CRYSTENGCOMM
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2019
·Vol. 22
·期 2
·275-282
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IF 3.382
Peng Yan,Jucai Yang,Xiangying Hao,Zhisheng Chen,Guanhua Shen,Yanhua Zhao,Deyun Ma,Jiaxin Zhu
A new Zn-based metal–organic framework with 8-connected hex topology constructed from bipyridine and carboxylate ligands, namely [Zn(cpna)3(tmbpy)]n·4DMF (1) (H2cpna = 6-(4-carboxyphenyl)nicotinic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine), has been synthesized under solvothermal conditions. The Zn-MOF was structurally characterized and retained a good crystal structure after activation (1a), an indication of permanent porosity. 1a exhibits a BET surface of 770 m2 g−1 and the maximum aperture of 8.60 Å. Single component adsorption isotherm measurements of C2H2, CO2, CH4, CO and N2 on 1a were performed both at 273 K and 298 K, and the selectivities for C2H2/CH4, C2H2/CO2, CO2/CO, CO2/CH4 and CO2/N2 were estimated on the basis of the ideal adsorbed solution theory (IAST). 1a shows the uptake of C2H2 (3.89 mmol g−1) and CO2 (3.52 mmol g−1) at 273 K and 100 kPa, respectively. Due to the Lewis basic pyridyl sites inside the channel of the framework, 1a showed good adsorption selectivities for C2H2/CH4(50 : 50) and C2H2/CO2(50 : 50) at 298 K (100 kPa).
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
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2024
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IF 2.2
Mohan Chen,Yichao Wang,Ziwen Fan,Yue Wang,Zheng Niu,Jianping Lang
Graphical We prepared a series of fluorinated MOFs through the post- synthesis modification of the classic Zr-based MOF-808. The fluorinated alkane pores within MOFs can enhance the forces between the framework and C 2 H 2 , therefore, the difference in the adsorption capacity to C 2 H 2 and C 2 H 4 making it possible to effectively separate the C 2 H 2 /C 2 H 4 mixture at room temperature. The separation of ethylene (C 2 H 4 ) and acetylene (C 2 H 2 ) is challenging due to their similar molecular dimensions and boiling points, making conventional methods like cryogenic distillation and solvent extraction inefficient and environmentally harmful. Fluorinated metal-organic frameworks (MOFs) have been proven to be an effective material for the separation of C 2 H 4 and C 2 H 2. However, their direct synthesis is relatively expensive and challenging. In this study, we report a facile post-synthetic modification strategy to introduce fluorinated alkane pores into a zirconium-based MOF, MOF-808. The construction of fluorine-containing pores within the MOFs prefers adsorption for C 2 H 2 attributed to the interaction between the fluorine atoms and C 2 H 2 . This series of fluorinated MOFs demonstrates potential for gas separation processes, with the highest separation ratio reaching 2.67 (1 : 99) at 298 K. Breakthrough experiments for C 2 H 2 /C 2 H 4 mixtures confirmed that fluorinated MOF is capable of separating C 2 H 2 /C 2 H 4 , making it a potential candidate for industrial application. Moreover, the simplicity of the post-synthetic modification method suggests a viable strategy for the synthesis of fluorinated MOFs.
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
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
·
IF 5.4
Qifan Yang,Haodong Xie,Xiang Ni,Li Liu,Yuan Xue,Yan Liu,Lei Wang,Hongjun Zhu
Adsorptive separation of C 2 H 2 from C 2 H 4 , which could deal with multi-steps for their similar kinetic diameter and physical properties, still poses a significant challenge. In this work, we prepared two metal cations (Co 2+ , Zn 2+ )-exchanged aluminosilicate FAU zeolites as an inorganic porous matrix, and grafted an organic zeolitic imidazole framework crystal layer to construct the inorganic–organic composites for gas separation process of C 2 H 4 among the mixed gas components. Such inorganic–organic porous composites can adsorb C 2 H 2 and hinder the large-sized C 2 H 4 . The Co-FAU@ZIF-8 composite was verified through breakthrough experiments and demonstrated a promising adsorptive volume of 1.46 mmol g −1 with an IAST selectivity of C 2 H 2 /C 2 H 4 of 5.6 at 298 K, respectively. Via powder X-ray diffraction crystallography and combined spectroscopy, we found that the exchanged metallic cation located at the accessible s 6 r , and served as the anchor point for the epitaxy of different crystals. Such tunable features ( i.e. , metallic centers and pore diameter) provide a potential pathway for the sub-sequential development of highly efficient adsorptive materials.
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
Analysis & Sensing
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2024
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IF 3.4
Yifeng Xu,Haixia Mei,Yu Bing,Fuyun Zhang,Ning Sui,Tingting Zhou,Xiaopeng Fan,Lijie Wang,Tong Zhang
Graphical In this article, a Sm−Pd bimetal doped SnO 2 -based MEMS C 2 H 2 sensor was prepared for detecting dissolved acetylene gas in transformer oil. It has the unique advantages of high sensitivity, high selectivity and low power consumption. Acetylene (C 2 H 2 ), as an important characteristic gas in transformer fault diagnosis, should be accurately detected and effectively distinguished from other dissolved gases (H 2 , CH 4 , C 2 H 6 , C 2 H 4 , CO, CO 2 ), which is crucial to determine whether the fault occurs and the fault type, but also faces challenges now. The rational design and employment of rare earth and noble metals are expected to address this issue. In this work, SnO 2 -3 at% Sm 2 O 3 -1 at% PdO based MEMS gas sensor was prepared to achieve high performance detection of C 2 H 2 which has a response value of 56 to 50 ppm C 2 H 2 , response/recovery time of 2 s/136 s, lower detection limit of 1 ppm, power consumption of 15.5 mW, and weak cross sensitivity to other transformer fault characteristic gases. Lewis acids and bases theory was used to explain the reason why rare earth Sm is a benefit element to improve selectivity to C 2 H 2 . The formation of oxygen vacancies and hetero junctions was used to explain the increased sensitivity of the material. This study proved the feasibility of rare earth and noble metals as potential additives to enable advanced gas-sensitive materials for highly selective transformer fault characteristic gas C 2 H 2 detection.
研究领域:
材料科学
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传感器技术
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电力设备监测
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Haiying Xu,Zhaoliang Wang,Hehua Liao,Dongmiao Li,Jinni Shen,Jinlin Long,Wenxin Dai,Xuxu Wang,Zizhong Zhang
Photocatalytic converting CO 2 into C 2 products is highly desirable but is extremely sensitive to catalyst structure. In this work, Ti-H species and oxygen vacancies are simultaneously integrated on hydrogenated SrTiO 3 surface by thermally treating with NaBH 4 , which promotes the activation of CO 2 into HCOO - and CO* intermediates. The proximity of oxygen vacancies and Ti-H species contributes to the C-C coupling of intermediates into acetylene (C 2 H 2 ) products. To the best of our knowledge, this is the first example for the photocatalytic CO 2 reduction into C 2 H 2 main products. The optimal hydrogenated SrTiO 3 has the C 2 H 2 yield of 39.0 μmol·g −1 with a 76.0 % selectivity among C 2 products. Therefore, this work provides an approach of designing the adjacent active sites for photocatalytic CO 2 conversion into C 2+ products.
研究领域:
材料科学
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环境科学
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Di-Ming Chen,Han-Dong Qiao,Pei-Feng Wang,Zi-Jun Zhao,Shao-Ming Fang
In this study, a porous Ni-MOF formulated as {(H 2 NMe 2 )[Ni 3 (μ 3 OH)(TPT)(TZB) 3 ](H 2 O) 6 (DMA) 7 } n (TZB = 4-(1H-tetrazol-5-yl)benzoate, TPT = 2,4,6-tri(4-pyridyl)-1,3,5-triazine, and DMA = N,N-dimethylacetamide) was prepared and its C 2 H 2 and CO 2 adsorption performances were systemically studied both experimentally and computationally. The structural analysis by single crystal X-ray diffraction studies reveals that the prepared Ni-MOF crystallizes in the space group P6 3 mc and features a porous pacs -type network composed of trigonal bipyramidal and octahedral cages. The activated Ni-MOF (Ni-MOF-a) shows a high C 2 H 2 uptake capacity of 157 cm 3 /g with a moderate C 2 H 2 /CO 2 IAST selectivity of 3.3 at 298 K and 1 bar. More importantly, Ni-MOF-a shows a low adsorption heat for C 2 H 2 ranging from 24.6 to 27.1 kJ/mol at 298 K with a high separation potential of 2.85 mol/kg. In the computational simulation section, six sets of point charge derived from different approaches (Qeq, Mulliken, PACMOF, mCBAC, Mepoml, PACMAN) and two different force-fields (UFF and Dreiding) were used to calculate the C 2 H 2 and CO 2 adsorption isotherms and then compared with the experimental values. Our results reveal that great care should be taken in the selection of point charges and force fields, and the unsuitable combinations might result in an inappropriate C 2 H 2 /CO 2 selectivity which is against the experimental results.
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
CHEMISTRY OF MATERIALS
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2025
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IF 7
Beibei Sun,Cheng Zeng,Suyun Deng,Yuewen Gu,Lei Gan,Huajun Yang
The separation of C2H2/CO2 under highly humid conditions by using metal–organic frameworks (MOFs) is extremely challenging because water vapor would reduce the C2H2 adsorption capacity or even degrade the structure of MOFs. In this work, a zirconium zeolitic metal–organic framework (NNM-5) with a small aperture and large cavities exhibits commendable C2H2/CO2 selectivity (16.6 at 298 K and 1 bar) and a high uptake ratio (3.13 at 298 K and 1 bar). More importantly, NNM-5 could maintain at least five breakthrough cycles under highly humid conditions (around 100% RH) without performance degradation compared to that under dry conditions. Our studies indicate that the kinetic mechanism is the key to excellent separation performance under highly humid conditions based on the fact that the material is hydrophilic with a high water uptake, but the diffusion rate of H2O is 2 orders slower than that of C2H2 and CO2 in NNM-5.
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
AICHE JOURNAL
·
2015
·Vol. 61
·期 6
·2016-2027
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IF 2.748
Xu Zhao,Qiwei Yang,Dan Xu,Zongbi Bao,Yi Zhang,Baogen Su,Qilong Ren,Huabin Xing
Ionic liquids (ILs) have been proposed as promising solvents for separating C 2 H 2 and C 2 H 4 , but screening an industrially attractive IL with high capacity from numerous available ILs remains challenging. In this work, a rapid screening method based on COSMO-RS was developed. We also present an efficient strategy to improve the C 2 H 2 capacity in ILs together with adequate C 2 H 2 /C 2 H 4 selectivity with the aid of COSMO-RS. The essence of this strategy is to increase molecular free volume of ILs and simultaneously enhance hydrogen-bond basicity of anions by introducing flexible and highly asymmetric structures, which is validated by a new class of tetraalkylphosphonium ILs featuring long-chain carboxylate anions. At 298.1 K and 1 bar, the solubility of C 2 H 2 in ILs reaches 0.476 mol/mol IL, very high for a physical absorption, with a selectivity of up to 21.4. The separation performance of tetraalkylphosphonium ILs to the mixture of C 2 H 2 /C 2 H 4 was also evaluated. © 2015 American Institute of Chemical Engineers AIChE J , 61: 2016–2027, 2015
研究领域:
化学工程
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材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jialang Hu,Yan Zhang,Mingyuan Jiang,Chao Xiong,Shenwei Chen,Jin Li,Xu Li,Ziyuan Zhu,Peng Hu,Hongbing Ji
Effective separation of acetylene/ethylene (C 2 H 2 /C 2 H 4 ) mixtures by adsorption is a challenging but green method given their similar molecular characters. An increasing number of metal-organic frameworks (MOFs) have addressed the diffusion-related challenges to achieve the separation, yet almost all of them just focus on diffusion rates and disregard the geometrical arrangement of adsorbed molecules which exerts important effects in boosting the diffusion behaviors. Herein, we now present a paradigm using an ultramicroporous zinc-MOF (Zn-MOF, referred to as 1 ) with assessable size of 3.4 × 3.3 Å 2 , as demonstrated by single-crystal and theoretical analysis, which realizes the effective separation of C 2 H 2 from its competitors. Static adsorption isotherms indicate that 1 possesses higher C 2 H 2 uptake of 28.4 cm 3 g −1 at 298 K and 0.1 bar, achieving a high IAST selectivity of 265 among the benchmark MOFs. Theoretical calculations reveal that C 2 H 2 molecules are grasped through multiple binding interactions and adsorbed in the pore surface rather than the center of the pore, thus forming C 2 H 2 tetramer through connecting four C 2 H 2 motifs. Further, time-dependent kinetic tests coupled with molecular dynamics confirm the faster diffusion behavior for C 2 H 2 , mainly attributing to unimpeded diffusion channel. Column breakthrough tests demonstrate that 1 can easily accomplish exclusive separation of C 2 H 2 from various binary ethane dehydrogenation (EDH) and senary non-oxidative coupling of methane (non-OCM) byproducts. Specially, structurally stable 1 can be readily synthesized utilizing inexpensive raw materials, yielding the cost of only $614 per kilogram. Accordingly, this work proposes a novel strategy of wall-trapped C 2 H 2 tetramer in MOF that can effectively promote the kinetic behavior through available diffusion channel, expecting to offer a new perspective and provide guidance for future research.
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 SOLID STATE CHEMISTRY
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2021
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IF 3.498
Di-Ming Chen,Yin-Ping Zheng,Shao-Ming Fang
The selective separation of C 2 H 2 from C 2 H 4 is a very important process for downstream industrial production, and porous metal-organic frameworks (MOFs) have shown great potential for such an application due to their tunable pore surroundings and adjustable building blocks. In this study, a new microporous MOF formulated as {(Et 2 NH 2 )[In(TBOT)(2,3-FDA)](DEF)(H 2 O) 2 } n ( 1 , H 3 TBOT = 4,4′,4’’-(((2,4,6-trimethylbenzene-1,3,5-triyl)tris(oxy))tris(methylene))tribenzoic acid, 2,3-HFDA = 2,3-difluorobenzoic acid and DEF = N , N -diethylformamide) with 2-fold interpenetrated network and 1D fluorine-decorated pores has been prepared via using an acid-acid mixed-ligand strategy. The activated complex 1 (named as 1a ) demonstrates apparently higher C 2 H 2 uptake than C 2 H 4 around room temperature , resulting in its relative high C 2 H 2 /C 2 H 4 (v:v = 1:99) IAST (Ideal Adsorbed Solution Theory) selectivity of 10.3 at 298 K and 1 bar. Furthermore, the GCMC (grand canonical Monte Carlo) simulation results indicate that the 2,3-FDA moieties serve as preferential binding sites for C 2 H 2 via the multipoint F 2 ⋯H–C C–H⋯F 2 interactions, implying the feasibility of the mixed-ligand approach for building porous MOFs with the targeted applications.
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
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 38
·9045-9051
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IF 5.16
Lingchang Jiang,Pengyuan Wang,Meiping Li,Panpan Zhang,Jialu Li,Jia Liu,Yanhang Ma,Hao Ren,Guangshan Zhu
Graphical Lapping it up : A thermally and chemically stable, crystalline polyimide porous organic framework, was constructed by imidization of linear naphthalene-1,4,5,8-tetracarboxylic dianhydride with triangular 1,3,5-tris(4-aminophenyl)benzene. This material is capable of selective adsorption of C 2 H 2 over C 2 H 4 and CO 2 over N 2 (see figure). Utilization of porous materials for gas capture and separation is a hot research topic. Removal of acetylene (C 2 H 2 ) from ethylene (C 2 H 4 ) is important in the oil refining and petrochemical industries, since C 2 H 2 impurities deactivate the catalysts and terminate the polymerization of C 2 H 4 . Carbon dioxide (CO 2 ) emission from power plants contributes to global climate change and threatens the survival of life on this planet. Herein, 2D crystalline polyimide porous organic framework PAF-120, which was constructed by imidization of linear naphthalene-1,4,5,8-tetracarboxylic dianhydride and triangular 1,3,5-tris(4-aminophenyl)benzene, showed significant thermal and chemical stability. Low-pressure gas adsorption isotherms revealed that PAF-120 exhibits good selective adsorption of C 2 H 2 over C 2 H 4 and CO 2 over N 2 . At 298 K and 1 bar, its C 2 H 2 and CO 2 selectivities were predicted to be 4.1 and 68.7, respectively. More importantly, PAF-120 exhibits the highest selectivity for C 2 H 2 /C 2 H 4 separation among porous organic frameworks. Thus PAF-120 could be a suitable candidate for selective separation of C 2 H 2 over C 2 H 4 and CO 2 over N 2 .
研究领域:
材料科学
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化学工程
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Hua Shuai,Junhui Liu,Yesong Teng,Xing Liu,Lingmin Wang,Hanting Xiong,Pengxiang Wang,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Shuguang Deng,Jun Wang
Energy-efficient adsorptive separation shows great potential for the one-step production of high-purity ethylene (C 2 H 4 ) from ternary C 2 hydrocarbons. However, it remains a formidable challenge to fabricate high-performance adsorbents that exhibit simultaneous high selectivity (>2) towards acetylene/ethylene (C 2 H 2 /C 2 H 4 ) and ethane/ethylene (C 2 H 6 /C 2 H 4 ). Herein, we report a pillar-layered metal–organic framework, Ni(sdba)(dabco) 0.5 (H 2 sdba = 4,4′-sulfonyldibenzoic acid; dabco = 1,4-diazabicyclo [2.2.2] octane), for preferential trapping of C 2 H 6 and C 2 H 2 over C 2 H 4 . The abundant accessible binding sites endow Ni(sdba)(dabco) 0.5 with outstanding C 2 H 2 /C 2 H 4 (2.28) and C 2 H 6 /C 2 H 4 (2.47) selectivity with high C 2 H 6 (3.15 mmol g −1 ) and C 2 H 2 (4.41 mmol g −1 ) uptake among porous materials reported for one-step C 2 H 4 purification. Dynamic breakthrough experiments demonstrated the feasibility of producing high-purity C 2 H 4 (>99.9%) from C 2 H 2 /C 2 H 6 /C 2 H 4 gas-mixtures (1/1/1 and 1/9/90, v/v/v ) in a single step. Computational simulations reveal that the aromatic-rich pore spaces, which decorated with accessible interlayer uncoordinated oxygen atoms of sulfonyl groups and alkyl functionalities, can provide multiple C-H···O, C-H···π, and C-H···H interactions for selectively recognizing C 2 H 6 and C 2 H 2 over C 2 H 4 .
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
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