SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Peng Hu,Jialang Hu,Long Li,Gui Shi,Mingyuan Jiang,Yuhan Chen,Lvming Jin,Chao Xiong,Hongbing Ji
Effective methane separation of gaseous C2-C3 alkanes from natural gas is crucial yet challenging industrial process. Herein, we report the impressive MOF ( 1a ) with rigid topology and ultramicroporous characters that can realize effective methane purification. Adsorption isotherms on 1a show the differential adsorption capacity, with values of 22.7 cm 3 g −1 for CH 4 , 69.1 cm 3 g −1 for C 2 H 6 and 83.6 cm 3 g −1 for C 3 H 8 at 298 K and 1 bar. IAST analysis reveals the calculated C 3 H 8 /CH 4 selectivity of 1a is 1228/1776 with the molar ratio of 50/50 and 10/90 at zero coverage, respectively. The higher selectivity is also demonstrated by C 2 H 6 /CH 4 mixtures. Breakthrough tests reveal the effective purification of CH 4 /C 2 H 6 /C 3 H 8 (85/10/5, v/v/v) mixtures, achieving >99.95 % CH 4 purity at a productivity of 88.7 L kg −1 . Further, scalable 1a with customized grain-size (3.4 g) also reveal the breakthrough performance under higher gas flux (30 sccm or 1.50 × 10 −3 kg h −1 ), indicative of great potential for industrial methane upgrading. Experimental and theoretical calculations show that the pore polarity of 1a can be effectively modulated upon the adsorption of C 3 H 8 molecules with abundant methyl groups without post-modification of MOF structure or introducing heterogeneous species (such as metals or ligands). This guests-induced self-regulatory strategy and decent adsorption orientation further enhances the gas diffusion and continuous adsorption of subsequent C 3 H 8 molecules. Such a strategy affords a novel perspective in adjusting pore polarity and enables methane upgrading from natural gas mixtures.
研究领域:
材料科学
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化学工程
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能源技术
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DOI
高影响因子
Journal of Materials Chemistry A
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2020
·Vol. 8
·期 26
·13132-13141
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IF 11.301
Yang Feng,Zhikun Wang,Weidong Fan,Zixi Kang,Shou Feng,Lili Fan,Songqing Hu,Daofeng Sun
The designability and adjustability of the pore structure are vital advantages of metal–organic framework (MOF) materials for separation. Their exploration in the field of membrane separation is still inadequate, especially for the regulation of the pore environment based on the inorganic secondary building unit (SBU). In this work, we have studied the effect of the pore environment regulated by the SBU on the gas separation performance of MOF membranes for the first time. The Fe3(μ3-O)(CH3COO)6 SBU of the parent framework (soc-MOF, a stable microporous Fe-MOF) was in situ modified with imidazole (IM) molecules to construct the soc-MOF-IM polycrystalline membrane. The exact location of the incorporated IM and the narrowed pore size are observed based on the determined crystal structure. The gas solubility, diffusivity and separation performance of the two membranes are evaluated. Compared to the soc-MOF membrane with a H2/CO2 selectivity of 6, the soc-MOF-IM polycrystalline membrane possesses a significantly enhanced H2/CO2 selectivity (48), which is mainly attributed to the triggered molecular sieving effect. Thanks to the facile introduction of functional molecules and precise adjustment of the pore environment, SBU modification can be a powerful strategy to improve the separation performance of MOF membranes.
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
Materials Today Chemistry
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2022
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IF 7.613
X.-T. Mu,Y.-S. Ouyang,L.-M. Pei,Z.-X. Peng,S.-Q. Shao,S.-M. Wang,H. Xiong,Y. Xiao,Q.-Y. Yang
Adsorptive separation of C 2 H 6 from C 2 H 4 by adsorbents is an energy-efficient and promising method to boost the polymer grades C 2 H 4 production. However, that C 2 H 6 and C 2 H 4 display very similar physical properties, making their separation extremely challenging. In this work, by regulating the pore environment in a family of chitosan-based carbon materials (C-CTS-1, C-CTS-2, C-CTS-4, and C-CTS-6)- we target ultrahigh C 2 H 6 uptake and C 2 H 6 /C 2 H 4 separation, which exceeds most benchmark carbon materials. Explicitly, the C 2 H 6 uptake of C-CTS-2 (166 cm 3 /g at 100 kPa and 298 K) has the second-highest adsorption capacity among all the porous materials. In addition, C-CTS-2 gives C 2 H 6 /C 2 H 4 selectivity of 1.75 toward a 1:15 mixture of C 2 H 6 /C 2 H 4 . Notably, the adsorption enthalpies for C 2 H 6 in C-CTS-2 are low (21.3 kJ/mol), which will facilitate regeneration in mild conditions. Furthermore, C 2 H 6 /C 2 H 4 separation performance was confirmed by binary breakthrough experiments. Under different ethane/ethylene ratios, C-CTS-X extracts a low ethane concentration from an ethane/ethylene mixture and produces high-purity C 2 H 4 in one step. Spectroscopic measurement and diffraction analysis provide critical insight into the adsorption/separation mechanism. The nitrogen functional groups on the surface play a vital role in improving C 2 H 6 /C 2 H 4 selectivity, and the adsorption capacities depend on the pore size and micropore volume. Moreover, these robust porous materials exhibit outstanding stability (up to 800 °C) and can be easily prepared on a large scale (kg) at a low cost (∼$26 per kg), which is very significant for potential industrial applications.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Catalysts
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2024
·Vol. 14
·期 10
·707
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IF 3.8
Zengjing Guo,Shuguang Ning,Shicheng Xu,Yongying Zhang,Yifan Dong,Hongjing Han
Ambient condition-determined chemical CO2fixation affords great promise for remitting the pressure of CO2release. The construction of a microporous environment easily captures CO2molecules around the reactive sites of the catalyst to reinforce the reaction process. Herein, multi-hydroxyl-containing hyper-crosslinked organic polymers (HCPs-OH-n) are synthesized by the polymerization of 1,4-dichlorobenzyl (DCX) andm-trihydroxybenzene in the monosaccharide form in a Friedel–Crafts alkylation hypercrosslinking process (FCAHP). By tuning the DCX ratio in the FCAHP, the structural properties can be regulated to create a more microporous surface in the HCPs-OH-n; meanwhile, the formed multi-hydroxyl species in the microporous environment could induce the easy interaction between hydroxyls and epoxides by forming a hydrogen bond, which improves the activation of epoxides during the cycloaddition reaction to synthesize the cyclic carbonates at ambient conditions. The structural properties suggest that HCPs-OH-npossess a large surface area with appreciable microporous and mesoporous distribution. As expected, the HCPs-OH-3 bearing the most abundant mesoporosity affords the highest reactivity in the chemical CO2fixation to cyclic carbonates and is endowed with rational recoverability.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Chaohui He,Yong Wang,Yang Chen,Xiaoqing Wang,Jiangfeng Yang,Libo Li,Jinping Li
The development of ethane (C 2 H 6 )-selective adsorbents displaying high uptake and selectivity to purify ethylene (C 2 H 4 ) to obtain polymer-grade raw materials is a meaningful, but challenging process. Tailoring the pore chemistry of a metal-organic framework is an effective strategy used to construct high performance adsorbents. Herein, BUT-10 with a tailored pore environment for tuning the C 2 H 6 adsorption ability has been synthesized via introducing functional sites into UiO-67. The single component gas adsorption capacity, adsorption heat and adsorption selectivity of BUT-10 have been proven to be effectively increased after modifying the pore environment. Computational studies have revealed that the stronger adsorption affinity for C 2 H 6 was achieved via multiple adsorbate-framework interactions in the appropriate pore environment. Breakthrough experiments using BUT-10 as a C 2 H 6 -selective adsorbent have shown that polymer grade C 2 H 4 was directly produced from C 2 H 6 /C 2 H 4 (1/15 v/v) mixtures using a single separation process under ambient conditions.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Mingming Xu,Kang Wang,Dongdong Zheng,Mo Li,Fei Xu,Peng Cui,Yao Jiang
The separation of acetylene (C 2 H 2 ) from mixtures with ethylene (C 2 H 4 ) and carbon dioxide (CO 2 ) is crucial yet challenging in the chemical industry. Based on the adsorption separation technology, it is desirable to design and develop efficient adsorbents for C 2 H 2 separation. In this work, we present an adenine-based metal-organic framework (Cu-AD-HEA), which features tailored pore environment with Lewis basic sites within the specific intersecting channels for the separation of C 2 H 2 from mixtures with C 2 H 4 and CO 2 . The obtained Cu-AD-HEA exhibits exceptional adsorption capacity for C 2 H 2 and demonstrates competitive adsorption selectivity for C 2 H 2 /C 2 H 4 and C 2 H 2 /CO 2 . Furthermore, dynamic breakthrough results further illustrate the superior dynamic separation of C 2 H 2 over C 2 H 4 and CO 2 . Moreover, detailed molecular simulations and density functional theory (DFT) calculations elucidate that C 2 H 2 is preferentially captured in a tailored pore environment of Cu-AD-HEA with stronger binding affinity through C H⋯N/O hydrogen bonds and C–H⋯π or π⋯π interactions. This work offers an effective MOF-based adsorbent for the separation of C 2 H 2 from mixtures with C 2 H 4 and CO 2 .
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
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Tong Li,Xiaoxia Jia,Hui Chen,Zeyu Chang,Libo Li,Yong Wang,Jinping Li
Adsorption separation technology using adsorbents is promising as an alternative to the energy-demanding cryogenic distillation of natural gas (CH4/N2) separation. Although a few adsorbents, such as metal–organic frameworks (MOFs), with high performance for CH4/N2 separation, have been reported, it is still challenging to target the desired adsorbents for the actual CH4/N2 separation under humid conditions because the adsorption capacity and selectivity of the adsorbents might be mainly dampened by water vapor. Except for the high CH4 uptake and CH4/N2 selectivity, the adsorption material should simultaneously have excellent stability against moisture and relatively low-water absorption affinity. Here, we tuned the ligands and metal sites of reticular MOFs, Zn-benzene-1,4-dicarboxylic acid–1,4-diazabicyclo[2.2.2]octane (Zn-BDC–DABCO) (DMOF), affording a series of isostructural MOFs (DMOF-N, DMOF-A1, DMOF-A2, and DMOF-A3). Because of the finely engineered pore size and introduced aromatic rings in the functional DMOF, gas sorption results reveal that the materials show improved performance with a benchmark CH4 uptake of 37 cm3/g and a high CH4/N2 adsorption selectivity of 7.2 for DMOF-A2 at 298 K and 1.0 bar. Moisture stability experiments show that DMOF-A2 is a robust MOF with low water vapor capacity even at ∼40% relative humidity (RH) because of the presence of more hydrophobic aromatic rings. Breakthrough experiments verify the excellent CH4/N2 separation performances of DMOF-A2 under high humidity.
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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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2022
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IF 4.889
Linqing Tian,Li Ha,Li Wang,Guangjin Chen,Frederic Coulon,Yuelu Jiang,Xin-Yang Zeng,Ruifeng Zhang,Guozhong Wu
Solidified natural gas technology shows significant potential for storing safely multi-fold volumes of natural gas in clathrate hydrates, but the main concern is the stochastic and slow process of hydrate nucleation making it unstable and unpredictable in practice. To overcome this limitation, methane hydrate was synthesized in a silicon carbide (SiC) ceramic foam packing trays reactor without stirring. Results suggested that the packing trays should be located near the gas-water interface instead of immersed in the aqueous phase, which decreased the induction time by about 98%. Results also highlighted the synergistic effects between the capillary wicking from the porous packings and the water suction from the initially formed hydrate clusters, which pumped water from the aqueous phase into the packings’ pores to provide an unsaturated porous environment for hydrate nucleation. It demonstrated that these two driving forces might also compete for water which became adverse to hydrate formation.
研究领域:
化学工程
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能源存储
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材料科学
✓ 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）