New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica
Abstract
Abstract A highly modular synthesis of designed catalysts with controlled bimetallic nanoparticle size and composition and a well‐defined structural hierarchy is demonstrated. Exemplary catalysts—bimetallic dilute Ag‐in‐Au nanoparticles partially embedded in a porous SiO 2 matrix (SiO 2 –Ag x Au y )—were synthesized by the decoration of polymeric colloids with the bimetallic nanoparticles followed by assembly into a colloidal crystal backfilled with the matrix precursor and subsequent removal of the polymeric template. This work reports that these new catalyst architectures are significantly better than nanoporous dilute AgAu alloy catalysts (nanoporous Ag 3 Au 97 ) while retaining a clear predictive relationship between their surface reactivity with that of single‐crystal Au surfaces. This paves the way for broadening the range of new catalyst architectures required for translating the designed principles developed under controlled conditions to designed catalysts under operating conditions for highly selective coupling of alcohols to form esters. Excellent catalytic performance of the porous SiO 2 –Ag x Au y structure for selective oxidation of both methanol and ethanol to produce esters with high conversion efficiency, selectivity, and stability was demonstrated, illustrating the ability to translate design principles developed for support‐free materialsmore »
- Authors:
-
- Harvard Univ., Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Harvard Univ., Cambridge, MA (United States). Energy Frontier Research Center (EFRC) Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1469871
- Alternate Identifier(s):
- OSTI ID: 1408783
- Grant/Contract Number:
- SC0012573
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Volume: 24; Journal Issue: 8; Related Information: IMASC partners with Harvard University (lead); Fritz Haber Institute; Lawrence Berkeley National Laboratory; Lawrence Livermore National Laboratory; University of Kansas; Tufts University; Journal ID: ISSN 0947-6539
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 42 ENGINEERING; 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; colloid templated porous materials; gold; heterogeneous catalysis; nanoparticles; selective oxidation; silver
Citation Formats
Shirman, Tanya, Lattimer, Judith, Luneau, Mathilde, Shirman, Elijah, Reece, Christian, Aizenberg, Michael, Madix, Robert J., Aizenberg, Joanna, and Friend, Cynthia M.. New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica. United States: N. p., 2017.
Web. doi:10.1002/chem.201704552.
Shirman, Tanya, Lattimer, Judith, Luneau, Mathilde, Shirman, Elijah, Reece, Christian, Aizenberg, Michael, Madix, Robert J., Aizenberg, Joanna, & Friend, Cynthia M.. New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica. United States. https://doi.org/10.1002/chem.201704552
Shirman, Tanya, Lattimer, Judith, Luneau, Mathilde, Shirman, Elijah, Reece, Christian, Aizenberg, Michael, Madix, Robert J., Aizenberg, Joanna, and Friend, Cynthia M.. Thu .
"New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica". United States. https://doi.org/10.1002/chem.201704552. https://www.osti.gov/servlets/purl/1469871.
@article{osti_1469871,
title = {New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica},
author = {Shirman, Tanya and Lattimer, Judith and Luneau, Mathilde and Shirman, Elijah and Reece, Christian and Aizenberg, Michael and Madix, Robert J. and Aizenberg, Joanna and Friend, Cynthia M.},
abstractNote = {Abstract A highly modular synthesis of designed catalysts with controlled bimetallic nanoparticle size and composition and a well‐defined structural hierarchy is demonstrated. Exemplary catalysts—bimetallic dilute Ag‐in‐Au nanoparticles partially embedded in a porous SiO 2 matrix (SiO 2 –Ag x Au y )—were synthesized by the decoration of polymeric colloids with the bimetallic nanoparticles followed by assembly into a colloidal crystal backfilled with the matrix precursor and subsequent removal of the polymeric template. This work reports that these new catalyst architectures are significantly better than nanoporous dilute AgAu alloy catalysts (nanoporous Ag 3 Au 97 ) while retaining a clear predictive relationship between their surface reactivity with that of single‐crystal Au surfaces. This paves the way for broadening the range of new catalyst architectures required for translating the designed principles developed under controlled conditions to designed catalysts under operating conditions for highly selective coupling of alcohols to form esters. Excellent catalytic performance of the porous SiO 2 –Ag x Au y structure for selective oxidation of both methanol and ethanol to produce esters with high conversion efficiency, selectivity, and stability was demonstrated, illustrating the ability to translate design principles developed for support‐free materials to the colloid‐templated structures. The synthetic methodology reported is customizable for the design of a wide range of robust catalytic systems inspired by design principles derived from model studies. Fine control over the composition, morphology, size, distribution, and availability of the supported nanoparticles was demonstrated.},
doi = {10.1002/chem.201704552},
journal = {Chemistry - A European Journal},
number = 8,
volume = 24,
place = {United States},
year = {Thu Sep 28 00:00:00 EDT 2017},
month = {Thu Sep 28 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Catalyst design for enhanced sustainability through fundamental surface chemistry
journal, February 2016
- Personick, Michelle L.; Montemore, Matthew M.; Kaxiras, Efthimios
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 374, Issue 2061
Nanostructure of wet-chemically prepared, polymer-stabilized silver–gold nanoalloys (6 nm) over the entire composition range
journal, January 2015
- Ristig, S.; Prymak, O.; Loza, K.
- Journal of Materials Chemistry B, Vol. 3, Issue 23
Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts
journal, December 2016
- Zugic, Branko; Wang, Lucun; Heine, Christian
- Nature Materials, Vol. 16, Issue 5
Extremely fast Au–Ag alloy–dealloy associated reversible plasmonic modifications in SiO 2 films
journal, January 2016
- Pramanik, Sourav; Chattopadhyay, Shreyasi; Das, Jugal Kishore
- Journal of Materials Chemistry C, Vol. 4, Issue 16
Continuous Catalytic Production of Methyl Acrylates from Unsaturated Alcohols by Gold: The Strong Effect of C═C Unsaturation on Reaction Selectivity
journal, February 2016
- Zugic, Branko; Karakalos, Stavros; Stowers, Kara J.
- ACS Catalysis, Vol. 6, Issue 3
Designing bimetallic catalysts for a green and sustainable future
journal, January 2012
- Sankar, Meenakshisundaram; Dimitratos, Nikolaos; Miedziak, Peter J.
- Chemical Society Reviews, Vol. 41, Issue 24
Active sites for methanol partial oxidation on nanoporous gold catalysts
journal, December 2016
- Wang, Lu-Cun; Personick, Michelle L.; Karakalos, Stavros
- Journal of Catalysis, Vol. 344
Nanoalloys: From Theory to Applications of Alloy Clusters and Nanoparticles
journal, March 2008
- Ferrando, Riccardo; Jellinek, Julius; Johnston, Roy L.
- Chemical Reviews, Vol. 108, Issue 3, p. 845-910
Exploiting basic principles to control the selectivity of the vapor phase catalytic oxidative cross-coupling of primary alcohols over nanoporous gold catalysts
journal, September 2015
- Wang, Lu-Cun; Stowers, Kara J.; Zugic, Branko
- Journal of Catalysis, Vol. 329
A colloidoscope of colloid-based porous materials and their uses
journal, January 2016
- Phillips, Katherine R.; England, Grant T.; Sunny, Steffi
- Chemical Society Reviews, Vol. 45, Issue 2
Correlating the Atomic Structure of Bimetallic Silver–Gold Nanoparticles to Their Antibacterial and Cytotoxic Activities
journal, March 2015
- Padmos, J. Daniel; Langman, Maxine; MacDonald, Katelyn
- The Journal of Physical Chemistry C, Vol. 119, Issue 13
Interaction of silica-supported small silver clusters with molecular oxygen. A computational study
journal, December 2014
- Shor, Aleksey M.; Laletina, Svetlana S.; Ivanova Shor, Elena A.
- Surface Science, Vol. 630
Experimental methods in catalytic kinetics
journal, September 1999
- Perego, C.
- Catalysis Today, Vol. 52, Issue 2-3
Gold Nanoshells on Polystyrene Cores for Control of Surface Plasmon Resonance
journal, February 2005
- Shi, Weili; Sahoo, Y.; Swihart, Mark T.
- Langmuir, Vol. 21, Issue 4
Synergistic Catalysis over Bimetallic Alloy Nanoparticles
journal, January 2013
- Singh, Ashish Kumar; Xu, Qiang
- ChemCatChem, Vol. 5, Issue 3
Superior long-term activity for a Pt-Re alloy compared to Pt in methanol oxidation reactions
journal, March 2017
- Duke, Audrey S.; Xie, Kangmin; Monnier, John R.
- Surface Science, Vol. 657
Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation
journal, June 2015
- Personick, Michelle L.; Zugic, Branko; Biener, Monika M.
- ACS Catalysis, Vol. 5, Issue 7
Nanoporous Gold Catalysts for Selective Gas-Phase Oxidative Coupling of Methanol at Low Temperature
journal, January 2010
- Wittstock, A.; Zielasek, V.; Biener, J.
- Science, Vol. 327, Issue 5963
Synergy in the Catalytic Activity of Bimetallic Nanoparticles and New Synthetic Methods for the Preparation of Fine Chemicals
journal, August 2014
- Notar Francesco, Irene; Fontaine-Vive, Fabien; Antoniotti, Sylvain
- ChemCatChem, Vol. 6, Issue 10
Modular Design of Advanced Catalytic Materials Using Hybrid Organic-Inorganic Raspberry Particles
journal, December 2017
- Shirman, Elijah; Shirman, Tanya; Shneidman, Anna V.
- Advanced Functional Materials, Vol. 28, Issue 27
Works referencing / citing this record:
New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd−Au Catalysts
journal, December 2019
- Guan, Erjia; Foucher, Alexandre C.; Marcella, Nicholas
- ChemCatChem, Vol. 12, Issue 3