Dynamic active sites over binary oxide catalysts: In situ/operando spectroscopic study of low-temperature CO oxidation over MnO sub(x)-CeO sub(2) catalysts
The determination of the dynamic active sites over binary oxide catalysts is of great challenge in heterogeneous catalysis. In this work, the origin of active sites toward low-temperature CO oxidation ( 130 degree C. Notably, the Mars-van Krevelen mechanism was proceeded in the whole temperature ran...
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| Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2016-08, Vol.191, p.179-191 |
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| container_title | Applied catalysis. B, Environmental |
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| creator | Zhanga, Xiao-man Denga, Ya-Qing Tiana, Pengfei Shanga, Huan-huan Xua, Jing Hana, Yi-Fan |
| description | The determination of the dynamic active sites over binary oxide catalysts is of great challenge in heterogeneous catalysis. In this work, the origin of active sites toward low-temperature CO oxidation ( 130 degree C. Notably, the Mars-van Krevelen mechanism was proceeded in the whole temperature range. We speculate that cheap binary oxides will substitute for noble metal as catalysts for the removal of CO and other toxic gases, especially operating under mild conditions. |
| doi_str_mv | 10.1016/j.apcatb.2016.03.030 |
| format | Article |
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In this work, the origin of active sites toward low-temperature CO oxidation (<200 degree C) were thoroughly studied using MnO sub(x)-CeO sub(2) composite oxide catalysts with different Mn/Ce molar ratios, synthesized by a redox co-precipitation method. The optimum Mn sub(1)Ce sub(1) catalyst (T sub(100) = 190 degree C), which showed excellent activity, has found to be composed of three phases: (1) CeO sub(2); (2) amorphous MnO sub(x); (3) MnO sub(x)-CeO sub(2) solid solution (active sites). With the combination of kinetics and characterization results, including Temperature-Programmed-Desorption/Reduction (TPD/TPR), operando Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS), the dynamic structures of catalysts were rationalized with the identification of the interface of MnO sub(x) and CeO sub(2). The mechanism for CO oxidation over MnO sub(x)-CeO sub(2) in the temperature range 100-190 degree C were proposed that the direct and the formate routes were followed at T < 130 degree C, and the carbonate route became dominant at T > 130 degree C. Notably, the Mars-van Krevelen mechanism was proceeded in the whole temperature range. We speculate that cheap binary oxides will substitute for noble metal as catalysts for the removal of CO and other toxic gases, especially operating under mild conditions.</description><identifier>ISSN: 0926-3373</identifier><identifier>DOI: 10.1016/j.apcatb.2016.03.030</identifier><language>eng</language><subject>Catalysis ; Catalysts ; Coprecipitation ; Dynamics ; Fourier transforms ; Oxidation ; Oxides ; Particulate composites</subject><ispartof>Applied catalysis. 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With the combination of kinetics and characterization results, including Temperature-Programmed-Desorption/Reduction (TPD/TPR), operando Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS), the dynamic structures of catalysts were rationalized with the identification of the interface of MnO sub(x) and CeO sub(2). The mechanism for CO oxidation over MnO sub(x)-CeO sub(2) in the temperature range 100-190 degree C were proposed that the direct and the formate routes were followed at T < 130 degree C, and the carbonate route became dominant at T > 130 degree C. Notably, the Mars-van Krevelen mechanism was proceeded in the whole temperature range. We speculate that cheap binary oxides will substitute for noble metal as catalysts for the removal of CO and other toxic gases, especially operating under mild conditions.</description><subject>Catalysis</subject><subject>Catalysts</subject><subject>Coprecipitation</subject><subject>Dynamics</subject><subject>Fourier transforms</subject><subject>Oxidation</subject><subject>Oxides</subject><subject>Particulate composites</subject><issn>0926-3373</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNqNj8tOwzAQRb0AiVL4AxZetosEPxI_2KHwqlTUTffVxHGkVKkdYqe038LPklIktkgjzVzNnXM1CN1RklJCxf02hc5ALFM2qpTwscgFmhDNRMK55FfoOoQtIYRxpibo6-noYNcYDCY2e4tDE23Afm97XDYO-iP2h6ayeERCewwxPOCFO7mGe9_ZHlzlceisib0PxncjKMShGq9q3PrPJNrdyRWH3uJi9cOC2Hh3Tnh3KxyGcnaYJ4U9j2z-F3WDLmtog7397VO0fnleF2_JcvW6KB6XSSeETKQEkBVXuTSsEuO32tYlo6ANhWxcKuCcMKWVrpikudKZ0XUmcg6C0Sq3fIpmZ2zX-4_BhrjZNcHYtgVn_RA2VLE8U1Rl8h9WooTMNFP8G3-bex8</recordid><startdate>20160815</startdate><enddate>20160815</enddate><creator>Zhanga, Xiao-man</creator><creator>Denga, Ya-Qing</creator><creator>Tiana, Pengfei</creator><creator>Shanga, Huan-huan</creator><creator>Xua, Jing</creator><creator>Hana, Yi-Fan</creator><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>20160815</creationdate><title>Dynamic active sites over binary oxide catalysts: In situ/operando spectroscopic study of low-temperature CO oxidation over MnO sub(x)-CeO sub(2) catalysts</title><author>Zhanga, Xiao-man ; Denga, Ya-Qing ; Tiana, Pengfei ; Shanga, Huan-huan ; Xua, Jing ; Hana, Yi-Fan</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p667-77aa7d3857c2d60309efb21a9c1a477a8a33028989d2715894c9f4653a621d5e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Catalysis</topic><topic>Catalysts</topic><topic>Coprecipitation</topic><topic>Dynamics</topic><topic>Fourier transforms</topic><topic>Oxidation</topic><topic>Oxides</topic><topic>Particulate composites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhanga, Xiao-man</creatorcontrib><creatorcontrib>Denga, Ya-Qing</creatorcontrib><creatorcontrib>Tiana, Pengfei</creatorcontrib><creatorcontrib>Shanga, Huan-huan</creatorcontrib><creatorcontrib>Xua, Jing</creatorcontrib><creatorcontrib>Hana, Yi-Fan</creatorcontrib><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>Zhanga, Xiao-man</au><au>Denga, Ya-Qing</au><au>Tiana, Pengfei</au><au>Shanga, Huan-huan</au><au>Xua, Jing</au><au>Hana, Yi-Fan</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Dynamic active sites over binary oxide catalysts: In situ/operando spectroscopic study of low-temperature CO oxidation over MnO sub(x)-CeO sub(2) catalysts</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2016-08-15</date><risdate>2016</risdate><volume>191</volume><spage>179</spage><epage>191</epage><pages>179-191</pages><issn>0926-3373</issn><abstract>The determination of the dynamic active sites over binary oxide catalysts is of great challenge in heterogeneous catalysis. In this work, the origin of active sites toward low-temperature CO oxidation (<200 degree C) were thoroughly studied using MnO sub(x)-CeO sub(2) composite oxide catalysts with different Mn/Ce molar ratios, synthesized by a redox co-precipitation method. The optimum Mn sub(1)Ce sub(1) catalyst (T sub(100) = 190 degree C), which showed excellent activity, has found to be composed of three phases: (1) CeO sub(2); (2) amorphous MnO sub(x); (3) MnO sub(x)-CeO sub(2) solid solution (active sites). With the combination of kinetics and characterization results, including Temperature-Programmed-Desorption/Reduction (TPD/TPR), operando Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS), the dynamic structures of catalysts were rationalized with the identification of the interface of MnO sub(x) and CeO sub(2). The mechanism for CO oxidation over MnO sub(x)-CeO sub(2) in the temperature range 100-190 degree C were proposed that the direct and the formate routes were followed at T < 130 degree C, and the carbonate route became dominant at T > 130 degree C. Notably, the Mars-van Krevelen mechanism was proceeded in the whole temperature range. We speculate that cheap binary oxides will substitute for noble metal as catalysts for the removal of CO and other toxic gases, especially operating under mild conditions.</abstract><doi>10.1016/j.apcatb.2016.03.030</doi><tpages>13</tpages></addata></record> |
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| subjects | Catalysis Catalysts Coprecipitation Dynamics Fourier transforms Oxidation Oxides Particulate composites |
| title | Dynamic active sites over binary oxide catalysts: In situ/operando spectroscopic study of low-temperature CO oxidation over MnO sub(x)-CeO sub(2) catalysts |
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