CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wan-Qi Sun,Jian-Bo Hu,Yun-Jia Jiang,Nuo Xu,Ling-Yao Wang,Jia-Hao Li,Yong-Qi Hu,Simon Duttwyler,Yuan-Bin Zhang
The separation of C 2 H 2 /CO 2 is an important process in industry but challenged by the trade-off of capacity and selectivity owning to their close physical properties and identical kinetic molecular size. Herein, we reported a new metal organic framework ZNU-3 (ZNU = Zhejiang Normal University) with flexibility controlled by abundant hydrogen-bonds for highly selective molecular sieving of C 2 H 2 from CO 2 , CH 4 , C 2 H 4 and C 2 H 6 using commercially available cost-effective ligands. At 1.0 bar and 298 K, the uptake capacity of C 2 H 2 is 81.0 cm 3 (STP) g −1 , while the CO 2 , C 2 H 4 , C 2 H 6 , CH 4 , N 2 uptake capacities are only 5.4, 5.3, 1.0, 1.1, 1.1 cm 3 (STP) g −1 , respectively. Such high uptake ratios of C 2 H 2 over other C2 and C1 gases have rarely been achieved. Particularly, the C 2 H 2 /CO 2 uptake ratio of 14.9 is only secondary to that of the benchmark UTSA-300a and much higher than those of all other porous materials. Dynamic breakthrough experiments with equimolar C 2 H 2 /CO 2 mixtures showed that the retaining time of C 2 H 2 is nearly 2 fold of that of CO 2 , indicating the excellent practical separation performance of ZNU-3 for C 2 H 2 /CO 2 mixtures. Modeling studies indicated that C 2 H 2 is mainly trapped by two opposite carboxylic groups with additional small contribution from π···π packing between pyridine ring and planar C≡C moiety.
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
Shuangqing Shang,Pengxiang Wang,Hanting Xiong,Xing Liu,Junhui Liu,Hua Shuai,Lingmin Wang,Zhenglong Zhu,Zhiwei Zhao,Yong Peng,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Jun Wang
The efficient separation of C 2 H 2 /CO 2 mixtures is critical yet and remains challenging owing to their closely similar physical properties and molecular sizes. Herein, we report a novel flexible microporous adsorbent, Zn-SDBA-bpy (SDBA=4,4′-sulfonyldibenzoic acid, bpy = 4,4′-bipyridine), for molecular sieving of C 2 H 2 from CO 2 . Zn-SDBA-bpy features contracted interlayer cavities with a highly negative electro-environment arising from abundant exposed oxygen atoms of SDBA. Charge transfers between C 2 H 2 and the framework result in strong C 2 H 2 -host interactions that induce a selective gate-opening effect towards C 2 H 2 . Therefore, Zn-SDBA-bpy exhibits substantial C 2 H 2 capture at low pressure (20.7 cm 3 g −1 at 0.1 bar) while excluding CO 2 , demonstrating high C 2 H 2 /CO 2 selectivity (490.2). Notably, Zn-SDBA-bpy features the lowest C 2 H 2 gate-opening threshold ( ca. 0.01 bar) among reported flexible adsorbents for C 2 H 2 /CO 2 separation. Dynamic breakthrough experiments confirm its excellent C 2 H 2 /CO 2 separation yielding high-purity C 2 H 2 (>99.5 %) products. Modeling studies reveal the strong host-C 2 H 2 interactions and underlying mechanisms of molecular sieving within Zn-SDBA-bpy.
研究领域:
化学
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材料科学
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环境科学
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DOI
高影响因子
mSphere
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2024
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IF 3.7
Chen Tang,Haifeng Wang,Xianjiang Jin,Wenwen Li,Yonglin Wang
Verticillium dahliae causes Verticillium wilt in more than 200 plant species worldwide. As a soilborne fungus, it forms melanized microsclerotia and colonizes the xylem of host plants. Our previous study revealed a subfamily of C2H2-homeobox transcription factors in V. dahliae, but their biological roles remain unknown. In this study, we systematically characterized the functions of seven C2H2-homeobox transcription factors in V. dahliae. Deletion of VdChtf3 and VdChtf6 significantly decreased the production of melanized microsclerotia, and knockout of VdChtf1 and VdChtf4 enhanced virulence. Loss of VdChtf2 and VdChtf6 increased conidium production, whereas loss of VdChtf5 and VdChtf7 did not affect growth, conidiation, microsclerotial formation, or virulence. Further research showed that VdChtf3 activated the expression of genes encoding pectic enzymes to participate in microsclerotial formation. In addition, VdChtf4 reduced the expression of VdSOD1 to disturb the scavenging of superoxide radicals but induced the expression of genes related to cell wall synthesis to maintain cell wall integrity. These findings highlight the diverse roles of different members of the C2H2-homeobox gene family in V. dahliae.
研究领域:
真菌学
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植物病理学
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转录调控
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Di-Ming Chen,Xue-Jing Zhang
Acetylene is an important industrial material for the production of acetaldehyde, acetic acid, benzene, synthetic rubber, synthetic fiber, etc., and its separation from the gas mixtures of C 2 H 2 /CO 2 is of great importance but a challenging task due to their similar physical properties and molecular sizes. In this study, taking the advantage of open-donor sites on the pore surface as the nano-traps for C 2 H 2 molecules, a new microporous metal-organic framework (MOF) formulated as {[C o 3 (OH) 2 (HCOO) 2 (CPT) 2 ](NMF) 2 (MeOH) 3 (H 2 O)} n ( 1 , NMF = N - methylformamide) has been prepared by virtue of a bifunctional organic ligand 4-(4H-1,2,4-triazol-4-yl)benzoic acid (HCPT), which showed discriminating sorption performance toward C 2 H 2 (113 cm 3 /g at 298 K and 1 bar) over CO 2 (33 cm 3 /g) under the same conditions. The different sorption behavior of {[C o 3 (OH) 2 (HCOO) 2 (CPT) 2 ]} n between C 2 H 2 and CO 2 results in a high uptake ration (3.4:1) and IAST selectivity (13) at 298 K and 1 bar. Furthermore, the force-field based grand canonical Monte Carlo (GCMC) simulation results demonstrate that the large electronegativity and polarizability of open O donor sites on the pore surface contribute to its high C 2 H 2 /CO 2 separation performance, leading to its more favorable C 2 H 2 uptakes than CO 2 .
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
MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Di-Ming Chen,Han-Dong Qiao,Cong-Li Gao,Shao-Ming Fang
Metal-organic frameworks (MOFs) have emerged as a multi-functional platform for selective gas capture and luminescent detection of harmful pollutants, in which their pore functionality and structural stability are two key factors to be considered for the targeted applications. In this contribution, we present the synthesis and structural evaluation of a new channel-type MOF formulated as {[In 3 (OH) 3 (TATAB) 2 ](DMA) 8 (CH 3 CN) 6 (H 2 O) 2 } n ( 1 , DMA is short for N,N-dimethylacetamide and TATAB is the abbreviation of 4,4′,4″-s-triazine-1,3,5-triyl-p-aminobenzoate) constructed from rod-like [In-(OH)-(COO) 2 ] n chains and the N-rich fluorescent triazine ligand H 3 TATAB. The noninterpenetrated framework of 1 features 1D rhombic channels (13.1 × 14.2 Å 2 ) along the c axis with abundant of free N sites on the pore walls. The solvent-removal framework of 1 ( 1a ) could adsorb large amount of C 2 H 2 (154 cm 3 /g) at 298 K and 1 bar with a moderate C 2 H 2 /CO 2 selectivity (3.7), and its separation performance has been further validated via the break-through experiments. Aqueous-phase sensing experiments demonstrate this MOF exhibits excellent performance of fluorescent detection of 2,4,6-trinitrophenol (TNP) via remarkable fluorescence quenching and obvious blue-shift of maximum emission. In connection to the sensing experiments, we used DFT calculations to reveal the underlying mechanism of such sensing performances via analyzing the energy lever together with electron transfer route.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2019
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IF 4.182
Peng Yan,Jucai Yang,Deyun Ma,Siyun Zhang,Shigong Zeng,Liting Feng,Sihui Zhan,Qiaquan Lin
A water-stable porous cobalt(II)–organic framework functionalized by ethoxyl groups with a chemical formula, {[Co 6 (5-EIA) 5 (tmbpy)(OH) 2 (H 2 O) 2 ]∙4(H 2 O)} n ( 1 ) (5-H 2 EIA = 5-ethoxy-isophthalic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine) has been constructed and studied in terms of structure and performance. 1 shows a 3D framework, and has a 1D channel of 8.1 × 6.0 Å 2 along the a axis. The framework 1 exhibits high humid and thermal stability according to PXRD and TGA results. The C 2 H 2 and CO 2 uptakes of the activated 1 ( 1a ) were up to 2.07 mmol g −1 and 1.89 mmol g −1 at 273 K (100 kPa), respectively. More importantly, 1a shows excellent C 2 H 2 /CH 4 (1:1) and CO 2 /CH 4 (1:1) separations with IAST selectivity of 23.7 and 11.4 at 298 K (100 kPa), respectively. Furthermore, 1a showed good reuse performance, suggesting that 1a could be applied to the separation of C 2 H 2 /CH 4 or CO 2 /CH 4 .
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
INORGANIC CHEMISTRY
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2024
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IF 4.3
Jia-Nuo Li,Ding Chen,Yunli Wang,Jia Li,Yuqiao Chai,Xunwen Xiao,Xing Li,Jin-Peng Xue
Multi-interpenetrated metal–organic frameworks (MOFs) have exhibited excellent performance in selective adsorption due to the variable post-interspersed flexibility, but the design and control remain challenging. Herein, two anthracene-based ligands, 4,4′-(anthracene-9,10-diyl)dibenzoic acid (H2L1) and 9,10-di(pyridin-4-yl)anthracene (L2), are used to construct a new three-dimensional 6-fold interpenetrated MOF [Zn(L1)(L2)]n (NBU-X1), which exhibits multiple C–H···π interactions that enhance the structural rigidity, thereby entangling with a C2H2/C2H4 separation performance. In this material, the incorporation of abundant anthracene rings within the framework not only partitions and restricts the pore window size to a quasi-double pore but also stabilizes it through host–host interactions. The structural stability upon heating or guest displacement/removal has been investigated by single-crystal X-ray diffraction and in situ variable-temperature powder X-ray diffraction, in contrast to the extreme flexibility of most multi-interpenetrated MOFs. The performance of purifying C2H4 from C2H2/C2H4 mixtures has been proved by dynamic breakthrough tests.
研究领域:
材料科学
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化学
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DOI
PubMed
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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DOI
高影响因子
JOURNAL OF RARE EARTHS
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2024
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IF 5.2
Chen Di-Ming,Han-Dong Qiao,Shao-Ming Fang
Introduction of porosity and fluorescent properties into lanthanide metal–organic frameworks (MOFs) with rational design to achieve multifunctional use is of great significance from the energy and environmental viewpoint. In this study, a microporous Tb(III)-based MOF with the formula of {[Tb 2 (oba) 3 (Phen) 2 ](DMF) 2 (H 2 O) 4 } n ( 1 ) was solvothermally prepared via using the mixed ligands of 1,10-phenanthroline (Phen) and 4,4′-oxybis(benzoic acid) (H 2 oba) as organic connecters. The structural evaluation results indicate that complex 1 is composed of binuclear Tb 2 (CO 2 ) 6 (Phen) 2 clusters which are extended by the oba 2− ligands to afford a two-fold interpenetrated framework with one-dimensional microporous channels along the b -axis. Gas sorption studies show that the activated 1 demonstrates a high ideal adsorption solution theory (IAST) sorption selectivity of 7.4 toward C 2 H 2 in a C 2 H 2 /CO 2 gas mixture, which are further supported by the dynamic breakthrough experiments. The grand canonical Monte Carlo (GCMC) simulation results indicate that the synergistic effects of the H-bond interactions of C 2 H 2 with oba 2− ligands and the C–H···π interactions with Phen ligand contribute to the strong binding of the framework toward C 2 H 2 molecules. What's more, the luminescent measurements reveal that the emission of 1 features both the characteristic peaks of Phen ligand and Tb(III) ion, which could be further applied as a self-calibrating sensor for the Cr(VI) detection in water. To the best of our knowledge, complex 1 represents the first example of Tb-MOF holding such a high C 2 H 2 /CO 2 selectivity together with ratiometric Cr(VI) detection performances.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Xionghui Liu,Jianfeng Du,Yu Ye,Yuchuan Liu,Shun Wang,Xianyu Meng,Xiaowei Song,Zhiqiang Liang,Wenfu Yan
Nitrogen-rich porous organic polymers have shown great potentials in gas adsorption/separation, photocatalysis , electrochemistry, sensing and so on. Herein, 1,2,3-triazole functionalized triazine-based porous organic polymers (TT-POPs) have been synthesized by the copper-catalyzed azide-alkyne cycloaddition (Cu-AAC) polymerization reactions of 1,3,5-tris(4-azidophenyl)-triazine with 1,4-diacetylene benzene and 1,3,5-triacetylenebenzene, respectively. The characterizations of N 2 adsorption at 77 K show TT-POPs possess permanent porosity with BET surface areas of 666 m 2 ·g −1 (TT-POP-1) and 406 m 2 ·g −1 (TT-POP-2). The adsorption capacities of TT-POPs for CO 2 , CH 4 , C 2 H 2 and C 2 H 4 , as well as the selective separation abilities of CO 2 /N 2 , CO 2 /CH 4 , C 2 H 2 /CH 4 and C 2 H 4 /CH 4 were evaluated. The gas selective separation ratio of TT-POPs was calculated by the ideal adsorbed solution theory (IAST) method, wherein the selective separation ratios of C 2 H 2 /CH 4 and C 2 H 4 /CH 4 of TT-POP-2 was 48.4 and 13.6 (298 K, 0.1 MPa), which is comparable to other adsorbents (5.6–120.6 for C 2 H 2 /CH 4 , 10–26 for C 2 H 4 /CH 4 ). This work shows that the 1,2,3-triazole functionalized triazine-based porous organic polymer has a good application prospect in natural gas purification.
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 JOURNAL
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2026
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IF 13.2
Bo Xue,Chuanruo Yang,Ruihan Wang,Ting Wang,Pengtao Guo,Gan Li,Dahuan Liu
The development of high-performance porous adsorbents for the efficient recovery of C 2 H 2 from C 2 H 2 /CO 2 mixtures holds significant industrial value. However, the separation of C 2 H 2 /CO 2 remains highly challenging due to their similarities in physicochemical properties. To tackle this key obstacle, we utilize a feasible fluorinated anion modulation strategy to optimize the negative electrostatic microenvironment of ultra-microporous MOFs for the preferential recognition of C 2 H 2 . Notably, compared to SIFSIX-dpds-Cu, TIFSIX-dpds-Cu exhibits higher C 2 H 2 uptake (81.0 cm 3 g −1 ) and C 2 H 2 /CO 2 selectivity (43.2). Furthermore, the C 2 H 2 packing density of TIFSIX-dpds-Cu can reach 522 g L −1 , outperforming most previously reported materials. Density functional theory calculations and in situ FT-IR spectra collaboratively demonstrate that the multiple C−H···F and C−H···C interactions are formed between TIFSIX-dpds-Cu and C 2 H 2 molecules. With the synergistic drive of multiple hydrogen bonds and van der Waals forces within the confined pores, ultimately achieving efficient C 2 H 2 purification. Breakthrough experiments reveal that TIFSIX-dpds-Cu achieves complete separation of C 2 H 2 /CO 2 mixtures, yielding the high-purity C 2 H 2 productivity (≥99.5 %) of 58.42 cm 3 g −1 in a single adsorption−desorption cycle.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Yadan Du,Yang Chen,Yong Wang,Chaohui He,Jiangfeng Yang,Libo Li,Jinping Li
Ethylene and acetylene are both important starting materials for the production of polyethylene , vinyl chloride, but-2-yne-1,4-diol, etc. To remove trace acetylene effectively from ethylene and the separation of acetylene from carbon dioxide are particularly challenging in the petrochemical industry. Although catalytic hydrogenation or cryogenic distillation for the separation of such light hydrocarbons is a very mature operation in the current petrochemical industry, it still requires huge capital and energy consumptions. Herein, a metal-organic framework (MOF), [Ni 2 (BTEC)(bipy) 3 ] (H 4 BTEC = 1,2,4,5-benzene tetracarboxylic acid, bipy = 4,4′-bipyridine), has been developed for efficient adsorptive separation of C 2 H 2 from C 2 H 2 /C 2 H 4 or C 2 H 2 /CO 2 mixtures. Ni 2 (BTEC)(bipy) 3 exhibited extraordinary two-step adsorption for C 2 H 2 with the adsorption capacity of 76.8 cm 3 /g at 298 K and 1 bar, significantly discriminating from C 2 H 4 (7.9 cm 3 /g) and CO 2 (13.0 cm 3 /g) in the same condition. The huge adsorption difference of Ni 2 (BTEC)(bipy) 3 between C 2 H 2 and C 2 H 4 /CO 2 resulted in the record high uptake ratio for C 2 H 2 /C 2 H 4 (9.7), C 2 H 2 /CO 2 (5.9) and very high ideal adsorption solution selectivity (104, 33.5) in robust MOFs at 298 K and 1 atm. The excellent separation performance was verified by breakthrough experiments; this material could effectively separate C 2 H 2 /C 2 H 4 or C 2 H 2 /CO 2 mixtures directly to obtain high purity of C 2 H 4 (>99.999%) and CO 2 (>99.99%) in one separation cycle. Furthermore, this material could be easily scaled up to be synthesized at room temperature under mild conditions, indicating the great potential in actual industrial applications.
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
危险品化学品经营许可证（带存储）