Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift reaction.However,the molecular reaction mechanism of water-gas shift reaction at these interfaces still rem...Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift reaction.However,the molecular reaction mechanism of water-gas shift reaction at these interfaces still remains unclear.Herein,water-gas shift reaction at Pt-NiO interfaces has been in-situ explored using surface-enhanced Raman spectroscopy by construction of Au@Pt@NiO nanostructures.Direct 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 intermediate.The carbonate species is generated through the reaction of adsorbed CO with gaseous water,and its decomposition is a slow step in water-gas shift reaction.Moreover,the Pt-NiO interfaces would promote the formation of this carbonate intermediate,thus leading to a higher activity compared with pure Pt.This spectral information deepens the fundamental understanding of the reaction mechanism of water-gas shift reaction,which would promote the design of more efficient catalysts.展开更多
Electrochemical energy devices such as fuel cells have received extensive concern in recent decades.However,the commercial applications of fuel cells have been restricted by the slow kinetics of oxygen reduction react...Electrochemical energy devices such as fuel cells have received extensive concern in recent decades.However,the commercial applications of fuel cells have been restricted by the slow kinetics of oxygen reduction reaction(ORR).Pd-based fuel cell catalysts are strong candidates for enhanced ORR activities,especially under alkaline conditions.Therefore,extensive exploration has been made to improve the performance of Pd-based nano-catalysts for oxygen reduction reaction.This paper reviews the research progress of preparation,electrocatalytic performance,and in-situ characterization of various Pd-based oxygen reduction catalysts,from zero-dimensional nanoparticles,to one-dimensional nanowires,to two-dimensional nanosheets,and to Pd single-atom catalysts.It may provide some help for improving the activity of Pd-based catalysts and understanding the reaction mecha-nisms and structure-activity relationships.展开更多
Core-shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies,catalysis,energy,and other fields because of their splendid properties such as...Core-shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies,catalysis,energy,and other fields because of their splendid properties such as multifunctionality,stability,and adjustability.In this article,we summarized the endeavors made by our group in the past decade about the core-shell nanostructures in the shell-isolated nanoparticle-enhanced Raman spectroscopy(SHINERS)and plasmon-enhanced spectroscopies.Meanwhile,the potential challenges and perspectives about core-shell nanostructures in spectroscopies have also been proposed.Thus,we believe this article would provide an avenue for a comprehensive understanding of enhanced spectroscopies with core-shell nanostructures.展开更多
文摘Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift reaction.However,the molecular reaction mechanism of water-gas shift reaction at these interfaces still remains unclear.Herein,water-gas shift reaction at Pt-NiO interfaces has been in-situ explored using surface-enhanced Raman spectroscopy by construction of Au@Pt@NiO nanostructures.Direct 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 intermediate.The carbonate species is generated through the reaction of adsorbed CO with gaseous water,and its decomposition is a slow step in water-gas shift reaction.Moreover,the Pt-NiO interfaces would promote the formation of this carbonate intermediate,thus leading to a higher activity compared with pure Pt.This spectral information deepens the fundamental understanding of the reaction mechanism of water-gas shift reaction,which would promote the design of more efficient catalysts.
基金National Key Research and Development Program of China(2020YFB1505800)National Natural Science Foundation of China(21925404,21972117,22122205,and 22021001)+1 种基金the Central Guidance on Local Science and Technology Development Fund of Shenzhen(2021Szvup065)the State Key Laboratory of Fine Chemicals(KF2002).
文摘Electrochemical energy devices such as fuel cells have received extensive concern in recent decades.However,the commercial applications of fuel cells have been restricted by the slow kinetics of oxygen reduction reaction(ORR).Pd-based fuel cell catalysts are strong candidates for enhanced ORR activities,especially under alkaline conditions.Therefore,extensive exploration has been made to improve the performance of Pd-based nano-catalysts for oxygen reduction reaction.This paper reviews the research progress of preparation,electrocatalytic performance,and in-situ characterization of various Pd-based oxygen reduction catalysts,from zero-dimensional nanoparticles,to one-dimensional nanowires,to two-dimensional nanosheets,and to Pd single-atom catalysts.It may provide some help for improving the activity of Pd-based catalysts and understanding the reaction mecha-nisms and structure-activity relationships.
基金the National Key Research and Development Program of China(Nos.2020YFB1505800 and 2019YFA0705400)the National Natural Science Foundation of China(NSFC)(Nos.21925404,22002128,21972117,and 21902137)+1 种基金the Fundamental Research Funds for the Central Universities(No.20720210069)the Science and Technology Planning Project of Fujian Province(No.2019Y4001).
文摘Core-shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies,catalysis,energy,and other fields because of their splendid properties such as multifunctionality,stability,and adjustability.In this article,we summarized the endeavors made by our group in the past decade about the core-shell nanostructures in the shell-isolated nanoparticle-enhanced Raman spectroscopy(SHINERS)and plasmon-enhanced spectroscopies.Meanwhile,the potential challenges and perspectives about core-shell nanostructures in spectroscopies have also been proposed.Thus,we believe this article would provide an avenue for a comprehensive understanding of enhanced spectroscopies with core-shell nanostructures.
