Metal-organic-framework derived Co-Pd bond is preferred over Fe-Pd for reductive upgrading of furfural to tetrahydrofurfuryl alcohol
Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report...
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| Published in | Dalton transactions : an international journal of inorganic chemistry Vol. 48; no. 24; pp. 8791 - 882 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Royal Society of Chemistry
2019
|
| Subjects | |
| Online Access | Get full text |
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| Abstract | Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo
3
O
4
and PdFe
3
O
4
nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix
via
facile
in situ
thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo
3
O
4
@NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe
3
O
4
@NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H
2
-TPR) for nanohybrids, we can conclude that the presence of PdCo-N
x
active sites, and the multiple synergistic effects between Co
3
O
4
and Pd(
ii
), Co
3
O
4
and Pd
0
, as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst
via
noble metal modified MOFs as precursors.
The metal-organic-framework-derived Co-Pd bond can more efficiently catalyze the reductive upgrading of furfural to tetrahydrofurfuryl alcohol production as compared to the Fe-Pd bond. |
|---|---|
| AbstractList | Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo3O4 and PdFe3O4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo3O4@NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe3O4@NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H2-TPR) for nanohybrids, we can conclude that the presence of PdCo-Nx active sites, and the multiple synergistic effects between Co3O4 and Pd(ii), Co3O4 and Pd0, as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors.Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo3O4 and PdFe3O4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo3O4@NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe3O4@NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H2-TPR) for nanohybrids, we can conclude that the presence of PdCo-Nx active sites, and the multiple synergistic effects between Co3O4 and Pd(ii), Co3O4 and Pd0, as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors. Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo 3 O 4 and PdFe 3 O 4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo 3 O 4 @NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe 3 O 4 @NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H 2 -TPR) for nanohybrids, we can conclude that the presence of PdCo-N x active sites, and the multiple synergistic effects between Co 3 O 4 and Pd( ii ), Co 3 O 4 and Pd 0 , as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors. The metal-organic-framework-derived Co-Pd bond can more efficiently catalyze the reductive upgrading of furfural to tetrahydrofurfuryl alcohol production as compared to the Fe-Pd bond. Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal–organic-framework (MOF) assisted preparation of PdCo 3 O 4 and PdFe 3 O 4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo 3 O 4 @NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd–Fe 3 O 4 @NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H 2 -TPR) for nanohybrids, we can conclude that the presence of PdCo-N x active sites, and the multiple synergistic effects between Co 3 O 4 and Pd( ii ), Co 3 O 4 and Pd 0 , as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors. Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo3O4 and PdFe3O4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo3O4@NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe3O4@NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H2-TPR) for nanohybrids, we can conclude that the presence of PdCo-Nx active sites, and the multiple synergistic effects between Co3O4 and Pd(ii), Co3O4 and Pd0, as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors. |
| Author | Mondal, John Bolla, Srinivasa Rao Lai, Zhiping Nakka, Lingaiah Pendem, Saikiran Morgan, David J Shinde, Digambar B |
| AuthorAffiliation | King Abdullah University of Science and Technology (KAUST) Cardiff Catalysis Institute Catalysis and fine chemicals Division Division of Physical Science and Engineering AcSIR-Indian Institute of Chemical Technology School of Chemistry CSIR-Indian Institute of Chemical Technology Cardiff University |
| AuthorAffiliation_xml | – name: CSIR-Indian Institute of Chemical Technology – name: Division of Physical Science and Engineering – name: Cardiff Catalysis Institute – name: Cardiff University – name: AcSIR-Indian Institute of Chemical Technology – name: King Abdullah University of Science and Technology (KAUST) – name: Catalysis and fine chemicals Division – name: School of Chemistry |
| Author_xml | – sequence: 1 givenname: Saikiran surname: Pendem fullname: Pendem, Saikiran – sequence: 2 givenname: Srinivasa Rao surname: Bolla fullname: Bolla, Srinivasa Rao – sequence: 3 givenname: David J surname: Morgan fullname: Morgan, David J – sequence: 4 givenname: Digambar B surname: Shinde fullname: Shinde, Digambar B – sequence: 5 givenname: Zhiping surname: Lai fullname: Lai, Zhiping – sequence: 6 givenname: Lingaiah surname: Nakka fullname: Nakka, Lingaiah – sequence: 7 givenname: John surname: Mondal fullname: Mondal, John |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31124551$$D View this record in MEDLINE/PubMed |
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| Notes | NC, O 1s XPS spectra of PdCo Electronic supplementary information (ESI) available: Characterization techniques, FE-SEM images of PVP-Pd@ZIF-67, wide angle powder XRD patterns and simulated pattern of Co-ZIF, XRD patterns of Fe-ZIF, pore-size distribution, & FE-SEM images of Pd-Co NC, Pd-Fe NC and PdFe NC, HR-TEM images and N NC, and plausible mechanistic pathway. See DOI O 2 adsorption/desorption isotherms of used Pd-Co 3 4 NC, Fe 2p XP spectra of used Pd-Fe 10.1039/c9dt01190k ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23 |
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| Snippet | Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a... |
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| SubjectTerms | Alcohol Biomass Catalysts Catalytic activity Catalytic converters Clean fuels Cobalt oxides Computer simulation Furfural Iron oxides Metal-organic frameworks Nanoparticles Noble metals Organic chemistry Palladium Scanning electron microscopy Selectivity Size distribution Transition metal alloys Transition metals X ray photoelectron spectroscopy |
| Title | Metal-organic-framework derived Co-Pd bond is preferred over Fe-Pd for reductive upgrading of furfural to tetrahydrofurfuryl alcohol |
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