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The influence of surface chemistry of activated carbons on the selective decomposition of hydrogen peroxide

Ribeiro, Rui; Silva, Ádrian; Figueiredo, José; Faria, Joaquim; Gomes, Helder
Fonte: Instituto Politécnico de Bragança Publicador: Instituto Politécnico de Bragança
Tipo: Conferência ou Objeto de Conferência
ENG
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Activated carbons can act as metal free catalysts on wet peroxide oxidation to generate the highly reactive HO• by means of H2O2 decomposition. To quantify the yield of HO• formed during the process (YHO•) the consumption of H2O2 and the oxygen formation were measured in experiments performed with and without an HO• scavenger. After 150 min of reaction, at T = 323 K, pH = 3 and catalyst load = 0.1 g L-1, the highest YHO• was obtained for the catalyst with higher surface basicity, obtained from the successive modification of the original activated carbon with nitric acid oxidation, hydrothermal treatment with urea and gas-phase thermal treatment under a N2 flow. A linear correlation between YHO• and the concentration of basic active sites at the carbons surface was obtained.

Sílicas e carbonos mesoestruturados organofuncionalizados e aplicação à liberação controlada de fármacos; Mesostructured organofunctionalized silicas and carbons and application to controlled release drug delivery

Ramon Kenned de Sousa Almeida
Fonte: Biblioteca Digital da Unicamp Publicador: Biblioteca Digital da Unicamp
Tipo: Tese de Doutorado Formato: application/pdf
Publicado em 27/08/2012 PT
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As sílicas mesoporosas SBA-15 e SBA-16 sintetizadas através do método hidrotérmico com os copolímeros direcionadores de estrutura P123 e F127 foram organofuncionalizadas com agentes sililantes que contêm grupos funcionais, como nitrogênio, oxigênio e enxofre. As sílicas foram caracterizadas por análise elementar, espectroscopia na região do infravermelho, ressonância magnética nuclear de carbono e silício no estado sólido, termogravimetria, área superficial, espalhamento de raios X a baixo ângulo, microscopia eletrônicas de varredura e transmissão. As caracterizações comprovam a efetivação das sínteses das sílicas SBA-15 e SBA-16 com estruturas hexagonal e cúbica, respectivamente. As sílicas organofuncionalizadas, mostraram maiores graus de ancoramento obtido quando funcionalizadas com organossilanos contendo nitrogênio. Além das sílicas, foram sintetizados carbonos mesoporosos usando as sílicas como direcionadores rígidos de estrutura. Os mesmos foram funcionalizados com anidrido malêico e subsequentes reações com água e hidreto de alumínio e lítio resultando em grupos carboxílicos e na redução dos mesmos, respectivamente. A efetividade da funcionalização foi comprovada, sobretudo por espectroscopia na região do infravermelho...

Influence of hydrocarbonization conditions on the porosity of derived carbon dioxide activated carbons

Roman, Silvia; Ledesma, Beatriz; Nabais, Joao; Laginhas, Carlos
Fonte: Universidade de Évora Publicador: Universidade de Évora
Tipo: Artigo de Revista Científica
POR
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Influence of hydrocarbonization conditions on the porosity of derived carbon dioxide activated carbons

Characterization of the Surface of Activated Carbons Produced from Tire Residues

Valente Nabais, Joao; Laginhas, Carlos; Carrott, Peter; Carrott, Manuela; Galacho, Cristina; Crespo Amoros, Jose; Nadal Gisbert, Antonio
Fonte: Materials Science Forum Publicador: Materials Science Forum
Tipo: Artigo de Revista Científica
ENG
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The surface characterisation of new activated carbons produced from tire residues by activation with carbon dioxide was studied. The activated carbons produced were mainly basic with point of zero charge values above 8.8. The main surface functional groups identified by FTIR were ether, quinones, lactones, ketones, hydroxyls (free and phenol) and pyrones. The XRD analysis shows that the materials produced have a microstructural organisation with microcrystallite height around 1.5nm and width from 3 to 5.3nm. This analysis indicates also the possible presence of oxides (single or mixture) of the following heteroatoms: Fe, Al, Ca, Mg, Ti, Si, K, Pb, Cd, Ba, Zn and Sn. The results have shown the significant potential of this type of residues for activated carbon production. Furthermore, the environment friendly use of an industrial residue is also noteworthy.

Porosity Development in Activated Carbons Prepared from Walnut Shells by Carbon Dioxide or Steam Activation

Roman, Silvia; Gonzalez, Jose; Garcia, Carmen; Valente Nabais, Joao; Ortiz, Antonio
Fonte: Ind. Eng. Chem. Res. Publicador: Ind. Eng. Chem. Res.
Tipo: Artigo de Revista Científica
ENG
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The influence of carbon dioxide and steam as activating agents on the porosity development of activated carbons produced from walnut shells was investigated. The study was made covering a wide range of burnoff (12-76%) and employing different temperatures and times: in carbon dioxide activation, 850 °C varying the activation time in the range 60-480 min, and in steam activation, 700, 850, and 900 °C (for 30-120 min). It was found that the gasifying agent has a profound influence on the activated carbon porosity development. First, steam is more reactive and produces, in general, activated carbons with greater N2 adsorption capacity. Second, the increase in the fraction of mesopores with activation time is more pronounced for steam. While steam generates micro-, meso-, and macropores from the early stages of the process, carbon dioxide produces highly microporous carbons, with broadening of the microporosity only for long activation times.

Phenol removal onto novel activated carbons made from lignocellulosic precursors: Influence of surface properties

Valente Nabais, Joao; Gomes, Jose; Suhas, Suhas; Carrott, Peter; Laginhas, Carlos; Roman, Silvia
Fonte: Journal of Hazardous Materials Publicador: Journal of Hazardous Materials
Tipo: Artigo de Revista Científica
ENG
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The adsorption of phenol from dilute aqueous solutions onto new activated carbons (AC) was studied. The novel activated carbon was produced from lignocellulosic (LC) precursors of rapeseed and kenaf. Samples oxidised with nitric acid in liquid phasewere also studied. The results have shown the significant potential of rapeseed and kenaf for the activated carbon production. The activated carbons produced by carbon dioxide activation were mainly microporous with BET apparent surface area up to 1350m2 g−1 and pore volume 0.5cm3 g−1. The effects of concentration (0.1–2mM) and pH (3–13) were studied. The phenol adsorption isotherms at 25 ◦C followed the Freundlichmodel withmaximumadsorption capacities of approximately 80 and 50mgg−1 for the pristine and oxidised activated carbons, respectively. The influence of pH on the adsorption has two trends for pH below and above 10. It was possible to conclude that when phenol is predominantly in the molecular form the most probable mechanism is based on the – dispersion interaction between the phenol aromatic ring and the delocalised electrons present in the activated carbon aromatic structure. When phenolate is the major component the electrostatic repulsion that occurs at high pH values is the most important aspect of the adsorption mechanism.

Decolourisation of a pulp mill effluent using commercial activated carbons

Valente Nabais, Joao; Carrott, Peter; Carrott, Manuela; Marques, Lilinana
Fonte: The British Carbon Group Publicador: The British Carbon Group
Tipo: Artigo de Revista Científica
ENG
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The decolourisation of industry effluents is a challenging and fundamental task related to pollution control, mainly in pulp mill and textile industries. The dark colour of the pulp mill effluent, depending on the river characteristics, can lead to the reduction of the light penetration into the aquatic environment with the consequent decrease of photosynthesis and aquatic life destruction. Also, the lignocelulosic material deposited on the margins and river bed can lead to a large depletion of the dissolved oxygen with the creation of anaerobic conditions that can give rise to the death of aquatic organisms (Ali, 2001). The chemical composition of the pulp mill effluent (referred as effluent) is very complex. Nevertheless, we can say that the lignin and tannin compounds are the main causes for the effluent´s dark brown colour. Among these compounds we can find hidroxyphenyl, siringyl and guaiacyl complexes (Mohan, 1997). These compounds are chemically stable, resistant to biodegradation and extremely difficult to separate by most methods in cost effective processes, such as membrane adsorption (Mutlu, 2002), cationic coagulants, ultrafiltration (Mutlu, 2002) and chemical oxidation (Malik, 2004). One of the most promising methods is the use of activated carbons for the removal of the effluent colour. In this work the use of 5 commercial activated samples with different shapes...

Production and characterisation of activated carbons made from coffee industry residues

Valente Nabais, Joao; Carrott, Manuela; Carrott, Peter; Luz, vania; Ortiz, Angel
Fonte: The British Carbon Group Publicador: The British Carbon Group
Tipo: Artigo de Revista Científica
POR
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Porous materials are usually heterogeneous both structurally and energetically. Activated carbon fibres (ACFs) are relatively novel fibrous adsorbents produced for example from pith, cellulose, lignocellulose, phenol resin and polyacrylonityile (Peebles, 1995; Ryu, 1999). ACFs show important advantages with respect to conventional activated carbons. Among these advantages it is worth noting their high adsorption capacity and easiness to handle. Their main inconvenience lays on the difficulty of choosing adequate activating agents and activation conditions that are required in order to maintain the fibrous morphology. The adsorption capacity of ACFs depends on many factors, such as raw materials, activation process, pore structure and surface functionalities (Suffet, 1981; Park, 1999). Surface roughness is an important factor that influences the adsorption properties of an activated carbon. Fractal dimension is a measure of roughness of a surface. The use of the fractal concept is becoming very popular as a tool to characterize the texture of complex materials, such as porous solids. The fractal properties of these porous systems were determined by means of several techniques such as gas adsorption, mercury porosimetry and Small-Angle X-Ray Scattering (SAXS and SANS). Kenaf is an herbaceous annual plant that belongs to the family of Malvaceae. Kenaf possesses both...

Study of the contributions of non-specific and specific interactions during fluoxetine adsorption onto activated carbons

Valente Nabais, Joao; Roman, Silvia; Gonzalez, Juan; Garcia, Carmen; Ortiz, Angel
Fonte: Clean – Soil, Air, Water Publicador: Clean – Soil, Air, Water
Tipo: Artigo de Revista Científica
ENG
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The adsorption of fluoxetine onto activated carbons (ACs) prepared from almond tree pruning by steam and CO2 activation under different temperature conditions (650– 9508C), was studied. In both series increasing the temperature caused an increase in the BET apparent surface area, yielding ACs with SBET up to 870 and 710m2 g 1 after steam and CO2 activation, respectively. Also, a slight widening of the porosity was found in both cases. In order to modify the functionality of the ACs, two of them were impregnated with triethylenediamine (TEDA) prior to the adsorption process, which caused a decrease in the AC apparent surface mainly due to micropore blockage. The fluoxetine adsorption isotherms at 258C showed maximum adsorption capacities between 110 and 224mgg 1. The adsorption isotherms were analyzed using Langmuir and Freundlich models. Although the impregnation reduced the pore volume, it did not cause a decrease in the fluoxetine maximum adsorption capacity, but a modification in the adsorption mechanism was observed.

Removal of amitriptyline from aqueous media using activated carbons

Valente Nabais, Joao; Ledesma, Beatriz; Laginhas, Carlos
Fonte: Adsorption Science and Technology Publicador: Adsorption Science and Technology
Tipo: Artigo de Revista Científica
ENG
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This paper reports the removal of amitriptyline, a widely used tricyclic anti-depressant, from aqueous solutions by six activated carbons produced from cork, coffee endocarp and eucalyptus pulp. The results of this study showed that samples from cork and eucalyptus pulp, activated at 800 °C, exhibited the highest adsorption capacity of 120 mg/g and 110 mg/g, respectively. Samples produced from coffee endocarp showed the lowest capacity. Amitriptyline adsorption was almost independent of the pH of the solution and occurred via three different mechanisms based on the dispersive and chemical interactions between amitriptyline molecules and the carbon surface.

Production and characterization of activated carbons made from sunflower stems

Valente Nabais, Joao; Laginhas, Carlos; Carrott, Peter; Ribeiro Carrott, Manuela
Fonte: 37th RIA Publicador: 37th RIA
Tipo: Artigo de Revista Científica
ENG
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Activated carbons (ACs) are artificial materials, prepared from natural or synthetic precursors that are worldwide extensively used. The ACs main characteristics are the noticeable adsorption capabilities provided by the highly developed porous structure and the rich surface chemistry. Because of their versatility and properties the final material can be tailored to have specific properties suitable for a wide range of applications such as medical uses, gas storage, removal of pollutants and odours, gas separation and purification as well as in catalysis. With the increase of activated carbon demand, one of the main challenges lies in the attempt to find new precursors, which are cheap and accessible with good valorisation potential, like industrial and agricultural residues. In the present work we report the production of ACs from sunflower stems, an agricultural by-product, through a physical activation process by CO2 and H2O, using a single step carbonisation at 400ºC, which as far as it came to our knowledge was never made for this precursor.

Pt-Ru Catalysts supported on mesoporous carbons for polymer electrolyte membrane fuel cells

Calderon, J. C.; Figueiredo, J. L.; Mahata, N.; Pereira, M. F. R.; Fernandes, Vitor R.; Rangel, C. M.; Pastor, E.; Calvillo, L.; Lázaro, M. J.
Fonte: Laboratório Nacional de Energia e Geologia Publicador: Laboratório Nacional de Energia e Geologia
Tipo: Conferência ou Objeto de Conferência
Publicado em 19/04/2010 ENG
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Pt-Ru electrocatalysts supported on xerogels and CMK-3 ordered mesoporous carbons were synthesized by reduction with formate ions (SFM method). Some of the carbon supports were chemically treated with HNO3 in order to generate oxygen groups on the surface, while other supports were heat treated. Physical characterization of the catalyst was obtained using X-ray dispersive energy (EDX) and X-ray diffraction (XRD) techniques. Results showed that Pt-Ru catalysts with similar metal content (20%) and atomic ratios (Pt:Ru 1:1) were obtained. The electrochemical activity was studied by cyclic voltammetry and chronoamperometry. Higher methanol oxidation current densities were found for catalyst deposited on chemically treated supports. Electrode preparation and MEA assembly allowed an in-house built direct methanol fuel to be fitted with the synthesized catalysts and supports in order to assess their performance. Cell and reactants were conditioned by a direct methanol test station. Polarisation curves were measured and confirmed data obtained by voltammetry, regarding the effect of heat treatment of the carbon support. Normalised power curves per weight of catalyst are discussed in terms of the significant impact on noble metal loading and attained cell maximum power...

Contribution to the study of the formation mechanism of ordered porous carbons from a soft-template method using the copolymer triblock (PEO140PPO39PEO140) and a phenolic resin

Santa,Cristiam F.; Sierra,Ligia
Fonte: Sociedade Brasileira de Química Publicador: Sociedade Brasileira de Química
Tipo: Artigo de Revista Científica Formato: text/html
Publicado em 01/12/2011 EN
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Different porous carbons were synthesized using direct self-assembly of a nonionic surfactant (PEO140PPO39PEO140, PEO poly(ethylene oxide) and PPO poly(propylene oxide)) and a phenolic resin. According to dynamic light scattering (DLS) experiments realized before the flocculation, the formation of covered hybrid micelles (precursors of ordered mesoporous materials) competes with the formation of resol particles depending on the surfactant concentration. High synthesis temperature increases the formation of mesoporosity. When monomers (instead of oligomers) are used as resin precursors, the mesoporosity is also enhanced. However in this case, the formation of resol particles is also favored. The obtained materials are mainly microporous, indicating that the formed polymer/surfactant hybrid micelles are not stable enough to template the formation of highly mesoporous carbons. Appropriate interaction between the surfactant micelles and resin precursor species, as well as the polymerization degree of the resin, is crucial for obtaining polymer/surfactant hybrid micelles that conduce to mesoporous carbons.

A pore network model for diffusion in nanoporous carbons: Validation by molecular dynamics simulation

Cai, Q.; Buts, A.; Seaton, N.; Biggs, M.
Fonte: Pergamon-Elsevier Science Ltd Publicador: Pergamon-Elsevier Science Ltd
Tipo: Artigo de Revista Científica
Publicado em //2008 EN
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A hybrid molecular dynamics simulation/pore network model (MD/PNM) approach is developed for predicting diffusion in nanoporous carbons. This approach is computationally fast, and related to the structure of the real material. The PNM takes into account both the geometrical (a distribution of pore sizes) and topological (the pore network connectivity) characteristics of nanoporous carbons, which are obtained by analysing adsorption data. The effective diffusion coefficient is calculated by taking the transport diffusion coefficients in single slit-shaped model pores from MD simulation and then computing the effective value over the PNM. The reliability of this approach is evaluated by comparing the results of the PNM analysis with a more rigorous, but much slower, simulation applied to a realistic model material, the virtual porous carbon (VPC). We obtain good agreement between the diffusion coefficients for the PNM and the VPC, indicating the reliability of the hybrid MD/PNM method and it can be used in industry for materials design; Q. Cai, A. Buts, N.A. Seaton and M.J. Biggs; Copyright © 2008 Elsevier Ltd

Virtual porous carbons: what they are and what they can be used for

Biggs, M.; Buts, A.
Fonte: Taylor & Francis Ltd Publicador: Taylor & Francis Ltd
Tipo: Artigo de Revista Científica
Publicado em //2006 EN
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We use the term “virtual porous carbon” (VPC) to describe computer-based molecular models of nanoporous carbons that go beyond the ubiquitous slit pore model and seek to engage with the geometric, topological and chemical heterogeneity that characterises almost every form of nanoporous carbon. A small number of these models have been developed and used since the early 1990s. These models and their use are reviewed. Included are three more detailed examples of the use of our VPC model. The first is concerned with the study of solid-like adsorbate in nanoporous carbons, the second with the absolute assessment of multi-isotherm based methods for determining the fractal dimension, and the final one is concerned with the fundamental study of diffusion in nanoporous carbons.; M. J. Biggs and A. Buts

Polyethyleneimine functionalized nano-carbons for the absorption of carbon dioxide

Dillon, Eoghan P.
Fonte: Universidade Rice Publicador: Universidade Rice
ENG
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The evolution of nanotechnology over the past 20 years has allowed researchers to use a wide variety of techniques and instruments to synthesize and characterize new materials on the nano scale. Due to their size, these nano materials have a wide variety of interesting properties, including, high tensile strength, novel electronic and optical properties and high surface areas. In any absorption system, a high surface areas is desirable, making carbon nano materials ideal candidates for use in absorption systems. To that end, we have prepared a variety of nano carbons, single walled carbon nanotubes, multi walled carbon nanotubes, graphite intercalation compounds, graphite oxide, phenylalanine modified graphite and fullerenes, for the absorption of carbon dioxide. These nano carbons are functionalized with the polymer, polyethyleneimine, and fully characterized using Raman spectroscopy, x-ray photoelectron spectroscopy, scanning electron microscopy, atomic force microscopy, solid state 13 C NMR, and thermogravimetric analysis. The carbon dioxide absorption potential of the PEI-nano carbons was evaluated using thermogravimetric analysis at standard room temperature and pressure. We have demonstrated the high gravimetric capacity of carbon dioxide capture on these materials with extremely high capacities for PEI-C 60 .

Correlation between heats of immersion and limiting capacitances in porous carbons

Álvarez Centeno, Teresa; Fernández López, José Antonio; Stoeckli, F.
Fonte: Elsevier Publicador: Elsevier
Tipo: Artículo Formato: 22195 bytes; application/pdf
ENG
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6 pages, 3 figures, 2 tables.-- Printed version published Jun 2008.; Based on more than 80 carbons, the paper shows that immersion calorimetry into benzene, water and carbon tetrachloride can be used to assess with a good accuracy the limiting capacitance Co at low current densities in both acidic (2 M H2SO4) and aprotic (1 M tetraethyl ammonium tetrafluoroborate in acetonitrile) electrolytic solutions. The enthalpies of immersion ΔiH(C6H6) and ΔiH(H2O) provide information on Co-acidic, where both the surface area and the oxygen content play a role. On the other hand, in the case of the organic electrolyte the oxygen content has only a small influence and Co-aprotic is directly related to ΔiH(C6H6) and ΔiH(CCl4). Carbon tetrachloride has a critical dimension (0.65 nm), which is close to the size of the (C2H5)4N+ ion (0.68 nm) and therefore ΔiH(CCl4) provides better information in the case of carbons with small micropores. The advantage of this approach lies in the fact that immersion calorimetry, in itself a useful tool for the structural and the chemical characterization of carbons, can also be used to evaluate directly the gravimetric capacitances of these solids at low current densities.; Peer reviewed

Synthesis of mesoporous carbons of high surface area and porosity by using polymer blends as template

Lin, Yu-Chien; Wu, Sheng-Ho; Liu, Che-Wei; Lim, Zheng-Yi; Huang, Cheng-Wei; Lin, Hong-Pin; Deng, Shiensen; Yang, Ming-Chang; Tang, Chih-Yuan; Lin, Ching-Yeh
Fonte: Springer Publicador: Springer
Tipo: Artigo de Revista Científica
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In this paper, we provided a new method to generate the carbonizable polymer-silica nanocomposite in one step by using different polymer blends of phenol formaldehyde (PF) and silica-gelling polymer (i.e., Pluronic F127, PEO6000 or gelatin) as the template. The PF-silica gelling polymer-silica nanocomposite was obtained from fast silicification in a highly diluted silica solution at pH∈≈∈5.0. Because the PF, one kind of carbon sources, was embedded in the as-synthesized nanocomposite, the mesoporous carbon was easily obtained from pyrolysis at 1,000°C and silica removal by diluted HF solution. The resulted mesoporous carbons possess a high surface area of 780-1,500 m2 g-1 and large pore size of 2.6-13.7 nm. In addition, the morphology of the mesoporous carbons can be tailored to nano-sized particles and hollow spheres by using different silica gelator-PF polymer blends. In practice, the electrically conducting mesoporous carbons of high surface area and large pore size can be considered as good material for preparing the supercapacitor. The mesoporous carbons exhibit electric capacity of 75-158 Fg-1 in 2.0 M H2SO4 electrolyte solution at scan rate of 1-50 mVs-1.

The influence of the textural properties of activated carbons on acetaminophen adsorption at different temperatures

Galhetas, M.; Andrade, Marta A.; Mestre, A. S.; Kangni-foli, Ekoé; Brito, Maria J. Villa de; Pinto, Moisés L.; Lopes, M. Helena; Carvalho, A. P.
Fonte: Royal Society of Chemistry Publicador: Royal Society of Chemistry
Tipo: Artigo de Revista Científica
Publicado em //2015 ENG
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The influence of temperature (20–40 °C) on the acetaminophen adsorption onto activated carbons with different textures was studied. Different temperature dependences, not explained by kinetic effects, were observed for carbons with different micropore size distribution patterns: adsorption capacity increased for pine gasification residues (Pi-fa) derived carbons and decreased for sisal based materials. No significant variation was seen for carbon CP. The species identified by 1H NMR spectroscopy on the back-extraction solution proved that during the adsorption process exist the conditions required to promote the formation of acetaminophen oligomers which have constrained access to the narrow microporosity. The rotation energy of the dihedral angle between monomers (estimated by electronic DFT methods) showed that conformations in the planar form are less stable than the non-planar conformation (energy barrier of 70 and 23 kJ mol-1), but have critical dimensions similar to the monomer and can access most of the micropore volume. The enthalpy change of the overall process showed that the energy gain of the system (endothermic) for Pi-fa samples (˜40 kJ mol-1) was enough to allow a change in the dimer, or even a larger oligomer...

Oxidative dehydrogenation of ethylbenzene to styrene on activated carbons derived from a native wood as catalyst

de Celis,J.P.; Villaverde,M.S.; Cukierman,A.L.; Amadeo,N.E.
Fonte: Latin American applied research Publicador: Latin American applied research
Tipo: Artigo de Revista Científica Formato: text/html
Publicado em 01/06/2009 EN
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Activated carbons were developed by phosphoric acid activation of a native wood (Prosopis ruscifolia) under a self-generated atmosphere or flowing air. Their potentiality as catalyst for oxidative dehydrogenation of ethylbenzene to styrene was examined at pre-established operating conditions. The carbons developed in the self-generated atmosphere showed specific surface area of 2281 m²/g and total pore volume of 1.7 cm³/g, whereas values of 1638 m²/g and 1.3 cm³/g, respectively, characterized those obtained in air. A commercial activated carbon (1200 m²/g and 0.7 cm³/g) was also used for comparison. Both wood-derived carbons resulted potentially suitable as catalyst for ethylbenzene oxidative dehydrogenation. Nevertheless, those developed in the self-generated atmosphere showed a better catalytic performance than the carbons obtained in air and the commercial sample. The behaviour could be due to its lower microporosity compared with the commercial sample, and to the formation of oxidative condensation products during the oxidative dehydrogenation of ethylbenzene with greater content of carbonyl groups than for the sample activated under flowing air. Chemical and textural characterization of the used carbons conclusively evidenced the presence of oxidative condensation products pointing to formation of new active surfaces.