Steam reforming of acetone over Ni- and Co-based catalysts: Effect of the composition of reactants and catalysts on reaction pathways

[Display omitted] •Co, Ni-based catalysts were oxidized in steam reforming of acetone at low temperatures.•Ni catalyst was reduced and active for reforming of acetone in H2 at low temperatures.•The reaction pathway was strongly influenced by reduction of the Co-Ni surface.•Steam reforming of acetone...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2016-10, Vol.195, p.16-28
Hauptverfasser: Braga, Adriano H., Sodré, Elaine R., Santos, João Batista O., de Paula Marques, Clelia M., Bueno, José Maria C.
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container_start_page 16
container_title Applied catalysis. B, Environmental
container_volume 195
creator Braga, Adriano H.
Sodré, Elaine R.
Santos, João Batista O.
de Paula Marques, Clelia M.
Bueno, José Maria C.
description [Display omitted] •Co, Ni-based catalysts were oxidized in steam reforming of acetone at low temperatures.•Ni catalyst was reduced and active for reforming of acetone in H2 at low temperatures.•The reaction pathway was strongly influenced by reduction of the Co-Ni surface.•Steam reforming of acetone was not possible at low temperatures over the Ni catalyst.•The fragments of acetone activation were hydrogenated to CH4 at low temperatures. The properties of Ni/Co/Co-Ni/MgAl2O4 catalysts in the steam reforming of acetone (SRA) were investigated regarding the metallic composition and nature of catalytic site. The catalysts were characterized by nitrogen physisorption, X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, and temperature programmed reduction and desorption of acetone. Experimental data revealed that the acetone conversion pathway on the Co, Co-Ni, or Ni catalysts was strongly dependent on the nature of the metal, reaction temperature, and the oxidation state of the metal atoms in nanoparticles surface atoms. Reaction data indicated that the acetone decomposition on reduced metal catalysts at high temperatures (>350°C) occurred mainly via the HC and CCO bonds cleavage, leading to the formation of CO, H2, and C on the metal surface. At low temperatures (200°C) and in the presence of H2 in the reactor feed, the Ni catalyst catalyzed the hydrogenation of the CO and CHx species formed from acetone activation on the metallic sites, producing CH4. For Co-containing catalysts, at low temperatures (200–350°C) the metal nanoparticles surface was in a higher oxidation degree and promoted the oxidation of acetone. At high temperatures (>350°C), the hydrogenation of CHx and CO species to CH4 was determined by the nanoparticle oxidation degree, which decreased in the order Ni>Co-Ni>Co. With increased temperature, the CHx species decomposed to C and H2, instead of being hydrogenated to CH4. The oxidation of C by H2O was favored on Co-containing catalysts. The reaction pathways are discussed based on theoretical data obtained from the literature.
doi_str_mv 10.1016/j.apcatb.2016.04.047
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The properties of Ni/Co/Co-Ni/MgAl2O4 catalysts in the steam reforming of acetone (SRA) were investigated regarding the metallic composition and nature of catalytic site. The catalysts were characterized by nitrogen physisorption, X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, and temperature programmed reduction and desorption of acetone. Experimental data revealed that the acetone conversion pathway on the Co, Co-Ni, or Ni catalysts was strongly dependent on the nature of the metal, reaction temperature, and the oxidation state of the metal atoms in nanoparticles surface atoms. Reaction data indicated that the acetone decomposition on reduced metal catalysts at high temperatures (&gt;350°C) occurred mainly via the HC and CCO bonds cleavage, leading to the formation of CO, H2, and C on the metal surface. At low temperatures (200°C) and in the presence of H2 in the reactor feed, the Ni catalyst catalyzed the hydrogenation of the CO and CHx species formed from acetone activation on the metallic sites, producing CH4. For Co-containing catalysts, at low temperatures (200–350°C) the metal nanoparticles surface was in a higher oxidation degree and promoted the oxidation of acetone. At high temperatures (&gt;350°C), the hydrogenation of CHx and CO species to CH4 was determined by the nanoparticle oxidation degree, which decreased in the order Ni&gt;Co-Ni&gt;Co. With increased temperature, the CHx species decomposed to C and H2, instead of being hydrogenated to CH4. The oxidation of C by H2O was favored on Co-containing catalysts. 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B, Environmental</title><description>[Display omitted] •Co, Ni-based catalysts were oxidized in steam reforming of acetone at low temperatures.•Ni catalyst was reduced and active for reforming of acetone in H2 at low temperatures.•The reaction pathway was strongly influenced by reduction of the Co-Ni surface.•Steam reforming of acetone was not possible at low temperatures over the Ni catalyst.•The fragments of acetone activation were hydrogenated to CH4 at low temperatures. The properties of Ni/Co/Co-Ni/MgAl2O4 catalysts in the steam reforming of acetone (SRA) were investigated regarding the metallic composition and nature of catalytic site. The catalysts were characterized by nitrogen physisorption, X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, and temperature programmed reduction and desorption of acetone. Experimental data revealed that the acetone conversion pathway on the Co, Co-Ni, or Ni catalysts was strongly dependent on the nature of the metal, reaction temperature, and the oxidation state of the metal atoms in nanoparticles surface atoms. Reaction data indicated that the acetone decomposition on reduced metal catalysts at high temperatures (&gt;350°C) occurred mainly via the HC and CCO bonds cleavage, leading to the formation of CO, H2, and C on the metal surface. At low temperatures (200°C) and in the presence of H2 in the reactor feed, the Ni catalyst catalyzed the hydrogenation of the CO and CHx species formed from acetone activation on the metallic sites, producing CH4. For Co-containing catalysts, at low temperatures (200–350°C) the metal nanoparticles surface was in a higher oxidation degree and promoted the oxidation of acetone. At high temperatures (&gt;350°C), the hydrogenation of CHx and CO species to CH4 was determined by the nanoparticle oxidation degree, which decreased in the order Ni&gt;Co-Ni&gt;Co. With increased temperature, the CHx species decomposed to C and H2, instead of being hydrogenated to CH4. The oxidation of C by H2O was favored on Co-containing catalysts. The reaction pathways are discussed based on theoretical data obtained from the literature.</description><subject>Acetone</subject><subject>Acetone reforming</subject><subject>Biomass conversion</subject><subject>Bonding</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Co catalyst</subject><subject>Cobalt</subject><subject>Heterogeneous catalysis</subject><subject>Hydrogen production</subject><subject>Ni catalyst</subject><subject>Nickel</subject><subject>Oxidation</subject><subject>Pathways</subject><subject>Reaction mechanism</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNqFUU1v1DAQtRBILC3_gIOPXLId24k_OCChVVuQKjgAZ2viONSrTRxst2h_QP83Thf1SKWRRjPz3ozmPULeMdgyYPJiv8XFYem3vFZbaGuoF2TDtBKN0Fq8JBswXDZCKPGavMl5DwBccL0hD9-Lx4kmP8Y0hfkXjSNF50ucPY33PtGvoaE4D3QXmx6zH2g9hIdjLvkDvRxH78pKKbeeujgtMYcS4ry2kkdXcC75kf7EonX6OFphC5bbP3jM5-TViIfs3_7LZ-Tn1eWP3efm5tv1l92nm8a1YErTM20kb5G1QvYAqpXKcNAdcMO6nqMZVDcI1xmHAoauAzmM0DOpQGEvOybOyPvT3iXF33c-FzuF7PzhgLOPd9kyzbtWGVGFex4KWjLOja7Q9gR1KeZcpbRLChOmo2VgV4Ps3p4MsqtBFtoa64WPJ5qvH98Hn2x2wc_ODyFVWe0Qw_8X_AUx4pr0</recordid><startdate>20161015</startdate><enddate>20161015</enddate><creator>Braga, Adriano H.</creator><creator>Sodré, Elaine R.</creator><creator>Santos, João Batista O.</creator><creator>de Paula Marques, Clelia M.</creator><creator>Bueno, José Maria C.</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7ST</scope><scope>C1K</scope><scope>SOI</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope></search><sort><creationdate>20161015</creationdate><title>Steam reforming of acetone over Ni- and Co-based catalysts: Effect of the composition of reactants and catalysts on reaction pathways</title><author>Braga, Adriano H. ; Sodré, Elaine R. ; Santos, João Batista O. ; de Paula Marques, Clelia M. ; Bueno, José Maria C.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c409t-b189624a1436b0074679208502915b2a9d75d3c59ca30d5506df0b16707ab6513</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Acetone</topic><topic>Acetone reforming</topic><topic>Biomass conversion</topic><topic>Bonding</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Co catalyst</topic><topic>Cobalt</topic><topic>Heterogeneous catalysis</topic><topic>Hydrogen production</topic><topic>Ni catalyst</topic><topic>Nickel</topic><topic>Oxidation</topic><topic>Pathways</topic><topic>Reaction mechanism</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Braga, Adriano H.</creatorcontrib><creatorcontrib>Sodré, Elaine R.</creatorcontrib><creatorcontrib>Santos, João Batista O.</creatorcontrib><creatorcontrib>de Paula Marques, Clelia M.</creatorcontrib><creatorcontrib>Bueno, José Maria C.</creatorcontrib><collection>CrossRef</collection><collection>Environment Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Environment Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Braga, Adriano H.</au><au>Sodré, Elaine R.</au><au>Santos, João Batista O.</au><au>de Paula Marques, Clelia M.</au><au>Bueno, José Maria C.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Steam reforming of acetone over Ni- and Co-based catalysts: Effect of the composition of reactants and catalysts on reaction pathways</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2016-10-15</date><risdate>2016</risdate><volume>195</volume><spage>16</spage><epage>28</epage><pages>16-28</pages><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted] •Co, Ni-based catalysts were oxidized in steam reforming of acetone at low temperatures.•Ni catalyst was reduced and active for reforming of acetone in H2 at low temperatures.•The reaction pathway was strongly influenced by reduction of the Co-Ni surface.•Steam reforming of acetone was not possible at low temperatures over the Ni catalyst.•The fragments of acetone activation were hydrogenated to CH4 at low temperatures. The properties of Ni/Co/Co-Ni/MgAl2O4 catalysts in the steam reforming of acetone (SRA) were investigated regarding the metallic composition and nature of catalytic site. The catalysts were characterized by nitrogen physisorption, X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, and temperature programmed reduction and desorption of acetone. Experimental data revealed that the acetone conversion pathway on the Co, Co-Ni, or Ni catalysts was strongly dependent on the nature of the metal, reaction temperature, and the oxidation state of the metal atoms in nanoparticles surface atoms. Reaction data indicated that the acetone decomposition on reduced metal catalysts at high temperatures (&gt;350°C) occurred mainly via the HC and CCO bonds cleavage, leading to the formation of CO, H2, and C on the metal surface. At low temperatures (200°C) and in the presence of H2 in the reactor feed, the Ni catalyst catalyzed the hydrogenation of the CO and CHx species formed from acetone activation on the metallic sites, producing CH4. For Co-containing catalysts, at low temperatures (200–350°C) the metal nanoparticles surface was in a higher oxidation degree and promoted the oxidation of acetone. At high temperatures (&gt;350°C), the hydrogenation of CHx and CO species to CH4 was determined by the nanoparticle oxidation degree, which decreased in the order Ni&gt;Co-Ni&gt;Co. With increased temperature, the CHx species decomposed to C and H2, instead of being hydrogenated to CH4. The oxidation of C by H2O was favored on Co-containing catalysts. The reaction pathways are discussed based on theoretical data obtained from the literature.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2016.04.047</doi><tpages>13</tpages></addata></record>
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subjects Acetone
Acetone reforming
Biomass conversion
Bonding
Catalysis
Catalysts
Co catalyst
Cobalt
Heterogeneous catalysis
Hydrogen production
Ni catalyst
Nickel
Oxidation
Pathways
Reaction mechanism
title Steam reforming of acetone over Ni- and Co-based catalysts: Effect of the composition of reactants and catalysts on reaction pathways
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