Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and a...Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and atomic-level insights into the structure-activity relationship of Pt_(n) remain a great challenge.Here,we present a combinatorial synthesis and analysis method to investigate the atomicity-activity relationships of Pt_(n) at the individual level.We employ single nanoparticle collision electrochemistry to facilitate the in-situ electrodeposition of a single precisely tunable Pt_(n) on the graphene quantum dot support,followed by instantaneous measurement of the intrinsic ORR activity of the resulting Pt_(n).By relying on highly sensitive electrochemical measurements,our investigations clarify the atomicity-specific ORR activity of Pt_(n),which is attributed to their distinct geometric and electronic structures at varying cluster sizes.Significantly,Pt_(n) with low atomicity,especially below 20,can reach extraordinarily high ORR activities due to atom-by-atom arrangement.Our work provides a simple and efficient method for investigating the atomicity-activity relationships of other nanoclusters under real reaction conditions,enabling a better design of the electrocatalysts at the atomic level.展开更多
基金financially supported by the National Natural Science Foundation of China(22272052)the Major Research Project(92061108)the Science and Technology Commission of Shanghai Municipality(24DX1400200)。
文摘Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and atomic-level insights into the structure-activity relationship of Pt_(n) remain a great challenge.Here,we present a combinatorial synthesis and analysis method to investigate the atomicity-activity relationships of Pt_(n) at the individual level.We employ single nanoparticle collision electrochemistry to facilitate the in-situ electrodeposition of a single precisely tunable Pt_(n) on the graphene quantum dot support,followed by instantaneous measurement of the intrinsic ORR activity of the resulting Pt_(n).By relying on highly sensitive electrochemical measurements,our investigations clarify the atomicity-specific ORR activity of Pt_(n),which is attributed to their distinct geometric and electronic structures at varying cluster sizes.Significantly,Pt_(n) with low atomicity,especially below 20,can reach extraordinarily high ORR activities due to atom-by-atom arrangement.Our work provides a simple and efficient method for investigating the atomicity-activity relationships of other nanoclusters under real reaction conditions,enabling a better design of the electrocatalysts at the atomic level.
