1 research outputs found
Facet Effect of Single-Crystalline Pd Nanocrystals for Aerobic Oxidation of 5‑Hydroxymethyl-2-furfural
Single-crystalline
Pd nanocrystals enclosed by {111} or {100} facets with controllable
sizes were synthesized and originally employed as catalysts in the
aerobic oxidation of 5-hydroxymethyl-2-furfural (HMF). The experimental
results indicated that the particle size and exposed facet of Pd nanocrystals
could obviously influence their catalytic performance. The size-dependent
effect of Pd nanocrystals in this reaction could only be derived from
the different Pd dispersions. Therefore, the facet effect of Pd nanocrystals
was first investigated in this work through experimental and theoretical
approaches. It was found that Pd-NOs enclosed by {111} facets were
more efficient than Pd-NCs enclosed by {100} facets for the aerobic
oxidation of HMF, especially for the oxidation step from 5-hydroxymethyl-2-furancarboxylic
acid (HMFCA) toward 5-formyl-2-furancarboxylic acid (FFCA). The TOF
value of Pd-NOsÂ(6 nm) was 2.6 times as high as that of Pd-NCsÂ(7 nm)
and 5.2 times higher than that of commercial Pd/C catalyst for HMF
oxidation. Through density functional theory (DFT) calculations, the
notably enhanced catalytic performance of Pd-NOs could be mainly attributed
to the lower energy barrier in the alcohol oxidation step (from HMFCA
to FFCA) and higher selectivity for O<sub>2</sub> hydrogenation to
produce peroxide