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

Abstract

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 SiO 2 matrix (SiO 2–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 Ag 3Au 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 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 widemore » 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.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. 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) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1469871
Alternate Identifier(s):
OSTI ID: 1408783
Grant/Contract Number:  
[SC0012573; 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. doi: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. doi: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 = {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–AgxAuy)—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–AgxAuy 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.},
doi = {10.1002/chem.201704552},
journal = {Chemistry - A European Journal},
number = [8],
volume = [24],
place = {United States},
year = {2017},
month = {9}
}

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