Assen, Ayalew Hussen Assen; Yassine, Omar; Shekhah, Osama; Eddaoudi, Mohamed; Salama, Khaled N.(ACS Sensors, American Chemical Society (ACS), 2017-08-15)[Article]
This work reports on the fabrication and deployment of a select metal-organic framework (MOF) thin film as an advanced chemical capacitive sensor for the sensing/detection of ammonia (NH3) at room temperature. Namely, the MOF thin film sensing layer consists of a rare-earth (RE) MOF (RE-fcu-MOF) deposited on a capacitive interdigitated electrode (IDE). Purposely, the chemically stable naphthalene-based RE-fcu-MOF (NDC-Y-fcu-MOF) was elected and prepared/arranged as a thin film on a pre-functionalized capacitive IDE via the solvothermal growth method. Unlike earlier realizations, the fabricated MOF-based sensor showed a notable detection sensitivity for NH3 at concentrations down to 1 ppm, with a detection limit appraised to be around 100 ppb (at room temperature) even in the presence of humidity and/or CO2. Distinctly, the NDC-Y-fcu-MOF based sensor exhibited the required stability to NH3, in contract to other reported MOFs, and a remarkable detection selectivity towards NH3 vs. CH4, NO2, H2 and C7H8. The NDC-Y-fcu-MOF based sensor exhibited excellent performance for sensing ammonia for simulated breathing system in the presence of the mixture of carbon dioxide and/or humidity (water vapor), with no major alteration in the detection signal.
Wang, Shuang; Belmabkhout, Youssef; Cairns, Amy; Li, Guanghua; Huo, Qisheng; Liu, Yunling; Eddaoudi, Mohamed(ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2017-07-11)[Article]
A strategy based on metal-ligand directed assembly of metal-organic squares (MOSs), built-up from four-membered ring (4MR) secondary building units (SBUs), has been employed for the design and construction of isoreticular zeolite-like supramolecular assemblies (ZSAs). Four porous Co-based ZSAs having the same underlying gis topology, but differing only with respect to the capping and bridging linkers, were successfully isolated and fully characterized. In this series, each MOS in ZSA-3-ZSA-6 possess an ideal square geometry and is connected to four neighboring MOS via a total of 16 hydrogen bonds to give a 3-periodic porous network.To systematically assess the effect of the pore system (size and functionality) on the gas adsorption properties, we evaluated the MOSs for their affinity for different probe molecules such as CO2 and light hydrocarbons. ZSA-3-ZSA-6 showed high thermal stability (up to 300 °C) and was proven highly porous as evidenced by gas adsorption studies. Notably, alkyl-functionalized MOSs were found to offer potential for selective separation of CO2, C3H6, and C3H8 from CH4 and H2 containing gas stream, such as natural gas and refinery-off gases.
AbdulHalim, Rasha; Bhatt, Prashant; Belmabkhout, Youssef; Shkurenko, Aleksander; Adil, Karim; Barbour, Leonard J.; Eddaoudi, Mohamed(Journal of the American Chemical Society, American Chemical Society (ACS), 2017-06-29)[Article]
Conventional adsorbents, namely zeolites and silica gel, are often used to control humidity by adsorbing water; however, adsorbents capable of dual functionality of humidification and dehumidification, offering the desired control of the moisture level at room temperature, has yet to be explored. Here we report Y-shp-MOF-5, a hybrid microporous highly-connected Rare-Earth based metal-organic framework (MOF), with dual functionality for moisture control within the recommended range of relative humidity (45% to 65% RH) set by the American Society of Heating, Refrigerating, and Air-Conditioning Engineers (ASHRAE). Y-shp-MOF-5 exhibits exceptional structural integrity, robustness and unique humidity-control performance as confirmed by the large number (thousand) of conducted water vapor adsorption-desorption cycles. The retained structural integrity and the mechanism of water sorption were corroborated using in situ single crystal X-ray diffraction (SCXRD) studies. The resultant working water uptake of 0.45 g.g-1 is solely regulated by a simple adjustment of the relative humidity, positioning this hydrolytically stable MOF as a prospective adsorbent for humidity control in confined spaces such as space shuttles, aircraft cabins and air-conditioned buildings.
Chen, Zhijie; Weselinski, Lukasz Jan; Adil, Karim; Belmabkhout, Youssef; Shkurenko, Aleksander; Jiang, Hao; Bhatt, Prashant; Guillerm, Vincent; Dauzon, Emilie; Xue, Dongxu; O’Keeffe, Michael; Eddaoudi, Mohamed(Journal of the American Chemical Society, American Chemical Society (ACS), 2017-02-15)[Article]
Highly connected and edge-transitive nets are of prime importance in crystal chemistry and are regarded as ideal blueprints for the rational design and construction of metal-organic frameworks (MOFs). We report the design and synthesis of highly connected MOFs based on reticulation of the sole two edge-transitive nets with a vertex figure as double six-membered-ring (d6R) building unit, namely the (4,12)-coordinated shp net (square and hexagonal-prism) and the (6,12)-coordinated alb net (aluminum diboride, hexagonal-prism and trigonal-prism). Decidedly, the combination of our recently isolated 12-connected (12-c) rare-earth (RE) nonanuclear [RE(μ-OH)(μ-O)(OC-)] carboxylate-based cluster, points of extension matching the 12 vertices of hexagonal-prism d6R, with 4-connected (4-c) square porphyrinic tetracarboxylate ligand led to the formation of the targeted RE-shp-MOF. This is the first time that RE-MOFs based on 12-c molecular building blocks (MBBs), d6R building units, have been deliberately targeted and successfully isolated, paving the way for the long-awaited (6,12)-c MOF with alb topology. Indeed, combination of a custom-designed hexacarboxylate ligand with RE salts led to the formation of the first related alb-MOF, RE-alb-MOF. Intuitively, we successfully transplanted the alb topology to another chemical system and constructed the first indium-based alb-MOF, In-alb-MOF, by employing trinuclear [In(μ-O)(OC-)] as the requisite 6-connected trigonal-prism and purposely made a dodecacarboxylate ligand as a compatible 12-c MBB. Prominently, the dodecacarboxylate ligand was employed to transplant shp topology into copper-based MOFs by employing the copper paddlewheel [Cu(OC-)] as the complementary square building unit, affording the first Cu-shp-MOF. We revealed that highly connected edge-transitive nets such shp and alb are ideal for topological transplantation and deliberate construction of related MOFs based on minimal edge-transitive nets.
Bootharaju, Megalamane Siddaramappa; Kozlov, Sergey; Cao, Zhen; Harb, Moussab; Maity, Niladri; Shkurenko, Aleksander; Parida, Manas R.; Hedhili, Mohamed N.; Eddaoudi, Mohamed; Mohammed, Omar F.; Bakr, Osman; Cavallo, Luigi; Basset, Jean-Marie(Journal of the American Chemical Society, American Chemical Society (ACS), 2017-01-12)[Article]
Atomically precise self-assembled architectures of noble metals with unique surface structures are necessary for prospective applications. However, the synthesis of such structures based on silver is challenging because of their instability. In this work, by developing a selective and controlled doping strategy, we synthesized and characterized a rod-shaped, charge-neutral, diplatinum-doped Ag nanocluster (NC) of [Pt2Ag23Cl7(PPh3)10]. Its crystal structure revealed the self-assembly of two Pt-centered Ag icosahedra through vertex sharing. Five bridging and two terminal chlorides and 10 PPh3 ligands were found to stabilize the cluster. Electronic structure simulations corroborated structural and optical characterization of the cluster and provided insights into the effect of the Pt dopants on the optical properties and stability of the cluster. Our study will open new avenues for designing novel self-assembled NCs using different elemental dopants.
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