The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization ...The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization of the electrochemical energy technology.Herein,we report a facile synthesis of cobalt(Co)and nitrogen(N)co‐doped carbon nanotube@porous carbon(Co/N/CNT@PC‐800)electrocatalyst through a one‐step pyrolysis of waste paper,dicyandiamide,and cobalt(II)acetylacetonate.The surface of the hierarchical porous carbon supported a large number of carbon nanotubes(CNTs),which were derived from dicyandiamide through the catalysis of Co.The addition of Co resulted in the formation of a hierarchical micro/mesoporous structure,which was beneficial for the exposure of active sites and rapid transportation of ORR‐relevant species(O2,H+,OH?,and H2O).The doped N and Co formed more active sites to enhance the ORR activity of the electrocatalyst.The Co/N/CNT@PC‐800 material exhibited optimal ORR performance with an onset potential of 0.005 V vs.Ag/AgCl and a half‐wave potential of?0.173 V vs.Ag/AgCl.Meanwhile,the electrocatalyst showed an excellent methanol tolerance and a long‐term operational durability than that of Pt/C,as well as a quasi‐four‐electron reaction pathway.The low‐cost and simple synthesis approach makes the Co/N/CNT@PC‐800 a prospective electrocatalyst for the ORR.Furthermore,this work provides an alternative approach for exploring the use of biomass‐derived electrocatalysts for renewable energy applications.展开更多
Deoxygenative upgrading of 5-hydromethylfurfural(HMF)into valuable chemicals has attracted intensive research interest in recent years,with product selectivity control remaining an important topic.Herein,TiO_(2) suppo...Deoxygenative upgrading of 5-hydromethylfurfural(HMF)into valuable chemicals has attracted intensive research interest in recent years,with product selectivity control remaining an important topic.Herein,TiO_(2) supported gold catalysts coated with a thin N-doped porous carbon(NPC)layer were developed via a polydopamine-coating-carbonization strategy and utilized for pathway-specific conversion of HMF into 5-methylfurfural(5-MF)with the use of renewable formic acid(FA)as the deoxygenation reagent.The as-fabricated Au/TiO_(2)@NPC exhibited excellent catalytic performance with a high yield of 5-MF(>95%).The catalytic behavior of Au@NPC-based catalysts was shown to be correlated with the suitable combination of highly dispersed Au nanoparticles and favorable interfacial interactions in the Au@NPC core-shell hetero-nanoarchitectures,thereby facilitating the preferential esterification of HMF with FA and suppressing unproductive FA dehydrogenation,which promoted the selective formylation/decarboxylation of hydroxy-methyl group in HMF in a pathway-specific manner.The present NPC/metal interfacial engineering strategy may provide a potential guide for the rational design of advanced catalysts for a wide variety of heterogeneous catalysis processes in terms of the conversion of biomass source.展开更多
基金supported by the National Nature Science Foundation of China(21476098,21471069,21576123)International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council(20150060)~~
文摘The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization of the electrochemical energy technology.Herein,we report a facile synthesis of cobalt(Co)and nitrogen(N)co‐doped carbon nanotube@porous carbon(Co/N/CNT@PC‐800)electrocatalyst through a one‐step pyrolysis of waste paper,dicyandiamide,and cobalt(II)acetylacetonate.The surface of the hierarchical porous carbon supported a large number of carbon nanotubes(CNTs),which were derived from dicyandiamide through the catalysis of Co.The addition of Co resulted in the formation of a hierarchical micro/mesoporous structure,which was beneficial for the exposure of active sites and rapid transportation of ORR‐relevant species(O2,H+,OH?,and H2O).The doped N and Co formed more active sites to enhance the ORR activity of the electrocatalyst.The Co/N/CNT@PC‐800 material exhibited optimal ORR performance with an onset potential of 0.005 V vs.Ag/AgCl and a half‐wave potential of?0.173 V vs.Ag/AgCl.Meanwhile,the electrocatalyst showed an excellent methanol tolerance and a long‐term operational durability than that of Pt/C,as well as a quasi‐four‐electron reaction pathway.The low‐cost and simple synthesis approach makes the Co/N/CNT@PC‐800 a prospective electrocatalyst for the ORR.Furthermore,this work provides an alternative approach for exploring the use of biomass‐derived electrocatalysts for renewable energy applications.
文摘Deoxygenative upgrading of 5-hydromethylfurfural(HMF)into valuable chemicals has attracted intensive research interest in recent years,with product selectivity control remaining an important topic.Herein,TiO_(2) supported gold catalysts coated with a thin N-doped porous carbon(NPC)layer were developed via a polydopamine-coating-carbonization strategy and utilized for pathway-specific conversion of HMF into 5-methylfurfural(5-MF)with the use of renewable formic acid(FA)as the deoxygenation reagent.The as-fabricated Au/TiO_(2)@NPC exhibited excellent catalytic performance with a high yield of 5-MF(>95%).The catalytic behavior of Au@NPC-based catalysts was shown to be correlated with the suitable combination of highly dispersed Au nanoparticles and favorable interfacial interactions in the Au@NPC core-shell hetero-nanoarchitectures,thereby facilitating the preferential esterification of HMF with FA and suppressing unproductive FA dehydrogenation,which promoted the selective formylation/decarboxylation of hydroxy-methyl group in HMF in a pathway-specific manner.The present NPC/metal interfacial engineering strategy may provide a potential guide for the rational design of advanced catalysts for a wide variety of heterogeneous catalysis processes in terms of the conversion of biomass source.
