共查询到20条相似文献,搜索用时 15 毫秒
1.
Jian Zhang Dr. Tao Wu Cong Zhou Shumei Chen Dr. Pingyun Feng Prof. Dr. Xianhui Bu Prof. Dr. 《Angewandte Chemie (International ed. in English)》2009,48(14):2542-2545
B‐hive? A family of crystalline materials analogous to porous AlPO4 but based on boron imidazolate frameworks (BIFs) can be formed by the crosslinking of various presynthesized boron imidazolates with monovalent cations (Li+ and Cu+, see picture). This synthetic method is capable of generating a large variety of open frameworks, ranging from the four‐connected zeolitic sodalite type to the three‐connected chiral (10,3)‐a type.
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Cristina Mottillo Prof. Tomislav Friščić 《Angewandte Chemie (International ed. in English)》2014,53(29):7471-7474
Zeolitic imidazolate frameworks of zinc, cobalt, and cadmium, including the framework ZIF‐8 commercially sold as Basolite Z1200, exhibit surprising sensitivity to carbon dioxide under mild conditions. The frameworks chemically react with CO2 in the presence of moisture or liquid water to form carbonates. This effect, which has been previously not reported in metal–organic framework chemistry, provides an explanation for conflicting reports on ZIF‐8 stability to water and is of outstanding significance for evaluating the potential applications of metal–organic frameworks, especially for CO2 sequestration. 相似文献
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Controllable Encapsulation of “Clean” Metal Clusters within MOFs through Kinetic Modulation: Towards Advanced Heterogeneous Nanocatalysts 下载免费PDF全文
Dr. Hongli Liu Lina Chang Cuihua Bai Liyu Chen Prof. Rafael Luque Prof. Yingwei Li 《Angewandte Chemie (International ed. in English)》2016,55(16):5019-5023
Surfactant‐free tiny Pt clusters were successfully encapsulated within MOFs with controllable size and spatial distribution by a novel kinetically modulated one‐step strategy. Our synthesis relies on the rational manipulation of the reduction rate of Pt ions and/or the growth rate of MOFs by using H2 as assistant reducing agent and/or acetic acid as MOF‐formation modulator. The as‐prepared Pt@MOF core–shell composites exhibited exceedingly high activity and excellent selectivity in the oxidation of alcohols as a result of the ultrafine “clean” Pt clusters, as well as interesting molecular‐sieving effects derived from the outer platinum‐free MOF shell. 相似文献
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Qing Zhang Zhengming Wu Yuan Lv Yali Li Yajing Zhao Rui Zhang Yushuang Xiao Xiaofei Shi Danrui Zhang Rui Hua Jianlin Yao Jun Guo Rong Huang Yi Cui Zhenhui Kang Subhadip Goswami Lee Robison Kepeng Song Xinghua Li Yu Han Lifeng Chi Omar K. Farha Guang Lu 《Angewandte Chemie (International ed. in English)》2019,58(4):1123-1128
Processing metal–organic frameworks (MOFs) as films with controllable thickness on a substrate is increasingly crucial for many applications to realize function integration and performance optimization. Herein, we report a facile cathodic deposition process that enables the large‐area preparation of uniform films of zeolitic imidazolate frameworks (ZIF‐8, ZIF‐71, and ZIF‐67) with highly tunable thickness ranging from approximately 24 nm to hundreds of nanometers. Importantly, this oxygen‐reduction‐triggered cathodic deposition does not lead to the plating of reduced metals (Zn and Co). It is also operable cost‐effectively in the absence of supporting electrolyte and facilitates the construction of well‐defined sub‐micrometer‐sized heterogeneous structures within ZIF films. 相似文献
6.
Juntao Li Dr. Srinivas Gadipelli 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(62):14167-14172
Metal–organic frameworks/zeolitic imidazolate frameworks (MOFs/ZIFs) and their post-synthesis modified nanostructures, such as oxides, hydroxides, and carbons have generated significant interest for electrocatalytic reactions. In this work, a high and durable oxygen evolution reaction (OER) performance directly from bimetallic Zn100−xCox-ZIF samples is reported, without carrying out high-temperature calcination and/or carbonization. ZIFs can be reproducibly and readily synthesized in large scale at ambient conditions. The bimetallic ZIFs show a systematic and gradually improved OER activity with increasing cobalt concentration. A further increase in OER activity is evidenced in ZIF-67 polyhedrons with controlled particle size of <200 nm among samples of different sizes between 50 nm and 2 μm. Building on this, a significantly enhanced, >50 %, OER activity is obtained with ZIF-67/carbon black, which shows a low overpotential of approximately 320 mV in 1.0 m KOH electrolyte. Such activity is comparable to or better than numerous MOF/ZIF-derived electrocatalysts. The optimized ZIF-67 sample also exhibits increased activity and durability over 24 h, which is attributed to an in situ developed active cobalt oxide/oxyhydroxide related nanophase. 相似文献
7.
Selective Capture of Carbon Dioxide under Humid Conditions by Hydrophobic Chabazite‐Type Zeolitic Imidazolate Frameworks 下载免费PDF全文
Nhung T. T. Nguyen Dr. Hiroyasu Furukawa Dr. Felipe Gándara Dr. Hoang T. Nguyen Kyle E. Cordova Prof. Omar M. Yaghi 《Angewandte Chemie (International ed. in English)》2014,53(40):10645-10648
Hydrophobic zeolitic imidazolate frameworks (ZIFs) with the chabazite ( CHA ) topology are synthesized by incorporating two distinct imidazolate links. Zn(2‐mIm)0.86(bbIm)1.14 (ZIF‐300), Zn(2‐mIm)0.94(cbIm)1.06 (ZIF‐301), and Zn(2‐mIm)0.67(mbIm)1.33 (ZIF‐302), where 2‐mIm=2‐methylimidazolate, bbIm=5(6)‐bromobenzimidazolate, cbIm=5(6)‐chlorobenzimidazolate, and mbIm=5(6)‐methylbenzimidazolate, were prepared by reacting zinc nitrate tetrahydrate and 2‐mIm with the respective bIm link in a mixture of N,N‐dimethylformamide (DMF) and water. Their structures were determined by single‐crystal X‐ray diffraction and their permanent porosity shown. All of these structures are hydrophobic as confirmed by water adsorption isotherms. All three ZIFs are equally effective at the dynamic separation of CO2 from N2 under both dry and humid conditions without any loss of performance over three cycles and can be regenerated simply by using a N2 flow at ambient temperature. 相似文献
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Yuchen Xiao Anh N. Hong Dandan Hu Yanxiang Wang Prof. Xianhui Bu Prof. Pingyun Feng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(71):16358-16365
Zeolitic imidazolate frameworks (ZIFs) are traditionally synthesized solvothermally by using cost- and waste-incurring organic solvents. Here, a direct synthesis method is reported for ZIF-8, ZIF-67, and their heterometallic versions from solid precursors only. This solvent-free crystallization method not only completely avoids organic solvents, but also provides an effective path for the synthesis of homogeneous mixed-metal ZIFs. Furthermore, under templating by NaCl/ZnCl2 eutectic salt, carbonization of the ZIF materials gives rise to a series of N-containing high-surface-area carbon materials with impressive catalytic properties for the oxygen reduction reaction. 相似文献
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Javier Pérez‐Pellitero Dr. Hedi Amrouche Flor R. Siperstein Dr. Gerhard Pirngruber Dr. Carlos Nieto‐Draghi Dr. Gérald Chaplais Dr. Angélique Simon‐Masseron Dr. Delphine Bazer‐Bachi Dr. David Peralta Nicolas Bats Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(5):1560-1571
Experimental measurements and molecular simulations were conducted for two zeolitic imidazolate frameworks, ZIF‐8 and ZIF‐76. The transferability of the force field was tested by comparing molecular simulation results of gas adsorption with experimental data available in the literature for other ZIF materials (ZIF‐69). Owing to the good agreement observed between simulation and experimental data, the simulation results can be used to identify preferential adsorption sites, which are located close to the organic linkers. Topological mapping of the potential‐energy surfaces makes it possible to relate the preferential adsorption sites, Henry constant, and isosteric heats of adsorption at zero coverage to the nature of the host–guest interactions and the chemical nature of the organic linker. The role played by the topology of the solid and the organic linkers, instead of the metal sites, upon gas adsorption on zeolite‐like metal–organic frameworks is discussed. 相似文献
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Synthesis of Densely Packaged,Ultrasmall Pt02 Clusters within a Thioether‐Functionalized MOF: Catalytic Activity in Industrial Reactions at Low Temperature 下载免费PDF全文
Marta Mon Miguel A. Rivero‐Crespo Dr. Jesús Ferrando‐Soria Alejandro Vidal‐Moya Dr. Mercedes Boronat Dr. Antonio Leyva‐Pérez Prof. Dr. Avelino Corma Dr. Juan C. Hernández‐Garrido Dr. Miguel López‐Haro Prof. Dr. José J. Calvino Giulio Ragazzon Prof. Dr. Alberto Credi Dr. Donatella Armentano Dr. Emilio Pardo 《Angewandte Chemie (International ed. in English)》2018,57(21):6186-6191
The gram‐scale synthesis, stabilization, and characterization of well‐defined ultrasmall subnanometric catalytic clusters on solids is a challenge. The chemical synthesis and X‐ray snapshots of Pt02 clusters, homogenously distributed and densely packaged within the channels of a metal–organic framework, is presented. This hybrid material catalyzes efficiently, and even more importantly from an economic and environmental viewpoint, at low temperature (25 to 140 °C), energetically costly industrial reactions in the gas phase such as HCN production, CO2 methanation, and alkene hydrogenations. These results open the way for the design of precisely defined catalytically active ultrasmall metal clusters in solids for technically easier, cheaper, and dramatically less‐dangerous industrial reactions. 相似文献
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Katherine Self Michael Telfer Dr. Heather F. Greer Prof. Wuzong Zhou 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(52):19090-19095
RHO zeolitic imidazolate framework (ZIF), Zn1.33(O.OH)0.33(nim)1.167(pur), crystals with a rhombic dodecahedral morphology were synthesized by a solvothermal process. The growth of the crystals was studied over time using scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X‐ray diffraction (PXRD) and Brunauer–Emmett–Teller (BET) analyses, and a reversed crystal growth mechanism was revealed. Initially, precursor materials joined together to form disordered aggregates, which then underwent surface recrystallization forming a core–shell structure, in which a disordered core is encased in a layer of denser, less porous crystal. When the growth continued, the shell became less and less porous, until it was a layer of true single crystal. The crystallization then extended from the surface to the core over a six‐week period until, eventually, true single crystals were formed. 相似文献
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Imidazolium Ionic Liquids,Imidazolylidene Heterocyclic Carbenes,and Zeolitic Imidazolate Frameworks for CO2 Capture and Photochemical Reduction 下载免费PDF全文
Imidazolium ionic liquids (ILs), imidazolylidene N‐heterocyclic carbenes (NHCs), and zeolitic imidazolate frameworks (ZIFs) are imidazolate motifs which have been extensively investigated for CO2 adsorption and conversion applications. Summarized in this minireview is the recent progress in the capture, activation, and photochemical reduction of CO2 with these three imidazolate building blocks, from homogeneous molecular entities (ILs and NHCs) to heterogeneous crystalline scaffolds (ZIFs). The developments and existing shortcomings of the imidazolate motifs for their use in CO2 utilizations is assessed, with more of focus on CO2 photoredox catalysis. The opportunities and challenges of imidazolate scaffolds for future advancement of CO2 photochemical conversion for artificial photosynthesis are discussed. 相似文献
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Controlling Dissolution and Transformation of Zeolitic Imidazolate Frameworks by using Electron‐Beam‐Induced Amorphization 下载免费PDF全文
Dr. Sabrina Conrad Prashant Kumar Feng Xue Dr. Limin Ren Sheryl Henning Chunhong Xiao Prof. K. Andre Mkhoyan Prof. Michael Tsapatsis 《Angewandte Chemie (International ed. in English)》2018,57(41):13592-13597
Amorphous zeolitic imidazolate frameworks (ZIFs) offer promising applications as novel functional materials. Herein, amorphization of ZIF‐L through scanning‐electron‐beam exposure is demonstrated, based on amorphization of individual ZIF‐L crystals. The amorphized ZIF product has drastically increased stability against dissolution in water. An electron dose that allows for complete preservation of amorphous particles after immersion in water is established, resulting in new shapes of amorphous ZIF‐L with spatial control at the sub‐micrometer length scale. Changed water stability as a consequence of scanning‐electron‐beam exposure is demonstrated for three additional metal–organic frameworks (ZIF‐8, Zn(BeIm)OAc, MIL‐101), highlighting the potential use of an electron beam for top‐down MOF patterning. Lastly, recrystallization of ZIF‐L in the presence of linker is studied and shows distinct differences for crystalline and amorphized material. 相似文献
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Modelling a Linker Mix‐and‐Match Approach for Controlling the Optical Excitation Gaps and Band Alignment of Zeolitic Imidazolate Frameworks 下载免费PDF全文
Dr. Ricardo Grau‐Crespo Alex Aziz Angus W. Collins Dr. Rachel Crespo‐Otero Dr. Norge C. Hernández Dr. L. Marleny Rodriguez‐Albelo Dr. A. Rabdel Ruiz‐Salvador Prof. Dr. Sofia Calero Dr. Said Hamad 《Angewandte Chemie (International ed. in English)》2016,55(52):16012-16016
Tuning the electronic structure of metal–organic frameworks is the key to extending their functionality to the photocatalytic conversion of absorbed gases. Herein we discuss how the band edge positions in zeolitic imidazolate frameworks (ZIFs) can be tuned by mixing different imidazole‐based linkers within the same structure. We present the band alignment for a number of known and hypothetical Zn‐based ZIFs with respect to the vacuum level. Structures with a single type of linker exhibit relatively wide band gaps; however, by mixing linkers of a low‐lying conduction edge with linkers of a high‐lying valence edge, we can predict materials with ideal band positions for visible‐light water splitting and CO2 reduction photocatalysis. By introducing copper in the tetrahedral position of the mixed‐linker ZIFs, it would be possible to increase both photo‐absorption and the electron–hole recombination times. 相似文献
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Dr. Thomas D. Bennett Dr. Paul J. Saines Prof. David A. Keen Dr. Jin‐Chong Tan Prof. Anthony K. Cheetham 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(22):7049-7055
The I2‐sorption and ‐retention properties of several existing zeolitic imidazolate frameworks (ZIF‐4, ‐8, ‐69) and a novel framework, ZIF‐mnIm ([Zn(mnIm)2]; mnIm=4‐methyl‐5‐nitroimidazolate), have been characterised using microanalysis, thermogravimetric analysis and X‐ray diffraction. The topologically identical ZIF‐8 ([Zn(mIm)2]; mIm=2‐methylimidazolate) and ZIF‐mnIm display similar sorption abilities, though strikingly different guest‐retention behaviour upon heating. We discover that this guest retention is greatly enhanced upon facile amorphisation by ball milling, particularly in the case of ZIF‐mnIm, for which I2 loss is retarded by as much as 200 °C. It is anticipated that this general approach should be applicable to the wide range of available metal–organic framework‐type materials for the permanent storage of harmful guest species. 相似文献
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Frontispiece: Modelling a Linker Mix‐and‐Match Approach for Controlling the Optical Excitation Gaps and Band Alignment of Zeolitic Imidazolate Frameworks 下载免费PDF全文
Dr. Ricardo Grau‐Crespo Alex Aziz Angus W. Collins Dr. Rachel Crespo‐Otero Dr. Norge C. Hernández Dr. L. Marleny Rodriguez‐Albelo Dr. A. Rabdel Ruiz‐Salvador Prof. Dr. Sofia Calero Dr. Said Hamad 《Angewandte Chemie (International ed. in English)》2016,55(52)
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Hongfeng Li Peng Wu Yawen Xiao Meng Shao Yu Shen Yun Fan Huanhuan Chen Ruijie Xie Wenlei Zhang Sheng Li Jiansheng Wu Yu Fu Bing Zheng Weina Zhang Fengwei Huo 《Angewandte Chemie (International ed. in English)》2020,59(12):4763-4769
Metal–organic frameworks (MOFs) are promising materials with fascinating properties. Their widespread applications are sometimes hindered by the intrinsic instability of frameworks. However, this instability of MOFs can also be exploited for useful purposes. Herein, we report the use of MOFs as metal ion precursors for constructing functional nanocomposites by utilizing the instability of MOFs. The heterogeneous growth process of nanostructures on substrates involves the release of metal ions, nucleation on substrates, and formation of a covering structure. Specifically, the synthesized CoS with carbon nanotubes as substrates display enhanced performance in a lithium‐ion battery. Such strategy not only presents a new way for exploiting the instability of MOFs but also supplies a prospect for designing versatile functional nanocomposites. 相似文献
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The First One‐Pot Synthesis of Metal–Organic Frameworks Functionalised with Two Transition‐Metal Complexes 下载免费PDF全文
Dr. Ana E. Platero‐Prats Dr. Antonio Bermejo Gómez Dr. Louise Samain Prof. Xiaodong Zou Prof. Belén Martín‐Matute 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(2):861-866
The synthesis of a metal–organic framework (UiO‐67) functionalised simultaneously with two different transition metal complexes (Ir and Pd or Rh) through a one‐pot procedure is reported for the first time. This has been achieved by an iterative modification of the synthesis parameters combined with characterisation of the resulting materials using different techniques, including X‐ray absorption spectroscopy (XAS). The method also allows the first synthesis of UiO‐67 with a very wide range of loadings (from 4 to 43 mol %) of an iridium complex ([IrCp*(bpydc)(Cl)Cl]2?; bpydc=2,2′‐bipyridine‐5,5′‐dicarboxylate, Cp*=pentamethylcyclopentadienyl) through a pre‐functionalisation methodology. 相似文献
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Zeolitic Imidazolate Framework/Graphene Oxide Hybrid Nanosheets as Seeds for the Growth of Ultrathin Molecular Sieving Membranes 下载免费PDF全文
Yaoxin Hu Dr. Jing Wei Yan Liang Dr. Huacheng Zhang Prof. Xiwang Zhang Prof. Wei Shen Prof. Huanting Wang 《Angewandte Chemie (International ed. in English)》2016,55(6):2048-2052
A defect‐free zeolitic imidazolate framework‐8 (ZIF‐8)/graphene oxide (GO) membrane with a thickness of 100 nm was prepared using two‐dimensional (2D) ZIF‐8/GO hybrid nanosheets as seeds. Hybrid nanosheets with a suitable amount of ZIF‐8 nanocrystals were essential for producing a uniform seeding layer that facilitates fast crystal intergrowth during membrane formation. Moreover, the seeding layer acts as a barrier between two different synthesis solutions, and self‐limits crystal growth and effectively eliminates defects during the contra‐diffusion process. The resulting ultrathin membranes show excellent molecular sieving gas separation properties, such as with a high CO2/N2 selectivity of 7.0. This 2D nano‐hybrid seeding strategy can be readily extended to the fabrication of other defect‐free and ultrathin MOF or zeolite molecular sieving membranes for a wide range of separation applications. 相似文献