Design of Pd@Graphene oxide framework nanocatalyst with improved activity and recyclability in Suzuki-Miyaura cross-coupling reaction

• Published in: Applied catalysis. A, General General, 2018-01, Vol.549, p.60-67
• Main Authors: Tran, Thuy Phuong Nhat, Thakur, Ashutosh, Trinh, Dai Xuan, Dao, Anh Thi Ngoc, Taniike, Toshiaki
• Format: Article
• Language: English
• Subjects: Benzene; Catalysis; Catalysts; Chemical reactions; Chemical synthesis; Coupling; Cross coupling; Design for recycling; Graphene; Graphene oxide framework; Interlayers; Nanoparticles; Noble metals; Palladium; Palladium nanocatalysts; Particle size distribution; Pore encapsulation; Recyclability; Salt; Solvents; Suzuki-Miyaura cross-coupling
• ISSN: 0926-860X; 1873-3875
• DOI: 10.1016/j.apcata.2017.09.026

[Display omitted] •A graphene oxide framework (GOF) obtained by the intercalation of diboronic ester was utilized as a solid support in heterogeneous catalysis.•The gallery space of GOF afforded well-dispersed and uniformly-sized Pd NPs.•The Pd@GOF exhibited superior performance in Suzuki-Miyaura cross-coupling reaction compared to the Pd/C and graphene oxide-supported Pd nanocatalysts.•Comparison of recyclability with Pd NPs supported on a monoboronic ester-intercalated GOF revealed the significance of a rigid framework in the stabilization of Pd NPs. We describe a new method to synthesize a catalyst comprising of Pd nanoparticles encapsulated in a graphene oxide framework (Pd@GOF). GO was first intercalated with benzene-1,4-diboronic acid to afford a three-dimensional (3D) framework with uniform interlayer spaces, in which Pd nanoparticles were generated through salt reduction. Thus formed Pd nanoparticles were highly dispersed and stabilized inside a graphitic gallery space with a narrow particle size distribution. Thus obtained Pd@GOF catalyst exhibited an outperforming activity toward the Suzuki-Miyaura cross-coupling reaction in both polar and apolar solvents. Moreover, it can be reused for at least five cycles without any significant loss of the activity, while commercial Pd/C and Pd/GO exhibited a clear drop in the activity. These findings would establish the GOF as a promising scaffold to host noble metal nanoparticles and to construct desired metal@GOF nanocatalysts with improved activity and durability, which must be attractive for a broad range of practical applications.