PdHx entrapped in covalent triazine framework modulates selectivity in glycerol oxidation [Modulation of palladium activity and stability by a covalent triazine framework]
Abstract
The confinement of a Pd nanoparticle within a nitrogen-containing covalent triazine framework (CTF) material was investigated to understand if the highly tunable CTF chemistry mediates the Pd catalytic properties through an ensemble effect with the CTF nitrogen atoms or a confinement effect within the CTF pores. The results surprisingly demonstrate that the CTF stabilizes the formation of 2.6 nm PdHx particles within the pores. These PdHx particles are very active for the liquid phase oxidation of glycerol due to the in situ formation of H2O2 which catalytically promotes the initial C-C cleavage. In addition the confined particles are stable over many catalytic cycles whereas nanoparticles trapped outside of the pores loose activity rapidly. These results indicate that there is the potential to tune the CTF chemistry to significantly modify the chemistry of the catalytic metals.
- Authors:
-
- Universita di Milano (Italy)
- Fritz Haber Institute of the Max Planck Society, Berlin (Germany)
- Istituto di Scienze e Tecnologie Molecolari del CNR, Milano (Italy)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Technische Univ. Berlin (Germany). Berlin Institute of Technology
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1207042
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 14; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Chan-Thaw, Carine E., Villa, Alberto, Wang, Di, Biroli, Alessio, Veith, Gabriel M, Thomas, Arne, and Prati, Laura. PdHx entrapped in covalent triazine framework modulates selectivity in glycerol oxidation [Modulation of palladium activity and stability by a covalent triazine framework]. United States: N. p., 2015.
Web. doi:10.1002/cctc.201500055.
Chan-Thaw, Carine E., Villa, Alberto, Wang, Di, Biroli, Alessio, Veith, Gabriel M, Thomas, Arne, & Prati, Laura. PdHx entrapped in covalent triazine framework modulates selectivity in glycerol oxidation [Modulation of palladium activity and stability by a covalent triazine framework]. United States. https://doi.org/10.1002/cctc.201500055
Chan-Thaw, Carine E., Villa, Alberto, Wang, Di, Biroli, Alessio, Veith, Gabriel M, Thomas, Arne, and Prati, Laura. Thu .
"PdHx entrapped in covalent triazine framework modulates selectivity in glycerol oxidation [Modulation of palladium activity and stability by a covalent triazine framework]". United States. https://doi.org/10.1002/cctc.201500055. https://www.osti.gov/servlets/purl/1207042.
@article{osti_1207042,
title = {PdHx entrapped in covalent triazine framework modulates selectivity in glycerol oxidation [Modulation of palladium activity and stability by a covalent triazine framework]},
author = {Chan-Thaw, Carine E. and Villa, Alberto and Wang, Di and Biroli, Alessio and Veith, Gabriel M and Thomas, Arne and Prati, Laura},
abstractNote = {The confinement of a Pd nanoparticle within a nitrogen-containing covalent triazine framework (CTF) material was investigated to understand if the highly tunable CTF chemistry mediates the Pd catalytic properties through an ensemble effect with the CTF nitrogen atoms or a confinement effect within the CTF pores. The results surprisingly demonstrate that the CTF stabilizes the formation of 2.6 nm PdHx particles within the pores. These PdHx particles are very active for the liquid phase oxidation of glycerol due to the in situ formation of H2O2 which catalytically promotes the initial C-C cleavage. In addition the confined particles are stable over many catalytic cycles whereas nanoparticles trapped outside of the pores loose activity rapidly. These results indicate that there is the potential to tune the CTF chemistry to significantly modify the chemistry of the catalytic metals.},
doi = {10.1002/cctc.201500055},
journal = {ChemCatChem},
number = 14,
volume = 7,
place = {United States},
year = {Thu Jun 25 00:00:00 EDT 2015},
month = {Thu Jun 25 00:00:00 EDT 2015}
}
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Works referenced in this record:
Porous, Covalent Triazine-Based Frameworks Prepared by Ionothermal Synthesis
journal, April 2008
- Kuhn, Pierre; Antonietti, Markus; Thomas, Arne
- Angewandte Chemie International Edition, Vol. 47, Issue 18
Ionothermalsynthese von porösen kovalenten Triazin- Polymernetzwerken
journal, April 2008
- Kuhn, Pierre; Antonietti, Markus; Thomas, Arne
- Angewandte Chemie, Vol. 120, Issue 18
Template-Free Tuning of Nanopores in Carbonaceous Polymers through Ionothermal Synthesis
journal, February 2009
- Kuhn, Pierre; Forget, Aurélien; Hartmann, Jürgen
- Advanced Materials, Vol. 21, Issue 8
Functional Materials: From Hard to Soft Porous Frameworks
journal, October 2010
- Thomas, Arne
- Angewandte Chemie International Edition, Vol. 49, Issue 45, p. 8328-8344
Funktionsmaterialien: von harten zu weichen porösen Netzwerken
journal, October 2010
- Thomas, Arne
- Angewandte Chemie, Vol. 122, Issue 45
Solid Catalysts for the Selective Low-Temperature Oxidation of Methane to Methanol
journal, September 2009
- Palkovits, Regina; Antonietti, Markus; Kuhn, Pierre
- Angewandte Chemie International Edition, Vol. 48, Issue 37
Feste Katalysatoren für die selektive Niedertemperaturoxidation von Methan zu Methanol
journal, September 2009
- Palkovits, Regina; Antonietti, Markus; Kuhn, Pierre
- Angewandte Chemie, Vol. 121, Issue 37
Covalent Triazine Framework as Catalytic Support for Liquid Phase Reaction
journal, February 2010
- Chan-Thaw, Carine E.; Villa, Alberto; Katekomol, Phisan
- Nano Letters, Vol. 10, Issue 2
Triazine-Based Polymers as Nanostructured Supports for the Liquid-Phase Oxidation of Alcohols
journal, November 2010
- Chan-Thaw, Carine E.; Villa, Alberto; Prati, Laura
- Chemistry - A European Journal, Vol. 17, Issue 3
Influence of Periodic Nitrogen Functionality on the Selective Oxidation of Alcohols
journal, December 2011
- Chan-Thaw, Carine E.; Villa, Alberto; Veith, Gabriel M.
- Chemistry - An Asian Journal, Vol. 7, Issue 2
Oxidation of alcohols with molecular oxygen on platinum metal catalysts in aqueous solutions
journal, March 1994
- Mallat, T.; Baiker, A.
- Catalysis Today, Vol. 19, Issue 2
From Microporous Regular Frameworks to Mesoporous Materials with Ultrahigh Surface Area: Dynamic Reorganization of Porous Polymer Networks
journal, October 2008
- Kuhn, Pierre; Forget, Aurélien; Su, Dangsheng
- Journal of the American Chemical Society, Vol. 130, Issue 40
Catalytic hydrogenation of alkadienes and alkynes by palladium catalysts supported on heterocyclic polyamides
journal, March 1998
- Michalska, Zofia M.; Ostaszewski, Bogdan; Zientarska, Jolanta
- Journal of Molecular Catalysis A: Chemical, Vol. 129, Issue 2-3
Neutral Ligands with Exceptional Donor Ability for Palladium-Catalyzed Alkene Hydrogenation
journal, July 2007
- Heckenroth, Marion; Kluser, Evelyne; Neels, Antonia
- Angewandte Chemie International Edition, Vol. 46, Issue 33
Neutral Ligands with Exceptional Donor Ability for Palladium-Catalyzed Alkene Hydrogenation
journal, August 2007
- Heckenroth, Marion; Kluser, Evelyne; Neels, Antonia
- Angewandte Chemie, Vol. 119, Issue 33
Size Effects in Electronic and Catalytic Properties of Unsupported Palladium Nanoparticles in Electrooxidation of Formic Acid
journal, July 2006
- Zhou, Wei Ping; Lewera, Adam; Larsen, Robert
- The Journal of Physical Chemistry B, Vol. 110, Issue 27, p. 13393-13398
Interaction of Palladium Nano-Crystals with Hydrogen During PECVD Growth of Carbon Nanotubes
book, July 2003
- Wunderlich, Wilfried; Tanemura, Masaki
- Advances in Solid State Physics
Transformation of Pd → PdH0.7 nanoparticles inside mesoporous Zr-modified SiO2 films in ambient conditions
journal, January 2011
- Saha, Jony; Dandapat, Anirban; De, Goutam
- Journal of Materials Chemistry, Vol. 21, Issue 31
Hydrogen induced lattice expansion and crystallinity degradation in palladium nanoparticles: Effect of hydrogen concentration, pressure, and temperature
journal, November 2009
- Khanuja, Manika; Mehta, B. R.; Agar, Pragya
- Journal of Applied Physics, Vol. 106, Issue 9
In-situ TEM on (de)hydrogenation of Pd at 0.5–4.5bar hydrogen pressure and 20–400°C
journal, January 2012
- Yokosawa, Tadahiro; Alan, Tuncay; Pandraud, Gregory
- Ultramicroscopy, Vol. 112, Issue 1
The use of active carbon pretreated at 2173K as a support for palladium catalysts for hydrodechlorination reactions
journal, July 2011
- Bonarowska, Magdalena; Raróg-Pilecka, Wioletta; Karpiński, Zbigniew
- Catalysis Today, Vol. 169, Issue 1
Au on MgAl2O4 spinels: The effect of support surface properties in glycerol oxidation
journal, September 2010
- Villa, Alberto; Gaiassi, Aureliano; Rossetti, Ilenia
- Journal of Catalysis, Vol. 275, Issue 1
Electronic, steric, and temperature effects in the Pd(II)-biquinoline catalyzed aerobic oxidation of benzylic alcohols in water
journal, April 2008
- Buffin, Brian P.; Belitz, Nadine L.; Verbeke, Sara L.
- Journal of Molecular Catalysis A: Chemical, Vol. 284, Issue 1-2
[Pd(NHC)(PR3)] (NHC = N-heterocyclic carbene) catalysed alcohol oxidation using molecular oxygen
journal, January 2012
- Jurčík, Václav; Schmid, Thibault E.; Dumont, Quentin
- Dalton Transactions, Vol. 41, Issue 40
Well-defined alkylpalladium complexes with pyridine-carboxylate ligands as catalysts for the aerobic oxidation of alcohols
journal, January 2012
- Melero, Cristóbal; Shishilov, Oleg N.; Álvarez, Eleuterio
- Dalton Transactions, Vol. 41, Issue 46
Influence of gold particle size on the aqueous-phase oxidation of carbon monoxide and glycerol
journal, August 2007
- Ketchie, W.; Fang, Y.; Wong, M.
- Journal of Catalysis, Vol. 250, Issue 1
From Renewable to Fine Chemicals Through Selective Oxidation: The Case of Glycerol
journal, January 2009
- Prati, Laura; Spontoni, Paolo; Gaiassi, Aureliano
- Topics in Catalysis, Vol. 52, Issue 3
Carbon-Supported Gold Nanocatalysts: Shape Effect in the Selective Glycerol Oxidation
journal, November 2012
- Wang, Di; Villa, Alberto; Su, Dangsheng
- ChemCatChem, Vol. 5, Issue 9
Oxidation of Glycerol to Glycolate by using Supported Gold and Palladium Nanoparticles
journal, December 2009
- Sankar, Meenakshisundaram; Dimitratos, Nikolaos; Knight, Davidâ W.
- ChemSusChem, Vol. 2, Issue 12
Au NPs on anionic-exchange resin as catalyst for polyols oxidation in batch and fixed bed reactor
journal, June 2010
- Villa, Alberto; Chan-Thaw, Carine E.; Prati, Laura
- Applied Catalysis B: Environmental, Vol. 96, Issue 3-4
Works referencing / citing this record:
Covalent Triazine-based Frameworks-Tailor-made Catalysts and Catalyst Supports for Molecular and Nanoparticulate Species
journal, March 2018
- Artz, Jens
- ChemCatChem, Vol. 10, Issue 8
Sulfur‐Linked Covalent Triazine Frameworks Doped with Coordinatively Unsaturated Cu(I) as Electrocatalysts for Oxygen Reduction
journal, January 2018
- Iwase, Kazuyuki; Kamiya, Kazuhide; Miyayama, Masaru
- ChemElectroChem, Vol. 5, Issue 5
Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis
journal, December 2019
- Jena, Himanshu Sekhar; Krishnaraj, Chidharth; Schmidt, Johannes
- Chemistry – A European Journal, Vol. 26, Issue 7
AuPd-nNiO as an effective catalyst for the base-free oxidation of HMF under mild reaction conditions
journal, January 2019
- Bonincontro, Danilo; Lolli, Alice; Villa, Alberto
- Green Chemistry, Vol. 21, Issue 15
Recent Advancements in the Synthesis of Covalent Triazine Frameworks for Energy and Environmental Applications
journal, December 2018
- Zhang, Ying; Jin, Shangbin
- Polymers, Vol. 11, Issue 1
Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports
journal, August 2019
- Tahir, Norini; Krishnaraj, Chidharth; Leus, Karen
- Polymers, Vol. 11, Issue 8
Playing with covalent triazine framework tiles for improved CO 2 adsorption properties and catalytic performance
journal, January 2019
- Tuci, Giulia; Iemhoff, Andree; Ba, Housseinou
- Beilstein Journal of Nanotechnology, Vol. 10
Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis
journal, December 2019
- Jena, Himanshu Sekhar; Krishnaraj, Chidharth; Schmidt, Johannes
- Chemistry – A European Journal
Tailored N-Containing Carbons as Catalyst Supports in Alcohol Oxidation
journal, February 2016
- Campisi, Sebastiano; Marzorati, Stefania; Spontoni, Paolo
- Materials, Vol. 9, Issue 2
Recent Advancements in the Synthesis of Covalent Triazine Frameworks for Energy and Environmental Applications
journal, December 2018
- Zhang, Ying; Jin, Shangbin
- Polymers, Vol. 11, Issue 1
Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports
journal, August 2019
- Tahir, Norini; Krishnaraj, Chidharth; Leus, Karen
- Polymers, Vol. 11, Issue 8