Tandem Catalysis by Palladium Nanoclusters Encapsulated in Metal–Organic Frameworks
A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS). Combining the oxidation activity of Pd NCs and the acetalization activity o...
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| Published in | ACS catalysis Vol. 4; no. 10; pp. 3490 - 3497 |
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| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
03.10.2014
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| Subjects | |
| Online Access | Get full text |
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| Abstract | A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS). Combining the oxidation activity of Pd NCs and the acetalization activity of the Lewis acid sites in UiO-66-NH2, this catalyst (Pd@UiO-66-NH2) exhibits excellent catalytic activity and selectivity in a one-pot tandem oxidation-acetalization reaction. This catalyst shows 99.9% selectivity to benzaldehyde ethylene acetal in the tandem reaction of benzyl alcohol and ethylene glycol at 99.9% conversion of benzyl alcohol. We also examined various substituted benzyl alcohols and found that alcohols with electron-donating groups showed better conversion and selectivity compared to those with electron-withdrawing groups. We further proved that there was no leaching of active catalytic species during the reaction and the catalyst can be recycled at least five times without significant deactivation. |
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| AbstractList | A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS). Combining the oxidation activity of Pd NCs and the acetalization activity of the Lewis acid sites in UiO-66-NH2, this catalyst (Pd@UiO-66-NH2) exhibits excellent catalytic activity and selectivity in a one-pot tandem oxidation-acetalization reaction. This catalyst shows 99.9% selectivity to benzaldehyde ethylene acetal in the tandem reaction of benzyl alcohol and ethylene glycol at 99.9% conversion of benzyl alcohol. We also examined various substituted benzyl alcohols and found that alcohols with electron-donating groups showed better conversion and selectivity compared to those with electron-withdrawing groups. As a result, we further proved that there was no leaching of active catalytic species during the reaction and the catalyst can be recycled at least five times without significant deactivation. A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS). Combining the oxidation activity of Pd NCs and the acetalization activity of the Lewis acid sites in UiO-66-NH2, this catalyst (Pd@UiO-66-NH2) exhibits excellent catalytic activity and selectivity in a one-pot tandem oxidation-acetalization reaction. This catalyst shows 99.9% selectivity to benzaldehyde ethylene acetal in the tandem reaction of benzyl alcohol and ethylene glycol at 99.9% conversion of benzyl alcohol. We also examined various substituted benzyl alcohols and found that alcohols with electron-donating groups showed better conversion and selectivity compared to those with electron-withdrawing groups. We further proved that there was no leaching of active catalytic species during the reaction and the catalyst can be recycled at least five times without significant deactivation. |
| Author | Guo, Zhiyong Goh, Tian Wei Huang, Wenyu Li, Xinle Xiao, Chaoxian Tesfagaber, Daniel |
| AuthorAffiliation | Department of Chemistry USDOE Iowa State University Ames Laboratory |
| AuthorAffiliation_xml | – name: Iowa State University – name: Department of Chemistry – name: USDOE – name: Ames Laboratory |
| Author_xml | – sequence: 1 givenname: Xinle surname: Li fullname: Li, Xinle organization: USDOE – sequence: 2 givenname: Zhiyong surname: Guo fullname: Guo, Zhiyong organization: USDOE – sequence: 3 givenname: Chaoxian surname: Xiao fullname: Xiao, Chaoxian organization: USDOE – sequence: 4 givenname: Tian Wei surname: Goh fullname: Goh, Tian Wei organization: USDOE – sequence: 5 givenname: Daniel surname: Tesfagaber fullname: Tesfagaber, Daniel organization: USDOE – sequence: 6 givenname: Wenyu surname: Huang fullname: Huang, Wenyu email: whuang@iastate.edu organization: USDOE |
| BackLink | https://www.osti.gov/servlets/purl/1225525$$D View this record in Osti.gov |
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| Keywords | acetal selective oxidation bifunctional catalysts acetalization UiO-66 solid acid tandem synthesis |
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| Snippet | A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron... |
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| SubjectTerms | acetalization bifunctional catalysts heterogeneous catalysis nanoclusters NANOSCIENCE AND NANOTECHNOLOGY tandem catalysis UiO-66 Zr-MOF |
| Title | Tandem Catalysis by Palladium Nanoclusters Encapsulated in Metal–Organic Frameworks |
| URI | http://dx.doi.org/10.1021/cs5006635 https://www.osti.gov/servlets/purl/1225525 |
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