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Displaying Results 151 - 175 of 4097 on page 7 of 164
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Thermal reversion of spirooxazine in ionic liquids containing the [NTf2]- anion
(2009)
Coleman, Simon; Byrne, Robert; Diamond, Dermot; Minkovska, Stela
Thermal reversion of spirooxazine in ionic liquids containing the [NTf2]- anion
(2009)
Coleman, Simon; Byrne, Robert; Diamond, Dermot; Minkovska, Stela
Abstract:
We have compared the rate of thermal reversion of Spirooxazine (SO) from its merocyanine (MC) form within ionic liquids and molecular solvents. Et(30) and Kamlet-Taft parameter studies indicate ILs are comparable to polar protic and aprotic solvents. The observed reversion kinetics within the ionic liquids were slower than that of molecular solvents with similar polarity, indicating a greater degree of interactions between the ionic liquid ions and the zwitterionic MC isomer, which led to increased lifetimes for the MC-ion complexes. Pre-metathesis cleaning of precursor salts was found to be necessary in order to obtain spectroscopic grade ILs for physiochemical analysis using solvatochromic probe dyes.
http://doras.dcu.ie/14788/
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Designer molecular probes for phosphonium ionic liquids
(2010)
Byrne, Robert; Coleman, Simon; Gallagher, Simon; Diamond, Dermot
Designer molecular probes for phosphonium ionic liquids
(2010)
Byrne, Robert; Coleman, Simon; Gallagher, Simon; Diamond, Dermot
Abstract:
Investigations into the extent of structuring present in phosphonium based ionic liquids (ILs) have been carried out using photochromic molecular probes. Three spiropyran derivatives containing hydroxyl (BSP-1), carboxylic acid (BSP-2) and aliphatic chain (C14H29) (BSP-3) functional groups have been analysed in a range of phosphonium based ionic liquids and their subsequent physico-chemical interactions were reported. It is believed that the functional groups locate the probe molecules into specific regions based upon the interaction of the functional groups with particular and defined regions of the ionic liquid. This structuring results in thermodynamic, kinetic and solvatochromic parameters that are not predictable from classical solvent models. BSP-1 and BSP-2 exhibit generally negative entropies of activation ranging from -50 J K-1 mol-1 to -90 J K-1 mol-1 implying relatively low solvent–solute interactions and possible anion interactions with IL polar functional groups. Higher...
http://doras.dcu.ie/15401/
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An investigation into the tropospheric chemistry of acidic aerosols and ammonia in the laboratory
(2009)
Townsend, Thomas Michael
An investigation into the tropospheric chemistry of acidic aerosols and ammonia in the laboratory
(2009)
Townsend, Thomas Michael
Abstract:
This thesis describes a broad range of experiments based on an aerosol flow-tube system to probe the interactions between atmospherically relevant aerosols with trace gases. This apparatus was used to obtain simultaneous optical and size distribution measurements using FTIR and SMPS measurements respectively as a function of relative humidity and aerosol chemical composition. Heterogeneous reactions between various ratios of ammonia gas and acidic aerosols were studied in aerosol form as opposed to bulk solutions. The apparatus is unique, in that it employed two aerosol generation methods to follow the size evolution of the aerosol while allowing detailed spectroscopic investigation of its chemical content. A novel chemiluminescence apparatus was also used to measure [NH4+]. SO2.H2O is an important species as it represents the first intermediate in the overall atmospheric oxidation process of sulfur dioxide to sulfuric acid. This complex was produced within gaseous, aqueous and aero...
http://hdl.handle.net/10468/192
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Photochromic imidazolium based ionic liquids based on spiropyran
(2010)
Coleman, Simon; Byrne, Robert; Alhashimy, Nameer; Fraser, Kevin J.; MacFarlane, Douglas...
Photochromic imidazolium based ionic liquids based on spiropyran
(2010)
Coleman, Simon; Byrne, Robert; Alhashimy, Nameer; Fraser, Kevin J.; MacFarlane, Douglas R.; Diamond, Dermot
Abstract:
We investigate the physicochemical properties of a novel imidazolium benzospiropyran derivative{,} SPIm{,} in imidazolium based ionic liquids (ILs). SPIm was prepared through alkylation of an imidazole to the photoswitchable compound and this derivative was characterised in imidazolium based ILs with increasing chain length to examine the stability of its merocyanine (MC) and spiropyran (SP) forms and compared to standard spiropyran{,} BSP. The rate of thermal relaxation of the new derivative is found to be about ten times faster than that of BSP as reflected in rates of 13.9 [times] 10-3 s-1 and 1.0 [times] 10-3 s-1 for SPIm and BSP{,} respectively{,} in [C6mIm][NTf2]. Since ILs are believed to form nano-structured domains it is proposed that the covalent attachment of the imidazolium side group of SPIm fully integrates the photoswitchable moiety into the non-polar region through side-chain association. In contrast{,} unbound BSP is relatively free to migrate between both polar and...
http://doras.dcu.ie/15403/
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Broadband optical cavity absorption spectroscopy in the near-ultraviolet: applications in atmospheric chemistry
(2011)
Chen, Jun
Broadband optical cavity absorption spectroscopy in the near-ultraviolet: applications in atmospheric chemistry
(2011)
Chen, Jun
Abstract:
A novel spectroscopic method, incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS), has been modified and extended to measure absorption spectra in the near-ultraviolet with high sensitivity. The near-ultraviolet region extends from 300 to 400 nm and is particularly important in tropospheric photochemistry; absorption of near-UV light can also be exploited for sensitive trace gas measurements of several key atmospheric constituents. In this work, several IBBCEAS instruments were developed to record reference spectra and to measure trace gas concentrations in the laboratory and field. An IBBCEAS instrument was coupled to a flow cell for measuring very weak absorption spectra between 335 and 375 nm. The instrument was validated against the literature absorption spectrum of SO2. Using the instrument, we report new absorption cross-sections of O3, acetone, 2-butanone, and 2-pentanone in this spectral region, where literature data diverge considerably owing to the extre...
http://hdl.handle.net/10468/435
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Investigating nano-structuring within imidazolium ionic liquids: A thermodynamic study using photochromic molecular probes
(2009)
Coleman, Simon; Byrne, Robert; Minkovska, Stela; Diamond, Dermot
Investigating nano-structuring within imidazolium ionic liquids: A thermodynamic study using photochromic molecular probes
(2009)
Coleman, Simon; Byrne, Robert; Minkovska, Stela; Diamond, Dermot
Abstract:
Following previous studies involving the thermal relaxation of spirocyclic compounds we extended our studies to investigate the formation of nano-structured domains in ionic liquids (ILs). Two compounds, spiropyran (BSP) and spirooxazine (SO) were added to imidazolium cation based ionic liquids with increasing chain lenghts (C2 –C12). Increasing side-chain length was found to have only minor effects on the rate of thermal relaxation of BSP and SO. BSP was found to be a suitable probe molecule as linear correlations in parameters were observed for this compound. This is believed to be due to the fact that BSP-IL interactions were based on hydrogen bonding between MCBSP and the cation compared to MCSO which is limited to electrostatic interactions thus enhancing the sensitivity of MCBSP to the charged polar regions. Increasing the side-chain of the cation resulted in slight increases in MC-BSP activation energy from 96.93 kJ.mol-1 in [C4mIm][NTf2] to 105.27 kJ.mol-1 in [C12mIm][NTf2]....
http://doras.dcu.ie/16121/
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Influence of plasma chemistry on oxygen triplets
(2011)
Milosavljevic, Vladimir; Ellingboe, Albert; Daniels, Stephen
Influence of plasma chemistry on oxygen triplets
(2011)
Milosavljevic, Vladimir; Ellingboe, Albert; Daniels, Stephen
Abstract:
The plasma chemistry of fluorocarbon-oxygen-argon discharges and its influence on prominent oxygen triplets are studied. The oxygen 777 triplet is very important for the measurement of atomic oxygen in low pressure plasmas, since the 777.417 nm spectral line is frequently used for actinometry. In this paper we identify changes in the individual 777 triplet lines arising from cascade effects from higher energy levels of oxygen, and from resonant energy transfer from energetic carbon atoms in carbon-rich plasmas. The lower energy levels of three oxygen triplets (544 nm, 616 nm, 645 nm) are the upper states of the 777 triplet. Increased emission intensity from the 544, 616, and 645 triplets result in changes to the relative intensity of the individual lines of the 777 triplet, and this can lead to errors in using the 777 triplet, e.g. for actinometry. Also, in operational conditions with strong carbon emission (around 601 nm), the relative intensity of the individual oxygen 777 lines...
http://doras.dcu.ie/16646/
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Photopatternable ionogels for electrochromic applications
(2011)
Kavanagh, Andrew; Copperwhite, Robert; Oubaha, Mohamed; Owens, Jessica; McDonagh, Colet...
Photopatternable ionogels for electrochromic applications
(2011)
Kavanagh, Andrew; Copperwhite, Robert; Oubaha, Mohamed; Owens, Jessica; McDonagh, Colette; Diamond, Dermot; Byrne, Robert
Abstract:
This work describes the development of photopatternable ionogels based on a hybrid organic/inorganic sol–gel material and both phosphonium (trihexyltetradecylphosphonium dicyanamide [P6,6,6,14][dca], trihexyltetradecylphosphonium bis(trifluoromethanesulfonyl)-amide [P6,6,6,14][NTf2]) and imidazolium (1-ethyl-3-methylimidazolium tris(pentafluoroethyl)trifluorophosphate [emIm][FAP]) room temperature ionic liquids (RTILs). Ionogels were prepared via a two step process with the RTIL content varied between 40 and 80 w/w%, and characterised via Raman and Electrochemical Impedance Spectroscopy. 1 and 2 photon polymerisation was performed on the hybrid ionogels using photolithography, resulting in three dimensional structures that were characterised using scanning electron microscopy. Electrochromic ionogels were prepared by addition of ethyl viologen dibromide (EV) to an ionogel containing [emIm][FAP] and hybrid sol–gel material. This composition was photopolymerised on ITO electrodes by ...
http://doras.dcu.ie/16364/
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Graphene-doped photo-patternable ionogels: tuning of conductivity and mechanical stability of 3D microstructures
(2012)
Oubaha, Mohamed; Kavanagh, Andrew; Gorin, Arnaud; Bickauskaite, Gabija; Byrne, Robert; ...
Graphene-doped photo-patternable ionogels: tuning of conductivity and mechanical stability of 3D microstructures
(2012)
Oubaha, Mohamed; Kavanagh, Andrew; Gorin, Arnaud; Bickauskaite, Gabija; Byrne, Robert; Farsari, Maria; Winfield, Richard; Diamond, Dermot; McDonagh, Colette; Copperwhite, Robert
Abstract:
This work reports for the first time the development of enhanced conductivity, graphene- doped photo-patternable hybrid organic-inorganic ionogels and the effect of the subsequent materials condensation on the conductivity and mechanical stability of three- dimensional microstructures fabricated by multi-photon polymerisation (MPP). Ionogels were based on photocurable silicon/zirconium hybrid sol-gel materials and phosphonium (trihexyltetradecylphosphonium dicyanamide [P6,6,6,14][DCA] ionic liquid (IL). To optimise the dispersion of graphene within the ionogel matrices, aqueous solutions of graphene were prepared, as opposed to the conventional graphene powder approach, and employed as catalysts of hydrolysis and condensation reactions occurring in the sol-gel process. Ionogels were prepared via a two step process by varying the hydrolysis degree from 25 to 50%, IL content between 0-50 w/w%, and the inorganic modifier (zirconate complex) concentration from 30 to 60 mol.% against the...
http://doras.dcu.ie/16962/
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Optical and electrochemical transduction of calixarene host-guest chemistry
(1996)
Grady, Teresa
Optical and electrochemical transduction of calixarene host-guest chemistry
(1996)
Grady, Teresa
Abstract:
The well-known selective receptor properties and ease of structural modification makes calixarene derivatives attractive materials for use in chemical sensors. This thesis represents a study of the performance of a range of calixarene compounds either as the active component of an optical sensor or as the lonophore in potentiometnc sensors. Determination of enantiomeric purity has become important in recent years due to increasing restrictions on the composition of pharmaceuticals whose efficacy depends on a chiral moiety. With the aim of enantiomeric selectivity, three novel fluorescent calixarenes were synthesised and their interaction with R and S enantiomers of phenylethylamine and norephedrine were investigated Stem-Volmer plots were used to evaluate the calixarenes and from this it was found that the calix[4]arene with a dinaphthylprolinol group attached to the lower nm exhibited the best selectivity of the three compounds investigated. Using this compound it was possible to ...
http://doras.dcu.ie/18784/
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The chemistry of group 6 metal carbonyls with N-Donor ligands
(1989)
Hegarty, Cormac
The chemistry of group 6 metal carbonyls with N-Donor ligands
(1989)
Hegarty, Cormac
Abstract:
The behaviour of the photochemically produced tungsten pentacarbonyl is investigated by laser flash photolysis and conventional ultraviolet/visible spectrophotometric methods. Rate constants for their reactions with 2- and 4-picoline and other pyridine derivatives are reported along with their proposed mechanisms. W(CO)5(L) complexes (L = pyridine, 2- or 4-phenylpyridine, or 2,2«dipyridylamine) are synthesised along with 3,6-bis(2-pyridyl)-l,4-dihydro-l,2,4,5-tetrazene derivatives of M(CO)6 (M = Cr, Mo, or W) These complexes are characterised by infrared, ultraviolet/visible, proton nuclear magnetic resonance spectroscopy, and by X-ray diffraction analysis Attempts to synthesise the W(CO)5(L) complexes (L = 2- aminomethylpyridine or bispicoylamine) were also reported The solvatochromie behaviour of these penta and tetra-carbonyl complexes was also investigated.
http://doras.dcu.ie/18842/
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Ground and excited state chemistry of some n-supstituted phthalimides
(1996)
McCormac, Paul B.
Ground and excited state chemistry of some n-supstituted phthalimides
(1996)
McCormac, Paul B.
Abstract:
The synthesis and photochemistry of a number of A/-(2-hydroxyethyl) phthalimides have been investigated. Irradiation of A/-(2-hydroxy-2- phenylethyl)phthaiimide results in rapid photofragmentation to form /V-methylphthalimide and benzaldehyde. This process is unusual as it involves intramolecular proton transfer from a hydroxyl group to an excited state phthalimido carbonyl as opposed to the expected y-hydrogen abstraction processes. The mechanism has been investigated in regard to role of hydroxyl group and the nature of the excited state involved. The scope of the fragmentation has been investigated by synthesising and irradiating a series of A/-(2-hydroxyethyl)phthalimides differing in the substituents located at the carbinyl carbon. Mono- and di- substitution led to products of fragmentation whereas the unsubstituted A/-(2-hydroxyethyl)phthalimide affords no photoproducts even after prolonged irradiation. A mechanism involving an excited state intramolecular proton transfer medi...
http://doras.dcu.ie/19016/
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Azaspiracid Shellfish Poisoning: A Review on the Chemistry, Ecology, and Toxicology with an Emphasis on Human Health Impacts
(2008)
Twiner, M J; Rehmann, N; Hess, P; Doucette, G J
Azaspiracid Shellfish Poisoning: A Review on the Chemistry, Ecology, and Toxicology with an Emphasis on Human Health Impacts
(2008)
Twiner, M J; Rehmann, N; Hess, P; Doucette, G J
Abstract:
Azaspiracids (AZA) are polyether marine toxins that accumulate in various shellfish species and have been associated with severe gastrointestinal human intoxications since 1995. This toxin class has since been reported from several countries, including Morocco and much of western Europe. A regulatory limit of 160 μg AZA/kg whole shellfish flesh was established by the EU in order to protect human health; however, in some cases, AZA concentrations far exceed the action level. Herein we discuss recent advances on the chemistry of various AZA analogs, review the ecology of AZAs, including the putative progenitor algal species, collectively interpret the in vitro and in vivo data on the toxicology of AZAs relating to human health issues, and outline the European legislature associated with AZAs.
http://hdl.handle.net/10793/413
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Optical switching of protein interactions on photosensitive–electroactive polymers measured by atomic force microscopy
(2013)
Gelmi, Amy; Zanoni, Michele; Higgins, Michael; Gambhir, Sanjeev; Officer, David; Diamon...
Optical switching of protein interactions on photosensitive–electroactive polymers measured by atomic force microscopy
(2013)
Gelmi, Amy; Zanoni, Michele; Higgins, Michael; Gambhir, Sanjeev; Officer, David; Diamond, Dermot; Wallace, Gordon
Abstract:
The ability to switch the physico-chemical properties of conducting polymers opens up new possibilities for a range of new applications. Appropriately functionalised materials can provide routes to multi-modal switching, for example in response light and/or electrochemical stimuli; this capability is important in the field of bionics, wherein remote control of the properties of materials opens new possibilities. For example, the ability to actuate a film via photonic stimuli is particularly interesting as it facilitates the modulation of interactions between surface host binding sites and potential guest molecules. In this work, we studied two different poly-terthiophenes: one was functionalized with a spiropyran photoswitch (pTTh-SP) and the second with a non photoswitchable methyl acetate moeity (pTTh-MA). These substrates were exposed to several cycles of illumination with light of different wavelengths and the resulting effect studied with UV-vis spectroscopy, contact angle and ...
http://doras.dcu.ie/17879/
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Regioselective functionalization of tetrabromophenanthroline-ruthenium complexes
(2004)
Rau, Sven; Fischer, Reinald; Jäger, Michael; Schäfer, Bernhard; Meyer, Susann; Kreisel,...
Regioselective functionalization of tetrabromophenanthroline-ruthenium complexes
(2004)
Rau, Sven; Fischer, Reinald; Jäger, Michael; Schäfer, Bernhard; Meyer, Susann; Kreisel, Günter; Görls, Helmar; Rudolf, Manfred; Henry, William; Vos, Johannes G.
Abstract:
Structural, photophysical and -chemical characterisation and reactivity of a novel polypyridyl ruthenium complex based on 3,5,6,8-tetra-bromophenanthroline are discussed. Signal storage at a molecular level is great challenge for chemistry.1 The possibility of connecting different functionalities selectively to one ligand of a metal complex may open the route towards higher integrated molecular units capable of processing various external stimuli in a predesignated order. The implementation of this concept demands ligands with a multitude of potential connecting groups which can selectively be transformed.2 3-bromo- and 3,8-dibromophenanthrolines have proved useful for the preparation of mononuclear3 and multiheteronuclear complexes.4 These systems have found applications ranging from DNA photoprobes5 to metalloligands in catalysis.6 A very useful feature of this bromophenanthroline ruthenium complexes is their susceptibility towards nucleophilic aromatic substitution which is very ...
http://doras.dcu.ie/35/
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A merocyanine-based conductive polymer
(2013)
Wagner, Klaudia; Zanoni, Michele; Elliott, Anastasia B.S.; Wagner, Pawel; Byrne, Robert...
A merocyanine-based conductive polymer
(2013)
Wagner, Klaudia; Zanoni, Michele; Elliott, Anastasia B.S.; Wagner, Pawel; Byrne, Robert; Florea, Larisa; Diamond, Dermot; Gordon, Keith; Wallace, Gordon; Officer, David
Abstract:
We report the first example of a conducting polymer with a merocyanine incorporated into the polymer backbone by electropolymerisation of a spiropyran moiety covalently linked between two alkoxythiophene units. Utilising the known metal coordination capabilities of merocyanines, introduction of cobalt ions into the electropolymerisation led to an enhancement of the conductivity, morphology and optical properties of the polymer films.
http://doras.dcu.ie/18285/
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Ionic liquid modulation of swelling and LCST behavior of nisopropylacrylamide polymer gels.
(2013)
Gallagher, Simon; Kavanagh, Andrew; Ziółkowski, Bartosz; Florea, Larisa; MacFarlane, Do...
Ionic liquid modulation of swelling and LCST behavior of nisopropylacrylamide polymer gels.
(2013)
Gallagher, Simon; Kavanagh, Andrew; Ziółkowski, Bartosz; Florea, Larisa; MacFarlane, Douglas R.; Fraser, Kevin J.; Diamond, Dermot
Abstract:
The physicochemical properties of free-standing cross-linked poly(N-isopropylacrylamide) (pNIPAAM) gels, generated in the presence of the Ionic Liquids (ILs), 1-ethyl-3-methylimidazolium [C2mIm]+ salts of ethylsulfate [EtSO4]-, dicyanamide [DCA]- , bis(trifluoromethylsulfonyl)imide [NTf2]-, and Trihexyltetradecylphosphonium dycanamide ([P6,6,6,14][DCA]) are described. The Lower Critical Solution Temperature (LCST) of the resulting ionogel was found to vary between 24 – 31 oC. The behaviour of swelling is found to be as high as 31.55% (± 0.47, n = 3) from the initial dehydrated state, while 28.04% (± 0.42, n = 3) shrinking from the hydrated swollen state is observed. For ionogels based on the [DCA]- anion an unexpected complete loss of the shrinking behaviour occurs, attributed to water interactions with the nitrile group of the [DCA]- anion. Scanning Electron Microscopy also reveals distinct morphological changes, for example [C2mim][EtSO4] displays a highly porous, nodule type morp...
http://doras.dcu.ie/19705/
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Probing the specific ion effects of biocompatible hydrated choline ionic liquids on lactate oxidase biofunctionality in sensor applications
(2013)
Curto, Vincenzo F.; Scheuermann, Stefan; Owens, Roisin; Ranganathan, Vijayaraghavan; Ma...
Probing the specific ion effects of biocompatible hydrated choline ionic liquids on lactate oxidase biofunctionality in sensor applications
(2013)
Curto, Vincenzo F.; Scheuermann, Stefan; Owens, Roisin; Ranganathan, Vijayaraghavan; MacFarlane, Douglas R.; Benito-Lopez, Fernando; Diamond, Dermot
Abstract:
This paper presents an extended study on the ion effects of a series of biocompatible hydrated choline based ionic liquids (ILs) on lactate oxidase (LOx), an important enzyme in biosensing technology for the in vitro detection of lactic acid. Secondary structural analysis revealed changes in the protein conformation in hydrated ILs, while thermal unfolding/aggregation dynamics showed different profiles in the presence or absence of ILs. Moreover, LOx thermally denaturised at 90 1C showed residual activity in the presence of chloride and dihydrogen phosphate anions. Kinetic and lifetime studies were also performed, providing a better understanding of the ion effects of ILs on the biocatalytic activity of the enzyme.
http://doras.dcu.ie/19709/
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PbO2: from semi-metal to transparent conducting oxide by defect chemistry control
(2013)
WATSON, GRAEME
PbO2: from semi-metal to transparent conducting oxide by defect chemistry control
(2013)
WATSON, GRAEME
Abstract:
Lead dioxide has been studied for over 150 years as a component of the lead-acid battery. Based on first-principles calculations, we predict that by tuning the concentration ofelectrons in the material, through control of the defect chemistry, PbO 2 can be rendered from black to optically transparent, thus opening up applications in the field of optoelectronics
http://hdl.handle.net/2262/66750
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The effects of season, habitat, hydroperiod and water chemistry on the distribution of turlough aquatic invertebrate communities
(2009)
Porst, Gwendolin
The effects of season, habitat, hydroperiod and water chemistry on the distribution of turlough aquatic invertebrate communities
(2009)
Porst, Gwendolin
Abstract:
The aim of this study was to investigate the effects of season, habitat, hydroperiod and water chemistry on the distribution of turlough aquatic invertebrate communities. Twenty-two turloughs, selected as representative of geographical distribution and hydrological conditions were included in the study. A comparative study of eight turloughs representing a nutrient gradient determined macroinvertebrate community distinctiveness in a stratified sampling design and related assemblage structures to environmental variables. Assessment of macroinvertebrate temporal and spatial variation was the objective of separate studies conducted in a subset of four turloughs, varying in hydrological and nutrient regimes. The influence of disturbance and habitat characteristics on macroinvertebrate community dynamics was tested. Across twenty-two turloughs macroinvertebrate and cladoceran zooplankton communities were analysed and their relation to varying trophic, hydrological and morphological regim...
http://hdl.handle.net/2262/61579
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Redox switching and oxygen evolution electrocatalysis in polymeric iron oxyhydroxide films
(2009)
LYONS, MICHAEL EDWARD
Redox switching and oxygen evolution electrocatalysis in polymeric iron oxyhydroxide films
(2009)
LYONS, MICHAEL EDWARD
Abstract:
peer-reviewed
Outstanding issues regarding the redox switching characteristics and the oxygen evolution reaction (OER) electrocatalytic behaviour of multicycled iron oxyhydroxide films in aqueous alkaline solution have been examined. Charge percolation through the hydrous layer has been quantified, using cyclic voltammetry, in terms of a charge transport diffusion coefficient DCT which admits a value of ca. 3 ? 10-10 cm2 s-1. Steady-state Tafel plot analysis and electrochemical impedance spectroscopy have been used to elucidate the kinetics and mechanism of oxygen evolution. Tafel slope values of ca. 60 mV dec-1 and ca. 120 mV dec-1 are found at low and high overpotentials respectively, whereas the reaction order with respect to hydroxide ion activity changes from ca. 3/2 to ca. 1 as the potential is increased. These observations are rationalised in terms of a kinetic scheme involving Temkin adsorption and the rate determining formation of a physisorbed hydrogen peroxide interme...
http://hdl.handle.net/2262/33790
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Understanding the p-Type Conduction Properties of the Transparent Conducting Oxide CuBO2: A Density Functional Theory Analysis
(2009)
WATSON, GRAEME; SCANLON, DAVID
Understanding the p-Type Conduction Properties of the Transparent Conducting Oxide CuBO2: A Density Functional Theory Analysis
(2009)
WATSON, GRAEME; SCANLON, DAVID
Abstract:
CuCrO2 is the most promising Cu-based delafossite for p-type optoelectronic devices. Despite this, little is known about the p-type conduction mechanism of this material, with both CuI/CuII and CrIII/CrIV hole mechanisms being proposed. In this article we examine the electronic structure, thermodynamic stability and the p-type defect chemistry of this ternary compound using density functional theory with three different approaches to the exchange and correlation; the generalized-gradient-approximation of Perdew, Burke and Ernzerhof (PBE), PBE with an additional correction for on-site Coulombic interactions (PBE + U) and the nonlocal, screened-exchange hybrid functional HSE06. The fundamental band gap of CuCrO2 is demonstrated to be indirect in nature. Under all growth conditions, the dominant intrinsic p-type defect will be the Cu vacancy, with hole formation centered solely on the Cu sublattice. Mg doping is found to be significantly lower in energy than intrinsic defect formation,...
http://hdl.handle.net/2262/62905
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Smart polymer surfaces: mapping chemical landscapes on the nanometre scale
(2010)
KOPF, ILONA
Smart polymer surfaces: mapping chemical landscapes on the nanometre scale
(2010)
KOPF, ILONA
Abstract:
We show that Scattering Infrared Near-field Microscopy (SNIM) allows chemical mapping of polymer monolayers that can serve as designed nanostructured surfaces with specific surface chemistry properties on a nm scale. Using s-SNIM a minimum volume of 100 nm 100 nm 15 nm is sufficient for a recording of a ``chemical?? IR signature which corresponds to an enhancement of at least four orders of magnitudes compared to conventional FT-IR microscopy. We could prove that even in cases where it is essentially difficult to distinguish between distinct polymer compositions based solely on topography, nanophase separated polymers can be clearly distinguished according to their characteristic near-field IR response.
http://hdl.handle.net/2262/56529
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Orientational/translational relaxation in aqueous electrolyte solutions : a molecular model for microwave/far-infrared ranges
(2001)
VIJ, JAGDISH KUMAR
Orientational/translational relaxation in aqueous electrolyte solutions : a molecular model for microwave/far-infrared ranges
(2001)
VIJ, JAGDISH KUMAR
Abstract:
A model is given where the complex permittivity of an electrolyte solution is calculated as a superposition of the contributions due to the translation of ions and the reorientation of water molecules, which occur in intermolecular potential wells during the lifetime of local order in liquids. Simple analytical expressions are found for the contributions of cations and anions to the linear-response spectral function. The one-dimensional rectangular potential well with perfectly elastic walls is considered. The contribution of water molecules to the orientational relaxation was calculated in terms of a hybrid model using the approach given recently in a book by Gaiduk (Dielectric Relaxation and Dynamics of Polar Molecules, World Scientific, Singapore, 1999). A modification of this model is also suggested in which the walls of the potential well undergo rather slow vibration. If the angular frequency is much less than the plasma frequency p of an ion, then the theory yields a nearly ...
http://hdl.handle.net/2262/40307
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Exploring the coordination chemistry of bifunctional organoarsonate ligands: Syntheses and characterisation of coordination polymers that contain 4-(1,2,4-triazol-4-yl)phenylarsonic acid
(2014)
VENKATESAN, MUNUSWAMY
Exploring the coordination chemistry of bifunctional organoarsonate ligands: Syntheses and characterisation of coordination polymers that contain 4-(1,2,4-triazol-4-yl)phenylarsonic acid
(2014)
VENKATESAN, MUNUSWAMY
Abstract:
This account describes the coordination chemistry of a novel bifunctional arsonic acid ligand, 4-(1,2,4-triazol-4-yl)phenylarsonic acid (H2TPAA) that contains a triazole group. Hydrothermal reactions of transition metal salts with H2TPAA produced five unprecedented coordination polymers: [Co(H2TPAA)(HTPAA)2]?H2O (1), M(HTPAA)Cl?2H2O (M = Cu (2), Co (3)) and M(HTPAA)2 (M = Mn (4), Cd (5)). These five polymers have been fully characterized by single crystal and powder X-ray diffraction, thermogravimetric analysis, infra-red spectroscopy and elemental analysis. Single crystal X-ray diffraction reveals that 1, 2 and 3 adopt 2-D layered structural motifs whereas 4 and 5 are 3-D frameworks. 1 and 3 are the first examples of arsonate-stabilised cobalt(II) coordination polymers. Likewise, 4 is recognised as the first record of a MnII arsonate coordination polymer with 3-D framework topology. Its isostructural Cd analogue 5 shows characteristic ligand-centered fluorescence properties. Magnet...
http://hdl.handle.net/2262/73308
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