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Thermodynamic Control of Metal Loading and Composition of Carbon Aerogel Supported Pt–Cu Alloy Nanoparticles by Supercritical Deposition
journal contribution
posted on 2016-02-19, 13:55 authored by S. E. Bozbag, U. Unal, M. A. Kurykin, C. J. Ayala, M. Aindow, C. ErkeyCarbon
aerogel (CA) supported Pt–Cu bimetallic nanoparticles
were synthesized via simultaneous adsorption of bis(1,1,1,3,5,5,6,6,6-nonafluorohexane-2,4-diiminate)copper
(CuDI6) and dimethyl(1,5-cyclooctadiene)platinum(II) (Pt(cod)me2) onto CAs in the presence of supercritical carbon dioxide
(scCO2) and subsequent thermal conversion at ambient pressure.
Binary adsorption isotherms of metal precursors on CAs in scCO2 were measured at 35 °C and 10.6 MPa by analyzing the
fluid phase concentrations in a batch system and could be predicted
from pure component adsorption isotherms using ideal adsorbed solution
theory (IAST). Homogeneously dispersed Pt–Cu nanoparticles
were formed on the surface of the CAs via the thermal conversion of
the precursors at 400 °C. As the Pt/Cu ratio decreased from 97:3
to 21:79, both the mean and the standard deviation of the particle
size increased from 2.9 to 7.2 nm and from 1.3 to 3.7 nm, respectively.
The alloying of Pt and Cu within the nanoparticles was confirmed via
XRD peak shifts, and XPS data indicated that the surfaces of these
Pt–Cu alloy nanoparticles were enriched in Pt.
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IASTbatch systemparticle sizenanoparticlescCO 2XPS data10.6 MPa3.7 nmPtfluid phase concentrationscarbon dioxideCarbon Aerogelambient pressureXRD peak shiftssolution theoryMetal Loadingmetal precursors7.2 nmCASupercritical DepositionCarbon aerogelBinary adsorption isothermscomponent adsorption isothermsThermodynamic Control
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