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Title: Solvothermal synthesis of porous beryllate containing materials
Author: Littlefield, Benjamin T. R.
Awarding Body: University of Southampton
Current Institution: University of Southampton
Date of Award: 2013
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Natural and synthetic zeolites have been the focus for extensive research owing to their many applications and huge potential number of new topologies. The work presented here represents the first major study into the formation of zeotypical materials incorporating BeO4 and T5+O4 (T5+ = As or P) tetrahedra and a large number of new structures have been produced. These novel materials have been synthesised via hydrothermal procedures and characterised via Single Crystal X-ray Diffraction, supported by Powder X-ray Diffraction, Thermogravimetric Analysis, Magic Angle Spinning Nuclear Magnetic Resonance and Electron Dispersive Spectroscopy. The berylloarsenates produced encompass the entire range of dimensionality, from cluster structures such as Na3.5[AsO4(BeF3)(BeF2)]•0.4H2O to the novel three dimensional framework [Hbis( 2-ethylhexyl)amine, NH4] [(AsO4)3(AsO3OH)Be3(BeOH)] and include analogues of known zeolite topologies; MER, AFI and WEI. Four completely novel fully connected three-dimensional zeolitic topologies are also reported with one already being assigned the Framework Type code of BOZ. These new topologies represent the most structurally complicated zeolites known and are remarkable in their high calculated internal pore volume. The berylloarsenates are supported by parallel research into the beryllophosphates which has produced unusual new structures of low dimensionality such as the one dimensional chain Na2[(BeO2OH)(PO2)]•H2O as well as structural analogues of the berylloarsenate structures including [H-pyridine][(BeO4)2BeO3(OH2)P3(OH)] which exhibits the AFI topology. These structures could potentially be used in catalysis, ion exchange and due to their low framework density, gas storage. A short investigation into other beryllate chemistry is also presented which includes the novel two dimensional structures Na[BeGeO3(OH)] and Ba[BeGeO3(OH)] which significantly contribute to the sparse field of beryllogermanates. This section also contains the first structural characterisation of Sr[Be(OH)4], a vital species in beryllium solution chemistry.
Supervisor: Raja, Robert Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: QD Chemistry