Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature
Identifieur interne : 000949 ( Main/Exploration ); précédent : 000948; suivant : 000950Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature
Auteurs : Roberto Wojcieszak [Belgique] ; Eric M. Gaigneaux [Belgique] ; Patricio Ruiz [Belgique]Source :
- ChemCatChem [ 1867-3880 ] ; 2013-01.
English descriptors
- Teeft :
- Acidity, Adsorption, Atomic ratio, Carbon number, Catal, Catalyst, Catalyst surface, Catalytic, Catalytic activity, Catalytic test, Catalytic tests, Chem, Chemcatchem, Chemical composition, Chemical properties, Chemical reduction, Chemisorption, Colloid, Colloid interface, Colloids surf, Core levels, Davis method, Formate, Gmbh, Hcho, High selectivity, High temperature, High temperatures, Higher temperature, Hydrazine, Hydrazine reduction, Isotherm, Kgaa, Lowest acidity, Metal nanoparticles, Metal particle size, Metal particles, Methanol, Methanol conversion, Methyl, Methyl formate, Microemulsion, Microemulsion method, Molar ratio, Nanoparticles, Nitrogen concentration, Organic surfactant, Organic surfactants, Oxidized palladium, Palladium, Palladium nanoparticles, Palladium particles, Papers figure, Particle size, Phys, Physical properties, Reaction conditions, Reduction degree, Selectivity, Small metal particles, Small palladium particles, Small particles, Specific surface area, Surface area, Surfactant, Tio2, Tio2 surface, Verlag, Verlag gmbh, Weinheim, Weinheim chemcatchem, Wojcieszak.
Abstract
Palladium nanoparticles of different sizes and supported on TiO2 (2 wt. %) were synthesized by using the water‐in‐oil microemulsion method. The control of palladium nanoparticles was investigated in terms of the nature of organic surfactant and solvent. Attention was paid to the reduction of palladium ions in solution during synthesis. Materials were characterized by N2‐BET at low temperature, XRD, XPS, H2 chemisorption, and TEM and were tested in the gas phase oxidation of methanol. The results confirmed the effect of microemulsion composition on the size of palladium nanoparticles. The direct formation of methyl formate from methanol was observed. Supported palladium catalysts produced methyl formate at low temperature (<150 °C) with a very high selectivity, and, in some cases, a selectivity of approximately 100 %. At higher temperature, methyl formate is not formed at all and the total oxidation to CO2 occurs. A linear correlation between palladium particle size and methanol conversion was observed. Conversion and selectivity were correlated with the acidity of the catalysts. Very small particles were more active but less selective. A mechanism was proposed to explain the formation of methyl formate from methanol.
A real challenge: Very active supported palladium nanoparticles have been used as selective catalysts in the oxidation of methanol to methyl formate in the presence of oxygen, but only at low temperature. At higher temperature, methyl formate is not formed at all and the formation of CO2 is promoted.
Url:
DOI: 10.1002/cctc.201200325
Affiliations:
- Belgique
- Province du Brabant wallon, Région wallonne
- Louvain-la-Neuve
- Université catholique de Louvain
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Le document en format XML
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The control of palladium nanoparticles was investigated in terms of the nature of organic surfactant and solvent. Attention was paid to the reduction of palladium ions in solution during synthesis. Materials were characterized by N2‐BET at low temperature, XRD, XPS, H2 chemisorption, and TEM and were tested in the gas phase oxidation of methanol. The results confirmed the effect of microemulsion composition on the size of palladium nanoparticles. The direct formation of methyl formate from methanol was observed. Supported palladium catalysts produced methyl formate at low temperature (<150 °C) with a very high selectivity, and, in some cases, a selectivity of approximately 100 %. At higher temperature, methyl formate is not formed at all and the total oxidation to CO2 occurs. A linear correlation between palladium particle size and methanol conversion was observed. Conversion and selectivity were correlated with the acidity of the catalysts. Very small particles were more active but less selective. A mechanism was proposed to explain the formation of methyl formate from methanol.</div><div type="abstract" xml:lang="en">A real challenge: Very active supported palladium nanoparticles have been used as selective catalysts in the oxidation of methanol to methyl formate in the presence of oxygen, but only at low temperature. At higher temperature, methyl formate is not formed at all and the formation of CO2 is promoted.</div></front></TEI><affiliations><list><country><li>Belgique</li></country><region><li>Province du Brabant wallon</li><li>Région wallonne</li></region><settlement><li>Louvain-la-Neuve</li></settlement><orgName><li>Université catholique de Louvain</li></orgName></list><tree><country name="Belgique"><region name="Région wallonne"><name sortKey="Wojcieszak, Roberto" sort="Wojcieszak, Roberto" uniqKey="Wojcieszak R" first="Roberto" last="Wojcieszak">Roberto Wojcieszak</name></region><name sortKey="Gaigneaux, Eric M" sort="Gaigneaux, Eric M" uniqKey="Gaigneaux E" first="Eric M." last="Gaigneaux">Eric M. Gaigneaux</name><name sortKey="Ruiz, Patricio" sort="Ruiz, Patricio" uniqKey="Ruiz P" first="Patricio" last="Ruiz">Patricio Ruiz</name><name sortKey="Wojcieszak, Roberto" sort="Wojcieszak, Roberto" uniqKey="Wojcieszak R" first="Roberto" last="Wojcieszak">Roberto Wojcieszak</name><name sortKey="Wojcieszak, Roberto" sort="Wojcieszak, Roberto" uniqKey="Wojcieszak R" first="Roberto" last="Wojcieszak">Roberto Wojcieszak</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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