Abstract

Nitrogen-doped graphene (NDG)-palladium (Pd)-based nanocatalysts (NDG@Pd) can be potentially applied as an efficient catalyst for the preparation of biaryls in a Suzuki–Miyaura coupling reaction. Herein, we report the one-pot facile synthesis of an NDG@Pd nanocatalyst, wherein the nanocatalyst was prepared by the simultaneous reduction of graphene oxide (GRO) and PdCl2 in the presence of hydrazine hydrate as a reducing agent, while ammonium hydroxide was used as a source of “N’’ on the surface of graphene. The as-synthesized NDG@Pd nanocatalyst, consisting of smaller-sized, spherical-shaped palladium nanoparticles (Pd-NPs) on the surface of NDG, was characterized by several spectroscopic and microscopic techniques, including high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), ultraviolet–visible spectroscopy (UV-Vis), Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and Brunauer–Emmett–Teller (BET). The nanocatalyst displayed outstanding catalytic activity in the Suzuki–Miyaura cross-coupling reactions of phenyl halides with phenyl boronic acids under facile conditions in water. The catalytic activity of NDG@Pd was found to be a more efficient catalyst when compared to pristine highly reduced graphene oxide (HRG) based Pd nanocatalyst (HRG@Pd). Furthermore, the reusability of the catalyst was also tested by repeatedly performing the same reaction using the recovered catalyst. The N-doped catalyst displayed excellent reusability even after several reactions.

Highlights

  • Graphene is a carbon allotrope in which an atomically thin layer of sp2 hybridized carbon atoms are densely packed, i.e., in a honeycomb crystal lattice [1,2]

  • In order to study the effect of nitrogen doping on the catalytic activity of nanocatalyst, the catalytic activity of the nitrogen-doped graphene (NDG)@Pd was compared to highly reduced graphene oxide (HRG)@Pd, which was prepared in the resultant nanocatalyst, the catalytic activity of the nitrogen-doped graphene-based palladium (NDG@Pd) was compared to highly reduced graphene-based palladium nanocatalysts (HRG@Pd), which the absence of a doping

  • We developed a one-pot method for the preparation of NDG@Pd nanocatalysts and studied their catalytic activity in Suzuki–Miyaura coupling reactions. This novel nitrogen-doped graphene-based palladium catalyst was prepared by using NH4 OH and hydrazine hydrate as doping and reducing agents

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Summary

Introduction

Graphene is a carbon allotrope in which an atomically thin layer of sp hybridized carbon atoms are densely packed, i.e., in a honeycomb crystal lattice [1,2] This ‘’2D” material displays exclusive electronic qualities and high crystal properties and is considered to be novel material for a variety of exciting applications, including catalysis [3,4,5]. Catalysts 2019, 9, 469 performance in several advanced applications ranging from the medical to the energy sector, including catalysis [7,8] In this regard, highly reduced graphene oxide (HRG) exhibits the potential to be a promising catalyst, and to function as an attractive support material in a variety of hybrid catalysts. Graphene-based palladium nanocomposites have been largely applied in a variety of catalytic applications

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