Integration of Bimetallic Electronic Synergy with Oxide Site Isolation Improves the Selective Hydrogenation of Acetylene
Semi‐hydrogenation of acetylene to ethylene is an important process to purify ethylene streams in industry. However, among current approaches reported in the literature, high ethylene selectivity has been generally achieved at the expense of activity. Herein, we show that a Ga2O3 coating of Ag@Pd co...
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Veröffentlicht in: | Angewandte Chemie International Edition 2021-08, Vol.60 (35), p.19324-19330 |
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description | Semi‐hydrogenation of acetylene to ethylene is an important process to purify ethylene streams in industry. However, among current approaches reported in the literature, high ethylene selectivity has been generally achieved at the expense of activity. Herein, we show that a Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalysts, allows improvement of the ethylene selectivity to a much greater extent than the coating of monometallic Pd nanoparticles, while preserving a remarkable intrinsic activity, approximately 50 times higher than the benchmark catalyst of Pd1Ag single‐atom alloys (SAAs). Importantly, the resulting catalyst also shows excellent long‐term stability, by suppressing coke formation efficiently. Spectroscopic characterization reveals that weakened ethylene adsorption by bimetallic electronic synergy, and oxide site isolation are both essential for the high ethylene selectivity and high‐coking resistance. H‐D exchange measurements further show that the Ga2O3‐coated Ag@Pd catalyst possesses a much higher activity of H2 activation than that of Pd1Ag SAAs, thus boosting the hydrogenation activity at the same time.
A Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalyst improves the ethylene selectivity compared with a coated Pd monometallic catalyst. The intrinsic activity is preserved and is approximately 50 times higher than the benchmark Pd1Ag single‐atom alloy catalysts. |
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A Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalyst improves the ethylene selectivity compared with a coated Pd monometallic catalyst. The intrinsic activity is preserved and is approximately 50 times higher than the benchmark Pd1Ag single‐atom alloy catalysts.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202105931</identifier><identifier>PMID: 34184379</identifier><language>eng</language><publisher>WEINHEIM: Wiley</publisher><subject>Acetylene ; atomic layer deposition ; bimetallic catalysts ; Bimetals ; Catalysts ; Chemistry ; Chemistry, Multidisciplinary ; Coatings ; Coking ; Ethylene ; Gallium oxides ; Hydrogenation ; Nanoparticles ; oxide overcoating ; Palladium ; Physical Sciences ; Science & Technology ; Selectivity ; Silver</subject><ispartof>Angewandte Chemie International Edition, 2021-08, Vol.60 (35), p.19324-19330</ispartof><rights>2021 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>true</woscitedreferencessubscribed><woscitedreferencescount>65</woscitedreferencescount><woscitedreferencesoriginalsourcerecordid>wos000677213400001</woscitedreferencesoriginalsourcerecordid><citedby>FETCH-LOGICAL-c3501-8044394cedc68a98981623afb085bbb161bc69aa3bc01324fe71aaab8e16e0c33</citedby><cites>FETCH-LOGICAL-c3501-8044394cedc68a98981623afb085bbb161bc69aa3bc01324fe71aaab8e16e0c33</cites><orcidid>0000-0002-2607-6869</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.202105931$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202105931$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>315,781,785,1418,27929,27930,39263,45579,45580</link.rule.ids></links><search><creatorcontrib>Liu, Fang</creatorcontrib><creatorcontrib>Xia, Yujia</creatorcontrib><creatorcontrib>Xu, Wenlong</creatorcontrib><creatorcontrib>Cao, Lina</creatorcontrib><creatorcontrib>Guan, Qiaoqiao</creatorcontrib><creatorcontrib>Gu, Qingqing</creatorcontrib><creatorcontrib>Yang, Bing</creatorcontrib><creatorcontrib>Lu, Junling</creatorcontrib><title>Integration of Bimetallic Electronic Synergy with Oxide Site Isolation Improves the Selective Hydrogenation of Acetylene</title><title>Angewandte Chemie International Edition</title><addtitle>ANGEW CHEM INT EDIT</addtitle><description>Semi‐hydrogenation of acetylene to ethylene is an important process to purify ethylene streams in industry. However, among current approaches reported in the literature, high ethylene selectivity has been generally achieved at the expense of activity. Herein, we show that a Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalysts, allows improvement of the ethylene selectivity to a much greater extent than the coating of monometallic Pd nanoparticles, while preserving a remarkable intrinsic activity, approximately 50 times higher than the benchmark catalyst of Pd1Ag single‐atom alloys (SAAs). Importantly, the resulting catalyst also shows excellent long‐term stability, by suppressing coke formation efficiently. Spectroscopic characterization reveals that weakened ethylene adsorption by bimetallic electronic synergy, and oxide site isolation are both essential for the high ethylene selectivity and high‐coking resistance. H‐D exchange measurements further show that the Ga2O3‐coated Ag@Pd catalyst possesses a much higher activity of H2 activation than that of Pd1Ag SAAs, thus boosting the hydrogenation activity at the same time.
A Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalyst improves the ethylene selectivity compared with a coated Pd monometallic catalyst. The intrinsic activity is preserved and is approximately 50 times higher than the benchmark Pd1Ag single‐atom alloy catalysts.</description><subject>Acetylene</subject><subject>atomic layer deposition</subject><subject>bimetallic catalysts</subject><subject>Bimetals</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Chemistry, Multidisciplinary</subject><subject>Coatings</subject><subject>Coking</subject><subject>Ethylene</subject><subject>Gallium oxides</subject><subject>Hydrogenation</subject><subject>Nanoparticles</subject><subject>oxide overcoating</subject><subject>Palladium</subject><subject>Physical Sciences</subject><subject>Science & Technology</subject><subject>Selectivity</subject><subject>Silver</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><sourceid>HGBXW</sourceid><recordid>eNqNkU1r3DAQhkVpaD7aa8-CXgrBG40l2_Jxu2wTQ2gOSc5G1o43CloplbRJ_O-r7YYt9NKe9IKeZ3iZIeQzsBkwVl4oZ3BWshJY1XJ4R06gKqHgTcPf5yw4LxpZwTE5jfEx81Ky-gM55gKk4E17Ql47l3AdVDLeUT_Sb2aDSVlrNF1a1Cl4l-Pt5DCsJ_pi0gO9eTUrpLcmIe2it3u12zwF_4yRpof8hzvVPCO9mlbBr9Ed5s81psmiw4_kaFQ24qe394zcf1_eLa6K65vLbjG_LjSvGBSSCcFboXGla6la2UqoS67GgclqGAaoYdB1qxQfNANeihEbUEoNEqFGpjk_I1_3c3O_n1uMqd-YqNFa5dBvY19Woq5aWck2o1_-Qh_9NrjcLlM15D0CF5ma7SkdfIwBx_4pmI0KUw-s392k392kP9wkC3IvvODgx6gNOo0HiTFWN02ZJ-fEYGHS710t_NalrJ7_v5rp9o02Fqd_1OrnP7rln5K_AIxxsE8</recordid><startdate>20210823</startdate><enddate>20210823</enddate><creator>Liu, Fang</creator><creator>Xia, Yujia</creator><creator>Xu, Wenlong</creator><creator>Cao, Lina</creator><creator>Guan, Qiaoqiao</creator><creator>Gu, Qingqing</creator><creator>Yang, Bing</creator><creator>Lu, Junling</creator><general>Wiley</general><general>Wiley Subscription Services, Inc</general><scope>BLEPL</scope><scope>DTL</scope><scope>HGBXW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-2607-6869</orcidid></search><sort><creationdate>20210823</creationdate><title>Integration of Bimetallic Electronic Synergy with Oxide Site Isolation Improves the Selective Hydrogenation of Acetylene</title><author>Liu, Fang ; Xia, Yujia ; Xu, Wenlong ; Cao, Lina ; Guan, Qiaoqiao ; Gu, Qingqing ; Yang, Bing ; Lu, Junling</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3501-8044394cedc68a98981623afb085bbb161bc69aa3bc01324fe71aaab8e16e0c33</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Acetylene</topic><topic>atomic layer deposition</topic><topic>bimetallic catalysts</topic><topic>Bimetals</topic><topic>Catalysts</topic><topic>Chemistry</topic><topic>Chemistry, Multidisciplinary</topic><topic>Coatings</topic><topic>Coking</topic><topic>Ethylene</topic><topic>Gallium oxides</topic><topic>Hydrogenation</topic><topic>Nanoparticles</topic><topic>oxide overcoating</topic><topic>Palladium</topic><topic>Physical Sciences</topic><topic>Science & Technology</topic><topic>Selectivity</topic><topic>Silver</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Liu, Fang</creatorcontrib><creatorcontrib>Xia, Yujia</creatorcontrib><creatorcontrib>Xu, Wenlong</creatorcontrib><creatorcontrib>Cao, Lina</creatorcontrib><creatorcontrib>Guan, Qiaoqiao</creatorcontrib><creatorcontrib>Gu, Qingqing</creatorcontrib><creatorcontrib>Yang, Bing</creatorcontrib><creatorcontrib>Lu, Junling</creatorcontrib><collection>Web of Science Core Collection</collection><collection>Science Citation Index Expanded</collection><collection>Web of Science - Science Citation Index Expanded - 2021</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Liu, Fang</au><au>Xia, Yujia</au><au>Xu, Wenlong</au><au>Cao, Lina</au><au>Guan, Qiaoqiao</au><au>Gu, Qingqing</au><au>Yang, Bing</au><au>Lu, Junling</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Integration of Bimetallic Electronic Synergy with Oxide Site Isolation Improves the Selective Hydrogenation of Acetylene</atitle><jtitle>Angewandte Chemie International Edition</jtitle><stitle>ANGEW CHEM INT EDIT</stitle><date>2021-08-23</date><risdate>2021</risdate><volume>60</volume><issue>35</issue><spage>19324</spage><epage>19330</epage><pages>19324-19330</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Semi‐hydrogenation of acetylene to ethylene is an important process to purify ethylene streams in industry. However, among current approaches reported in the literature, high ethylene selectivity has been generally achieved at the expense of activity. Herein, we show that a Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalysts, allows improvement of the ethylene selectivity to a much greater extent than the coating of monometallic Pd nanoparticles, while preserving a remarkable intrinsic activity, approximately 50 times higher than the benchmark catalyst of Pd1Ag single‐atom alloys (SAAs). Importantly, the resulting catalyst also shows excellent long‐term stability, by suppressing coke formation efficiently. Spectroscopic characterization reveals that weakened ethylene adsorption by bimetallic electronic synergy, and oxide site isolation are both essential for the high ethylene selectivity and high‐coking resistance. H‐D exchange measurements further show that the Ga2O3‐coated Ag@Pd catalyst possesses a much higher activity of H2 activation than that of Pd1Ag SAAs, thus boosting the hydrogenation activity at the same time.
A Ga2O3 coating of Ag@Pd core–shell bimetallic nanoparticle catalyst improves the ethylene selectivity compared with a coated Pd monometallic catalyst. The intrinsic activity is preserved and is approximately 50 times higher than the benchmark Pd1Ag single‐atom alloy catalysts.</abstract><cop>WEINHEIM</cop><pub>Wiley</pub><pmid>34184379</pmid><doi>10.1002/anie.202105931</doi><tpages>7</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-2607-6869</orcidid></addata></record> |
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subjects | Acetylene atomic layer deposition bimetallic catalysts Bimetals Catalysts Chemistry Chemistry, Multidisciplinary Coatings Coking Ethylene Gallium oxides Hydrogenation Nanoparticles oxide overcoating Palladium Physical Sciences Science & Technology Selectivity Silver |
title | Integration of Bimetallic Electronic Synergy with Oxide Site Isolation Improves the Selective Hydrogenation of Acetylene |
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