从沉积应力到表面反应性：依赖应变的溅射铂薄片氢演化
From Deposition Stress to Surface Reactivity: Strain-Dependent Hydrogen Evolution on Sputtered Platinum Thin Films
AI总结：
研究通过调节溅射压力改变铂薄片的应力状态，发现低压力下薄片具有更高的氢演化反应活性，而高压力导致活性降低，揭示了残余应变、微结构和氢覆盖度的相互作用机制。
摘要：
应变已成为调节电催化性能的有前景方法，但其在溅射沉积薄片中的作用仍不明确。本文通过调节溅射压力制备了不同应力状态的溅射铂薄片，利用互补表征技术和密度泛函理论计算研究了微结构、残余应变和氢演化反应（HER）活性的变化。结构分析显示，(111)取向的铂薄片在低压力下呈致密光滑状态，而在高压力下转变为更多孔的微结构并具有增加的粗糙度。电化学测量显示，低溅射压力下薄片表现出最高的HER活性，而高溅射压力尽管增加了表面积却导致活性降低。DFT计算表明，晶格应变改变了铂(111)上的氢吸附能和表面覆盖度，为观察到的活性趋势提供了机理解释。总体而言，结果强调溅射铂薄片的HER活性由残余应变、微结构和氢覆盖度的相互作用决定。
英文摘要：
Strain has emerged as a promising approach for tuning electrocatalytic properties, yet its role in sputter-deposited thin films remains poorly understood. In this work, magnetron-sputtered platinum (Pt) thin films with different stress states were prepared by varying the sputter pressure. The resulting changes in microstructure, residual strain, and hydrogen evolution reaction (HER) activity were investigated using complementary characterization techniques and density functional theory (DFT) calculations. Structural analysis reveals a transition of (111)-textured Pt thin films from dense and smooth films at low pressures, to more porous microstructures with increased roughness at higher pressures. Electrochemical measurements show that films deposited at low sputter pressure exhibit the highest HER activity, while higher sputter pressures lead to reduced activity despite increased surface area. DFT calculations demonstrate that lattice strain alters hydrogen adsorption energetics and surface coverage on Pt(111), providing a mechanistic explanation for the observed activity trends. Overall, the results highlight that HER activity in sputtered Pt thin films is governed by the interplay of residual strain, microstructure, and hydrogen coverage.
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