摘要：Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift ***,the molecular reaction mechanism of water-gas shift reaction at these interfaces still remains ***,water-gas shift reaction at Pt-NiO interfaces has been in-situ explored using surface-enhanced Raman spectroscopy by construction of Au@Pt@NiO *** Raman spectroscopic evidence demonstrates that water-gas shift reaction at Pt-NiO interfaces proceeds via an associative mechanism with the carbonate species as a key *** carbonate species is generated through the reaction of adsorbed CO with gaseous water,and its decomposition is a slow step in water-gas shift ***,the Pt-NiO interfaces would promote the formation of this carbonate intermediate,thus leading to a higher activity compared with pure *** spectral information deepens the fundamental understanding of the reaction mechanism of water-gas shift reaction,which would promote the design of more efficient catalysts.

摘要：Alloying Pt with transition metals can significantly improve the catalytic properties for the oxygen reduction reaction(ORR).However,the application of Pt-transition metal alloys in fuel cells is largely limited by poor long-term durability because transition metals can easily *** this study,we developed a nonmetallic doping approach and prepared a P-doped Pt catalyst with excellent durability for the ***-supported core-shell nanoparticles with a P-doped Pt core and Pt shell(denoted as PtPx@Pt/C)were synthesized via heat-treatment phosphorization of commercial Pt/C,followed by acid *** analysis using electron energy loss spectroscopy and X-ray photoelectron spectroscopy clearly demonstrated that Pt was enriched in the near-surface region(approximately 1 nm)of the carbon-supported core-shell *** to P doping,the ORR specific activity and mass activity of the PtP_(1.4)@Pt/C catalyst were as high as 0.62 mA cm^(–2)and 0.31 mAμgPt–^(1),respectively,at 0.90 V,and they were enhanced by 2.8 and 2.1 times,respectively,in comparison with the Pt/C *** importantly,PtP_(1.4)@Pt/C exhibited superior stability with negligible mass activity loss(6%after 30000 potential cycles and 25%after 90000 potential cycles),while Pt/C lost 46%mass activity after 30000 potential *** high ORR activity and durability were mainly attributed to the core-shell nanostructure,the electronic structure effect,and the resistance of Pt nanoparticles against aggregation,which originated from the enhanced ability of the PtP_(1.4)@Pt to anchor to the carbon *** study provides a new approach for constructing nonmetal-doped Pt-based catalysts with excellent activity and durability for the ORR.