Ultrafine PdAu nanoparticles immobilized on amine functionalized carbon black toward fast dehydrogenation of formic acid at room temperature

Abstract

Ultrafine and highly dispersed PdAu nanoparticles were immobilized on amine functionalized carbon black (VXC-72-NH₂) for dehydrogenation of formic acid (FA). The introduction of amines is of vital importance for the formation of ultrafine PdAu nanoparticles (∼1.5 nm). Moreover, the presence of the amino groups also increased the electron density of PdAu nanoparticles, and this effect facilitated the formation of metal-formate, which further enhanced the rate of the catalytic dehydrogenation of FA. The as-prepared Pd_0.6Au_0.4/VXC-72-NH₂ exhibited high catalytic activity and 100% H₂ selectivity for dehydrogenation of formic acid without any additive, with turnover frequency (TOF) values of 7385 h⁻¹ at 298 K and 17 724 h⁻¹ at 333 K, which are the highest TOF values ever reported among heterogeneous catalysts for FA dehydrogenation.