Atomically dispersed Ru catalysts for polychlorinated aromatic hydrocarbon oxidation

Abstract

The development of cost-efficient catalysts with good catalytic activity is an urgent task for polychlorinated aromatic hydrocarbon (PCAH) oxidation. Herein, atomically dispersed Ru catalysts (denoted as Ru ADCs) proved by aberration corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy were synthesized for PCAH oxidation. The oxidation results showed that 0.2 Ru ADCs exhibited enhanced catalytic activity (T_50% < 250 °C, T_90% < 300 °C) compared with the T_90% > 300 °C on 0.2 Ru nanoparticles (NPs). Besides, 0.2 Ru ADCs demonstrated high CO₂ yield with >60% CO₂ ratio, along with good stability (>80% conversion for 800 mins). The better performance of 0.2 Ru ADCs was verified by kinetic experiments, in which, the apparent activation energy associated with 0.2 Ru ADCs (50.8 kJ mol⁻¹) was significantly lower compared with that with 0.2 Ru NPs (80.0 kJ mol⁻¹). The superior oxidation activity of 0.2 Ru ADCs was also applied to toluene oxidation. H₂ temperature-programmed reduction ensured the stronger interaction of Ru species with the supports in Ru ADCs than that in Ru NPs, thus inhibiting Ru species aggregation and favoring their higher dispersion ensured by CO temperature-programmed desorption. The present work provides a potential strategy to maximize the usage of noble metal catalysts for PCAH oxidation.