Dataset of "Different conditions, different composition: Reactive environment-induced surface composition dynamics in Pt-based bimetallic alloys"

In this study, we utilize near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) to monitor in real time, the redox-driven surface restructuring of model Pt–M alloys (M = Co, Ni, Cu) with systematically tailored compositions. Samples underwent sequential oxidative (5 mbar O₂) and reductive (5 mbar H₂) treatments across a temperature range from room temperature to 300°C, for real-time tracking of surface composition, oxidation states, and electronic structure as a functions of reactive environment, temperature, alloy type and stoichiometry. Results reveal that exposure to reactive gas atmospheres induces substantial surface dynamics. Overall, in oxidative atmospheres, the less noble component preferentially oxidized and segregated to the surface, triggering dealloying, while in subsequent reductive atmospheres, its reduction induces partial realloying with Pt. The extent and reversibility of these processes are discussed depending on alloy type and composition, providing insights into redox-driven surface dynamics and offer a basis for the rational design of durable, high-performance Pt-based multimetallic catalysts.本研究采用近常压X射线光电子能谱（NAP-XPS），实时监测具有系统调控组分的模型Pt-M合金（M=Co、Ni、Cu）的氧化还原驱动表面重构过程。实验样品在室温至300℃的温度区间内，依次进行氧化（5 mbar O₂）与还原（5 mbar H₂）处理，以实时追踪随反应环境、温度、合金种类及化学计量比变化的表面组分、氧化态与电子结构。研究结果表明，暴露于反应性气体氛围可引发显著的表面动态变化。总体而言，在氧化氛围中，合金中的非贵金属组分优先发生氧化并偏析至表面，引发脱合金过程；而在后续的还原氛围中，该组分的还原会触发其与Pt发生部分再合金化。本研究探讨了这些过程的程度与可逆性随合金种类及组成的变化规律，为解析氧化还原驱动的表面动态机制，并为合理设计耐用、高性能的Pt基多金属催化剂提供了理论依据。