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Ekaterina A Dolgopolova, Allison M Rice, Corey R Martin, Natalia B Shustova
In this review, we highlight how recent advances achieved in the fields of photochemistry and photophysics of metal-organic frameworks (MOFs) could be applied towards the engineering of next generation MOF-based sensing devices. In addition to high surface area and structural tunability, which are crucial for efficient sensor development, progress in the field of MOF-based sensors could rely on the combination of MOF light-harvesting ability, understanding energy transfer processes within a framework, and application of MOF-based photocatalysis towards sensing enhancement...
March 16, 2018: Chemical Society Reviews
Junjie Zhao, Berc Kalanyan, Heather F Barton, Brent A Sperling, Gregory N Parsons
In situ chemical measurements of solution/surface reactions during metal-organic framework (MOF) thin film growth can provide valuable information about the mechanistic and kinetic aspects of key reaction steps, and allow control over crystal quality and material properties. Here, we report a new approach to study the growth of MOF thin films in a flow cell using attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR). Real-time spectra recorded during continuous flow synthesis were used to investigate the mechanism and kinetics that govern the formation of (Zn, Cu) hydroxy double salts (HDSs) from ZnO thin films and the subsequent conversion of HDS to HKUST-1...
October 24, 2017: Chemistry of Materials: a Publication of the American Chemical Society
Jia Wen, Ying Fang, Guangming Zeng
The efficient removal of heavy metals (HMs) from the environment has become an important issue from both biological and environmental perspectives. Recently, porous metal-organic frameworks (MOFs), combining central metals and organic ligands, have been proposed as promising materials in the capture of various toxic substances, including HMs, due to their unique characteristics. Here we review recent progress in the field of water remediation from the perspective of primary HMs (including divalent metals and variable-valent metals) in water pollution and the corresponding MOFs (including virgin and modified MOFs, magnetic MOFs composites and so on) that can remove these metals from water...
March 6, 2018: Chemosphere
Duong Tung Pham, Joseph Paul Baboo, Jinju Song, Sungjin Kim, Jeonggeun Jo, Vinod Mathew, Muhammad Hilmy Alfaruqi, Balaji Sambandam, Jaekook Kim
Pyrite (FeS2 ) is a promising electrode material for lithium ion batteries (LIBs) because of its high natural availability, low toxicity, cost-effectiveness, high theoretical capacity (894 mA h g-1 ) and high theoretical specific energy density (1270 W h kg-1 , 4e- /FeS2 ). Nevertheless, the use of FeS2 in electrochemical capacitors was restricted due to fast capacity fading as a result of polysulfide (S/Sn 2- ) formation during the initial electrochemical cycling. In order to avoid the formation of polysulfides, we employed the strategy of utilizing an ether based electrolyte (1...
March 15, 2018: Nanoscale
Erika Virmani, Julian M Rotter, Andre Mähringer, Tobias von Zons, Adelheid Godt, Thomas Bein, Stefan Wuttke, Dana D Medina
Controlled on-surface film growth of porous and crystalline frameworks is a central requisite for incorporating these materials into functional platforms and operational devices. Here, we present the synthesis of thin zirconium-based metal-organic framework (MOF) films by vapor-assisted conversion (VAC). We established protocols adequate for the growth of UiO-66, UiO-66(NH2 ), UiO-67, and UiO-68(NH2 ) as well as the porous interpenetrated Zr-organic framework (PPPP-PIZOF-1) as highly oriented thin films. Through the VAC approach, precursors in a cast solution layer on a bare gold substrate are reacting to form a porous continuous MOF film, oriented along the [111] crystal axis by an exposure to a solvent vapor under elevated temperatures of 100 °C and 3 h reaction times...
March 15, 2018: Journal of the American Chemical Society
Sheta M Sheta, Said M El-Sheikh, Mohkles M Abd-Elzaher
Novel copper metal organic framework nanoparticles Cu-MOF-NPs (C1) were prepared via two simple alternative methods and confirmed by analytical characterization using mass, IR, Raman, XRD spectrum, HR-TEM and TGA-DSC. Mass spectroscopy revealed the molecular ion peak at 647 m/z for the monomeric unit structure n[Cu(AIP)2 (PIY)(H2 O)2 ]·4H2 O, the presence of which was further supported by mass fragmentation. The Raman spectrum revealed two separate peaks corresponding to D and G bands of carbon in the structure of C1...
March 15, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Shogo Amemori, Rakesh Kumar Gupta, Marcus Leo Böhm, James Xiao, Uyen Huynh, Tomoki Oyama, Kenji Kaneko, Akshay Rao, Nobuhiro Yanai, Nobuo Kimizuka
Hybrid materials consisting of semiconductor nanocrystals and metal-organic frameworks (MOFs) were prepared for the first time to achieve photon upconversion based on triplet-triplet annihilation (TTA-UC) in the solid-state, which allowed TTA-UC with large anti-Stokes shifts in the visible and near-infrared regions.
March 15, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Meng-Ting Li, Ning Kong, Ya-Qian Lan, Zhong-Min Su
We utilise the dual synthesis strategy in terms of bimetallic inorganic building blocks and sulfur containing organic ligand. A novel sulfur-containing bimetallic metal organic framework (Fe2 Co-TPDC) with two types of 4-fold meso-helical structures has been successfully synthesized. Benefitting from the uniform distribution of active sulfur sites and the structural stability of the mixed-metallic method, Fe2 Co-TPDC can efficiently prevent a shuttle behavior of sulfur and endow a commendable specific capacity...
March 15, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Senja Barthel, Eugeny V Alexandrov, Davide M Proserpio, Berend Smit
We consider two metal-organic frameworks as identical if they share the same bond network respecting the atom types. An algorithm is presented that decides whether two metal-organic frameworks are the same. It is based on distinguishing structures by comparing a set of descriptors that is obtained from the bond network. We demonstrate our algorithm by analyzing the CoRe MOF database of DFT optimized structures with DDEC partial atomic charges using the program package ToposPro.
March 7, 2018: Crystal Growth & Design
Zongbi Bao, Danyan Xie, Ganggang Chang, Hui Wu, Liangying Li, Wei Zhou, Hailong Wang, Zhiguo Zhang, Huabin Xing, Qiwei Yang, Michael J Zaworotko, Qilong Ren, Banglin Chen
Research on HOFs has been developed for quite a long time; however, those with both established permanent porosities and functional properties are extremely rare due to weak hydrogen-bonding interactions among molecular organic linkers which are much more fragile and difficult to stabilize. Herein, through judiciously combining the superiority of both the moderately stable coordination bonds in MOFs and hydrogen bonds, we have realized a microporous hydrogen-bonded organometallic framework HOF-21, which not only shows permanent porosity but also exhibits highly selective separation performance of C2H2/C2H4 at room temperature...
March 14, 2018: Journal of the American Chemical Society
Kai Lv, Chu-Ting Yang, Yi Liu, Sheng Hu, Xiao-Lin Wang
To aid the design of a hierarchically porous unconventional metal-phosphonate framework (HP-UMPF) for practical radioanalytical separation, a systematic investigation of the hydrolytic stability of bulk phase against acidic corrosion has been carried out for an archetypical HP-UMPF. Bulk dissolution results suggest that aqueous acidity has a more paramount effect on incongruent leaching than the temperature, and the kinetic stability reaches equilibrium by way of an accumulation of a partial leached species on the corrosion conduits...
March 14, 2018: Nanomaterials
Martin Drost, Fan Tu, Luisa Berger, Christian Preischl, Wencai Zhou, Hartmut Gliemann, Christof Wöll, Hubertus Marbach
We demonstrate that Surface-Anchored Metal-Organic Frameworks (SURMOFs) are extraordinary well-suited as resists for high-resolution Focused Electron Beam Induced Processing (FEBIP) techniques. The combination of such powerful lithographic protocols with the huge versatility of MOF materials are investigated in respect to their potential in nanostructures fabrication. The applied FEBIP methods rely on the local decomposition of Fe(CO)5 and Co(CO)3 NO as precursors, either by the direct impact of the focused electron beam (Electron Beam Induced Deposition, EBID) or through the interaction of the precursor molecules with preirradiated/activated SURMOF areas (Electron Beam Induced Surface Activation, EBISA)...
March 14, 2018: ACS Nano
Zhishun He, Kai Wang, Shasha Zhu, Liang-Ai Huang, Miaomiao Chen, Jianfeng Guo, Shien Pei, Haibo Shao, Jianming Wang
Hierarchically nanostructured binary/multiple transition metal oxides with electrically conductive coatings are very attractive for lithium-ion batteries (LIBs) owing to their excellent electrochemical properties induced by their unique compositions and microstructures. Herein, hierarchical MnO doped Fe3O4@C composite nanospheres are prepared by a simple one-step annealing in Ar atmosphere, using Mn-doped Fe-based metal organic frameworks (Mn-doped MIL-53(Fe)) as precursor. The MnO doped Fe3O4@C composite particles have a uniform nanosphere structure with a diameter of ~100 nm, and each nanosphere is composed of clustered primary nanoparticles with an amorphous carbon shell, forming a unique hierarchical nanoarchitecture...
March 14, 2018: ACS Applied Materials & Interfaces
Jiahui Kou, Lin-Bing Sun
Due to their diverse structure, high porosity, and tunable functionality, metal-organic frameworks (MOFs) are of great inter-est for diverse applications including catalysis. However, the poor hydrostability of most reported MOFs hinders their cata-lytic applications seriously. In addition, the development of an effective method to improve the catalytic activity of MOFs is another challenge. Here, we report for the first time the development of a double-solvent strategy to fabricate MOFs inside silica nanopores...
March 14, 2018: ACS Applied Materials & Interfaces
Oriana Brea, Alberto Luna, Cristina Díaz, Ines Corral Perez
H₂ has been proposed as a long-term non-fossil fuel to be used in a future ideal carbon neutral energetic economy. However, its low volumetric energy density hinders its storage and transportation. MOFs represent very promising materials for this purpose, due to their very extended surface areas. Azolates and, in particular tetrazolates, are together with carboxylate functionalities very common organic linkers connecting metallic secondary building units in MOFs. This study addresses from a theoretical perspective the H₂ adsorptive properties of tetrazolate linkers at molecular level, following a size progressive approach...
March 14, 2018: Chemphyschem: a European Journal of Chemical Physics and Physical Chemistry
Xizhen Lian, Yanyan Huang, Yuanyuan Zhu, Yu Fang, Rui Zhao, Elizabeth Joseph, Jialuo Li, Jean-Phillipe Pellois, Hongcai Zhou
Prodrug activation by exogenously administered enzymes for cancer therapy is an approach to achieve better selectivity and less systemic toxicity than conventional chemotherapy. However, the short half-lives of the activating enzymes in bloodstream has limited its success. Here, we demonstrate that a tyrosinase-MOF nanoreactor activates the prodrug paracetamol in cancer cells in a long-lasting manner. By generating reactive oxygen species (ROS) and depleting glutathione (GSH), the product of enzymatic conversion of paracetamol is toxic to drug-resistant cancer cells...
March 13, 2018: Angewandte Chemie
Hiang Kwee Lee, Charlynn Sher Lin Koh, Yih Hong Lee, Chong Liu, In Yee Phang, Xuemei Han, Chia-Kuang Tsung, Xing Yi Ling
Electrochemical nitrogen-to-ammonia fixation is emerging as a sustainable strategy to tackle the hydrogen- and energy-intensive operations by Haber-Bosch process for ammonia production. However, current electrochemical nitrogen reduction reaction (NRR) progress is impeded by overwhelming competition from the hydrogen evolution reaction (HER) across all traditional NRR catalysts and the requirement for elevated temperature/pressure. We achieve both excellent NRR selectivity (~90%) and a significant boost to Faradic efficiency by 10 percentage points even at ambient operations by coating a superhydrophobic metal-organic framework (MOF) layer over the NRR electrocatalyst...
March 2018: Science Advances
Ang Qiao, Thomas D Bennett, Haizheng Tao, Andraž Krajnc, Gregor Mali, Cara M Doherty, Aaron W Thornton, John C Mauro, G Neville Greaves, Yuanzheng Yue
Glass-forming ability (GFA) is the ability of a liquid to avoid crystallization during cooling. Metal-organic frameworks (MOFs) are a new class of glass formers ( 1 - 3 ), with hitherto unknown dynamic and thermodynamic properties. We report the discovery of a new series of tetrahedral glass systems, zeolitic imidazolate framework-62 (ZIF-62) [Zn(Im2- x bIm x )], which have ultrahigh GFA, superior to any other known glass formers. This ultrahigh GFA is evidenced by a high viscosity η (105 Pa·s) at the melting temperature T m , a large crystal-glass network density deficit (Δρ/ρg )network , no crystallization in supercooled region on laboratory time scales, a low fragility ( m = 23), an extremely high Poisson's ratio (ν = 0...
March 2018: Science Advances
Ayda Nemati Vesali Azar, Seda Keskin
Efficient separation of acetylene (C2 H2 ) from CO2 and CH4 is important to meet the requirement of high-purity acetylene in various industrial applications. Metal organic frameworks (MOFs) are great candidates for adsorption-based C2 H2 /CO2 and C2 H2 /CH4 separations due to their unique properties such as wide range of pore sizes and tunable chemistries. Experimental studies on the limited number of MOFs revealed that MOFs offer remarkable C2 H2 /CO2 and C2 H2 /CH4 selectivities based on single-component adsorption data...
2018: Frontiers in Chemistry
Roberto Christian Arbulu, Ying-Bing Jiang, Eric John Peterson, Yang Qin
New mechanisms of controlled growth of one-dimensional (1D) metal-organic framework (MOF) nano- and super-structures under size-confinement and surface directing effects have been discovered. Through applying interfacial synthesis templated by track-etched polycarbonate (PCTE) membranes, congruent polycrystalline zeolitic imidazolate framework-8 (ZIF-8) solid nanorods and hollow nanotubes were found to form within 100 nm membrane pores, while single crystalline ZIF-8 nanowires grew inside 30 nm pores, all of which possess large aspect ratios up to 60 and show preferential crystal orientation with the {100} planes aligned parallel to the pore's long axis...
March 13, 2018: Angewandte Chemie
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