This work demonstrates a two-step method to produce oxide-derived Cu nanowires on Cu mesh surface to offer a monolithic catalyst that outstandingly improves the hydrogen production from reforming formaldehyde and wate...This work demonstrates a two-step method to produce oxide-derived Cu nanowires on Cu mesh surface to offer a monolithic catalyst that outstandingly improves the hydrogen production from reforming formaldehyde and water under ambient conditions.Our results not only reveal that the special oxidederived nanostructure can significantly improve the formaldehyde reforming performance of Cu,but also display that the hydrogen production has a linear relationship with oxygen pressure.Specially,a maximum of 36 times increment in hydrogen generation rate is observed than that without oxygen during the reaction.Density functional theory calculations show that the formaldehyde molecule is adsorbed on Cu surface only when the adsorbed oxygen is in adjacency,and hydrogen release process is the ratedetermining step.This work highlights that the activity of deliberately synthesized catalyst can further be promoted by dynamic chemical modulation of surface states during working.展开更多
The surface reactivity of metals is fundamentally dependent on the local electronic structure generally tailored by atomic compositions and configurations during the synthesis.Herein,we demonstrate that Cu,which is in...The surface reactivity of metals is fundamentally dependent on the local electronic structure generally tailored by atomic compositions and configurations during the synthesis.Herein,we demonstrate that Cu,which is inert for oxygen reduction reaction(ORR)due to the fully occupied d-orbital,could be activated by applying a visible-light irradiation at ambient temperature.The ORR current is increased to 3.3 times higher in the potential range between-0.1 and 0.4 V under the light of 400 mW·cm^-2,and the activity enhancement is proportional to the light intensity.Together with the help of the first-principle calculation,the remarkably enhanced electrocatalytic activity is expected to stem mainly from the decreased metal-adsorbate binding by photoexcita-tion.This finding provides an additional degree of freedom for controlling and manipulating the surface reactivity of metal catalysts besides materials strategy.展开更多
基金supported by the China Bao Wu Low Carbon Metallurgical Innovation Foundation(No.BWLCF202113)the Fundamental Research Funds for the Central Universities(Nos.N2202012,N180206004)the National Natural Science Foundation of China(No.51971059)。
文摘This work demonstrates a two-step method to produce oxide-derived Cu nanowires on Cu mesh surface to offer a monolithic catalyst that outstandingly improves the hydrogen production from reforming formaldehyde and water under ambient conditions.Our results not only reveal that the special oxidederived nanostructure can significantly improve the formaldehyde reforming performance of Cu,but also display that the hydrogen production has a linear relationship with oxygen pressure.Specially,a maximum of 36 times increment in hydrogen generation rate is observed than that without oxygen during the reaction.Density functional theory calculations show that the formaldehyde molecule is adsorbed on Cu surface only when the adsorbed oxygen is in adjacency,and hydrogen release process is the ratedetermining step.This work highlights that the activity of deliberately synthesized catalyst can further be promoted by dynamic chemical modulation of surface states during working.
基金supported by the National Natural Science Foundation of China(Grant No.51771047)the Fundamental Research Funds for the Central Universities(N180204014)。
文摘The surface reactivity of metals is fundamentally dependent on the local electronic structure generally tailored by atomic compositions and configurations during the synthesis.Herein,we demonstrate that Cu,which is inert for oxygen reduction reaction(ORR)due to the fully occupied d-orbital,could be activated by applying a visible-light irradiation at ambient temperature.The ORR current is increased to 3.3 times higher in the potential range between-0.1 and 0.4 V under the light of 400 mW·cm^-2,and the activity enhancement is proportional to the light intensity.Together with the help of the first-principle calculation,the remarkably enhanced electrocatalytic activity is expected to stem mainly from the decreased metal-adsorbate binding by photoexcita-tion.This finding provides an additional degree of freedom for controlling and manipulating the surface reactivity of metal catalysts besides materials strategy.
