Improving Catalytic Activity towards the Direct Synthesis of H2O2 through Cu Incorporation into AuPd Catalysts

Abstract

With a focus on catalysts prepared by an excess-chloride wet impregnation procedure and supported on the zeolite ZSM-5(30), the introduction of low concentrations of tertiary base metals, in particular Cu, into supported AuPd nanoparticles can be observed to enhance catalytic activity towards the direct synthesis of H2O2. Indeed the optimal catalyst formulation (1%AuPd(0.975)Cu(0.025)/ZSM-5) is able to achieve rates of H2O2 synthesis (115 molH2O2kgcat−1h−1) approximately 1.7 times that of the bi-metallic analogue (69 molH2O2kgcat−1h−1) and rival that previously reported over comparable materials which use Pt as a dopant. Notably, the introduction of Cu at higher loadings results in an inhibition of performance. Detailed analysis by CO-DRFITS and XPS reveals that the improved performance observed over the optimal catalyst can be attributed to the electronic modification of the Pd species and the formation of domains of a mixed Pd2+/Pd0 oxidation state as well as structural changed within the nanoalloy.