution processability. The Zr-MOP cages reinforce the hydrogel hydrogen-bond network, enabling high CO 2 -philic performance with a CO 2 /H 2 separation factor of 44 and CO 2 permeability of 7025 Barrer. Upon dehydration, membrane shrinkage induces cage rearrangement and exposure of molecular sieving windows, switching the separation behavior to a highly H 2 -selective mode with an H 2 /CO 2 separation factor of 798. This transition is reversible and can be further regulated by pH stimuli. This work introduces a strategy for membranes with switchable and inverted separation functions.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2023
·Vol. 29
·期 18
·e202203152
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IF 4.3
Yan Long,Jie He,Hang Zhang,Yingkang Chen,Kang Liu,Junwei Fu,Hongmei Li,Li Zhu,Zhang Lin,Andrei Stefancu,Emiliano Cortes,Mingshan Zhu,Min Liu
Graphical Ag/Al 2 O 3 catalytic controllable synthesis of N-monomethylated amines by using CO 2 /H 2 as C 1 source has been demonstrated in a first example. The reactivity of methylated amines was reduced by the heterolytic dissociation of H 2 over the catalyst, and hence conversion of various amines to corresponding monomethylated amines was enabled with excellent selectivity. The selective synthesis of monomethylated amines with CO 2 is particularly challenging because the formation of tertiary amines is thermodynamically more favorable. Herein, a new strategy for the controllable synthesis of N-monomethylated amines from primary amines and CO 2 /H 2 is explored. First-principle calculations reveal that the dissociation of H 2 via an heterolytic route reduces the reactivity of methylated amines and thus inhibit successive methylation. In situ DRIFTS proves the process of formation and decomposition of ammonium salt by secondary amine reversible binding with H + on the Ag/Al 2 O 3 catalyst, thereby reducing its reactivity. Meanwhile, the energy barrier for the rate-determining step of monomethylation was much lower than that of overmethylation (0.34 eV vs. 0.58 eV) means amines monomethylation in preference to successive methylation. Under optimal reaction conditions, a variety of amines were converted to the corresponding monomethylated amines in good to excellent yields, and more than 90 % yield of product was obtained.
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Haoyi Guo,Pan Cao,Muxian Liu,Guohui Dai,Bei Liu,Changyu Sun,Chun Deng,Guangjin Chen
Hydrogen is regarded as a promising alternative to fossil fuels; however, approximately 95% of the global hydrogen supply still comes from “gray hydrogen”, with high carbon emissions. Efficient separation of CO2 and H2 is a key challenge in gray hydrogen production. This study proposes a novel H2 recovery process based on an aqueous solution of 2-methylimidazole (2-MeIm). The 2-MeIm aqueous solution possesses both strong CO2 absorption capacity and easy desorption performance, which can reduce energy consumption. Pure component solubility experiments were carried out at temperatures ranging from 283.15 to 353.15 K and pressures ranging from 0 to 2.0 MPa, yielding 66 sets of pure CO2 solubility data and 15 sets of pure H2 solubility data, which were used to regress the binary interaction parameters of the NRTL model. Comparison between the fitted NRTL model parameters and the experimental data indicates that the mean relative error of CO2 is 5.19%, whereas that of H2 is only 0.18%. Further, single-equilibrium-stage phase equilibrium experiments were conducted using a mixed gas stream with a CO2/H2 molar ratio of 40:60 to further validate the accuracy of the fitted NRTL parameters. The results demonstrate that the solubility-based fitted model achieves a mean absolute error (MAE) of 0.03 for gaseous CO2 and a mean relative error (MRE) of 0.93% for liquid-phase CO2, indicating high predictive accuracy. Based on Aspen Plus, this study has developed a rigorous process simulation model with a processing capacity of 100,000 N m3/h. The operating conditions were defined through sensitivity analysis, resulting in the following optimized parameters: 7 theoretical stages for the absorber, an operating pressure of 3.8 MPa, a volumetric gas-to-liquid ratio of 200, and a desorption temperature of 373.15 K. Under these conditions, H2 purity and recovery reached 99.99% and 99.13%, with specific energy consumption of only 260.27 kgoe/t H2 (10.88GJ/t H2). Compared with the conventional Rectisol process, the 2-MeIm-based process not only achieves higher H2 purity and recovery rate, but also significantly reduces total energy consumption by 32.07%. This marked performance enhancement underscores the outstanding energy-saving potential of the 2-MeIm system in the field of H2/CO2 separation.
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高影响因子
FUEL
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2026
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IF 7.5
Xuanyu Lin,Yiming Qin,Xinyu Feng,Hanzhen Liu,Zhenhang Lu,Xin Tang
CO 2 as a rich source of carbon can provide an alternative route to produce value-added chemicals. Electrocatalysis is one of the most promising approaches to convert CO 2 captured from the atmosphere into valuable chemicals. However, the CO 2 molecule is relatively stable and requires a large amount of energy to activate CO 2 for conversion. We develop a new creative type of solid-state CO 2 fuel cell that can generate high-value-added chemicals through electrochemical reduction of CO 2 without external electrical energy input while achieving self-power generation, operating in the medium temperature range of 400–700 ℃. This study demonstrates a fuel cell operating at 570 °C, which achieves a current density of 686.0 A·m −2 and a power density of 98.8 W·m −2 . Under these conditions, the fuel cell achieved a product formation rate of 140.0 μmol·g cat −1 ·h −1 . The system’s operational parameters enable its integration into combined heat and power (CHP) generation, simultaneously facilitating CO 2 conversion, thereby aligning with sustainable energy and emissions reduction strategies.
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 135
·期 5
·45765
·
IF 1.86
Leiqing Hu,Jun Cheng,Yannan Li,Jianzhong Liu,Junhu Zhou,Kefa Cen
To optimize the CO 2 permeation and CO 2 /H 2 separation performance of hollow fiber-supported polydimethylsiloxane (PDMS) membranes, the effect of the viscosity of the PDMS coating solution on surface morphologies, thickness of PDMS layer, and solution intrusion into surface pores of hollow fiber supports was investigated. Increases in both stirring time and standing time could increase the viscosity of the PDMS solution. The PDMS layer thickness increased when the coating solution viscosity increased, whereas the surface roughness of the PDMS layer markedly decreased and then slightly changed. Moreover, when the stirring time of the PDMS coating solution was 9 min and the standing time was increased from 2 min to 25 min, the CO 2 permeance first decreased, then increased to ∼2250 GPU probably due to the decreased intrusion depth, and finally decreased because of the substantially increased thickness of the PDMS layer. However, the CO 2 /H 2 selectivity increased to 3.4 with an increase in coating solution viscosity. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 45765.
研究领域:
材料科学
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化学工程
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高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200063
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IF 9.14
Qing Ji,Xiaoping Chen,Ya-Jun Cheng,Qingyu Dong,Yanbin Shen,Zhaohui Yang,Binjie Hu,Yonggao Xia
Graphical Carbon, the master : Constructed with unique carbon emcoating structure through CO 2 acivation, NbO 2 benefited from an effective and highly conductive carbon network, giving rise to exceptional electrochemical performances in terms of reversible capacities, rate capability, and cyclic stability. As a promising alternative as lithium-ion anode, niobium dioxide appeals to researchers due to high theoretical capacity and good electron conductivity. However, rarely work about NbO 2 based high performance anode is reported. Here, NbO 2 nanoparticles emcoated in continuous carbon matrix is constructed through CO 2 /H 2 coupling treatment. CO 2 activation introduces unique carbon emcoating structure, which builds interconnected electron conductive network with low carbon content. Furthermore, crystallographic phase of NbO 2 is enhanced during H 2 treatment, which increases the lithium storage ability. Electrochemical performance of NbO 2 anodes is significantly improved based on the carbon emcoating structure. A high reversible capacity of 391 mAh g −1 is retained after 350 cycles at 0.2 C. Additionally, at a current density of 1 A g −1 , the reversible capacity reaches 139 mAh g −1 . Compared with conventional NbO 2 /C nanohybrids, the lithium diffusion coefficient of carbon-emcoated sample shows improvement of three orders of magnitude. Moreover, the in situ XRD investigation shows a reversible lithium insertion behaviour with a limited volume change.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiaoman He,Zhangdi Peng,Peilin Shen,Chenjia Miao,Jiale Xie,Chen Deng,Panagiotis G. Kougias,Dekui Shen,Richen Lin
Conversion of CO2 and H2 into biomethane is a promising technology within the concept of power-to-X. However, the integration of high-value-added products can enhance the economic viability and diversify future biobased production chains. Herein, an integrated biosystem converting CO2/H2 into acetic acid, which is further converted to C4+ fatty acids, was demonstrated with the aim to assess the role of carbonaceous materials (model nanomaterial graphene and cost-effective biochar) and external electron donor (ethanol). With the supplementation of ethanol as the electron donor, carbonaceous materials significantly increased the production and selectivity of butyrate (C4) and caproate (C6) due to enhanced microbial growth and chain elongation efficiency. The highest concentration of butyrate (2512.35 ± 60.05 mg/L) was observed in the graphene-added group, while the highest concentration of caproate (396.74 ± 14.83 mg/L) was observed in the biochar group, suggesting different mechanisms induced by carbonaceous materials. Microbial community analysis revealed that carbonaceous materials primarily enriched members of the genus Clostridium_sensu_stricto_12, which are identified as typical carbon chain elongating microorganisms. Functional prediction revealed that carbonaceous materials increased the relative abundance of functional genes encoding crucial enzymes involved in both the Wood–Ljungdahl pathway and the fatty acid biosynthesis pathway. This study demonstrated an integrated approach for the efficient conversion of CO2 to value-added green chemicals.
研究领域:
环境生物学
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微生物学
·
合成生物学
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高影响因子
FUEL
·
2025
·
IF 7.5
Zhangkai Qian,Jia-qi Bai,Mei Ma,Huangfei Liu,Mengdie Cai,Jingshuai Chen,Song Sun
N -methylation of amines, nitro compounds and nitriles with CO 2 and H 2 offers a promising strategy for CO 2 utilization. However, developing highly efficient and stable Cu-based catalysts for selective mono- N -methylation of aniline remains challenging. Herein, we report the successful synthesis of a Cu-ZnO/TiO 2 catalyst, with the optimized 5 %Cu-7.5 %ZnO/TiO 2 catalyst achieving a 96.7 % yield of N -methylaniline (MA) and an initial turnover frequency (TOF) of 7.4 h −1 after 6 h under 453 K, 2 MPa CO 2 and 4 MPa H 2 . This performance surpasses all reported Cu-based catalysts and rivals noble metal-based systems. The catalyst demonstrated reusability at least four cycles and versatility in the N -methylation of various amines, nitro compounds, and nitriles. Kinetic studies revealed reaction orders of 0 with respect to aniline concentration and CO 2 pressure, and 1 with respect to H 2 pressure. Based on kinetics and extensive characterization, we propose a reaction mechanism over 5 %Cu-7.5 %ZnO/TiO 2 , identifying Cu nanoparticles as the active sites. The process proceeds via N -phenylcarbamic acid and N -phenylformamide intermediates, with the hydrogenation of N -phenylcarbamic acid as the rate-determining step.
研究领域:
化学工程
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催化科学
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环境科学
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhiwei Dong,Yudong Ding,Fei Chen,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
The inefficient conversion of carbon dioxide (CO 2 ) to methane often restricts the advancement of CO 2 biomethanation technologies . This study explored the degrading performance, microbial community compositions, and functional gene abundance to examine the impact of zirconium metal-organic frameworks (Zr-MOFs) on the CO 2 biomethanation process. The results showed that the maximum utilization rates of CO 2 and H 2 increased by 2.77 times and 2.36 times after the addition of Zr-MOFs, respectively, and the corresponding conversion rate of CO 2 to methane also increased by 57.53%. Additionally, Zr-MOFs enhanced the COD removal efficiency and hydrolysis of tryptophan-like proteins and humic acid-like substances, resulting in more volatile organic compounds, such as tetradecane, 2-pentanone, and hexadecanoic acid. The analysis of microbial community structure revealed that the relative abundance of Methanothrix and Metanobacterium increased by 24.40% and 36.02% after the addition of Zr-MOFs, respectively. The methane metabolism revealed that Metanobacterium was a member of the same aceticlastic methanogenic pathway as Metanothrix , which encodes acetyl-CoA synthetase to catalyze the synthesis of acetyl-CoA from acetate, and Zr-MOFs also increased the relative abundance of genes that encode the enzyme responsible for converting intermediates to methane. Finally, Zr-MOFs improved the biogenesis and utilization of acetate and hydrogen (H 2 ) by enhancing the activity of enzymes, thereby providing more nutrients for methanogenesis . This study provided thorough explanations for the application and improvement of Zr-MOFs in CO 2 biomethanation technology.
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