Abstract

Graphdiyne (GD), a novel two dimensional (2D) carbon material, has earned a lot of attention in recent years. Constructing a novel hybrid nanomaterial based on GD, macrocyclic host and Au nanoparticles is an effective strategy for heterogeneous catalysis applications. While tremendous advancements in the preparation of two dimensional (2D) materials anchoring Au nanoparticles have been made, it is an urgent requirement to explore a green, efficient and facile approach for obtaining small-sized Au nanoparticles. The use of the 2D material graphdiyne (GD) presents more-promising candidates for constructing excellent sites for loading metal nanoparticles. In this study, a novel 2D heterogeneous hybrid nanomaterial (P5A-Au-GD) based on GD and pillar[5]arene (P5A)-reduced Au nanoparticles (P5A-Au) was successfully prepared. In this strategy, the P5A can reduce HAuCl4 with the aid of NaOH in the dispersion of GD. Accordingly, the generated P5A-Au can immediately interact with GD to form the P5A-Au-GD hybrid nanomaterial without any harsh reduced materials or other energies. The Au nanoparticles with average diameter of 2–3 nm are homogeneously dispersed on the surface of GD. The heterogeneous 2D catalyst of P5A-Au-GD shows high catalytic performances in the reduction of 4-nitrophenol and methylene blue by comparing commercial Pd/C catalyst. Meanwhile, the unique 2D heterogeneous hybrid material P5A-Au-GD exhibits durable recyclability and stability during the catalytic reaction. Considering the outstanding merits of the heterogeneous 2D catalyst of P5A-Au-GD as well as the simple and green preparation, this study might not only present enormous opportunities for the stabilized, high-performance and sustainable catalysts but also be applied in other frontier studies of sustainable functionalized nanocomposites and advanced materials.

Highlights

  • Carbon materials, such as carbon nanotube, porous carbons and graphene, have received enormous attention owing to their potential technological value in sensing, catalysis, batteries, nanoelectronics and so forth.[1,2,3] Among these carbon materials, the two dimensional (2D) carbon materials are frequently studied due to their excellent properties including optical electrical properties

  • Characterization of P5A-Au-GD The prepared materials of GD and P5A-Au-GD were characterized by Fourier transform infrared (FTIR) spectroscopy

  • High resolution transmission electron microscopy (TEM) (HRTEM) image of P5A-AuGD demonstrates the highlighted crystal lattice spacing with 0.228 nm Au nanoparticles (Fig. 2c) and the size of Au nanoparticles is measured as shown in Fig. 2d, which implies that the diameter of Au nanoparticles is approximately 2.75 Æ 0.62 nm

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Summary

Introduction

Carbon materials, such as carbon nanotube, porous carbons and graphene, have received enormous attention owing to their potential technological value in sensing, catalysis, batteries, nanoelectronics and so forth.[1,2,3] Among these carbon materials, the two dimensional (2D) carbon materials are frequently studied due to their excellent properties including optical electrical properties. The 2D polymers, constructed by covalent bond linkages are the novel 2D materials.[4,5] Graphdiyne (GD), generated by sp- and sp2-hybridized 2D graphene-like material, shows highly conjugated p system, controllable electronic property and conformably distributed pores, and can be used in different elds comparable to conventional sp2-hybridized With these outstanding features in mind, we study the integration of the at sp- and sp2-hybridized GD and Au nanoparticles for catalytic applications.[20] We anticipate that the interaction between Au nanoparticles and the alkyne and aryl pconjugated networks of GD would be bene cial for stabilizing Au nanoparticles from aggregation.[21,22] In addition, the preeminent porous structure of GD could embed the Au nanoparticles with a forceful adsorption energy.[23,24] the splendid chemical stability and electrical conductivity allow GD to act as 2D material support for the catalysts. The Au nanoparticles were facilely obtained by the redox reaction between hydroxyl pillar[5]arene (P5A) and HAuCl4 at room temperature without using any harsh reducing agent This process of synthesizing Au nanoparticles was carried out in the presence of GD. Considering the outstanding merits of P5A-Au-GD heterogeneous 2D catalyst as well as the simple and green preparation, this research might present enormous opportunities for the stabilized, high-performance and sustainable catalyst and be applied in other frontier studies of sustainable functionalized nanocomposites and advanced materials (Scheme 1)

Materials
Synthesis of GD
Preparation of P5A-Au-GD
Catalytic activity of P5A-Au-GD towards the reduction of 4-NP and MB
Results and discussion
Microstructure characterization of P5A-Au-GD
Catalytic activity of P5A-Au-GD
Conclusions
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