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. 2017 Jan 7;41(1):177-183.
doi: 10.1039/C6NJ02898E. Epub 2016 Nov 11.

Influence of Graphene Oxide Supports on Solution-Phase Catalysis of Thiolate-Protected Palladium Nanoparticles in Water

Vivian Chen  1 , Hanqing Pan  1 , Roxanne Jacobs  1 , Shahab Derakhshan  1 , Young-Seok Shon  1
Affiliations

Influence of Graphene Oxide Supports on Solution-Phase Catalysis of Thiolate-Protected Palladium Nanoparticles in Water

Vivian Chen et al. New J Chem. .

Abstract

The influence of graphene oxide supports and thiolate surface ligands on the catalytic activity of colloidal Pd nanoparticles for alkyne hydrogenation in water is investigated. The studies show that unsupported, water-soluble thiolate-capped Pd nanoparticle catalysts favor the semi-hydrogenation over full-hydrogenation of dimethyl acetylene dicarboxylate (DMAD) under the atmospheric pressure and at room temperature. Pd nanoparticles supported on graphene oxide exhibit a similar activity for the hydrogenation of DMAD, but they show an improved long-term colloidal stability in aqueous solution after multiple catalytic cycles. After the heat treatment of Pd nanoparticles supported on graphene oxide at 300 °C, these heated hybrids exhibit an enhanced catalytic activity towards the full-hydrogenation. Overall, the studies suggest some influences of graphene oxide supports on the stability and thiolate surface ligands on the activity and selectivity of Pd nanoparticle catalysts.

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Figures

Fig 1
Fig 1
TEM images and histograms of (a) PdNP and (b) PdNP/GO hybrids. Scale bars are 20 nm.
Fig 2
Fig 2
TEM image of PdNP/GO heated at 300 °C. Scale bar is 20 nm.
Fig 3
Fig 3
Kinetic plot of hydrogenation of DMAD using PdNP, PdNP/GO, and the heated PdNP/GO (300 °C) catalysts. The complete hydrogenation of alkyne to alkene requires the degree of hydrogenation to be 2.
Fig 4
Fig 4
Results from the 3rd recycling reactions for all three catalysts compared to the average of catalytic reactions using fresh catalysts (1st use). The catalysis result from the reaction using the regenerated PdNP/GO at 300 °C is also included in the figure. The complete hydrogenation of alkyne to alkene requires the degree of hydrogenation to be 2.
Fig 5
Fig 5
Reaction systems before and after 24 hour DMAD hydrogenation reactions with (a) PdNP, (b) PdNP/GO, and (c) PdNP/GO heated at 300°C.
Scheme 1
Scheme 1
Synthetic scheme for ω-carboxylate-1-hexanethiolate-capped palladium nanoparticles (PdNP).
See this image and copyright information in PMC

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