ORCID Profile
0000-0002-9910-7603
Current Organisation
University of Nottingham
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Publisher: Wiley
Date: 14-05-2014
Abstract: Solvothermal reaction of H4L (L = biphenyl-3,3',5,5'-tetracarboxylate) and Bi(NO3)3⋅(H2O)5 in a mixture of DMF/MeCN/H2O in the presence of piperazine and nitric acid at 100 °C for 10 h affords the solvated metal-organic polymer [Bi2(L)1.5(H2O)2]⋅(DMF)3.5⋅(H2O)3 (NOTT-220-solv). A single crystal X-ray structure determination confirms that it crystallises in space group P2/c and has a neutral and non-interpenetrated structure comprising binuclear {Bi2} centres bridged by tetracarboxylate ligands. NOTT-220-solv shows a 3,6-connected network having a framework topology with a {4⋅6(2)}2{4(2)⋅6(5)⋅8(8)}{6(2)⋅8} point symbol. The desolvated material NOTT-220a shows exceptionally high adsorption uptakes for CH4 and CO2 on a volumetric basis at moderate pressures and temperatures with a CO2 uptake of 553 g L(-1) (20 bar, 293 K) with a saturation uptake of 688 g L(-1) (1 bar, 195 K). The corresponding CH4 uptake was measured as 165 V(STP)/V (20 bar, 293 K) and 189 V(STP/V) (35 bar, 293 K) with a maximum CH4 uptake for NOTT-220a recorded at 20 bar and 195 K to be 287 V(STP)/V, while H2 uptake of NOTT-220a at 20 bar, 77 K is 42 g L(-1). These gas uptakes have been modelled by grand canonical Monte Carlo (GCMC) and density functional theory (DFT) calculations, which confirm the experimental data and give insights into the nature of the binding sites of CH4 and CO2 in this porous hybrid material.
Publisher: Proceedings of the National Academy of Sciences
Date: 09-03-2017
Abstract: A family of stable porous materials incorporating organic linkers and Cu(II) cations is reported. Their pores can be altered systematically by elongation of the ligands allowing a strategy of selective pore extension along one dimension. These materials show remarkable gas adsorption properties with high working capacities for CH 4 (0.24 g g −1 , 163 cm 3 cm −3 at 298 K, 5–65 bar) for the most porous system. The mechanism of rotation of the organic groups in the solid state has been analyzed by NMR spectroscopy and rotational rates and transition temperatures analyzed. Significantly, we show that framework dynamics can be controlled by ligand design only, and this paves the way to understanding the role of molecular rotors within these materials.
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2SC20443F
Publisher: Springer Science and Business Media LLC
Date: 03-06-2012
DOI: 10.1038/NMAT3343
Abstract: The selective capture of carbon dioxide in porous materials has potential for the storage and purification of fuel and flue gases. However, adsorption capacities under dynamic conditions are often insufficient for practical applications, and strategies to enhance CO(2)-host selectivity are required. The unique partially interpenetrated metal-organic framework NOTT-202 represents a new class of dynamic material that undergoes pronounced framework phase transition on desolvation. We report temperature-dependent adsorption/desorption hysteresis in desolvated NOTT-202a that responds selectively to CO(2). The CO(2) isotherm shows three steps in the adsorption profile at 195 K, and stepwise filling of pores generated within the observed partially interpenetrated structure has been modelled by grand canonical Monte Carlo simulations. Adsorption of N(2), CH(4), O(2), Ar and H(2) exhibits reversible isotherms without hysteresis under the same conditions, and this allows capture of gases at high pressure, but selectively leaves CO(2) trapped in the nanopores at low pressure.
Publisher: American Chemical Society (ACS)
Date: 23-04-2018
Publisher: Informa UK Limited
Date: 13-04-2023
Publisher: American Chemical Society (ACS)
Date: 03-09-2014
DOI: 10.1021/JA506577G
Publisher: American Chemical Society (ACS)
Date: 12-10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CC08029G
Abstract: Carbon nanotube encapsulation offers a mechanism to trap kinetically rather than thermodynamically favoured supramolecular arrays.
Publisher: American Chemical Society (ACS)
Date: 11-2016
DOI: 10.1021/JACS.6B08059
Publisher: Wiley
Date: 07-05-2014
Abstract: The porous framework [Cu2(H2O)2L]⋅4 H2O⋅2 DMA (H4L = oxalylbis(azanediyl)diisophthalic acid DMA = N,N-dimethylacetamide), denoted NOTT-125, is formed by connection of {Cu2(RCOO)4} paddlewheels with the isophthalate linkers in L(4-). A single crystal structure determination reveals that NOTT-125 crystallises in monoclinic unit cell with a = 27.9161(6), b = 18.6627(4) and c = 32.3643(8) Å, β = 112.655(3)°, space group P2(1)/c. The structure of this material shows fof topology, which can be viewed as the packing of two types of cages (cage A and cage B) in three-dimensional space. Cage A is constructed from twelve {Cu2(OOCR)4} paddlewheels and six linkers to form an ellipsoid-shaped cavity approximately 24.0 Å along its long axis and 9.6 Å across its central diameter. Cage B consists of six {Cu2(OOCR)4} units and twelve linkers and has a spherical diameter of 12.7 Å taking into account the van der Waals radii of the atoms. NOTT-125 incorporates oxamide functionality within the pore walls, and this, combined with high porosity in desolvated NOTT-125a, is responsible for excellent CO2 uptake (40.1 wt % at 273 K and 1 bar) and selectivity for CO2 over CH4 or N2. Grand canonical Monte Carlo (GCMC) simulations show excellent agreement with the experimental gas isotherm data, and a computational study of the specific interactions and binding energies of both CO2 and CH4 with the linkers in NOTT-125 reveals a set of strong interactions between CO2 and the oxamide motif that are not possible with a single amide.
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Elena Besley.