Active sites for CO₂ hydrogenation to methanol on Cu/ZnO catalysts
The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al₂O₃) catalysts for carbon dioxide (CO₂) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. We report a direct comparison between the activity...
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| Veröffentlicht in: | Science (American Association for the Advancement of Science) 2017-03, Vol.355 (6331), p.1296-1299 |
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| creator | Kattel, Shyam Ramírez, Pedro J. Chen, Jingguang G. Rodriguez, José A. Liu, Ping |
| description | The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al₂O₃) catalysts for carbon dioxide (CO₂) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates. |
| doi_str_mv | 10.1126/science.aal3573 |
| format | Article |
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We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.</description><identifier>ISSN: 0036-8075</identifier><identifier>EISSN: 1095-9203</identifier><identifier>DOI: 10.1126/science.aal3573</identifier><language>eng</language><publisher>Washington: American Association for the Advancement of Science</publisher><subject>Aluminum ; Aluminum oxide ; Bimetals ; Carbon dioxide ; Catalysis ; Catalysts ; Chemical synthesis ; Computer simulation ; Copper ; Density functional theory ; Hydrogenation ; Industrial production ; Intermediates ; Methanol ; Methyl alcohol ; Monte Carlo simulation ; Oxidation ; Photoelectric emission ; Photoelectron spectroscopy ; Spectroscopy ; Surface chemistry ; Zinc ; Zinc oxide ; Zinc oxides</subject><ispartof>Science (American Association for the Advancement of Science), 2017-03, Vol.355 (6331), p.1296-1299</ispartof><rights>Copyright © 2017 American Association for the Advancement of Science</rights><rights>Copyright © 2017, American Association for the Advancement of Science</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/24918071$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/24918071$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>314,780,784,803,27924,27925,58017,58250</link.rule.ids></links><search><creatorcontrib>Kattel, Shyam</creatorcontrib><creatorcontrib>Ramírez, Pedro J.</creatorcontrib><creatorcontrib>Chen, Jingguang G.</creatorcontrib><creatorcontrib>Rodriguez, José A.</creatorcontrib><creatorcontrib>Liu, Ping</creatorcontrib><title>Active sites for CO₂ hydrogenation to methanol on Cu/ZnO catalysts</title><title>Science (American Association for the Advancement of Science)</title><description>The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al₂O₃) catalysts for carbon dioxide (CO₂) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.</description><subject>Aluminum</subject><subject>Aluminum oxide</subject><subject>Bimetals</subject><subject>Carbon dioxide</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemical synthesis</subject><subject>Computer simulation</subject><subject>Copper</subject><subject>Density functional theory</subject><subject>Hydrogenation</subject><subject>Industrial production</subject><subject>Intermediates</subject><subject>Methanol</subject><subject>Methyl alcohol</subject><subject>Monte Carlo simulation</subject><subject>Oxidation</subject><subject>Photoelectric emission</subject><subject>Photoelectron spectroscopy</subject><subject>Spectroscopy</subject><subject>Surface chemistry</subject><subject>Zinc</subject><subject>Zinc oxide</subject><subject>Zinc oxides</subject><issn>0036-8075</issn><issn>1095-9203</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNqN0D1PwzAQBmALgUQpzExIllhY0tpx7PjGKnxKlbrAwhK5zqVNldoldpC69qfySwgqExPT6XSPXuleQq45m3CeqmmwDTqLE2NaIXNxQkacgUwgZeKUjBgTKtEsl-fkIoQNY8MNxIjcz2xsPpGGJmKgte9osfg6HOh6X3V-hc7ExjsaPd1iXBvnWzqsRT99dwtqTTTtPsRwSc5q0wa8-p1j8vb48Fo8J_PF00sxmyerNBUxMUoLaSznWmopamk0VpxLXlXCwDKzFcosq0Fx4MucMQ1LAKVRZahR6FyIMbk75u46_9FjiOW2CRbb1jj0fSi5BgFMAcA_qB5KS0Gygd7-oRvfd2545KjyVOufwJuj2oTou3LXNVvT7cs0Az7UysU3-stzGA</recordid><startdate>20170324</startdate><enddate>20170324</enddate><creator>Kattel, Shyam</creator><creator>Ramírez, Pedro J.</creator><creator>Chen, Jingguang G.</creator><creator>Rodriguez, José A.</creator><creator>Liu, Ping</creator><general>American Association for the Advancement of Science</general><general>The American Association for the Advancement of Science</general><scope>7QF</scope><scope>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QQ</scope><scope>7QR</scope><scope>7SC</scope><scope>7SE</scope><scope>7SN</scope><scope>7SP</scope><scope>7SR</scope><scope>7SS</scope><scope>7T7</scope><scope>7TA</scope><scope>7TB</scope><scope>7TK</scope><scope>7TM</scope><scope>7U5</scope><scope>7U9</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>H94</scope><scope>JG9</scope><scope>JQ2</scope><scope>K9.</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>7X8</scope></search><sort><creationdate>20170324</creationdate><title>Active sites for CO₂ hydrogenation to methanol on Cu/ZnO catalysts</title><author>Kattel, Shyam ; 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We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.</abstract><cop>Washington</cop><pub>American Association for the Advancement of Science</pub><doi>10.1126/science.aal3573</doi><tpages>4</tpages></addata></record> |
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| source | Science Online_科学在线; JSTOR |
| subjects | Aluminum Aluminum oxide Bimetals Carbon dioxide Catalysis Catalysts Chemical synthesis Computer simulation Copper Density functional theory Hydrogenation Industrial production Intermediates Methanol Methyl alcohol Monte Carlo simulation Oxidation Photoelectric emission Photoelectron spectroscopy Spectroscopy Surface chemistry Zinc Zinc oxide Zinc oxides |
| title | Active sites for CO₂ hydrogenation to methanol on Cu/ZnO catalysts |
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