Structural Ni0–Niδ+ Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines
Supported metal pair sites have sparked interest due to their tremendous potential as bifunctional catalysts. Here, we report the structural Ni0–Niδ+ pair sites constructed in a well-defined nanocrystal phase of Ni3P. These Ni0–Niδ+ pair sites exhibited a remarkable product formation rate of 123 mol...
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| Veröffentlicht in: | Journal of the American Chemical Society 2024-08, Vol.146 (31), p.21623-21633 |
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| container_issue | 31 |
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| container_title | Journal of the American Chemical Society |
| container_volume | 146 |
| creator | Lyu, Kyeinfar Jian, Xianfeng Nie, Kaiqi Liu, Shaoxiong Huai, Mengjiao Kang, Zhenyu Liu, Dehuai Lan, Xiaocheng Wang, Tiefeng |
| description | Supported metal pair sites have sparked interest due to their tremendous potential as bifunctional catalysts. Here, we report the structural Ni0–Niδ+ pair sites constructed in a well-defined nanocrystal phase of Ni3P. These Ni0–Niδ+ pair sites exhibited a remarkable product formation rate of 123 molBA/molmetal/h for the hydrogenation of benzonitrile (BN) to benzylamine (BA). The heterogeneity of surface Ni atoms over the Ni3P crystal created two types of metal centers, Ni0 and Niδ+, with a specific spatial distance of 4–5 Å. The Ni0 site acted as the center for H2 activation, while the Niδ+ site served as the adsorption and activation center for the C ≡ N group. The highly efficient cooperation effect of Ni0–Niδ+ pair sites resulted in a TOF of 2915 h–1 in BN hydrogenation, which is 2.4 and 9.7 times higher than that over the mono-Ni0 and -Niδ+ sites, respectively. |
| doi_str_mv | 10.1021/jacs.4c05572 |
| format | Article |
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Here, we report the structural Ni0–Niδ+ pair sites constructed in a well-defined nanocrystal phase of Ni3P. These Ni0–Niδ+ pair sites exhibited a remarkable product formation rate of 123 molBA/molmetal/h for the hydrogenation of benzonitrile (BN) to benzylamine (BA). The heterogeneity of surface Ni atoms over the Ni3P crystal created two types of metal centers, Ni0 and Niδ+, with a specific spatial distance of 4–5 Å. The Ni0 site acted as the center for H2 activation, while the Niδ+ site served as the adsorption and activation center for the C ≡ N group. The highly efficient cooperation effect of Ni0–Niδ+ pair sites resulted in a TOF of 2915 h–1 in BN hydrogenation, which is 2.4 and 9.7 times higher than that over the mono-Ni0 and -Niδ+ sites, respectively.</description><identifier>ISSN: 0002-7863</identifier><identifier>ISSN: 1520-5126</identifier><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/jacs.4c05572</identifier><language>eng</language><publisher>American Chemical Society</publisher><subject>adsorption ; benzylamines ; hydrogenation ; nanocrystals ; nitriles</subject><ispartof>Journal of the American Chemical Society, 2024-08, Vol.146 (31), p.21623-21633</ispartof><rights>2024 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-4607-8650</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jacs.4c05572$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jacs.4c05572$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,27055,27903,27904,56716,56766</link.rule.ids></links><search><creatorcontrib>Lyu, Kyeinfar</creatorcontrib><creatorcontrib>Jian, Xianfeng</creatorcontrib><creatorcontrib>Nie, Kaiqi</creatorcontrib><creatorcontrib>Liu, Shaoxiong</creatorcontrib><creatorcontrib>Huai, Mengjiao</creatorcontrib><creatorcontrib>Kang, Zhenyu</creatorcontrib><creatorcontrib>Liu, Dehuai</creatorcontrib><creatorcontrib>Lan, Xiaocheng</creatorcontrib><creatorcontrib>Wang, Tiefeng</creatorcontrib><title>Structural Ni0–Niδ+ Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines</title><title>Journal of the American Chemical Society</title><addtitle>J. Am. Chem. Soc</addtitle><description>Supported metal pair sites have sparked interest due to their tremendous potential as bifunctional catalysts. Here, we report the structural Ni0–Niδ+ pair sites constructed in a well-defined nanocrystal phase of Ni3P. These Ni0–Niδ+ pair sites exhibited a remarkable product formation rate of 123 molBA/molmetal/h for the hydrogenation of benzonitrile (BN) to benzylamine (BA). The heterogeneity of surface Ni atoms over the Ni3P crystal created two types of metal centers, Ni0 and Niδ+, with a specific spatial distance of 4–5 Å. The Ni0 site acted as the center for H2 activation, while the Niδ+ site served as the adsorption and activation center for the C ≡ N group. The highly efficient cooperation effect of Ni0–Niδ+ pair sites resulted in a TOF of 2915 h–1 in BN hydrogenation, which is 2.4 and 9.7 times higher than that over the mono-Ni0 and -Niδ+ sites, respectively.</description><subject>adsorption</subject><subject>benzylamines</subject><subject>hydrogenation</subject><subject>nanocrystals</subject><subject>nitriles</subject><issn>0002-7863</issn><issn>1520-5126</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkM1KAzEUhYMoWKs7HyBLQabm5r_LUtQKpRaq65BOMzVlOtEkI3TnO_gqPocP4ZM4YsGlq8uB7xy4H0LnQAZAKFxtbJkGvCRCKHqAeiAoKQRQeYh6hBBaKC3ZMTpJadNFTjX0kFnk2Ja5jbbGM0--3t5n_vPjEs-tj3jhs0u4ChFP_Pqp3uFRmf2rw5PdKoa1a2z2ocGh6po5-rpjc8Dz6Lc2duzWNy6doqPK1smd7W8fPd5cP4wnxfT-9m48mhYWNM-FFrRcCWUJEAJCM60I0yuxXK6GjFYSONdLJ4mQbgi8gkpVlpRcsrIjAeSQ9dHF7-5zDC-tS9lsfSpdXdvGhTYZBoIppiXQ_1GiuVJCSfmHdmLNJrSx6X4wQMyPbvOj2-x1s2-P33K8</recordid><startdate>20240807</startdate><enddate>20240807</enddate><creator>Lyu, Kyeinfar</creator><creator>Jian, Xianfeng</creator><creator>Nie, Kaiqi</creator><creator>Liu, Shaoxiong</creator><creator>Huai, Mengjiao</creator><creator>Kang, Zhenyu</creator><creator>Liu, Dehuai</creator><creator>Lan, Xiaocheng</creator><creator>Wang, Tiefeng</creator><general>American Chemical Society</general><scope>7X8</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0002-4607-8650</orcidid></search><sort><creationdate>20240807</creationdate><title>Structural Ni0–Niδ+ Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines</title><author>Lyu, Kyeinfar ; Jian, Xianfeng ; Nie, Kaiqi ; Liu, Shaoxiong ; Huai, Mengjiao ; Kang, Zhenyu ; Liu, Dehuai ; Lan, Xiaocheng ; Wang, Tiefeng</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a184t-852cd57a0100158387038d5bbd932f61448be6056e914f1f7fa0c463c38711693</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>adsorption</topic><topic>benzylamines</topic><topic>hydrogenation</topic><topic>nanocrystals</topic><topic>nitriles</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lyu, Kyeinfar</creatorcontrib><creatorcontrib>Jian, Xianfeng</creatorcontrib><creatorcontrib>Nie, Kaiqi</creatorcontrib><creatorcontrib>Liu, Shaoxiong</creatorcontrib><creatorcontrib>Huai, Mengjiao</creatorcontrib><creatorcontrib>Kang, Zhenyu</creatorcontrib><creatorcontrib>Liu, Dehuai</creatorcontrib><creatorcontrib>Lan, Xiaocheng</creatorcontrib><creatorcontrib>Wang, Tiefeng</creatorcontrib><collection>MEDLINE - Academic</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lyu, Kyeinfar</au><au>Jian, Xianfeng</au><au>Nie, Kaiqi</au><au>Liu, Shaoxiong</au><au>Huai, Mengjiao</au><au>Kang, Zhenyu</au><au>Liu, Dehuai</au><au>Lan, Xiaocheng</au><au>Wang, Tiefeng</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Structural Ni0–Niδ+ Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. Am. Chem. Soc</addtitle><date>2024-08-07</date><risdate>2024</risdate><volume>146</volume><issue>31</issue><spage>21623</spage><epage>21633</epage><pages>21623-21633</pages><issn>0002-7863</issn><issn>1520-5126</issn><eissn>1520-5126</eissn><abstract>Supported metal pair sites have sparked interest due to their tremendous potential as bifunctional catalysts. Here, we report the structural Ni0–Niδ+ pair sites constructed in a well-defined nanocrystal phase of Ni3P. These Ni0–Niδ+ pair sites exhibited a remarkable product formation rate of 123 molBA/molmetal/h for the hydrogenation of benzonitrile (BN) to benzylamine (BA). The heterogeneity of surface Ni atoms over the Ni3P crystal created two types of metal centers, Ni0 and Niδ+, with a specific spatial distance of 4–5 Å. The Ni0 site acted as the center for H2 activation, while the Niδ+ site served as the adsorption and activation center for the C ≡ N group. The highly efficient cooperation effect of Ni0–Niδ+ pair sites resulted in a TOF of 2915 h–1 in BN hydrogenation, which is 2.4 and 9.7 times higher than that over the mono-Ni0 and -Niδ+ sites, respectively.</abstract><pub>American Chemical Society</pub><doi>10.1021/jacs.4c05572</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0002-4607-8650</orcidid></addata></record> |
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| source | American Chemical Society Web Editions |
| subjects | adsorption benzylamines hydrogenation nanocrystals nitriles |
| title | Structural Ni0–Niδ+ Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines |
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