One-pot synthesis of porous silica-supported ultrafine Ni nanoparticles as efficient and stable catalyst for selective hydrogenation of benzophenone
[Display omitted] •Ni(7%)@pSiO2-Alg was developed by a facile one-pot co-assembly syntheses strategy.•Ni(II) chelated alginate hydrogel acts as metal precursor and sacrificial template.•In-situ generated Na2CO3 is the key factor for improved selectivity of benzhydrol.•This catalyst exhibited good ac...
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Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2019-12, Vol.259, p.118111, Article 118111 |
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container_title | Applied catalysis. B, Environmental |
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creator | Qiao, Xianliang She, Tiantian Zhang, Huiling Wen, Xin Niu, Libo Ricardez-Sandoval, Luis Li, Jingde Bai, Guoyi |
description | [Display omitted]
•Ni(7%)@pSiO2-Alg was developed by a facile one-pot co-assembly syntheses strategy.•Ni(II) chelated alginate hydrogel acts as metal precursor and sacrificial template.•In-situ generated Na2CO3 is the key factor for improved selectivity of benzhydrol.•This catalyst exhibited good activity and stability in benzophenone hydrogenation.
In this work, we report a silica-supported ultrafine Ni catalyst for the selective hydrogenation of benzophenone. This material was developed by a facile one-pot co-assembly syntheses strategy, using Ni(II) chelated alginate hydrogel as metal precursor and sacrificial template. Due to the highly active and uniformly dispersed Ni nanoparticles (NPs), 99.8% of benzophenone conversion was achieved. Remarkably, it also reached a 97.7% of selectivity for benzhydrol during benzophenone hydrogenation. Temperature-programmed desorption of ammonia (NH3-TPD) and Density Functional Theory (DFT) results reveal that the in-situ generated sodium carbonate (Na2CO3) derived from sodium alginate is essential in tuning the selectivity of benzhydrol: the existence of Na2CO3 reduces the surface acidity of catalyst and promotes the desorption of intermediate benzhydrol, preventing its further hydrogenolysis on the surface acidic sites of catalyst. Moreover, the supported Ni catalyst shows no significant loss of its activity during 20 times of recycling. |
doi_str_mv | 10.1016/j.apcatb.2019.118111 |
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•Ni(7%)@pSiO2-Alg was developed by a facile one-pot co-assembly syntheses strategy.•Ni(II) chelated alginate hydrogel acts as metal precursor and sacrificial template.•In-situ generated Na2CO3 is the key factor for improved selectivity of benzhydrol.•This catalyst exhibited good activity and stability in benzophenone hydrogenation.
In this work, we report a silica-supported ultrafine Ni catalyst for the selective hydrogenation of benzophenone. This material was developed by a facile one-pot co-assembly syntheses strategy, using Ni(II) chelated alginate hydrogel as metal precursor and sacrificial template. Due to the highly active and uniformly dispersed Ni nanoparticles (NPs), 99.8% of benzophenone conversion was achieved. Remarkably, it also reached a 97.7% of selectivity for benzhydrol during benzophenone hydrogenation. Temperature-programmed desorption of ammonia (NH3-TPD) and Density Functional Theory (DFT) results reveal that the in-situ generated sodium carbonate (Na2CO3) derived from sodium alginate is essential in tuning the selectivity of benzhydrol: the existence of Na2CO3 reduces the surface acidity of catalyst and promotes the desorption of intermediate benzhydrol, preventing its further hydrogenolysis on the surface acidic sites of catalyst. Moreover, the supported Ni catalyst shows no significant loss of its activity during 20 times of recycling.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2019.118111</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Acidity ; Alginate hydrogel ; Alginic acid ; Ammonia ; Benzophenone ; Benzophenone hydrogenation ; Catalysts ; Density functional theory ; Desorption ; High selectivity ; Hydrogels ; Hydrogenation ; Hydrogenolysis ; Nanoparticles ; Ni nanoparticles ; Nickel ; Selectivity ; Silica ; Silicon dioxide ; Sodium ; Sodium alginate ; Sodium carbonate ; Stability ; Ultrafines</subject><ispartof>Applied catalysis. B, Environmental, 2019-12, Vol.259, p.118111, Article 118111</ispartof><rights>2019 Elsevier B.V.</rights><rights>Copyright Elsevier BV Dec 15, 2019</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c417t-ac7a8378dfa75d4c5695b8825ca238dcd65d63f9f9c6fdd70e9b820679670af73</citedby><cites>FETCH-LOGICAL-c417t-ac7a8378dfa75d4c5695b8825ca238dcd65d63f9f9c6fdd70e9b820679670af73</cites><orcidid>0000-0002-1300-1630</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0926337319308586$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>Qiao, Xianliang</creatorcontrib><creatorcontrib>She, Tiantian</creatorcontrib><creatorcontrib>Zhang, Huiling</creatorcontrib><creatorcontrib>Wen, Xin</creatorcontrib><creatorcontrib>Niu, Libo</creatorcontrib><creatorcontrib>Ricardez-Sandoval, Luis</creatorcontrib><creatorcontrib>Li, Jingde</creatorcontrib><creatorcontrib>Bai, Guoyi</creatorcontrib><title>One-pot synthesis of porous silica-supported ultrafine Ni nanoparticles as efficient and stable catalyst for selective hydrogenation of benzophenone</title><title>Applied catalysis. B, Environmental</title><description>[Display omitted]
•Ni(7%)@pSiO2-Alg was developed by a facile one-pot co-assembly syntheses strategy.•Ni(II) chelated alginate hydrogel acts as metal precursor and sacrificial template.•In-situ generated Na2CO3 is the key factor for improved selectivity of benzhydrol.•This catalyst exhibited good activity and stability in benzophenone hydrogenation.
In this work, we report a silica-supported ultrafine Ni catalyst for the selective hydrogenation of benzophenone. This material was developed by a facile one-pot co-assembly syntheses strategy, using Ni(II) chelated alginate hydrogel as metal precursor and sacrificial template. Due to the highly active and uniformly dispersed Ni nanoparticles (NPs), 99.8% of benzophenone conversion was achieved. Remarkably, it also reached a 97.7% of selectivity for benzhydrol during benzophenone hydrogenation. Temperature-programmed desorption of ammonia (NH3-TPD) and Density Functional Theory (DFT) results reveal that the in-situ generated sodium carbonate (Na2CO3) derived from sodium alginate is essential in tuning the selectivity of benzhydrol: the existence of Na2CO3 reduces the surface acidity of catalyst and promotes the desorption of intermediate benzhydrol, preventing its further hydrogenolysis on the surface acidic sites of catalyst. Moreover, the supported Ni catalyst shows no significant loss of its activity during 20 times of recycling.</description><subject>Acidity</subject><subject>Alginate hydrogel</subject><subject>Alginic acid</subject><subject>Ammonia</subject><subject>Benzophenone</subject><subject>Benzophenone hydrogenation</subject><subject>Catalysts</subject><subject>Density functional theory</subject><subject>Desorption</subject><subject>High selectivity</subject><subject>Hydrogels</subject><subject>Hydrogenation</subject><subject>Hydrogenolysis</subject><subject>Nanoparticles</subject><subject>Ni nanoparticles</subject><subject>Nickel</subject><subject>Selectivity</subject><subject>Silica</subject><subject>Silicon dioxide</subject><subject>Sodium</subject><subject>Sodium alginate</subject><subject>Sodium carbonate</subject><subject>Stability</subject><subject>Ultrafines</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNp9kEtr3DAQx01pIdu036AHQc_e6LG25EuhhL4gJJf0LMbSqKvFlVyNHNh-jnzgenHOPQ0M_8fMr2k-CL4XXPQ3pz3MDuq4l1wMeyGMEOJVsxNGq1YZo143Oz7IvlVKq6vmLdGJcy6VNLvm-SFhO-fK6JzqESkSy4HNueSFGMUpOmhpmddFRc-WqRYIMSG7jyxByjOUGt2ExIAYhhBdxFQZJM-owjghW--C6UyVhVwY4YSuxidkx7Mv-RcmqDGnS-WI6W-ej5hywnfNmwAT4fuXed38_Prl8fZ7e_fw7cft57vWHYSuLTgNRmnjA-jOH1zXD91ojOwcSGW8833nexWGMLg-eK85DqORvNdDrzkEra6bj1vuXPKfBanaU15KWiutVCtKIQ9GrqrDpnIlExUMdi7xN5SzFdxe-NuT3fjbC3-78V9tnzYbrh88RSyWLnAc-lhWCNbn-P-Af0u8lGE</recordid><startdate>20191215</startdate><enddate>20191215</enddate><creator>Qiao, Xianliang</creator><creator>She, Tiantian</creator><creator>Zhang, Huiling</creator><creator>Wen, Xin</creator><creator>Niu, Libo</creator><creator>Ricardez-Sandoval, Luis</creator><creator>Li, Jingde</creator><creator>Bai, Guoyi</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0002-1300-1630</orcidid></search><sort><creationdate>20191215</creationdate><title>One-pot synthesis of porous silica-supported ultrafine Ni nanoparticles as efficient and stable catalyst for selective hydrogenation of benzophenone</title><author>Qiao, Xianliang ; She, Tiantian ; Zhang, Huiling ; Wen, Xin ; Niu, Libo ; Ricardez-Sandoval, Luis ; Li, Jingde ; Bai, Guoyi</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c417t-ac7a8378dfa75d4c5695b8825ca238dcd65d63f9f9c6fdd70e9b820679670af73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Acidity</topic><topic>Alginate hydrogel</topic><topic>Alginic acid</topic><topic>Ammonia</topic><topic>Benzophenone</topic><topic>Benzophenone hydrogenation</topic><topic>Catalysts</topic><topic>Density functional theory</topic><topic>Desorption</topic><topic>High selectivity</topic><topic>Hydrogels</topic><topic>Hydrogenation</topic><topic>Hydrogenolysis</topic><topic>Nanoparticles</topic><topic>Ni nanoparticles</topic><topic>Nickel</topic><topic>Selectivity</topic><topic>Silica</topic><topic>Silicon dioxide</topic><topic>Sodium</topic><topic>Sodium alginate</topic><topic>Sodium carbonate</topic><topic>Stability</topic><topic>Ultrafines</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Qiao, Xianliang</creatorcontrib><creatorcontrib>She, Tiantian</creatorcontrib><creatorcontrib>Zhang, Huiling</creatorcontrib><creatorcontrib>Wen, Xin</creatorcontrib><creatorcontrib>Niu, Libo</creatorcontrib><creatorcontrib>Ricardez-Sandoval, Luis</creatorcontrib><creatorcontrib>Li, Jingde</creatorcontrib><creatorcontrib>Bai, Guoyi</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Qiao, Xianliang</au><au>She, Tiantian</au><au>Zhang, Huiling</au><au>Wen, Xin</au><au>Niu, Libo</au><au>Ricardez-Sandoval, Luis</au><au>Li, Jingde</au><au>Bai, Guoyi</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>One-pot synthesis of porous silica-supported ultrafine Ni nanoparticles as efficient and stable catalyst for selective hydrogenation of benzophenone</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2019-12-15</date><risdate>2019</risdate><volume>259</volume><spage>118111</spage><pages>118111-</pages><artnum>118111</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted]
•Ni(7%)@pSiO2-Alg was developed by a facile one-pot co-assembly syntheses strategy.•Ni(II) chelated alginate hydrogel acts as metal precursor and sacrificial template.•In-situ generated Na2CO3 is the key factor for improved selectivity of benzhydrol.•This catalyst exhibited good activity and stability in benzophenone hydrogenation.
In this work, we report a silica-supported ultrafine Ni catalyst for the selective hydrogenation of benzophenone. This material was developed by a facile one-pot co-assembly syntheses strategy, using Ni(II) chelated alginate hydrogel as metal precursor and sacrificial template. Due to the highly active and uniformly dispersed Ni nanoparticles (NPs), 99.8% of benzophenone conversion was achieved. Remarkably, it also reached a 97.7% of selectivity for benzhydrol during benzophenone hydrogenation. Temperature-programmed desorption of ammonia (NH3-TPD) and Density Functional Theory (DFT) results reveal that the in-situ generated sodium carbonate (Na2CO3) derived from sodium alginate is essential in tuning the selectivity of benzhydrol: the existence of Na2CO3 reduces the surface acidity of catalyst and promotes the desorption of intermediate benzhydrol, preventing its further hydrogenolysis on the surface acidic sites of catalyst. Moreover, the supported Ni catalyst shows no significant loss of its activity during 20 times of recycling.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2019.118111</doi><orcidid>https://orcid.org/0000-0002-1300-1630</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Acidity Alginate hydrogel Alginic acid Ammonia Benzophenone Benzophenone hydrogenation Catalysts Density functional theory Desorption High selectivity Hydrogels Hydrogenation Hydrogenolysis Nanoparticles Ni nanoparticles Nickel Selectivity Silica Silicon dioxide Sodium Sodium alginate Sodium carbonate Stability Ultrafines |
title | One-pot synthesis of porous silica-supported ultrafine Ni nanoparticles as efficient and stable catalyst for selective hydrogenation of benzophenone |
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