Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature
Identifieur interne : 001462 ( Istex/Corpus ); précédent : 001461; suivant : 001463Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature
Auteurs : Roberto Wojcieszak ; Eric M. Gaigneaux ; Patricio RuizSource :
- 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
Links to Exploration step
ISTEX:C1934926C0A711D65E205437D3C7D3C670621B7ALe 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. 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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. 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<ref target="http://www.tei-c.org/">We use TEI</ref></desc></application></appInfo></encodingDesc><profileDesc><abstract xml:lang="en" style="main"><head>Abstract</head><p>Palladium nanoparticles of different sizes and supported on TiO<hi rend="subscript">2</hi> (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 N<hi rend="subscript">2</hi>‐BET at low temperature, XRD, XPS, H<hi rend="subscript">2</hi> 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 CO<hi rend="subscript">2</hi> 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.</p></abstract><abstract xml:lang="en" style="graphical"><p><hi rend="bold">A real challenge:</hi> 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 CO<hi rend="subscript">2</hi> is promoted.<figure type="box"><media mimeType="image" url="urn:x-wiley:18673880:media:CCTC201200325:content"></media></figure></p></abstract><textClass><keywords xml:lang="en"><term xml:id="kwd1">microemulsion</term><term xml:id="kwd2">nanoparticles</term><term xml:id="kwd3">palladium</term><term xml:id="kwd4">XPS</term></keywords><keywords rend="articleCategory"><term>Full Paper</term></keywords><keywords rend="tocHeading1"><term>Full Papers</term></keywords></textClass><langUsage><language ident="en"></language></langUsage></profileDesc><revisionDesc><change when="2019-12-20" who="#istex" xml:id="pub2tei">formatting</change></revisionDesc></teiHeader></istex:fulltextTEI><json:item><extension>txt</extension><original>false</original><mimetype>text/plain</mimetype><uri>https://api.istex.fr/ark:/67375/WNG-RCXPKD08-0/fulltext.txt</uri></json:item></fulltext><metadata><istex:metadataXml wicri:clean="Wiley, elements deleted: body"><istex:xmlDeclaration>version="1.0" encoding="UTF-8" standalone="yes"</istex:xmlDeclaration><istex:document><component version="2.0" type="serialArticle" xml:lang="en"><header><publicationMeta level="product"><publisherInfo><publisherName>WILEY‐VCH Verlag</publisherName><publisherLoc>Weinheim</publisherLoc></publisherInfo><doi registered="yes">10.1002/(ISSN)1867-3899</doi><issn type="print">1867-3880</issn><issn type="electronic">1867-3899</issn><idGroup><id type="product" value="CCTC"></id></idGroup><titleGroup><title type="main" xml:lang="en" sort="CHEMCATCHEM">ChemCatChem</title><title type="short">ChemCatChem</title></titleGroup></publicationMeta><publicationMeta level="part" position="10"><doi origin="wiley" registered="yes">10.1002/cctc.v5.1</doi><numberingGroup><numbering type="journalVolume" number="5">5</numbering><numbering type="journalIssue">1</numbering></numberingGroup><coverDate startDate="2013-01">January 2013</coverDate></publicationMeta><publicationMeta level="unit" type="article" position="44" status="forIssue"><doi origin="wiley" registered="yes">10.1002/cctc.201200325</doi><idGroup><id type="unit" value="CCTC201200325"></id></idGroup><countGroup><count type="pageTotal" number="10"></count></countGroup><titleGroup><title type="articleCategory">Full Paper</title><title type="tocHeading1">Full Papers</title></titleGroup><copyright ownership="publisher">Copyright © 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim</copyright><eventGroup><event type="manuscriptReceived" date="2012-05-17"></event><event type="manuscriptRevised" date="2012-07-10"></event><event type="xmlConverted" agent="Converter:JWSART34_TO_WML3G version:3.4.1 mode:FullText mathml2tex" date="2015-02-25"></event><event type="xmlConverted" agent="Converter:WILEY_ML3G_TO_WILEY_ML3GV2 version:3.4.1 mode:FullText" date="2015-02-25"></event><event type="publishedOnlineEarlyUnpaginated" date="2012-11-19"></event><event type="publishedOnlineFinalForm" date="2012-12-23"></event><event type="firstOnline" date="2012-11-19"></event><event type="xmlConverted" agent="Converter:WML3G_To_WML3G version:4.6.4 mode:FullText" date="2015-10-02"></event></eventGroup><numberingGroup><numbering type="pageFirst">339</numbering><numbering type="pageLast">348</numbering></numberingGroup><correspondenceTo>Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</correspondenceTo><linkGroup><link type="toTypesetVersion" href="file:CCTC.CCTC201200325.pdf"></link></linkGroup></publicationMeta><contentMeta><countGroup><count type="figureTotal" number="8"></count><count type="tableTotal" number="5"></count><count type="referenceTotal" number="31"></count></countGroup><titleGroup><title type="main" xml:lang="en">Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature</title></titleGroup><creators><creator xml:id="au1" creatorRole="author" affiliationRef="#aa" corresponding="yes"><personName><givenNames>Roberto</givenNames><familyName>Wojcieszak</familyName></personName><contactDetails><email>robert.wojcieszak@uclouvain.be</email></contactDetails></creator><creator xml:id="au2" creatorRole="author" affiliationRef="#aa"><personName><honorifics>Prof. </honorifics><givenNames>Eric M.</givenNames><familyName>Gaigneaux</familyName></personName></creator><creator xml:id="au3" creatorRole="author" affiliationRef="#aa"><personName><givenNames>Patricio</givenNames><familyName>Ruiz</familyName></personName></creator></creators><affiliationGroup><affiliation xml:id="aa" countryCode="BE" type="organization"><unparsedAffiliation>Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</unparsedAffiliation></affiliation></affiliationGroup><keywordGroup xml:lang="en" type="author"><keyword xml:id="kwd1">microemulsion</keyword><keyword xml:id="kwd2">nanoparticles</keyword><keyword xml:id="kwd3">palladium</keyword><keyword xml:id="kwd4">XPS</keyword></keywordGroup><fundingInfo><fundingAgency>Fonds National de la Recherche Scientifique</fundingAgency></fundingInfo><fundingInfo><fundingAgency>Public Fédéral de Programmation Politique Scientifique</fundingAgency></fundingInfo><abstractGroup><abstract type="main" xml:lang="en"><title type="main">Abstract</title><p>Palladium nanoparticles of different sizes and supported on TiO<sub>2</sub> (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 N<sub>2</sub>‐BET at low temperature, XRD, XPS, H<sub>2</sub> 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 CO<sub>2</sub> 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.</p></abstract><abstract type="graphical" xml:lang="en"><p><b>A real challenge:</b> 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 CO<sub>2</sub> is promoted.<blockFixed type="graphic"><mediaResourceGroup><mediaResource alt="image" eRights="yes" copyright="WILEY-VCH" href="urn:x-wiley:18673880:media:CCTC201200325:content"></mediaResource></mediaResourceGroup></blockFixed></p></abstract></abstractGroup></contentMeta></header></component></istex:document></istex:metadataXml><mods version="3.6"><titleInfo lang="en"><title>Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature</title></titleInfo><titleInfo type="alternative" contentType="CDATA" lang="en"><title>Direct Methyl Formate Formation from Methanol over Supported Palladium Nanoparticles at Low Temperature</title></titleInfo><name type="personal"><namePart type="given">Roberto</namePart><namePart type="family">Wojcieszak</namePart><affiliation>Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</affiliation><affiliation>E-mail: robert.wojcieszak@uclouvain.be</affiliation><affiliation>Correspondence address: Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="termsOfAddress">Prof. </namePart><namePart type="given">Eric M.</namePart><namePart type="family">Gaigneaux</namePart><affiliation>Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">Patricio</namePart><namePart type="family">Ruiz</namePart><affiliation>Institute of Condensed Matter and Nanosciences (IMCN), Division “Molecules, Solids and Reactivity (MOST)”, Université catholique de Louvain, Croix du Sud, 2/17, 1348 Louvain la Neuve (Belgique)</affiliation><role><roleTerm type="text">author</roleTerm></role></name><typeOfResource>text</typeOfResource><genre type="article" displayLabel="article" authority="ISTEX" authorityURI="https://content-type.data.istex.fr" valueURI="https://content-type.data.istex.fr/ark:/67375/XTP-6N5SZHKN-D">article</genre><originInfo><publisher>WILEY‐VCH Verlag</publisher><place><placeTerm type="text">Weinheim</placeTerm></place><dateIssued encoding="w3cdtf">2013-01</dateIssued><dateCaptured encoding="w3cdtf">2012-05-17</dateCaptured><copyrightDate encoding="w3cdtf">2013</copyrightDate></originInfo><language><languageTerm type="code" authority="rfc3066">en</languageTerm><languageTerm type="code" authority="iso639-2b">eng</languageTerm></language><physicalDescription><extent unit="figures">8</extent><extent unit="tables">5</extent><extent unit="references">31</extent></physicalDescription><abstract lang="en">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.</abstract><abstract type="graphical" 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.</abstract><note type="funding">Fonds National de la Recherche Scientifique</note><note type="funding">Public Fédéral de Programmation Politique Scientifique</note><subject lang="en"><genre>keywords</genre><topic>microemulsion</topic><topic>nanoparticles</topic><topic>palladium</topic><topic>XPS</topic></subject><relatedItem type="host"><titleInfo><title>ChemCatChem</title></titleInfo><titleInfo type="abbreviated"><title>ChemCatChem</title></titleInfo><genre type="journal" authority="ISTEX" authorityURI="https://publication-type.data.istex.fr" valueURI="https://publication-type.data.istex.fr/ark:/67375/JMC-0GLKJH51-B">journal</genre><subject><genre>article-category</genre><topic>Full Paper</topic><topic>Full Papers</topic></subject><identifier type="ISSN">1867-3880</identifier><identifier type="eISSN">1867-3899</identifier><identifier type="DOI">10.1002/(ISSN)1867-3899</identifier><identifier type="PublisherID">CCTC</identifier><part><date>2013</date><detail type="volume"><caption>vol.</caption><number>5</number></detail><detail type="issue"><caption>no.</caption><number>1</number></detail><extent unit="pages"><start>339</start><end>348</end><total>10</total></extent></part></relatedItem><relatedItem type="references" displayLabel="cit1"><titleInfo><title>Chem. 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