Palladium on S,N-Containing Carbon Materials Derived from Covalent Triazine-Based Frameworks (CTF) for C-C Coupling and Electrocatalytic Hydrogen Production

Abstract

In light of increasing population pressures, constrained natural resources and escalating energy requirements, the advancement of energy research and pharmaceutical development has become urgent. In this regard, we employed an ionothermal method to synthesize a covalent triazine framework (CTF) using 2,3,6,7-tetra(4-cyanophenyl)tetrathiafulvalene (TTFCN) and ZnCl₂ (1:10 molar ratio) at 400 °C. Subsequently, palladium ions or palladium nanoparticles (Pd-NPs) supported CTF material, named as CTFTTF@Pd has been prepared through an in-situ process in the absence of any reducing agent. The synthesized CTFTTF@Pd was characterized using FTIR, PXRD, X-ray photoelectron spectroscopy (XPS), SEM, TEM, and N₂ sorption measurements. The presence of C, N, S and Pd was confirmed by XPS analysis. TEM analysis confirmed the uniform distribution of Pd(II) and Pd(0) sites within CTFTTF@Pd, with an average particle size of approximately 8 nm. The catalyst CTFTTF@Pd exhibited superior efficiency and reusability in Suzuki–Miyaura cross-coupling reactions. The small Pd-NPs in CTFTTF@Pd enhanced the surface-active site density, driving superior catalytic activity. In addition, the electrocatalytic hydrogen evolution performance in alkaline media was investigated, exhibiting excellent long-term cycling stability. This work highlights the potential of S,N-containing carbon materials to generate catalytically active metal ions without the use of reducing agents, offering a strategy for designing recyclable catalysts for efficient chemical and energy production.