CO2-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy
Identifieur interne : 001F81 ( Main/Repository ); précédent : 001F80; suivant : 001F82CO2-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy
Auteurs : RBID : Pascal:12-0457222Descripteurs français
- Pascal (Inist)
- Méthanol, Reformage vapeur, In situ, Spectrométrie photoélectron, Rayon X, Alliage, Feuille, Déshydrogénation, Eau, Activation, Catalyse hétérogène, Réaction catalytique, Corrélation, Température ambiante, Dépôt, Recuit, Couche multimoléculaire, Structure électronique, Indium, Caractérisation, Sélectivité, Support, Nanoparticule, Formaldéhyde, Oxyde, Synergie, Conversion, Inverse, Monocouche.
- Wicri :
English descriptors
- KwdEn :
- Activation, Alloys, Annealing, Catalytic reaction, Characterization, Conversion, Correlation, Dehydrogenation, Deposition, Electronic structure, Foil, Formaldehyde, Heterogeneous catalysis, In situ, Indium, Inverse, Methanol, Multilayer, Nanoparticle, Oxides, Photoelectron spectrometry, Room temperature, Selectivity, Steam reforming, Support, Synergism, Water, X ray.
Abstract
In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa. Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd1In1 phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd1Zn1 counterpart. Catalytic characterization of the multilayer Pd1In1 phase in MSR yielded a CO2-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In2O3-supported Pdln nanoparticles and pure In2O3, intermediate formaldehyde is only partially converted to CO2 using this Pd1In1 phase. Strongly correlated with PdZn, on an In-diluted Pdln intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed. To achieve CO2-TOF values on the isolated Pd1In1 intermetallic phase as high as on supported Pdln/ In2O3, at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO2 conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd1In1 inhibited inverse water-gas-shift reaction on In2O3 and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO2-selectivity of the supported catalyst.
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-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy</title>
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<author><name sortKey="Schlogl, Robert" uniqKey="Schlogl R">Robert Schlögl</name>
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<author><name sortKey="Klotzer, Bernhard" uniqKey="Klotzer B">Bernhard Klötzer</name>
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<profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Activation</term>
<term>Alloys</term>
<term>Annealing</term>
<term>Catalytic reaction</term>
<term>Characterization</term>
<term>Conversion</term>
<term>Correlation</term>
<term>Dehydrogenation</term>
<term>Deposition</term>
<term>Electronic structure</term>
<term>Foil</term>
<term>Formaldehyde</term>
<term>Heterogeneous catalysis</term>
<term>In situ</term>
<term>Indium</term>
<term>Inverse</term>
<term>Methanol</term>
<term>Multilayer</term>
<term>Nanoparticle</term>
<term>Oxides</term>
<term>Photoelectron spectrometry</term>
<term>Room temperature</term>
<term>Selectivity</term>
<term>Steam reforming</term>
<term>Support</term>
<term>Synergism</term>
<term>Water</term>
<term>X ray</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Méthanol</term>
<term>Reformage vapeur</term>
<term>In situ</term>
<term>Spectrométrie photoélectron</term>
<term>Rayon X</term>
<term>Alliage</term>
<term>Feuille</term>
<term>Déshydrogénation</term>
<term>Eau</term>
<term>Activation</term>
<term>Catalyse hétérogène</term>
<term>Réaction catalytique</term>
<term>Corrélation</term>
<term>Température ambiante</term>
<term>Dépôt</term>
<term>Recuit</term>
<term>Couche multimoléculaire</term>
<term>Structure électronique</term>
<term>Indium</term>
<term>Caractérisation</term>
<term>Sélectivité</term>
<term>Support</term>
<term>Nanoparticule</term>
<term>Formaldéhyde</term>
<term>Oxyde</term>
<term>Synergie</term>
<term>Conversion</term>
<term>Inverse</term>
<term>Monocouche</term>
</keywords>
<keywords scheme="Wicri" type="concept" xml:lang="fr"><term>Méthanol</term>
<term>Alliage</term>
<term>Eau</term>
<term>Oxyde</term>
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<front><div type="abstract" xml:lang="en">In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa. Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd<sub>1</sub>
In<sub>1</sub>
phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd<sub>1</sub>
Zn<sub>1</sub>
counterpart. Catalytic characterization of the multilayer Pd<sub>1</sub>
In<sub>1</sub>
phase in MSR yielded a CO<sub>2</sub>
-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In<sub>2</sub>
O<sub>3</sub>
-supported Pdln nanoparticles and pure In<sub>2</sub>
O<sub>3</sub>
, intermediate formaldehyde is only partially converted to CO<sub>2</sub>
using this Pd<sub>1</sub>
In<sub>1</sub>
phase. Strongly correlated with PdZn, on an In-diluted Pdln intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed. To achieve CO<sub>2</sub>
-TOF values on the isolated Pd<sub>1</sub>
In<sub>1</sub>
intermetallic phase as high as on supported Pdln/ In<sub>2</sub>
O<sub>3</sub>
, at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO<sub>2</sub>
conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd<sub>1</sub>
In<sub>1</sub>
inhibited inverse water-gas-shift reaction on In<sub>2</sub>
O<sub>3</sub>
and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO<sub>2</sub>
-selectivity of the supported catalyst.</div>
</front>
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<fA08 i1="01" i2="1" l="ENG"><s1>CO<sub>2</sub>
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<fA11 i1="01" i2="1"><s1>RAMESHAN (Christoph)</s1>
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In<sub>1</sub>
phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd<sub>1</sub>
Zn<sub>1</sub>
counterpart. Catalytic characterization of the multilayer Pd<sub>1</sub>
In<sub>1</sub>
phase in MSR yielded a CO<sub>2</sub>
-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In<sub>2</sub>
O<sub>3</sub>
-supported Pdln nanoparticles and pure In<sub>2</sub>
O<sub>3</sub>
, intermediate formaldehyde is only partially converted to CO<sub>2</sub>
using this Pd<sub>1</sub>
In<sub>1</sub>
phase. Strongly correlated with PdZn, on an In-diluted Pdln intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed. To achieve CO<sub>2</sub>
-TOF values on the isolated Pd<sub>1</sub>
In<sub>1</sub>
intermetallic phase as high as on supported Pdln/ In<sub>2</sub>
O<sub>3</sub>
, at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO<sub>2</sub>
conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd<sub>1</sub>
In<sub>1</sub>
inhibited inverse water-gas-shift reaction on In<sub>2</sub>
O<sub>3</sub>
and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO<sub>2</sub>
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<s5>05</s5>
</fC03>
<fC03 i1="06" i2="X" l="FRE"><s0>Alliage</s0>
<s2>NA</s2>
<s5>06</s5>
</fC03>
<fC03 i1="06" i2="X" l="ENG"><s0>Alloys</s0>
<s2>NA</s2>
<s5>06</s5>
</fC03>
<fC03 i1="06" i2="X" l="SPA"><s0>Aleación</s0>
<s2>NA</s2>
<s5>06</s5>
</fC03>
<fC03 i1="07" i2="X" l="FRE"><s0>Feuille</s0>
<s5>07</s5>
</fC03>
<fC03 i1="07" i2="X" l="ENG"><s0>Foil</s0>
<s5>07</s5>
</fC03>
<fC03 i1="07" i2="X" l="SPA"><s0>Hoja</s0>
<s5>07</s5>
</fC03>
<fC03 i1="08" i2="X" l="FRE"><s0>Déshydrogénation</s0>
<s5>08</s5>
</fC03>
<fC03 i1="08" i2="X" l="ENG"><s0>Dehydrogenation</s0>
<s5>08</s5>
</fC03>
<fC03 i1="08" i2="X" l="SPA"><s0>Deshidrogenación</s0>
<s5>08</s5>
</fC03>
<fC03 i1="09" i2="X" l="FRE"><s0>Eau</s0>
<s5>09</s5>
</fC03>
<fC03 i1="09" i2="X" l="ENG"><s0>Water</s0>
<s5>09</s5>
</fC03>
<fC03 i1="09" i2="X" l="SPA"><s0>Agua</s0>
<s5>09</s5>
</fC03>
<fC03 i1="10" i2="X" l="FRE"><s0>Activation</s0>
<s5>10</s5>
</fC03>
<fC03 i1="10" i2="X" l="ENG"><s0>Activation</s0>
<s5>10</s5>
</fC03>
<fC03 i1="10" i2="X" l="SPA"><s0>Activación</s0>
<s5>10</s5>
</fC03>
<fC03 i1="11" i2="X" l="FRE"><s0>Catalyse hétérogène</s0>
<s5>11</s5>
</fC03>
<fC03 i1="11" i2="X" l="ENG"><s0>Heterogeneous catalysis</s0>
<s5>11</s5>
</fC03>
<fC03 i1="11" i2="X" l="SPA"><s0>Catálisis heterogénea</s0>
<s5>11</s5>
</fC03>
<fC03 i1="12" i2="X" l="FRE"><s0>Réaction catalytique</s0>
<s5>14</s5>
</fC03>
<fC03 i1="12" i2="X" l="ENG"><s0>Catalytic reaction</s0>
<s5>14</s5>
</fC03>
<fC03 i1="12" i2="X" l="SPA"><s0>Reacción catalítica</s0>
<s5>14</s5>
</fC03>
<fC03 i1="13" i2="X" l="FRE"><s0>Corrélation</s0>
<s5>15</s5>
</fC03>
<fC03 i1="13" i2="X" l="ENG"><s0>Correlation</s0>
<s5>15</s5>
</fC03>
<fC03 i1="13" i2="X" l="SPA"><s0>Correlación</s0>
<s5>15</s5>
</fC03>
<fC03 i1="14" i2="X" l="FRE"><s0>Température ambiante</s0>
<s5>16</s5>
</fC03>
<fC03 i1="14" i2="X" l="ENG"><s0>Room temperature</s0>
<s5>16</s5>
</fC03>
<fC03 i1="14" i2="X" l="SPA"><s0>Temperatura ambiente</s0>
<s5>16</s5>
</fC03>
<fC03 i1="15" i2="X" l="FRE"><s0>Dépôt</s0>
<s5>17</s5>
</fC03>
<fC03 i1="15" i2="X" l="ENG"><s0>Deposition</s0>
<s5>17</s5>
</fC03>
<fC03 i1="15" i2="X" l="SPA"><s0>Depósito</s0>
<s5>17</s5>
</fC03>
<fC03 i1="16" i2="X" l="FRE"><s0>Recuit</s0>
<s5>18</s5>
</fC03>
<fC03 i1="16" i2="X" l="ENG"><s0>Annealing</s0>
<s5>18</s5>
</fC03>
<fC03 i1="16" i2="X" l="SPA"><s0>Recocido</s0>
<s5>18</s5>
</fC03>
<fC03 i1="17" i2="X" l="FRE"><s0>Couche multimoléculaire</s0>
<s5>19</s5>
</fC03>
<fC03 i1="17" i2="X" l="ENG"><s0>Multilayer</s0>
<s5>19</s5>
</fC03>
<fC03 i1="17" i2="X" l="SPA"><s0>Capa multimolecular</s0>
<s5>19</s5>
</fC03>
<fC03 i1="18" i2="X" l="FRE"><s0>Structure électronique</s0>
<s5>20</s5>
</fC03>
<fC03 i1="18" i2="X" l="ENG"><s0>Electronic structure</s0>
<s5>20</s5>
</fC03>
<fC03 i1="18" i2="X" l="SPA"><s0>Estructura electrónica</s0>
<s5>20</s5>
</fC03>
<fC03 i1="19" i2="X" l="FRE"><s0>Indium</s0>
<s2>NC</s2>
<s5>21</s5>
</fC03>
<fC03 i1="19" i2="X" l="ENG"><s0>Indium</s0>
<s2>NC</s2>
<s5>21</s5>
</fC03>
<fC03 i1="19" i2="X" l="SPA"><s0>Indio</s0>
<s2>NC</s2>
<s5>21</s5>
</fC03>
<fC03 i1="20" i2="X" l="FRE"><s0>Caractérisation</s0>
<s5>22</s5>
</fC03>
<fC03 i1="20" i2="X" l="ENG"><s0>Characterization</s0>
<s5>22</s5>
</fC03>
<fC03 i1="20" i2="X" l="SPA"><s0>Caracterización</s0>
<s5>22</s5>
</fC03>
<fC03 i1="21" i2="X" l="FRE"><s0>Sélectivité</s0>
<s5>23</s5>
</fC03>
<fC03 i1="21" i2="X" l="ENG"><s0>Selectivity</s0>
<s5>23</s5>
</fC03>
<fC03 i1="21" i2="X" l="SPA"><s0>Selectividad</s0>
<s5>23</s5>
</fC03>
<fC03 i1="22" i2="X" l="FRE"><s0>Support</s0>
<s5>24</s5>
</fC03>
<fC03 i1="22" i2="X" l="ENG"><s0>Support</s0>
<s5>24</s5>
</fC03>
<fC03 i1="22" i2="X" l="SPA"><s0>Soporte</s0>
<s5>24</s5>
</fC03>
<fC03 i1="23" i2="X" l="FRE"><s0>Nanoparticule</s0>
<s5>25</s5>
</fC03>
<fC03 i1="23" i2="X" l="ENG"><s0>Nanoparticle</s0>
<s5>25</s5>
</fC03>
<fC03 i1="23" i2="X" l="SPA"><s0>Nanopartícula</s0>
<s5>25</s5>
</fC03>
<fC03 i1="24" i2="X" l="FRE"><s0>Formaldéhyde</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>26</s5>
</fC03>
<fC03 i1="24" i2="X" l="ENG"><s0>Formaldehyde</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>26</s5>
</fC03>
<fC03 i1="24" i2="X" l="SPA"><s0>Formaldehído</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>26</s5>
</fC03>
<fC03 i1="25" i2="X" l="FRE"><s0>Oxyde</s0>
<s2>NA</s2>
<s5>27</s5>
</fC03>
<fC03 i1="25" i2="X" l="ENG"><s0>Oxides</s0>
<s2>NA</s2>
<s5>27</s5>
</fC03>
<fC03 i1="25" i2="X" l="SPA"><s0>Óxido</s0>
<s2>NA</s2>
<s5>27</s5>
</fC03>
<fC03 i1="26" i2="X" l="FRE"><s0>Synergie</s0>
<s5>28</s5>
</fC03>
<fC03 i1="26" i2="X" l="ENG"><s0>Synergism</s0>
<s5>28</s5>
</fC03>
<fC03 i1="26" i2="X" l="SPA"><s0>Sinergia</s0>
<s5>28</s5>
</fC03>
<fC03 i1="27" i2="X" l="FRE"><s0>Conversion</s0>
<s5>29</s5>
</fC03>
<fC03 i1="27" i2="X" l="ENG"><s0>Conversion</s0>
<s5>29</s5>
</fC03>
<fC03 i1="27" i2="X" l="SPA"><s0>Conversión</s0>
<s5>29</s5>
</fC03>
<fC03 i1="28" i2="X" l="FRE"><s0>Inverse</s0>
<s5>30</s5>
</fC03>
<fC03 i1="28" i2="X" l="ENG"><s0>Inverse</s0>
<s5>30</s5>
</fC03>
<fC03 i1="28" i2="X" l="SPA"><s0>Inverso</s0>
<s5>30</s5>
</fC03>
<fC03 i1="29" i2="X" l="FRE"><s0>Monocouche</s0>
<s4>INC</s4>
<s5>32</s5>
</fC03>
<fC07 i1="01" i2="X" l="FRE"><s0>Alcanol</s0>
<s5>12</s5>
</fC07>
<fC07 i1="01" i2="X" l="ENG"><s0>Alkanol</s0>
<s5>12</s5>
</fC07>
<fC07 i1="01" i2="X" l="SPA"><s0>Alcanol</s0>
<s5>12</s5>
</fC07>
<fC07 i1="02" i2="X" l="FRE"><s0>Alcool</s0>
<s5>13</s5>
</fC07>
<fC07 i1="02" i2="X" l="ENG"><s0>Alcohol</s0>
<s5>13</s5>
</fC07>
<fC07 i1="02" i2="X" l="SPA"><s0>Alcohol</s0>
<s5>13</s5>
</fC07>
<fN21><s1>353</s1>
</fN21>
<fN44 i1="01"><s1>OTO</s1>
</fN44>
<fN82><s1>OTO</s1>
</fN82>
</pA>
</standard>
</inist>
</record>
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