Computational design of bimetallic core-shell nanoparticles for hot-carrier photocatalysis  

作　　者：Luigi Ranno Stefano Dal Forno Johannes Lischner 

机构地区：[1]Department of Materials,Imperial College London,London SW72AZ,UK [2]Department of Physics,Imperial College London,London SW72AZ,UK [3]Department of Physics and Department of Materials,and the Thomas Young Centre for Theory and Simulation of Materials,Imperial College London,London SW72AZ,UK

出　　处：《npj Computational Materials》2018年第1期389-395,共7页计算材料学（英文）

基　　金：S.D.F.and J.L.acknowledge support from EPSRC under Grant No.EP/N005244/1 and also from the Thomas Young Center under Grant No.TYC-101.Via J.L.‘s membership of the UK’s HEC Materials Chemistry Consortium,which is funded by EPSRC(EP/L000202);this work used the ARCHER UK National Supercomputing Service.S.D.F.and J.L.acknowledge support from EPSRC under Grant No.EP/N005244/1 and also from the Thomas Young Center under Grant No.TYC-101.

摘　　要：Computational design can accelerate the discovery of new materials with tailored properties,but applying this approach to plasmonic nanoparticles with diameters larger than a few nanometers is challenging as atomistic first-principles calculations are not feasible for such systems.In this paper,we employ a recently developed material-specific approach that combines effective mass theory for electrons with a quasistatic description of the localized surface plasmon to identify promising bimetallic core-shell nanoparticles for hot-electron photocatalysis.Specifically,we calculate hot-carrier generation rates of 100 different core-shell nanoparticles and find that systems with an alkali-metal core and a transition-metal shell exhibit high figures of merit for water splitting and are stable in aqueous environments.Our analysis reveals that the high efficiency of these systems is related to their electronic structure,which features a two-dimensional electron gas in the shell.Our calculations further demonstrate that hotcarrier properties are highly tunable and depend sensitively on core and shell sizes.The design rules resulting from our work can guide experimental progress towards improved solar energy conversion devices.

关 键 词：APPLYING ALKALI DIAMETERS 

分 类 号：O64[理学—物理化学]