Rationally designing mixed Cu-(μ-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation
The direct conversion of methane to methanol on [Cu(μ-O)M] (M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M] (M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite pro...
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| Veröffentlicht in: | Physical chemistry chemical physics : PCCP 2018-11, Vol.20 (41), p.26522-26531 |
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| creator | Wang, Guiru Huang, Ling Chen, Wei Zhou, Jian Zheng, Anmin |
| description | The direct conversion of methane to methanol on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH
activation decreases in the sequence [Cu(μ-O)Ag]
> [Cu(μ-O)Au]
> [Cu(μ-O)Cu]
> [Cu(μ-O)Zn]
. (2) There are two factors that can dramatically enhance C-H bond activation: a greater spin density and a less negative charge of the μ-O atom. (3) The angles ∠CuOM play a minor role in the reactivity difference among [CuOM]
-ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes. |
| doi_str_mv | 10.1039/c8cp04872j |
| format | Article |
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(M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH
activation decreases in the sequence [Cu(μ-O)Ag]
> [Cu(μ-O)Au]
> [Cu(μ-O)Cu]
> [Cu(μ-O)Zn]
. (2) There are two factors that can dramatically enhance C-H bond activation: a greater spin density and a less negative charge of the μ-O atom. (3) The angles ∠CuOM play a minor role in the reactivity difference among [CuOM]
-ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes.</description><identifier>ISSN: 1463-9076</identifier><identifier>EISSN: 1463-9084</identifier><identifier>DOI: 10.1039/c8cp04872j</identifier><identifier>PMID: 30306980</identifier><language>eng</language><publisher>England: Royal Society of Chemistry</publisher><subject>Angles (geometry) ; Bimetals ; Catalysis ; Catalytic activity ; Cobalt ; Copper ; Density functional theory ; Direct conversion ; Gold ; Hydrogen bonds ; Mathematical analysis ; Methane ; Nickel ; Silver ; Zeolites ; Zinc</subject><ispartof>Physical chemistry chemical physics : PCCP, 2018-11, Vol.20 (41), p.26522-26531</ispartof><rights>Copyright Royal Society of Chemistry 2018</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c352t-b1ab003e90adb0d5e1e7fb7e4cc9db8fdef186c192f176b945f6ea02a28801143</citedby><cites>FETCH-LOGICAL-c352t-b1ab003e90adb0d5e1e7fb7e4cc9db8fdef186c192f176b945f6ea02a28801143</cites><orcidid>0000-0002-3713-5107 ; 0000-0001-7115-6510</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/30306980$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Wang, Guiru</creatorcontrib><creatorcontrib>Huang, Ling</creatorcontrib><creatorcontrib>Chen, Wei</creatorcontrib><creatorcontrib>Zhou, Jian</creatorcontrib><creatorcontrib>Zheng, Anmin</creatorcontrib><title>Rationally designing mixed Cu-(μ-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation</title><title>Physical chemistry chemical physics : PCCP</title><addtitle>Phys Chem Chem Phys</addtitle><description>The direct conversion of methane to methanol on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH
activation decreases in the sequence [Cu(μ-O)Ag]
> [Cu(μ-O)Au]
> [Cu(μ-O)Cu]
> [Cu(μ-O)Zn]
. (2) There are two factors that can dramatically enhance C-H bond activation: a greater spin density and a less negative charge of the μ-O atom. (3) The angles ∠CuOM play a minor role in the reactivity difference among [CuOM]
-ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes.</description><subject>Angles (geometry)</subject><subject>Bimetals</subject><subject>Catalysis</subject><subject>Catalytic activity</subject><subject>Cobalt</subject><subject>Copper</subject><subject>Density functional theory</subject><subject>Direct conversion</subject><subject>Gold</subject><subject>Hydrogen bonds</subject><subject>Mathematical analysis</subject><subject>Methane</subject><subject>Nickel</subject><subject>Silver</subject><subject>Zeolites</subject><subject>Zinc</subject><issn>1463-9076</issn><issn>1463-9084</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNpdkc9OFEEQxjtGI4hefABTiZfFMFA9PX96Dh7IBEUCwRC9eJn09NTs9mb-rN094PIYPo_P4DPRywIHTlX56ldfKvUx9p7jIUdRHGmpV5jIPF6-YLs8yURUoExePvV5tsPeOLdERJ5y8ZrtCBSYFRJ32d8r5c04qK5bQ0POzAczzKE3f6iBcopm__9Fl_vRBcwu4HMQDuB4fgC_hlCnfdA0eLIOxmuycEtjZzxBr4JmVOfgxvgFLMx8AVp51a290aC0N9fGr8GPN8o2DnryCzXQdnB_y1v2qg3r9O6h7rGfX05-lKfR-eXXb-XxeaRFGvuo5qpGFFSgampsUuKUt3VOidZFU8u2oZbLTPMibnme1UWSthkpjFUsJXKeiD022_qu7Ph7Iuer3jhNXRfOGSdXxZxLgTKVG_TjM3Q5TjZ8bUPF4ctpkmOgPm0pbUfnLLXVyppe2XXFsdokVZWy_H6f1FmAPzxYTnVPzRP6GI24A1lGjqc</recordid><startdate>20181107</startdate><enddate>20181107</enddate><creator>Wang, Guiru</creator><creator>Huang, Ling</creator><creator>Chen, Wei</creator><creator>Zhou, Jian</creator><creator>Zheng, Anmin</creator><general>Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-3713-5107</orcidid><orcidid>https://orcid.org/0000-0001-7115-6510</orcidid></search><sort><creationdate>20181107</creationdate><title>Rationally designing mixed Cu-(μ-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation</title><author>Wang, Guiru ; Huang, Ling ; Chen, Wei ; Zhou, Jian ; Zheng, Anmin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c352t-b1ab003e90adb0d5e1e7fb7e4cc9db8fdef186c192f176b945f6ea02a28801143</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Angles (geometry)</topic><topic>Bimetals</topic><topic>Catalysis</topic><topic>Catalytic activity</topic><topic>Cobalt</topic><topic>Copper</topic><topic>Density functional theory</topic><topic>Direct conversion</topic><topic>Gold</topic><topic>Hydrogen bonds</topic><topic>Mathematical analysis</topic><topic>Methane</topic><topic>Nickel</topic><topic>Silver</topic><topic>Zeolites</topic><topic>Zinc</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Guiru</creatorcontrib><creatorcontrib>Huang, Ling</creatorcontrib><creatorcontrib>Chen, Wei</creatorcontrib><creatorcontrib>Zhou, Jian</creatorcontrib><creatorcontrib>Zheng, Anmin</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>Physical chemistry chemical physics : PCCP</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Guiru</au><au>Huang, Ling</au><au>Chen, Wei</au><au>Zhou, Jian</au><au>Zheng, Anmin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Rationally designing mixed Cu-(μ-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation</atitle><jtitle>Physical chemistry chemical physics : PCCP</jtitle><addtitle>Phys Chem Chem Phys</addtitle><date>2018-11-07</date><risdate>2018</risdate><volume>20</volume><issue>41</issue><spage>26522</spage><epage>26531</epage><pages>26522-26531</pages><issn>1463-9076</issn><eissn>1463-9084</eissn><abstract>The direct conversion of methane to methanol on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M]
(M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH
activation decreases in the sequence [Cu(μ-O)Ag]
> [Cu(μ-O)Au]
> [Cu(μ-O)Cu]
> [Cu(μ-O)Zn]
. (2) There are two factors that can dramatically enhance C-H bond activation: a greater spin density and a less negative charge of the μ-O atom. (3) The angles ∠CuOM play a minor role in the reactivity difference among [CuOM]
-ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes.</abstract><cop>England</cop><pub>Royal Society of Chemistry</pub><pmid>30306980</pmid><doi>10.1039/c8cp04872j</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-3713-5107</orcidid><orcidid>https://orcid.org/0000-0001-7115-6510</orcidid></addata></record> |
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| source | Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
| subjects | Angles (geometry) Bimetals Catalysis Catalytic activity Cobalt Copper Density functional theory Direct conversion Gold Hydrogen bonds Mathematical analysis Methane Nickel Silver Zeolites Zinc |
| title | Rationally designing mixed Cu-(μ-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation |
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