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. 2015;7(3):307-315.
doi: 10.1007/s40820-015-0044-6. Epub 2015 Jun 9.

Green-chemistry Compatible Approach to TiO2-supported PdAu Bimetallic Nanoparticles for Solvent-free 1-Phenylethanol Oxidation under Mild Conditions

Jian-Bing Chang  1 , Chang-Hai Liu  1 , Jie Liu  1 , Yu-Yan Zhou  1 , Xu Gao  1 , Sui-Dong Wang  1
Affiliations

Green-chemistry Compatible Approach to TiO2-supported PdAu Bimetallic Nanoparticles for Solvent-free 1-Phenylethanol Oxidation under Mild Conditions

Jian-Bing Chang et al. Nanomicro Lett. 2015.

Abstract

TiO2-supported PdAu bimetallic nanoparticles (NPs) with small size and good dispersity were prepared by the room-temperature ionic liquid-assisted bimetal sputtering, which is simple, environmentally friendly, and free of additives and byproducts. Pd/Au atomic ratio can be tuned by controlling the sputtering conditions simply. High catalytic activity was found in PdAu-NPs-TiO2 hybrids for solvent-free selective oxidation of 1-phenylethanol using O2 as the oxidant at the low temperature of 50 °C and low pressure of 1 atm. It was found that Pd/Au ratio strongly affected the catalytical activity, and the highest conversion of about 35 % and turnover frequency of about 421 h-1 were achieved at 1:1 of Pd/Au atomic ratio. The synergistic effect in PdAu NPs was also discussed based on the comprehensive characterization results. The present approach may offer an alternative platform for future development of green-chemistry compatible bimetallic nanocatalysts.

Keywords: Electronic structure; PdAu nanoparticles; TiO2 nanosupport.

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Figures

Scheme 1
Scheme 1
Preparation method for PdAu–NPs–TiO2 hybrids: Successive sputtering of Au and Pd onto RTIL of [BMIm][BF4], in which TiO2 NPs are pre-dispersed
Fig. 1
Fig. 1
TEM images and NPs size distributions of a TiO2 NPs as the support, b Au NPs on TiO2, c PdAu (1:4) NPs on TiO2, d PdAu (1:1) NPs on TiO2, e PdAu (4:1) NPs on TiO2, and f Pd NPs on TiO2. TEM images in the middle are magnified square region shown in the left
Fig. 2
Fig. 2
HAADF-STEM images of PdAu (1:1) NPs on TiO2 a in large scale and b in selective small scale. Elemental mapping for c Au, d Pd, e Ti, and f O
Fig. 3
Fig. 3
UV–Vis absorption spectra of TiO2-supported metal NPs with different Pd/Au atomic ratios
Fig. 4
Fig. 4
a XPS Au 4f spectra, b XANES Au L 3-edge spectra, and c XPS Pd 3d spectra of TiO2-supported metal NPs with different Pd/Au atomic ratios. Inset in b is magnified whiteline region, where Au L 3-edge jump is normalized
Fig. 5
Fig. 5
XRD patterns of TiO2 NPs (anatase) and TiO2-supported metal NPs with different Pd/Au atomic ratios
Fig. 6
Fig. 6
Dependences of catalytic activity for 1-phenylethanol oxidation on Pd/Au atomic ratio in TiO2-supported metal NPs: a conversion (square) and selectivity (diamond); b turnover frequency (circle). The catalytic reaction is carried out at 323 K and 1 atm using O2 as the oxidant
See this image and copyright information in PMC

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