New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica

Shirman, Tanya; Lattimer, Judith; Luneau, Mathilde; Shirman, Elijah; Reece, Christian; Aizenberg, Michael; Madix, Robert J.; Aizenberg, Joanna; Friend, Cynthia M.

doi:10.1002/chem.201704552

New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica

Journal Article · Thu Sep 28 04:00:00 EDT 2017 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.201704552· OSTI ID:1469871

Shirman, Tanya ^[1]; Lattimer, Judith ^[1]; Luneau, Mathilde ^[1]; Shirman, Elijah ^[1]; Reece, Christian ^[1]; Aizenberg, Michael ^[1]; Madix, Robert J. ^[1]; Aizenberg, Joanna ^[1]; Friend, Cynthia M. ^[1]

Harvard Univ., Cambridge, MA (United States)

A highly modular synthesis of designed catalysts with controlled bimetallic nanoparticle size and composition and a well-defined structural hierarchy is shown. Exemplary catalysts—bimetallic dilute Ag-in-Au nanoparticles partially embedded in a porous SiO₂ matrix (SiO₂–Ag_xAu_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 Ag₃Au₉₇) 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 SiO₂–Ag_xAu_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 discussed.

View Accepted Manuscript (DOE)

Research Organization:: Harvard Univ., Cambridge, MA (United States). Energy Frontier Research Center (EFRC) Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)

Grant/Contract Number:: SC0012573

OSTI ID:: 1469871

Alternate ID(s):: OSTI ID: 1408783

Journal Information:: Chemistry - A European Journal, Journal Name: Chemistry - A European Journal Journal Issue: 8 Vol. 24; ISSN 0947-6539

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

References (20)

Modular Design of Advanced Catalytic Materials Using Hybrid Organic-Inorganic Raspberry Particles Shirman, Elijah; Shirman, Tanya; Shneidman, Anna V. Advanced Functional Materials, Vol. 28, Issue 27 https://doi.org/10.1002/adfm.201704559	journal	December 2017
Synergistic Catalysis over Bimetallic Alloy Nanoparticles Singh, Ashish Kumar; Xu, Qiang ChemCatChem, Vol. 5, Issue 3 https://doi.org/10.1002/cctc.201200591	journal	January 2013
Synergy in the Catalytic Activity of Bimetallic Nanoparticles and New Synthetic Methods for the Preparation of Fine Chemicals Notar Francesco, Irene; Fontaine-Vive, Fabien; Antoniotti, Sylvain ChemCatChem, Vol. 6, Issue 10 https://doi.org/10.1002/cctc.201402252	journal	August 2014
Experimental methods in catalytic kinetics Perego, C. Catalysis Today, Vol. 52, Issue 2-3 https://doi.org/10.1016/S0920-5861(99)00071-1	journal	September 1999
Exploiting basic principles to control the selectivity of the vapor phase catalytic oxidative cross-coupling of primary alcohols over nanoporous gold catalysts Wang, Lu-Cun; Stowers, Kara J.; Zugic, Branko Journal of Catalysis, Vol. 329 https://doi.org/10.1016/j.jcat.2015.04.022	journal	September 2015
Active sites for methanol partial oxidation on nanoporous gold catalysts Wang, Lu-Cun; Personick, Michelle L.; Karakalos, Stavros Journal of Catalysis, Vol. 344 https://doi.org/10.1016/j.jcat.2016.08.012	journal	December 2016
Interaction of silica-supported small silver clusters with molecular oxygen. A computational study Shor, Aleksey M.; Laletina, Svetlana S.; Ivanova Shor, Elena A. Surface Science, Vol. 630 https://doi.org/10.1016/j.susc.2014.08.022	journal	December 2014
Superior long-term activity for a Pt-Re alloy compared to Pt in methanol oxidation reactions Duke, Audrey S.; Xie, Kangmin; Monnier, John R. Surface Science, Vol. 657 https://doi.org/10.1016/j.susc.2016.11.007	journal	March 2017
Correlating the Atomic Structure of Bimetallic Silver–Gold Nanoparticles to Their Antibacterial and Cytotoxic Activities Padmos, J. Daniel; Langman, Maxine; MacDonald, Katelyn The Journal of Physical Chemistry C, Vol. 119, Issue 13 https://doi.org/10.1021/acs.jpcc.5b00145	journal	March 2015
Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation Personick, Michelle L.; Zugic, Branko; Biener, Monika M. ACS Catalysis, Vol. 5, Issue 7 https://doi.org/10.1021/acscatal.5b00330	journal	June 2015
Continuous Catalytic Production of Methyl Acrylates from Unsaturated Alcohols by Gold: The Strong Effect of C═C Unsaturation on Reaction Selectivity Zugic, Branko; Karakalos, Stavros; Stowers, Kara J. ACS Catalysis, Vol. 6, Issue 3 https://doi.org/10.1021/acscatal.5b02902	journal	February 2016
Nanoalloys: From Theory to Applications of Alloy Clusters and Nanoparticles Ferrando, Riccardo; Jellinek, Julius; Johnston, Roy L. Chemical Reviews, Vol. 108, Issue 3, p. 845-910 https://doi.org/10.1021/cr040090g	journal	March 2008
Gold Nanoshells on Polystyrene Cores for Control of Surface Plasmon Resonance Shi, Weili; Sahoo, Y.; Swihart, Mark T. Langmuir, Vol. 21, Issue 4 https://doi.org/10.1021/la047628y	journal	February 2005
Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts Zugic, Branko; Wang, Lucun; Heine, Christian Nature Materials, Vol. 16, Issue 5 https://doi.org/10.1038/nmat4824	journal	December 2016
A colloidoscope of colloid-based porous materials and their uses Phillips, Katherine R.; England, Grant T.; Sunny, Steffi Chemical Society Reviews, Vol. 45, Issue 2 https://doi.org/10.1039/C5CS00533G	journal	January 2016
Nanostructure of wet-chemically prepared, polymer-stabilized silver–gold nanoalloys (6 nm) over the entire composition range Ristig, S.; Prymak, O.; Loza, K. Journal of Materials Chemistry B, Vol. 3, Issue 23 https://doi.org/10.1039/C5TB00644A	journal	January 2015
Extremely fast Au–Ag alloy–dealloy associated reversible plasmonic modifications in SiO ₂ films Pramanik, Sourav; Chattopadhyay, Shreyasi; Das, Jugal Kishore Journal of Materials Chemistry C, Vol. 4, Issue 16 https://doi.org/10.1039/C5TC03123K	journal	January 2016
Designing bimetallic catalysts for a green and sustainable future Sankar, Meenakshisundaram; Dimitratos, Nikolaos; Miedziak, Peter J. Chemical Society Reviews, Vol. 41, Issue 24 https://doi.org/10.1039/c2cs35296f	journal	January 2012
Catalyst design for enhanced sustainability through fundamental surface chemistry Personick, Michelle L.; Montemore, Matthew M.; Kaxiras, Efthimios Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 374, Issue 2061 https://doi.org/10.1098/rsta.2015.0077	journal	February 2016
Nanoporous Gold Catalysts for Selective Gas-Phase Oxidative Coupling of Methanol at Low Temperature Wittstock, A.; Zielasek, V.; Biener, J. Science, Vol. 327, Issue 5963 https://doi.org/10.1126/science.1183591	journal	January 2010

Cited By (2)

New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd−Au Catalysts Guan, Erjia; Foucher, Alexandre C.; Marcella, Nicholas ChemCatChem, Vol. 12, Issue 3 https://doi.org/10.1002/cctc.201901847	journal	December 2019
Silica–titania hybrids for structurally robust inverse opals with controllable refractive index Phillips, Katherine R.; Shirman, Tanya; Aizenberg, Michael Journal of Materials Chemistry C, Vol. 8, Issue 1 https://doi.org/10.1039/c9tc05103a	journal	January 2020

Similar Records

Dilute Pd-in-Au alloy RCT-SiO₂ catalysts for enhanced oxidative methanol coupling

Journal Article · Wed Jun 09 00:00:00 EDT 2021 · Journal of Catalysis · OSTI ID:1977245

Effect of nanoscale flows on the surface structure of nanoporous catalysts

Journal Article · Thu Jun 01 00:00:00 EDT 2017 · Journal of Chemical Physics · OSTI ID:1388894

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
77 NANOSCIENCE AND NANOTECHNOLOGY
colloid templated porous materials
gold
heterogeneous catalysis
nanoparticles
selective oxidation
silver

New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica

Citation Formats

References (20)

Cited By (2)

Similar Records

Related Subjects