Materials
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2020
·Vol. 13
·期 5
·1126
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IF 3.057
Yongfeng Li,Jiaojiao Su,Guiping Li,Xiufeng Meng
Super-microporous material (pore size 1–2 nm) can bridge the pore size gap between the zeolites (<1 nm) and the mesoporous oxides (>2 nm). A series of super-microporous titania–alumina materials has been successfully prepared via a facile one-pot evaporation-induced self-assembly (EISA) strategy by different solvents using fatty alcohol polyoxyethylene ether (AEO-7) as the template. Moreover, no extra acid or base is added in our synthesis process. When titanium isopropylate is used as the titanium source, these materials exhibit high BET surface areas (from 275 to 396 m2/g) and pore volumes (from 0.14 to 0.18 cm3/g). The sample prepared using methanol as the solvent shows the largest Brunauer–Emmett–Teller (BET) surface area of 396 m2/g. When tetrabutyl titanate is used as the titanium source, these materials exhibit high BET surface areas (from 282 to 396 m2/g) and pore volumes (from 0.13 to 0.18 cm3/g). The sample prepared using ethanol as the solvent shows the largest BET surface area of 396 m2/g.Keywords:super-microporous alumina–titania;different solvents;fatty alcohol polyoxyethylene ether;high BET surface areas
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Kunpeng Liu,Yixuan Yu,Qi Wang,Lingtong Kong,Tianjun Sun
A comprehensive investigation was conducted to explore the adsorption behaviors of CH 4 over N 2 on ultra-microporous Al/Zr-FDCA frameworks, which were synthesized specifically using the eco-friendly and bio-sourced 2,5-furandicarboxylic acid (FDCA). Characterization results revealed that both Al-FDCA and Zr-FDCA exhibited similar specific surface area and surface groups, leading to comparable methane uptake per-unit mass at atmospheric pressure. However, the presence of Zr nodes generated ultra-micropores around 0.43 nm in size, leading to a pronounced affinity for CH 4 . Zr-FDCA demonstrated a higher CH 4 /N 2 selectivity (8.90) calculated from the isotherms compared to Al-FDCA (3.86). Furthermore, breakthrough experiments indicated that under the same dynamic conditions, Zr-FDCA exhibited 1.5 times higher CH 4 uptake per unit volume and 2.5 times higher CH 4 /N 2 selectivity when compared to Al-FDCA. Initially, a four-step VPSA process was simulated to investigate the separation of CH 4 /N 2 mixture, in which the effects of feed-gas flow rate, adsorption time, adsorption pressure, and desorption pressure in VPSA cycle were extensively evaluated to enhance the purity and recovery of methane. Subsequently, a six-step process was employed for further optimization, achieving a purity of 95.9 % and a recovery of 99.1 %. The obtained results demonstrated the reliability of the established model and highlighted the significant potential of Zr-FDCA for CH 4 /N 2 separation.
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
JOURNAL OF CHEMICAL THERMODYNAMICS
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2015
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IF 2.679
Na Kong,Hui-Hui Zhang,Jie Wang,Zhi-Hong Liu
Two pure dehydrated borogermanates with microporous structure, β -K 2 [B 2 Ge 3 O 10 ] and NH 4 [BGe 3 O 8 ], have been synthesized and characterized by XRD, FT-IR, TG techniques. The molar enthalpies of solution of 2.51 mg of GeO 2 (s)/0.99 mg of H 3 BO 3 (s)/1.98 mg of H 3 BO 3 (s) in 2.00 cm 3 of 1 mol · dm −3 NaOH (aq) were measured, respectively. The molar enthalpies of solution of 2.44 mg of K 2 B 4 O 7 · 4H 2 O (s) and 2.18 mg of NH 4 B 5 O 8 · 4H 2 O (s) in the mixture solvent of 2.00 cm 3 of 1 mol · dm −3 NaOH (aq) which contains 2.51 mg of GeO 2 (s) were measured, respectively. The molar enthalpies of solution of 3.82 mg of β -K 2 [B 2 Ge 3 O 10 ] (s) in the mixture solvent of 2.00 cm 3 of 1 mol · dm −3 NaOH (aq) which contains 0.99 mg of H 3 BO 3 (s), and 3.00 mg of NH 4 [BGe 3 O 8 ] (s) in the mixture solvent of 2.00 cm 3 of 1 mol · dm −3 NaOH (aq) which contains 1.98 mg of H 3 BO 3 ) (s) were also measured, respectively. With the use of standard molar enthalpies of formation for NH 4 B 5 O 8 · 4H 2 O (s), K 2 B 4 O 7 · 4H 2 O (s), GeO 2 (s), H 3 BO 3 (s) and H 2 O (l), the standard molar enthalpies of formation of – (3937.1 ± 4.7) kJ · mol −1 for β -K 2 [B 2 Ge 3 O 10 ] and – (2713.7 ± 6.0) kJ · mol −1 for NH 4 [BGe 3 O 8 ] at T = 298.15 K were obtained on the basis of the appropriate thermochemical cycles, respectively.
研究领域:
无机化学
·
物理化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2017
·
IF 3.615
Chang Wang,Jiaqi Liu,Jiangfeng Yang,Jinping Li
Synthesis of ultra-high silica (SiO 2 /Al 2 O 3 > 1800) MFI type zeolite such as silicalite-1 is still considered to be luxury because of the long synthesis time (5–12 days). Here, this material with a highly uniform mesoporous (20 nm) structure was crystallized in a shorter time (20 h) using a crystal-seeds method when an appropriate amount of potassium fluoride was added. Characterization techniques including XRD , SEM, TEM and liquid nitrogen adsorption provided detailed information on the two kinds of porous structure silicalite-1. Due to the “smooth” adsorption surface of silicalite-1 containing few equilibrium ions, it is ideal for the separation of gas mixtures containing non-polar molecules with similar physical properties. Moreover, the CH 4 , N 2 , CO 2 and C 2 H 6 adsorption properties were also investigated. Microporous silicalite-1 has a high adsorption capacity for CH 4 , N 2 , CO 2 and C 2 H 6 and adsorption selectivity for CH 4 /N 2 , CO 2 /N 2 , CO 2 /CH 4 and C 2 H 6 /CH 4 . Although a lower adsorption capacity was observed for mesoporous silicalite-1, the pore size did not affect the outstanding adsorption selectivity, on the contrary, the selectivity of mesoporous silicalite-1 was improved.
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
POLYMER
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2024
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IF 4.1
Dongpeng Li,Zhao Ke,Ke Xu,Tao Li,Dandan Li,Wei Wang,Guangtao Qian,Chunhai Chen
Two novel spiro-bis-benzimidazole-based diamines were synthesized and polymerized with commercial 4,4′-(hexafluoroisopropylidene)diphthalic anhydride dianhydride (6FDA) to produce two types of spiro-bis-benzimidazole-based polyimides (PIM-PBZIs). The resulting polymer membranes, PIM-PBZI-1 and PIM-PBZI-2, exhibited excellent thermal and mechanical properties, including glass transition temperature (T g ) of 417 and 413 °C, 5 % thermal decomposition temperature (T d5% ) above 500 °C, tensile strength of 72 and 74 MPa, and an elongation at break of 6.6 and 5.4 %. Additionally, these PIM-PBZIs were confirmed as novel microporous polymers with BET surface areas of 473–546 m 2 /g and pore sizes ranging from 4 to 9 Å. Furthermore, PIM-PBZI-1, modified with N -phenyl, demonstrated excellent organic solubility and gas separation performance, with CO 2 /CH 4 gas pair permeability selectivity exceeding the 1991 Robeson upper bound, providing an effective pathway for the development of high-performance gas separation membranes.
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
ACS Applied Engineering Materials
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2023
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IF 0
Xue Han,Ruisheng Xue
Hypercross-linked porous polymer materials have good stability and can be used as needed by adjusting the hydrophobic/hydrophilic degree of its functional groups/ions and surface, and they can achieve high gas adsorption. In this study, a series of hypercross-linked porous polymer materials with a rich pore structure and excellent gas adsorption ability were synthesized from polynaphthalene and dimethoxymethane by adjusting the added amount of the catalyst and cross-linker. The sample prepared under the optimized conditions of adding 18 mmol catalyst and 9 mmol cross-linker gained the specific surface area of 786 m2 g–1 and 0.58 nm ultramicropores taking up 80% of total pores. In addition, its CO2 uptake was up to 2.75 mmol g–1 at 273.15 K/1.0 bar. After carbonization at 800 °C, this sample had a 710 m2 g–1 specific surface area and a monodisperse pore structure with a pore diameter of about 0.4 nm, and its CO2 uptake increased to 3.81 mmol g–1 at 273.15 K/1.0 bar. The adsorption selectivity coefficients of CO2/N2 and CO2/CH4 for the carbonized sample were 8.5 and 2.3, respectively, by using Henry’s law initial slope method.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
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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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Chenyang Shu,Chaozhong Guo,Xinru Xu,Lingtao Sun,Yao Liu,Hongdian Chen,Chuanlan Xu,Rong Jin,Yujun Si,Haifeng Chen
Designing micropore-rich carbon materials with large specific surface area (SSA) as a carbon-based oxygen reduction reaction (ORR) electrocatalyst is still frontier but remains challenging in catalysis of zinc-air batteries. Here we propose a new strategy for synthesis of nitrogen atoms co-doped carbon sheets and carbon quantum dots (N-C@CQDs) with an SSA of 1485.3 m 2 g −1 and 98.8 % micro-porosity from α-cellulose via using a complex salt (ZnCl 2 -NH 4 Cl) with low eutectic point (179 °C) as a pore regulator and K 2 FeO 4 as a graphitization catalyst, which can serve as an active and stable carbon-based ORR electrocatalyst. The role of K 2 FeO 4 not only promotes graphitization but also oxidizes the large-sized graphitic carbon particles into a huge amount of uniformly distributed CQDs. This catalyst has exhibited a comparable ORR activity and superior stability to the Pt/C, but a Zn-air battery assembled with the former has delivered a higher peak power density (214 mW cm −2 ) and a larger gravimetric energy density (ED) of (959 Wh k g Z n - 1 ), especially in which it also displays an outstanding catalytic durability with 98.7 % ED retention during a ∼110 h continuous discharge. This work provides a new pathway for design of high-performance carbon-based ORR catalysts in various energy devices.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shuang Guo,Chuanjie Fang,Jiaqi Li,Yongbing Zhuang,Liping Zhu
Polymers of intrinsic microporosity (PIMs) are widely recognized for having great potential in reforming membrane technology for molecular separation within organic solvents, due to their rich and appropriate pore structures with a size < 2 nm. However, the swelling in organic solvents has a significant effect on their pore structures due to the amorphous and linear nature, resulting in the permeability and selectivity performances of developed PIM membranes being far from ideal. In this work, we synthesized an advanced polyimide of intrinsic microporosity by integrating a Tröger’s base (TB) structure with an synergistic structure of aromatic (naphthalenediimide, NDI) and alicyclic (bicyclooctenediimide, BCODI) linking groups. The TB with a rigid and twisted structure was used to furnish a basis for inhibiting chain packing for high overall free volume. The ultra-rigid NDI units maintained such a tailored high free volume and provided superior solvent resistance. The relatively flexible and polar BCODI units promoted local chain mobility to tailor uniform pore size distribution and increased affinity for polar solvents. The innovative design fostered the formation of stable, uniform, and highly solvent-accessible intrinsic micropores. The prepared TFC membrane exhibited good organic solvent separation capabilities, achieving an ethanol permeance of 7.6 L m -2 h −1 bar −1 and a low molecular weight cut-off (MWCO) of approximately 470 Da. This work contributes significantly to the strategic design of PIMs for preparing high-performance membranes for realistic chemical-related separation application scenarios.
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
·
IF 8.1
Hafezeh Nabipour,Yuan Hu,Sohrab Rohani
A novel complex, resulting from the synthesis of a guanazole ligand coordinated with Zn(II), has been successfully synthesized through an environmentally friendly method and carefully characterized using a combination of analytical techniques, including Fourier-transform infrared (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), N 2 adsorption–desorption, scanning electron microscope (SEM), and X-ray photoelectron spectroscopy (XPS). The Brunauer–Emmett–Teller surface (BET) surface area of the guanazole complex is determined to be approximately 407.50 m 2 /g, featuring pore diameters and pore volume of 1.84 nm and 0.187 cm 3 /g, respectively. The emergence of micropores in the guanazole complex significantly enhances its CO 2 adsorption capacity. The maximum CO 2 adsorption capacity of the complex is observed to be 3.18, 2.08, and 1.51 mmol/g at temperatures of 273, 298, and 313 K, respectively. This study presents novel prospects for the controlled synthesis of nitrogen-rich complexes and their potential application in CO 2 capture.
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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产品关联
DOI
高影响因子
Green Chemical Engineering
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2020
·
IF 0
Zhong Gao,Yanan Wang,Hong Wu,Yanxiong Ren,Zheyuan Guo,Xu Liang,Yingzhen Wu,Yutao Liu,Zhongyi Jiang
Membrane separation technology offers a green, efficient and energy-saving approach for biogas upgrading. Membranes with high selectivity and high permeability are the key to achieve high performance. Polymers of Intrinsic Microporosity (PIMs) materials have shown excellent gas permeability but low selectivity which limits their practical application. Herein, a polyphenol, tannic acid, was coated on the PIM-1 membrane surface by a facile dipping method to fabricate composite membranes. Tannic acid containing a large number of polar oxygen-containing groups (quinone, phenolic hydroxyl) self-polymerized on the membrane surface to form a CO 2 -philic, defect-free and thin layer. The CO 2 /CH 4 selectivity of the resultant composite membranes was increased after tannic acid coating while the permeability remained comparable to or even higher than pristine PIM-1 membrane, exceeding the reported 2008 upper bound.
研究领域:
材料科学
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环境工程
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yijun Liu,Yongchao Sun,Fake Sun,Hongjin Li,Jianyu Guan,Lu Bai,Zeyuan Gao,Tianyou Li,Fangxu Fan,Gaohong He,Canghai Ma
Ester-crosslinking has proven to be an effective strategy for enhancing gas selectivity and CO 2 -induced plasticization resistance. However, achieving ester-crosslinked membranes that surpass the 2019 CO 2 /N 2 upper bound remains a significant challenge. To address this, we used polymer of intrinsic microporosity (PIM-1) as a precursor, followed by hydrolysis to prepare PIM-COOH. Subsequently, 1,4-butylene glycol was employed as a crosslinker to react with PIM-COOH, forming M-PIM, which is then thermally crosslinked at different conditions. The ester-crosslinked membrane treated at 250 °C for 8 h demonstrated a CO 2 permeability of 7184 Barrer, with a selectivity of 36.7 for CO 2 /N 2 and 30.4 for CO 2 /CH 4 , both surpassing the 2019 upper bounds. Additionally, the ester-crosslinked membrane demonstrated resistance to CO 2 -induced plasticization even at a test pressure of 35 bar. These results suggest that esterification and crosslinking modification significantly enhance both the gas separation performance and plasticization resistance of PIM-1 membranes. The approach presented in this work provides a promising pathway for designing high-performance membranes that exceed the 2019 CO 2 separation upper bounds and improve resistance to CO 2 plasticization, with potential applications in natural gas purification and CO 2 capture.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子