摘要
The excellent catalysts for anodic methanol oxidation reaction(MOR)of direct methanol fuel cells(DMFCs)require a weaker*CO adsorption but a stronger*OH adsorption.Nevertheless,the adsorption strength of the benchmark Pt-based electrocatalysts to the oxygen-containing species is generally a scaling relationship.To solve this problem,a stable Pt_(3)Sn_(0.7)Cr_(0.3)intermetallic structure with appropriate adsorption energies of dualintermediates is designed and achieved.Both experimental and density functional theory calculations corroborate that the addition of Cr brought more electron transfer and stronger orbital hybridization,which upgrades the electron density of Pt but reversely downgrades that of Sn.Consequently,the adsorption site of*OH as well as the adsorption energies of*CO and*OH on Pt_(3)Sn_(0.7)Cr_(0.3)surface were optimized at the same time.Beyond providing a promising DMFC electrocatalyst that breaks the scaling adsorption relationship of oxygen-containing species,this work presents valuable insights into the atomic-level rational design of catalysts according to the reaction mechanism.
基金
supported by the Guizhou Provincial Basic Research Program(Natural Science)(No.QianKeHeJiChu ZK[2024]YiBan008)
the Special Fund for Natural Science of Guizhou University(Nos.202134,202133)
the 2023 Open Fund of Guangdong Provincial Key Laboratory of Fuel Cell Technology(No.FC202321)。
