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Back Cover: Ligand Symmetry Modulation for Designing a Mesoporous Metal–Organic Framework: Dual Reactivity to Transition and Lanthanide Metals for Enhanced Functionalization (Chem. Eur. J. 27/2015) 下载免费PDF全文
Prof. Miao Du Xi Wang Dr. Min Chen Dr. Cheng‐Peng Li Jia‐Yue Tian Zhuo‐Wei Wang Prof. Chun‐Sen Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(27):9916-9916
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Dr. Yiyin Mao Danke Chen Pan Hu Dr. Yi Guo Dr. Yulong Ying Dr. Wen Ying Prof. Dr. Xinsheng Peng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(43):15127-15132
Hierarchical porous materials are promising for catalyst, separation and sorption applications. A ligand‐assisted etching process is developed for template‐free synthesis of hierarchical mesoporous MOFs as single crystals and well‐intergrown membranes at 40 °C. At 223 K, the hierarchical porous structures significantly improve the CO2 capture capacity of HKUST‐1 by more than 44 % at pressures up to 20 kPa and 13 % at 100 kPa. Even at 323 K, the enhancement of CO2 uptake is above 25 % at pressures up to 20 kPa and 7 % at 100 kPa. The mesoporous structures not only enhance the CO2 uptake capacity but also improve the diffusion and mass transportation of CO2. Similarly, well‐intergrown mesoporous HKUST‐1 membranes are synthesized, which hold the potential for film‐like porous devices. Mesoporous MOF‐5 crystals are also obtained by a similar ligand‐assisted etching process. This may provide a facile way to prepare hierarchical porous MOF single crystals and membranes for wide‐ranging applications. 相似文献
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Ligand Functionalization in Metal–Organic Frameworks for Enhanced Carbon Dioxide Adsorption 下载免费PDF全文
Ligand functionalization in metal–organic frameworks (MOFs) has been studied extensively and has been demonstrated to enhance gas adsorption and induce interesting gas adsorption phenomena. This account summarizes our recent study of three series of MOFs by ligand functionalization, as well as their carbon dioxide adsorption properties. While ligand functionalization does not change the overall structure of the frameworks, it can influence their gas adsorption behavior. In the first two series, we show how ligand functionalization influences the CO2 affinity and adsorption capacity of MOFs. We also show a special case in which subtle changes in ligand functionality alter the CO2 adsorption profile.
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A Highly Stable Zeotype Mesoporous Zirconium Metal–Organic Framework with Ultralarge Pores 下载免费PDF全文
Dawei Feng Kecheng Wang Dr. Jie Su Dr. Tian‐Fu Liu Jihye Park Dr. Zhangwen Wei Mathieu Bosch Dr. Andrey Yakovenko Prof. Dr. Xiaodong Zou Prof. Dr. Hong‐Cai Zhou 《Angewandte Chemie (International ed. in English)》2015,54(1):149-154
Through topological rationalization, a zeotype mesoporous Zr‐containing metal–organic framework (MOF), namely PCN‐777, has been designed and synthesized. PCN‐777 exhibits the largest cage size of 3.8 nm and the highest pore volume of 2.8 cm3 g?1 among reported Zr‐MOFs. Moreover, PCN‐777 shows excellent stability in aqueous environments, which makes it an ideal candidate as a support to incorporate different functional moieties. Through facile internal surface modification, the interaction between PCN‐777 and different guests can be varied to realize efficient immobilization. 相似文献
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Dr. Chun‐Yi Sun Prof. Xin‐Long Wang Chao Qin Jun‐Ling Jin Zhong‐Min Su Peng Huang Kui‐Zhan Shao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(11):3639-3645
Two anionic metal–organic frameworks (MOFs) with 1D mesoporous tubes ( 1 ) and chiral mesoporous cages ( 2 ) have been rationally constructed by means of a predesigned size‐extended hexatopic ligand, namely, 5,5′,5′′‐(1,3,5‐triazine‐2,4,6‐triyl)tris‐ (azanediyl)triisophthalate (TATAT). Charge neutrality is achieved by protonated dimethylamine cations. Notably, the two MOFs can be used to separate large molecules based on ionic selectivity rather than the size‐exclusion effect so far reported in the literature. Owing to the imino triazine backbone and carboxyl groups of the hexatopic ligand, which provide important host–guest interactions, rare solvatochromic phenomena of 1 and 2 are observed on incorporating acetone and ethanol guests. Furthermore, guest‐dependent luminescence properties of compound 2 were investigated, and the results show that luminescence intensity is significantly enhanced in toluene and benzene, while quenching effects are observed in acetone and ethanol. Thus, compound 2 may be a potential material for luminescent probes. 相似文献
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Adsorption on Mesoporous Metal–Organic Frameworks in Solution: Aromatic and Heterocyclic Compounds 下载免费PDF全文
Dr. Alexander Samokhvalov 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(47):16726-16742
Adsorption and desorption play major roles in separations, purification of water, waste streams, liquid fuels, catalysis, biomedicine and chromatography. Mesoporous metal–organic frameworks (MOFs) with pore sizes 2–50 nm are particularly suitable for adsorption of organic compounds in solution. Tens of thousands of aromatic and heterocyclic compounds are major components of liquid fuels, feedstock for industrial synthesis, solvents, dyestuffs, agricultural chemicals, medicinal drugs, food additives, and so forth. This Review provides a systematization and analysis of studies on adsorption/desorption on mesoporous MOFs in solution and their underlying chemical mechanisms. The (in)stability of mesoporous MOFs in water is critically discussed. Adsorption capacity and selectivity are covered for organic dyes, medicinal drugs, major components of liquid fuels, and miscellaneous industrial chemicals. Ionic interactions, Brønsted acid–base interactions, hydrogen bonding, coordination bonding, π–π interactions, and non‐specific interactions are covered amongst adsorption mechanisms. The effects of post‐synthetic modifications of mesoporous MOFs on their stability, adsorption capacity, selectivity, and mechanisms of adsorption and desorption are analyzed. To encourage research in this quickly growing field, we identify “niches” for which no application‐oriented and/or mechanistic studies were reported. Perspectives and limitations of a wide use of mesoporous MOFs as industrial sorbents are discussed. 相似文献
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A Microporous Anionic Metal–Organic Framework for Sensing Luminescence of Lanthanide(III) Ions and Selective Absorption of Dyes by Ionic Exchange 下载免费PDF全文
Dr. Jun‐Sheng Qin Dr. Shu‐Ran Zhang Dr. Dong‐Ying Du Ping Shen Shao‐Juan Bao Prof. Ya‐Qian Lan Prof. Zhong‐Min Su 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(19):5625-5630
Herein, a novel anionic framework with primitive centered cubic (pcu) topology, [(CH3)2NH2]4[(Zn4dttz6)Zn3]?15 DMF?4.5 H2O, ( IFMC‐2 ; H3dttz=4,5‐di(1H‐tetrazol‐5‐yl)‐2H‐1,2,3‐triazole) was solvothermally isolated. A new example of a tetranuclear zinc cluster {Zn4dttz6} served as a secondary building unit in IFMC‐2 . Furthermore, the metal cluster was connected by ZnII ions to give rise to a 3D open microporous structure. The lanthanide(III)‐loaded metal–organic framework (MOF) materials Ln3+@IFMC‐2 , were successfully prepared by using ion‐exchange experiments owing to the anionic framework of IFMC‐2 . Moreover, the emission spectra of the as‐prepared Ln3+@IFMC‐2 were investigated, and the results suggested that IFMC‐2 could be utilized as a potential luminescent probe toward different Ln3+ ions. Additionally, the absorption ability of IFMC‐2 toward ionic dyes was also performed. Cationic dyes can be absorbed, but not neutral and anionic dyes, thus indicating that IFMC‐2 exhibits selective absorption toward cationic dyes. Furthermore, the cationic dyes can be gradually released in the presence of NaCl. 相似文献
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Dr. Hui Liu Dr. Yonggang Zhao Zhijuan Zhang Nour Nijem Prof. Dr. Yves J. Chabal Prof. Dr. Xiangfang Peng Prof. Dr. Heping Zeng Prof. Dr. Jing Li 《化学:亚洲杂志》2013,8(4):778-785
We report two new 3D structures, [Zn3(bpdc)3(2,2′‐dmbpy)] (DMF)x(H2O)y ( 1 ) and [Zn3(bpdc)3(3,3′‐dmbpy)]?(DMF)4(H2O)0.5 ( 2 ), by methyl functionalization of the pillar ligand in [Zn3(bpdc)3(bpy)] (DMF)4?(H2O) ( 3 ) (bpdc=biphenyl‐4,4′‐dicarboxylic acid; z,z′‐dmbpy=z,z′‐dimethyl‐4,4′‐bipyridine; bpy=4,4′‐bipyridine). Single‐crystal X‐ray diffraction analysis indicates that 2 is isostructural to 3 , and the power X‐ray diffraction (PXRD) study shows a very similar framework of 1 to 2 and 3 . Both 1 and 2 are 3D porous structures made of Zn3(COO)6 secondary building units (SBUs) and 2,2′‐ or 3,3′‐dmbpy as pillar ligand. Thermogravimetric analysis (TGA) and PXRD studies reveal high thermal and water stability for both compounds. Gas‐adsorption studies show that the reduction of surface area and pore volume by introducing a methyl group to the bpy ligand leads to a decrease in H2 uptake for both compounds. However, CO2 adsorption experiments with 1′ (guest‐free 1 ) indicate significant enhancement in CO2 uptake, whereas for 2′ (guest‐free 2 ) the adsorbed amount is decreased. These results suggest that there are two opposing and competitive effects brought on by methyl functionalization: the enhancement due to increased isosteric heats of CO2 adsorption (Qst), and the detraction due to the reduction of surface area and pore volume. For 1′ , the enhancement effect dominates, which leads to a significantly higher uptake of CO2 than its parent compound 3′ (guest‐free 3 ). For 2′ , the detraction effect predominates, thereby resulting in reduced CO2 uptake relative to its parent structure 3′ . IR and Raman spectroscopic studies also present evidence for strong interaction between CO2 and methyl‐functionalized π moieties. Furthermore, all compounds exhibit high separation capability for CO2 over other small gases including CH4, CO, N2, and O2. 相似文献
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Jie Lu Ju‐Kang Wu Yao Jiang Peng Tan Lin Zhang Yu Lei Xiao‐Qin Liu Lin‐Bing Sun 《Angewandte Chemie (International ed. in English)》2020,59(16):6428-6434
Hierarchically porous metal–organic frameworks (HP‐MOFs) are promising in various applications. Most reported HP‐MOFs are prepared based on the generation of mesopores in microporous frameworks, and the formed mesopores are connected by microporous channels, limiting the accessibility of mesopores for bulky molecules. A hierarchical structure is formed by constructing microporous MOFs in uninterrupted mesoporous tunnels. Using the confined space in as‐prepared mesoporous silica, highly dispersed metal precursors for MOFs are coated on the internal surface of mesoporous tunnels. Ligand vapor‐induced crystallization is employed to enable quantitative formation of MOFs in situ, in which sublimated ligands diffuse into mesoporous tunnels and react with metal precursors. The obtained hierarchically porous composites exhibit record‐high adsorption capacity for the bulky molecule trypsin. The thermal and storage stability of trypsin is improved upon immobilization on the composites. 相似文献
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Jun Liang Alexander Nuhnen Simon Millan Hergen Breitzke Vasily Gvilava Gerd Buntkowsky Christoph Janiak 《Angewandte Chemie (International ed. in English)》2020,59(15):6068-6073
We present a facile approach to encapsulate functional porous organic cages (POCs) into a robust MOF by an incipient‐wetness impregnation method. Porous cucurbit[6]uril (CB6) cages with high CO2 affinity were successfully encapsulated into the nanospace of Cr‐based MIL‐101 while retaining the crystal framework, morphology, and high stability of MIL‐101. The encapsulated CB6 amount is controllable. Importantly, as the CB6 molecule with intrinsic micropores is smaller than the inner mesopores of MIL‐101, more affinity sites for CO2 are created in the resulting CB6@MIL‐101 composites, leading to enhanced CO2 uptake capacity and CO2/N2, CO2/CH4 separation performance at low pressures. This POC@MOF encapsulation strategy provides a facile route to introduce functional POCs into stable MOFs for various potential applications. 相似文献
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Flexible and Hierarchical Metal–Organic Framework Composites for High‐Performance Catalysis 下载免费PDF全文
Dr. Ning Huang Hannah Drake Jialuo Li Dr. Jiandong Pang Dr. Ying Wang Shuai Yuan Qi Wang Peiyu Cai Dr. Junsheng Qin Prof. Dr. Hong‐Cai Zhou 《Angewandte Chemie (International ed. in English)》2018,57(29):8916-8920
The development of porous composite materials is of great significance for their potentially improved performance over those of individual components and extensive applications in separation, energy storage, and heterogeneous catalysis. Now mesoporous metal–organic frameworks (MOFs) with macroporous melamine foam (MF) have been integrated using a one‐pot process, generating a series of MOF/MF composite materials with preserved crystallinity, hierarchical porosity, and increased stability over that of melamine foam. The MOF nanocrystals were threaded by the melamine foam networks, resembling a ball‐and‐stick model overall. The resulting MOF/MF composite materials were employed as an effective heterogeneous catalyst for the epoxidation of cholesteryl esters. Combining the advantages of interpenetrative mesoporous and macroporous structures, the MOF/melamine foam composite has higher dispersibility and more accessibility of catalytic sites, exhibiting excellent catalytic performance. 相似文献
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Young Eun Cheon Myunghyun Paik Suh Prof. 《Angewandte Chemie (International ed. in English)》2009,48(16):2899-2903
Quick on the uptake : Palladium nanoparticles were fabricated simply by immersing {[Zn3(ntb)2(EtOH)2]?4 EtOH}n ( 1 ) in an MeCN solution of Pd(NO3)2 at room temperature, without any extra reducing agent. 3 wt % PdNPs@[ 1 ]0.54+(NO3?)0.54 significantly increase H2 uptake capacities, both at 77 K and 1 bar and at 298 K and high pressures (see picture, red curve) compared to [Zn3(ntb)2]n (black). ntb=4,4′,4′′‐nitrilotrisbenzoate.
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Assembly of Mesoporous Metal–Organic Framework Templated by an Ionic Liquid/Ethylene Glycol Interface 下载免费PDF全文
Xinxin Sang Prof. Jianling Zhang Li Peng Chengcheng Liu Xue Ma Prof. Buxing Han Guanying Yang 《Chemphyschem》2015,16(11):2317-2321
We propose a facile room‐temperature synthesis of a metal–organic framework (MOF) with a bimodal mesoporous structure (3.9 and 17‐28 nm) in an ionic liquid (IL)/ethylene glycol (EG) mixture. The X‐ray diffraction analysis reveals that MOF formation can be efficiently promoted by the presence of the EG/IL interface at room temperature. The MOFs with mesoporous networks are characterized by SEM and TEM. The formation mechanism of the mesoporous MOF in EG/IL mixture is investigated. It is proposed that the EG nanodroplets in the IL work as templates for the formation of the large mesopores. The as‐synthesized mesoporous metal–organic framework is an effective and reusable heterogeneous catalyst to catalyze the aerobic oxidation of benzylic alcohols. 相似文献