One-Step Pyrolysis Preparation of 1.1.1 Oriented Gold Nanoplatelets Supported on Graphene and Six Orders of Magnitude Enhancement of the Resulting Catalytic Activity.

Pyrolysis of chitosan films containing Au(3+) renders 1.1.1 oriented Au nanoplatelets (20 nm lateral size, 3-4 nm height) on a few layers of N-doped graphene (Au/fl-G), while the lateral sides were 0.0.1 oriented. Comparison of the catalytic activity of Au/fl-G films with powders of unoriented Au NPs supported on graphene showed that Au/fl-G films exhibit six orders of magnitude enhancement for three gold-catalyzed reactions, namely, Ullmann-like homocoupling, C-N cross coupling, and the oxidative coupling of benzene to benzoic acid. This enhancement is the result of the defined morphology, facet orientation of Au nanocrystals, and strong gold-graphene interaction.

Construction of N, P Co-Doped Carbon Frames Anchored with Fe Single Atoms and Fe2 P Nanoparticles as a Robust Coupling Catalyst for Electrocatalytic Oxygen Reduction.

A coupling catalyst of highly dispersed N, P co-doped carbon frames (NPCFs) anchored with Fe single atoms (SAs) and Fe2 P nanoparticles (NPs) is synthesized by a novel in situ doping-adsorption-phosphatization strategy for the electrocatalytic oxygen reduction reaction (ORR). The optimized Fe SAs-Fe2 P NPs/NPCFs-2.5 catalyst shows a superior ORR activity and stability in 0.5 m H2 SO4 and 0.1 m KOH, respectively. Theoretical calculations reveal a synergistic effect, in that the existence of Fe2 P weakens the adsorption of ORR intermediates on active sites and lowers the reaction free energy. The doped P atoms with a strong electron-donating ability elevate the energy level of Fe-3d orbitals and facilitate the adsorption of O2 . The active Fe atoms exist in a low oxidation state and are less positively charged, and they serve as an electron reservoir capable of donating and releasing electrons, thus improving the ORR activity. Operando and in situ characterization results indicate that the atomically dispersed FeN4 /FeP coupled active centers in the Fe SAs-Fe2 P NPs/NPCFs-2.5 catalyst are characteristic of the different catalytic mechanisms in acidic and alkaline media. This work proposes a novel idea for constructing coupling catalysts with atomic-level precision and provides a strong reference for the development of high-efficiency ORR electrocatalysts for practical application.