New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica
- Harvard Univ., Cambridge, MA (United States)
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.
- 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); National Science Foundation (NSF)
- Grant/Contract Number:
- SC0012573
- OSTI ID:
- 1469871
- Alternate ID(s):
- OSTI ID: 1408783
- Journal Information:
- Chemistry - A European Journal, Vol. 24, 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; ISSN 0947-6539
- Publisher:
- ChemPubSoc EuropeCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd−Au Catalysts
|
journal | December 2019 |
Similar Records
Dilute Pd-in-Au alloy RCT-SiO2 catalysts for enhanced oxidative methanol coupling
Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2