Methanol Steam Reforming over Indium-Promoted Pt/Al2O3 Catalyst: Nature of the Active Surface
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Abstract
The surface state of the Pt/In2O3/Al2O3 catalyst coated onto a microchannel stainless steel reactor was investigated under working conditions using synchrotron-based ambient pressure photoelectron (APPES) and X-ray absorption near-edge structure (XANES) spectroscopies, combined with online mass spectrometry. The surface of the fresh catalyst consists of metallic Pt, In2O3, and Al2O3. Reduction under 0.2 mbar of H2 at 250 °C leads to surface enhancement of Pt and partial reduction of In2O3, while Al2O3 remains unchanged. Reoxidation in O2 atmosphere stimulates surface segregation of In2O3 over Pt, accompanied by partial oxidation of Pt to PtOx. Based on these results a dynamic, gas-phase-dependent surface state is demonstrated. Under methanol steam reforming conditions, the surface state rapidly adapts under the reaction stream regardless of the pretreatment. However, correlation of gas phase with spectroscopic results under working conditions pointed out the beneficial effect of surface indium to reduce the CO selectivity. Finally, evidence of a distorted symmetry of Al sites on Pt/In2O3/Al2O3 catalyst compared to that of γ-Al2O3, is given. The findings obtained in the present study are of fundamental significance in understanding the relation between the surface state and the catalytic performance of a functional methanol reforming catalyst.
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en" level="a">Methanol Steam Reforming over Indium-Promoted Pt/Al<sub>2</sub>O<sub>3</sub> Catalyst: Nature of the Active Surface</title><author><name sortKey="Barbosa, Roland L" uniqKey="Barbosa R">Roland L. Barbosa</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé (ICPEES), UMR 7515 Strasbourg, 25, rue Becquerel</s1><s2>67087 Strasbourg</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ><sZ>10 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Alsace</region><settlement type="city">Strasbourg</settlement></placeName></affiliation></author><author><name sortKey="Papaefthimiou, Vasiliki" uniqKey="Papaefthimiou V">Vasiliki Papaefthimiou</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé (ICPEES), UMR 7515 Strasbourg, 25, rue Becquerel</s1><s2>67087 Strasbourg</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ><sZ>10 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Alsace</region><settlement type="city">Strasbourg</settlement></placeName></affiliation></author><author><name sortKey="Law, Yeuk T" uniqKey="Law Y">Yeuk T. Law</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé (ICPEES), UMR 7515 Strasbourg, 25, rue Becquerel</s1><s2>67087 Strasbourg</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ><sZ>10 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Alsace</region><settlement type="city">Strasbourg</settlement></placeName></affiliation></author><author><name sortKey="Teschner, Detre" uniqKey="Teschner D">Detre Teschner</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Fritz-Haber-Institut der MPG, Faradayweg 4-6</s1><s2>14195 Berlin (Dahlem)</s2><s3>DEU</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>9 aut.</sZ></inist:fA14><country>Allemagne</country><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation></author><author><name sortKey="H Vecker, Michael" uniqKey="H Vecker M">Michael H Vecker</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Fritz-Haber-Institut der MPG, Faradayweg 4-6</s1><s2>14195 Berlin (Dahlem)</s2><s3>DEU</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>9 aut.</sZ></inist:fA14><country>Allemagne</country><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation><affiliation wicri:level="3"><inist:fA14 i1="04"><s1>Helmholtz-Zentrum Berlin/BESSY II, Albert-Einstein-Str. 15</s1><s2>12489 Berlin</s2><s3>DEU</s3><sZ>5 aut.</sZ></inist:fA14><country>Allemagne</country><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation></author><author><name sortKey="Knop Gericke, Axel" uniqKey="Knop Gericke A">Axel Knop-Gericke</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Fritz-Haber-Institut der MPG, Faradayweg 4-6</s1><s2>14195 Berlin (Dahlem)</s2><s3>DEU</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>9 aut.</sZ></inist:fA14><country>Allemagne</country><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation></author><author><name sortKey="Zapf, Ralf" uniqKey="Zapf R">Ralf Zapf</name><affiliation wicri:level="1"><inist:fA14 i1="03"><s1>Institut fur Mikrotech Mainz GmbH IMM</s1><s2>55129 Mainz</s2><s3>DEU</s3><sZ>7 aut.</sZ><sZ>8 aut.</sZ></inist:fA14><country>Allemagne</country><wicri:noRegion>55129 Mainz</wicri:noRegion><wicri:noRegion>Institut fur Mikrotech Mainz GmbH IMM</wicri:noRegion><wicri:noRegion>Institut fur Mikrotech Mainz GmbH IMM</wicri:noRegion></affiliation></author><author><name sortKey="Kolb, Gunther" uniqKey="Kolb G">Gunther Kolb</name><affiliation wicri:level="1"><inist:fA14 i1="03"><s1>Institut fur Mikrotech Mainz GmbH IMM</s1><s2>55129 Mainz</s2><s3>DEU</s3><sZ>7 aut.</sZ><sZ>8 aut.</sZ></inist:fA14><country>Allemagne</country><wicri:noRegion>55129 Mainz</wicri:noRegion><wicri:noRegion>Institut fur Mikrotech Mainz GmbH IMM</wicri:noRegion><wicri:noRegion>Institut fur Mikrotech Mainz GmbH IMM</wicri:noRegion></affiliation></author><author><name sortKey="Schlogl, Robert" uniqKey="Schlogl R">Robert Schlögl</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Fritz-Haber-Institut der MPG, Faradayweg 4-6</s1><s2>14195 Berlin (Dahlem)</s2><s3>DEU</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>9 aut.</sZ></inist:fA14><country>Allemagne</country><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation></author><author><name sortKey="Zafeiratos, Spyridon" uniqKey="Zafeiratos S">Spyridon Zafeiratos</name><affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé (ICPEES), UMR 7515 Strasbourg, 25, rue Becquerel</s1><s2>67087 Strasbourg</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ><sZ>10 aut.</sZ></inist:fA14><country>France</country><wicri:noRegion>67087 Strasbourg</wicri:noRegion><placeName><settlement type="city">Strasbourg</settlement><region type="région" nuts="2">Alsace</region></placeName></affiliation></author></titleStmt><publicationStmt><idno type="inist">13-0338125</idno><date when="2013">2013</date><idno type="stanalyst">PASCAL 13-0338125 INIST</idno><idno type="RBID">Pascal:13-0338125</idno><idno type="wicri:Area/Main/Corpus">000586</idno><idno type="wicri:Area/Main/Repository">000907</idno></publicationStmt><seriesStmt><idno type="ISSN">1932-7447</idno><title level="j" type="abbreviated">J. phys. chem., C</title><title level="j" type="main">Journal of physical chemistry. C</title></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Aluminium oxide</term><term>Catalyst</term><term>Catalytic reforming</term><term>Methanol</term><term>Photoelectron spectrum</term><term>Platinum</term><term>Surface conditions</term><term>Synchrotron radiation</term><term>XANES</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Catalyseur</term><term>Spectre photoélectron</term><term>Rayonnement synchrotron</term><term>XANES</term><term>Reformage catalytique</term><term>Etat surface</term><term>Méthanol</term><term>Oxyde d'aluminium</term><term>Platine</term></keywords><keywords scheme="Wicri" type="concept" xml:lang="fr"><term>Méthanol</term><term>Platine</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">The surface state of the Pt/In<sub>2</sub>O<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst coated onto a microchannel stainless steel reactor was investigated under working conditions using synchrotron-based ambient pressure photoelectron (APPES) and X-ray absorption near-edge structure (XANES) spectroscopies, combined with online mass spectrometry. The surface of the fresh catalyst consists of metallic Pt, In<sub>2</sub>O<sub>3</sub>, and Al<sub>2</sub>O<sub>3</sub>. Reduction under 0.2 mbar of H<sub>2</sub> at 250 °C leads to surface enhancement of Pt and partial reduction of In<sub>2</sub>O<sub>3</sub>, while Al<sub>2</sub>O<sub>3</sub> remains unchanged. Reoxidation in O<sub>2</sub> atmosphere stimulates surface segregation of In<sub>2</sub>O<sub>3</sub> over Pt, accompanied by partial oxidation of Pt to PtO<sub>x</sub>. Based on these results a dynamic, gas-phase-dependent surface state is demonstrated. Under methanol steam reforming conditions, the surface state rapidly adapts under the reaction stream regardless of the pretreatment. However, correlation of gas phase with spectroscopic results under working conditions pointed out the beneficial effect of surface indium to reduce the CO selectivity. Finally, evidence of a distorted symmetry of Al sites on Pt/In<sub>2</sub>O<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst compared to that of γ-Al<sub>2</sub>O<sub>3</sub>, is given. The findings obtained in the present study are of fundamental significance in understanding the relation between the surface state and the catalytic performance of a functional methanol reforming catalyst.</div></front></TEI><inist><standard h6="B"><pA><fA01 i1="01" i2="1"><s0>1932-7447</s0></fA01><fA03 i2="1"><s0>J. phys. chem., C</s0></fA03><fA05><s2>117</s2></fA05><fA06><s2>12</s2></fA06><fA08 i1="01" i2="1" l="ENG"><s1>Methanol Steam Reforming over Indium-Promoted Pt/Al<sub>2</sub>O<sub>3</sub> Catalyst: Nature of the Active Surface</s1></fA08><fA11 i1="01" i2="1"><s1>BARBOSA (Roland L.)</s1></fA11><fA11 i1="02" i2="1"><s1>PAPAEFTHIMIOU (Vasiliki)</s1></fA11><fA11 i1="03" i2="1"><s1>LAW (Yeuk T.)</s1></fA11><fA11 i1="04" i2="1"><s1>TESCHNER (Detre)</s1></fA11><fA11 i1="05" i2="1"><s1>HÄVECKER (Michael)</s1></fA11><fA11 i1="06" i2="1"><s1>KNOP-GERICKE (Axel)</s1></fA11><fA11 i1="07" i2="1"><s1>ZAPF (Ralf)</s1></fA11><fA11 i1="08" i2="1"><s1>KOLB (Gunther)</s1></fA11><fA11 i1="09" i2="1"><s1>SCHLÖGL (Robert)</s1></fA11><fA11 i1="10" i2="1"><s1>ZAFEIRATOS (Spyridon)</s1></fA11><fA14 i1="01"><s1>Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé (ICPEES), UMR 7515 Strasbourg, 25, rue Becquerel</s1><s2>67087 Strasbourg</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ><sZ>10 aut.</sZ></fA14><fA14 i1="02"><s1>Fritz-Haber-Institut der MPG, Faradayweg 4-6</s1><s2>14195 Berlin (Dahlem)</s2><s3>DEU</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>9 aut.</sZ></fA14><fA14 i1="03"><s1>Institut fur Mikrotech Mainz GmbH IMM</s1><s2>55129 Mainz</s2><s3>DEU</s3><sZ>7 aut.</sZ><sZ>8 aut.</sZ></fA14><fA14 i1="04"><s1>Helmholtz-Zentrum Berlin/BESSY II, Albert-Einstein-Str. 15</s1><s2>12489 Berlin</s2><s3>DEU</s3><sZ>5 aut.</sZ></fA14><fA20><s1>6143-6150</s1></fA20><fA21><s1>2013</s1></fA21><fA23 i1="01"><s0>ENG</s0></fA23><fA43 i1="01"><s1>INIST</s1><s2>549C</s2><s5>354000173297730170</s5></fA43><fA44><s0>0000</s0><s1>© 2013 INIST-CNRS. All rights reserved.</s1></fA44><fA45><s0>39 ref.</s0></fA45><fA47 i1="01" i2="1"><s0>13-0338125</s0></fA47><fA60><s1>P</s1></fA60><fA61><s0>A</s0></fA61><fA64 i1="01" i2="1"><s0>Journal of physical chemistry. C</s0></fA64><fA66 i1="01"><s0>USA</s0></fA66><fC01 i1="01" l="ENG"><s0>The surface state of the Pt/In<sub>2</sub>O<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst coated onto a microchannel stainless steel reactor was investigated under working conditions using synchrotron-based ambient pressure photoelectron (APPES) and X-ray absorption near-edge structure (XANES) spectroscopies, combined with online mass spectrometry. The surface of the fresh catalyst consists of metallic Pt, In<sub>2</sub>O<sub>3</sub>, and Al<sub>2</sub>O<sub>3</sub>. Reduction under 0.2 mbar of H<sub>2</sub> at 250 °C leads to surface enhancement of Pt and partial reduction of In<sub>2</sub>O<sub>3</sub>, while Al<sub>2</sub>O<sub>3</sub> remains unchanged. Reoxidation in O<sub>2</sub> atmosphere stimulates surface segregation of In<sub>2</sub>O<sub>3</sub> over Pt, accompanied by partial oxidation of Pt to PtO<sub>x</sub>. Based on these results a dynamic, gas-phase-dependent surface state is demonstrated. Under methanol steam reforming conditions, the surface state rapidly adapts under the reaction stream regardless of the pretreatment. However, correlation of gas phase with spectroscopic results under working conditions pointed out the beneficial effect of surface indium to reduce the CO selectivity. Finally, evidence of a distorted symmetry of Al sites on Pt/In<sub>2</sub>O<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst compared to that of γ-Al<sub>2</sub>O<sub>3</sub>, is given. The findings obtained in the present study are of fundamental significance in understanding the relation between the surface state and the catalytic performance of a functional methanol reforming catalyst.</s0></fC01><fC02 i1="01" i2="X"><s0>001C01A03B</s0></fC02><fC03 i1="01" i2="X" l="FRE"><s0>Catalyseur</s0><s5>02</s5></fC03><fC03 i1="01" i2="X" l="ENG"><s0>Catalyst</s0><s5>02</s5></fC03><fC03 i1="01" i2="X" l="SPA"><s0>Catalizador</s0><s5>02</s5></fC03><fC03 i1="02" i2="X" l="FRE"><s0>Spectre photoélectron</s0><s5>03</s5></fC03><fC03 i1="02" i2="X" l="ENG"><s0>Photoelectron spectrum</s0><s5>03</s5></fC03><fC03 i1="02" i2="X" l="SPA"><s0>Espectro fotoelectrones</s0><s5>03</s5></fC03><fC03 i1="03" i2="X" l="FRE"><s0>Rayonnement synchrotron</s0><s5>04</s5></fC03><fC03 i1="03" i2="X" l="ENG"><s0>Synchrotron radiation</s0><s5>04</s5></fC03><fC03 i1="03" i2="X" l="SPA"><s0>Radiación sincrotrón</s0><s5>04</s5></fC03><fC03 i1="04" i2="3" l="FRE"><s0>XANES</s0><s5>05</s5></fC03><fC03 i1="04" i2="3" l="ENG"><s0>XANES</s0><s5>05</s5></fC03><fC03 i1="05" i2="X" l="FRE"><s0>Reformage catalytique</s0><s5>11</s5></fC03><fC03 i1="05" i2="X" l="ENG"><s0>Catalytic reforming</s0><s5>11</s5></fC03><fC03 i1="05" i2="X" l="SPA"><s0>Reformación catalítica</s0><s5>11</s5></fC03><fC03 i1="06" i2="X" l="FRE"><s0>Etat surface</s0><s5>12</s5></fC03><fC03 i1="06" i2="X" l="ENG"><s0>Surface conditions</s0><s5>12</s5></fC03><fC03 i1="06" i2="X" l="SPA"><s0>Estado superficie</s0><s5>12</s5></fC03><fC03 i1="07" i2="X" l="FRE"><s0>Méthanol</s0><s2>NK</s2><s2>FX</s2><s5>15</s5></fC03><fC03 i1="07" i2="X" l="ENG"><s0>Methanol</s0><s2>NK</s2><s2>FX</s2><s5>15</s5></fC03><fC03 i1="07" i2="X" l="SPA"><s0>Metanol</s0><s2>NK</s2><s2>FX</s2><s5>15</s5></fC03><fC03 i1="08" i2="X" l="FRE"><s0>Oxyde d'aluminium</s0><s5>16</s5></fC03><fC03 i1="08" i2="X" l="ENG"><s0>Aluminium oxide</s0><s5>16</s5></fC03><fC03 i1="08" i2="X" l="SPA"><s0>Aluminio óxido</s0><s5>16</s5></fC03><fC03 i1="09" i2="X" l="FRE"><s0>Platine</s0><s2>NC</s2><s5>17</s5></fC03><fC03 i1="09" i2="X" l="ENG"><s0>Platinum</s0><s2>NC</s2><s5>17</s5></fC03><fC03 i1="09" i2="X" l="SPA"><s0>Platino</s0><s2>NC</s2><s5>17</s5></fC03><fN21><s1>322</s1></fN21></pA></standard></inist></record>Pour manipuler ce document sous Unix (Dilib)
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