Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols
Metal–organic frameworks (MOFs) featuring multiple catalytic units are excellent platforms for heterogeneous catalysis. However, the synergism between multiple catalytic units for catalysis is far from being well understood. Herein, we reported the synthesis of a robust 2,2,6,6-tetramethylpiperidiny...
Gespeichert in:
| Veröffentlicht in: | ACS applied materials & interfaces 2019-01, Vol.11 (3), p.3034-3043 |
|---|---|
| Hauptverfasser: | , , , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 3043 |
|---|---|
| container_issue | 3 |
| container_start_page | 3034 |
| container_title | ACS applied materials & interfaces |
| container_volume | 11 |
| creator | Zhuang, Jin-Liang Liu, Xiang-Yue Zhang, Yu Wang, Chen Mao, Hui-Ling Guo, Jun Du, Xuan Zhu, Shao-Bin Ren, Bin Terfort, Andreas |
| description | Metal–organic frameworks (MOFs) featuring multiple catalytic units are excellent platforms for heterogeneous catalysis. However, the synergism between multiple catalytic units for catalysis is far from being well understood. Herein, we reported the synthesis of a robust 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) radical-functionalized Zr-MOF (UiO-68-TEMPO) in the form of single-crystalline and microsized crystals with varied missing linker defects. Detailed catalytic studies and theoretical calculations reveal that the synergistic effect between the TEMPO radicals and hydrophilic and defective Zr-nodes endows UiO-68-TEMPO with superior catalytic activity toward aerobic oxidation of alcohols. Our work not only offers a new route to design and synthesize highly effective MOF catalysts but also provides insights into the synergism between multiple catalytic sites. |
| doi_str_mv | 10.1021/acsami.8b18370 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_miscellaneous_2160731587</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2160731587</sourcerecordid><originalsourceid>FETCH-LOGICAL-a396t-5d74f96e02fc0e8afb4460eae5def850382a15fad9abeccbbddcc469a3835d4c3</originalsourceid><addsrcrecordid>eNp1kcFu1DAQhi0EoqVw5Yh8REhZ7NjOOty2ZZcitSyCcuESTezx1iWJFztR2RvvwAPwbjwJrnbpjdPM4fv-0egn5DlnM85K_hpMgt7PdMu1mLMH5JjXUha6VOXD-13KI_IkpRvGKlEy9ZgcCaa0klodk99fY3GJI3R_fv5axw0M3tBVhB5vQ_yW6AphnKIfNvRqeflxTT-B9Qa69IZ-3g0YNz6NWVg6h2akLY63iMMBhcHS852NYXvtuwzlQx-CRfoW7-BET0PIck5eYAxtBtY_vIXRh4EGRxedCdehS0_JI5fv4bPDPCFfVsurs_PiYv3u_dniogBRV2Oh7Fy6ukJWOsNQg2ulrBgCKotOKyZ0CVw5sDW0aEzbWmuMrGoQWigrjTghL_e52xi-T5jGpvfJYNfBgGFKTckrNhdc6XlGZ3vUxJBSRNdso-8h7hrOmrtSmn0pzaGULLw4ZE9tj_Ye_9dCBl7tgSw2N2GKQ371f2l_AR5NmyQ</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2160731587</pqid></control><display><type>article</type><title>Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols</title><source>ACS Publications</source><creator>Zhuang, Jin-Liang ; Liu, Xiang-Yue ; Zhang, Yu ; Wang, Chen ; Mao, Hui-Ling ; Guo, Jun ; Du, Xuan ; Zhu, Shao-Bin ; Ren, Bin ; Terfort, Andreas</creator><creatorcontrib>Zhuang, Jin-Liang ; Liu, Xiang-Yue ; Zhang, Yu ; Wang, Chen ; Mao, Hui-Ling ; Guo, Jun ; Du, Xuan ; Zhu, Shao-Bin ; Ren, Bin ; Terfort, Andreas</creatorcontrib><description>Metal–organic frameworks (MOFs) featuring multiple catalytic units are excellent platforms for heterogeneous catalysis. However, the synergism between multiple catalytic units for catalysis is far from being well understood. Herein, we reported the synthesis of a robust 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) radical-functionalized Zr-MOF (UiO-68-TEMPO) in the form of single-crystalline and microsized crystals with varied missing linker defects. Detailed catalytic studies and theoretical calculations reveal that the synergistic effect between the TEMPO radicals and hydrophilic and defective Zr-nodes endows UiO-68-TEMPO with superior catalytic activity toward aerobic oxidation of alcohols. Our work not only offers a new route to design and synthesize highly effective MOF catalysts but also provides insights into the synergism between multiple catalytic sites.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.8b18370</identifier><identifier>PMID: 30585485</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><ispartof>ACS applied materials & interfaces, 2019-01, Vol.11 (3), p.3034-3043</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a396t-5d74f96e02fc0e8afb4460eae5def850382a15fad9abeccbbddcc469a3835d4c3</citedby><cites>FETCH-LOGICAL-a396t-5d74f96e02fc0e8afb4460eae5def850382a15fad9abeccbbddcc469a3835d4c3</cites><orcidid>0000-0002-9821-5864 ; 0000-0003-2369-5151 ; 0000-0001-5704-6569</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/acsami.8b18370$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsami.8b18370$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/30585485$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhuang, Jin-Liang</creatorcontrib><creatorcontrib>Liu, Xiang-Yue</creatorcontrib><creatorcontrib>Zhang, Yu</creatorcontrib><creatorcontrib>Wang, Chen</creatorcontrib><creatorcontrib>Mao, Hui-Ling</creatorcontrib><creatorcontrib>Guo, Jun</creatorcontrib><creatorcontrib>Du, Xuan</creatorcontrib><creatorcontrib>Zhu, Shao-Bin</creatorcontrib><creatorcontrib>Ren, Bin</creatorcontrib><creatorcontrib>Terfort, Andreas</creatorcontrib><title>Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>Metal–organic frameworks (MOFs) featuring multiple catalytic units are excellent platforms for heterogeneous catalysis. However, the synergism between multiple catalytic units for catalysis is far from being well understood. Herein, we reported the synthesis of a robust 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) radical-functionalized Zr-MOF (UiO-68-TEMPO) in the form of single-crystalline and microsized crystals with varied missing linker defects. Detailed catalytic studies and theoretical calculations reveal that the synergistic effect between the TEMPO radicals and hydrophilic and defective Zr-nodes endows UiO-68-TEMPO with superior catalytic activity toward aerobic oxidation of alcohols. Our work not only offers a new route to design and synthesize highly effective MOF catalysts but also provides insights into the synergism between multiple catalytic sites.</description><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNp1kcFu1DAQhi0EoqVw5Yh8REhZ7NjOOty2ZZcitSyCcuESTezx1iWJFztR2RvvwAPwbjwJrnbpjdPM4fv-0egn5DlnM85K_hpMgt7PdMu1mLMH5JjXUha6VOXD-13KI_IkpRvGKlEy9ZgcCaa0klodk99fY3GJI3R_fv5axw0M3tBVhB5vQ_yW6AphnKIfNvRqeflxTT-B9Qa69IZ-3g0YNz6NWVg6h2akLY63iMMBhcHS852NYXvtuwzlQx-CRfoW7-BET0PIck5eYAxtBtY_vIXRh4EGRxedCdehS0_JI5fv4bPDPCFfVsurs_PiYv3u_dniogBRV2Oh7Fy6ukJWOsNQg2ulrBgCKotOKyZ0CVw5sDW0aEzbWmuMrGoQWigrjTghL_e52xi-T5jGpvfJYNfBgGFKTckrNhdc6XlGZ3vUxJBSRNdso-8h7hrOmrtSmn0pzaGULLw4ZE9tj_Ye_9dCBl7tgSw2N2GKQ371f2l_AR5NmyQ</recordid><startdate>20190123</startdate><enddate>20190123</enddate><creator>Zhuang, Jin-Liang</creator><creator>Liu, Xiang-Yue</creator><creator>Zhang, Yu</creator><creator>Wang, Chen</creator><creator>Mao, Hui-Ling</creator><creator>Guo, Jun</creator><creator>Du, Xuan</creator><creator>Zhu, Shao-Bin</creator><creator>Ren, Bin</creator><creator>Terfort, Andreas</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-9821-5864</orcidid><orcidid>https://orcid.org/0000-0003-2369-5151</orcidid><orcidid>https://orcid.org/0000-0001-5704-6569</orcidid></search><sort><creationdate>20190123</creationdate><title>Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols</title><author>Zhuang, Jin-Liang ; Liu, Xiang-Yue ; Zhang, Yu ; Wang, Chen ; Mao, Hui-Ling ; Guo, Jun ; Du, Xuan ; Zhu, Shao-Bin ; Ren, Bin ; Terfort, Andreas</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a396t-5d74f96e02fc0e8afb4460eae5def850382a15fad9abeccbbddcc469a3835d4c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhuang, Jin-Liang</creatorcontrib><creatorcontrib>Liu, Xiang-Yue</creatorcontrib><creatorcontrib>Zhang, Yu</creatorcontrib><creatorcontrib>Wang, Chen</creatorcontrib><creatorcontrib>Mao, Hui-Ling</creatorcontrib><creatorcontrib>Guo, Jun</creatorcontrib><creatorcontrib>Du, Xuan</creatorcontrib><creatorcontrib>Zhu, Shao-Bin</creatorcontrib><creatorcontrib>Ren, Bin</creatorcontrib><creatorcontrib>Terfort, Andreas</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhuang, Jin-Liang</au><au>Liu, Xiang-Yue</au><au>Zhang, Yu</au><au>Wang, Chen</au><au>Mao, Hui-Ling</au><au>Guo, Jun</au><au>Du, Xuan</au><au>Zhu, Shao-Bin</au><au>Ren, Bin</au><au>Terfort, Andreas</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl. Mater. Interfaces</addtitle><date>2019-01-23</date><risdate>2019</risdate><volume>11</volume><issue>3</issue><spage>3034</spage><epage>3043</epage><pages>3034-3043</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>Metal–organic frameworks (MOFs) featuring multiple catalytic units are excellent platforms for heterogeneous catalysis. However, the synergism between multiple catalytic units for catalysis is far from being well understood. Herein, we reported the synthesis of a robust 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) radical-functionalized Zr-MOF (UiO-68-TEMPO) in the form of single-crystalline and microsized crystals with varied missing linker defects. Detailed catalytic studies and theoretical calculations reveal that the synergistic effect between the TEMPO radicals and hydrophilic and defective Zr-nodes endows UiO-68-TEMPO with superior catalytic activity toward aerobic oxidation of alcohols. Our work not only offers a new route to design and synthesize highly effective MOF catalysts but also provides insights into the synergism between multiple catalytic sites.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>30585485</pmid><doi>10.1021/acsami.8b18370</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-9821-5864</orcidid><orcidid>https://orcid.org/0000-0003-2369-5151</orcidid><orcidid>https://orcid.org/0000-0001-5704-6569</orcidid></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1944-8244 |
| ispartof | ACS applied materials & interfaces, 2019-01, Vol.11 (3), p.3034-3043 |
| issn | 1944-8244 1944-8252 |
| language | eng |
| recordid | cdi_proquest_miscellaneous_2160731587 |
| source | ACS Publications |
| title | Zr-Metal–Organic Frameworks Featuring TEMPO Radicals: Synergistic Effect between TEMPO and Hydrophilic Zr-Node Defects Boosting Aerobic Oxidation of Alcohols |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-02-13T21%3A40%3A13IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Zr-Metal%E2%80%93Organic%20Frameworks%20Featuring%20TEMPO%20Radicals:%20Synergistic%20Effect%20between%20TEMPO%20and%20Hydrophilic%20Zr-Node%20Defects%20Boosting%20Aerobic%20Oxidation%20of%20Alcohols&rft.jtitle=ACS%20applied%20materials%20&%20interfaces&rft.au=Zhuang,%20Jin-Liang&rft.date=2019-01-23&rft.volume=11&rft.issue=3&rft.spage=3034&rft.epage=3043&rft.pages=3034-3043&rft.issn=1944-8244&rft.eissn=1944-8252&rft_id=info:doi/10.1021/acsami.8b18370&rft_dat=%3Cproquest_cross%3E2160731587%3C/proquest_cross%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2160731587&rft_id=info:pmid/30585485&rfr_iscdi=true |