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1.
Environ Sci Pollut Res Int ; 25(32): 32001-32014, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30215209

RESUMO

The simultaneous photocatalytic removal of nitrate from aqueous environment in presence of organic hole scavenger using TiO2 has long been explored. However, the use of unmodified TiO2 in such reaction resulted in non-performance or release of significant amount of undesirable reaction products in the process, a problem that triggered surface modification of TiO2 for enhanced photocatalytic performance. Previous studies focused on decreasing rate of charge carrier recombination and absorption of light in the visible region. Yet, increasing active sites and adsorption capacity by combining TiO2 with a high surface area adsorbent such as activated carbon (AC) remains unexploited. This study reports the potential of such modification in simultaneous removal of nitrates and oxalic acid in aqueous environment. The adsorptive behaviour of nitrate and oxalic acid on TiO2 and TiO2/AC composites were studied. The Langmuir adsorption coefficient for nitrate was four times greater than that of oxalic acid. However, the amount of oxalic acid adsorbed was about 10 times greater than the amount of nitrate taken up. Despite this advantage, the materials did not appear to produce more active photocatalysts for the simultaneous degradation of nitrate and oxalic acid. The photocatalytic activity of TiO2 and its carbon-based composites was improved by combination with Cu2O particles. Consequently, 2.5 Cu2O/TiO2 exhibited the maximum photocatalytic performance with 57.6 and 99.8% removal of nitrate and oxalic acid, respectively, while selectivity stood at 45.7, 12.4 and 41.9% for NH4+, NO2- and N2, respectively. For the carbon based, 2.5 Cu2O/TiO2-20AC showed removal of 12.7% nitrate and 80.3% oxalic acid and achieved 21.6, 0 and 78.4% selectivity for NH4+, NO2- and N2, respectively. Using the optimal AC loading (20 wt%) resulted in significant decrease in the selectivity for NH4+ with no formation of NO2-, which unveils that selectivity for N2 and low/no selectivity for undesirable products can be manipulated by controlling the rate of consumption of oxalic acid. In contract, no nitrate reduction was observed with Cu2O promoted TiO2-T and its TiO2-(T)-20AC, which may be connected to amorphous nature of TiO2-T and perhaps served as charge carrier trapping sites that impeded activity.


Assuntos
Carvão Vegetal/química , Nitratos/química , Titânio/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Ácido Oxálico , Purificação da Água/instrumentação
2.
Faraday Discuss ; 206: 535-547, 2018 01 01.
Artigo em Inglês | MEDLINE | ID: mdl-28930329

RESUMO

This study reports the behaviour of SCILL based catalysts in the oxidative S-S coupling of aliphatic and aromatic thiols, namely 1-butanethiol and thiophenol, to dibutyl disulfide and diphenyl disulfide. A range of ionic liquids (1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide) and metal supported catalysts (5% Pt/SiO2; 5% Ru/SiO2; 5% Ru/C; 5% Pt/OMS-2) were used to prepare the SCILL catalysts and all were found to be active for the reaction following the trend 5% Pt-OMS-2 > 5% Pt/SiO2 > 5% Ru/C > 5% Ru/SiO2. The presence of SCILL catalysts afforded high selectivity to the disulfide, and the activity of the SCILL catalyst was dependent on the ionic liquid used. A significant increase in the stability of all the supported metal catalysts was found in the presence of the ionic liquid, and there was no change in the selectivity towards disulfides. This demonstrated that the ionic liquids protect the active sites of the catalyst against sulfation, thus providing more stable and active catalysts.

3.
Chem Commun (Camb) ; 52(54): 8335-41, 2016 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-27307017

RESUMO

The Faraday Discussion on the design of new heterogeneous catalysts took place from 4-6 April 2016 in London, United Kingdom. It brought together world leading scientists actively involved in the synthesis, characterisation, modelling and testing of solid catalysts, attracting more than one hundred delegates from a broad spectrum of backgrounds and experience levels - academic and industrial researchers, experimentalists and theoreticians, and students. The meeting was a reflection of how big of an impact the ability to control and design catalysts with specific properties for particular processes can potentially have on the chemical industry, environment, economy and society as a whole. In the following, we give an overview of the topics covered during this meeting and briefly highlight the content of each presentation.

4.
Phys Chem Chem Phys ; 18(26): 17237-43, 2016 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-27052196

RESUMO

Total neutron scattering has been used to follow the hydrogenation of toluene-d8 to methylcyclohexane-d14 over 3 wt% platinum supported on highly ordered mesoporous silica (MCM-41) at 298 K and under 150 mbar D2 pressure. The detailed kinetic information so revealed indicates that liquid reorganisation inside pores is the slowest step of the whole process. Additionally, the results were compared with the reaction performed under 250 mbar D2 pressure as well as with toluene-h8 hydrogenation using D2 at 150 mbar.

5.
Faraday Discuss ; 188: 451-466, 2016 07 04.
Artigo em Inglês | MEDLINE | ID: mdl-27095631

RESUMO

Porous manganese oxide (OMS-2) and platinum supported on OMS-2 catalysts have been shown to facilitate the hydrogenation of the nitro group in chloronitrobenzene to give chloroaniline with no dehalogenation. Complete conversion was obtained within 2 h at 25 °C and, although the rate of reaction increased with increasing temperature up to 100 °C, the selectivity to chloroaniline remained at 99.0%. Use of Pd/OMS-2 or Pt/Al2O3 resulted in significant dechlorination even at 25 °C and 2 bar hydrogen pressure giving a selectivity to chloroaniline of 34.5% and 77.8%, respectively, at complete conversion. This demonstrates the potential of using platinum group metal free catalysts for the selective hydrogenation of halogenated aromatics. Two pathways were observed for the analogous nitrobenzene hydrogenation depending on the catalyst used. The hydrogenation of nitrobenzene was found to follow a direct pathway to aniline and nitrosobenzene over Pd/OMS-2 in contrast to the OMS and Pt/OMS-2 catalysts which resulted in formation of nitrosobenzene, azoxybenzene and azobenzene/hydrazobenzene intermediates before complete conversion to aniline. These results indicate that for Pt/OMS-2 the hydrogenation proceeds predominantly over the support with the metal acting to dissociate hydrogen. In the case of Pd/OMS-2 both the hydrogenation and hydrogen adsorption occur on the metal sites.

6.
Chemphyschem ; 17(13): 2043-55, 2016 07 04.
Artigo em Inglês | MEDLINE | ID: mdl-26990367

RESUMO

Organic solvents, such as cyclohexane, cyclohexene, methylcyclohexane, benzene and toluene, are widely used as both reagents and solvents in industrial processes. Despite the ubiquity of these liquids, the local structures that govern the chemical properties have not been studied extensively. Herein, we report neutron diffraction measurements on liquid cyclohexane, cyclohexene, methylcyclohexane, benzene and toluene at 298 K to obtain a detailed description of the local structure in these compounds. The radial distribution functions of the centres of the molecules, as well as the partial distribution functions for the double bond for cyclohexene and methyl group for methylcyclohexane and toluene have been calculated. Additionally, probability density functions and angular radial distribution functions were extracted to provide a full description of the local structure within the chosen liquids. Structural motifs are discussed and compared for all liquids, referring specifically to the functional group and aromaticity present in the different liquids.

7.
Dalton Trans ; 41(1): 219-27, 2012 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-22101503

RESUMO

Two stable nanofluids comprising of mixed valent copper(I,II) oxide clusters (<1 nm) suspended in 1-butyl-3-methylimidazolium acetate, [C(4)mim][OAc], and copper(II) oxide nanoparticles (<50 nm) suspended in trioctyl(dodecyl)phosphonium acetate, [P(8 8 8 12)][OAc], were synthesised in a facile one-pot reaction from solutions of copper(II) acetate hydrate in the corresponding ionic liquids. Formation of the nanostructures was studied using (13)C NMR spectroscopy and differential scanning calorimetry (DSC). From a solution of Cu(OAc)(2) in 1-ethyl-3-methylimidazolium acetate, [C(2)mim][OAc], crystals were obtained that revealed the structure of [C(2)mim][Cu(3)(OAc)(5)(OH)(2)(H(2)O)]·H(2)O, indicating the formation of copper hydroxo-clusters in the course of the reaction. Synthesised nanostructures were studied using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Physical properties of the prepared IL-nanofluids were examined using IR and UV-VIS spectroscopy, thermogravimetric analysis (TGA), differential scanning calorimetry (DSC) and densitometry.

8.
Chem Commun (Camb) ; 47(23): 6590-2, 2011 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-21573273

RESUMO

Determination of metal oxidation state under relevant working conditions is crucial to understand catalytic behaviour. The reduction behaviour of Pt and Re was evaluated simultaneously as a function of support and solvent in a pressurized reactor (autoclave). The bimetallic catalysts are used in selective hydrogenation of carboxylic acids and amides. Gas phase reduction reduced the metals more efficiently, in particular Pt.


Assuntos
Gases/química , Platina/química , Rênio/química , Amidas/química , Ácidos Carboxílicos/química , Catálise , Hidrogenação , Oxirredução , Pressão , Solventes/química
9.
J Colloid Interface Sci ; 354(2): 511-6, 2011 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-21145558

RESUMO

ZnS nanoparticles were synthesized in four component "water in oil" microemulsions formed by a cationic surfactant (cetyltrimethylammonium bromide, CTAB), a cosurfactant (pentanol or butanol), n-hexane and water. The effect of various parameters (nature of cosurfactant, water/surfactant W(0), and alcohol/surfactant P(0)) on the formation and stability of ZnS nanoparticles was investigated thoroughly. UV-Vis spectroscopy was employed to directly follow the formation of ZnS systems in the microemulsions. Thus, particle size was estimated from the position of the first excitonic transition by employing an approximate finite-depth equation and an empirical correlation, giving average diameters in the ranges 2.3-2.5 and 3.0-3.5nm, respectively. Stable ZnS nanoparticles were obtained by employing low water and high cosurfactant amounts. This suggests that at high concentration the cosurfactant molecules act as capping agents on the surface of the inverse micelles, while low water amounts are needful to obtain water droplets with a radius close to that of the interfacial film spontaneous curvature. HRTEM analysis showed that the samples are formed by a few crystalline ZnS nanoparticles of spherical shape, embedded in and amorphous organic matrix, with a coherent scattering domain between 2 and 4nm.

10.
Chem Commun (Camb) ; 46(34): 6279-81, 2010 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-20664876

RESUMO

Selective hydrogenation of carboxylic acids to alcohols and alkanes has been achieved under remarkably mild reaction temperatures and H(2) pressures (333 K, 0.5 MPa) using Pt/TiO(2) catalyst.


Assuntos
Álcoois/química , Álcoois/síntese química , Ácidos Carboxílicos/química , Platina/química , Titânio/química , Alcanos/síntese química , Alcanos/química , Catálise , Hidrogenação
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