金属单分子层命令：纳米晶体表面的欠电位沉积：定量操作电化学透射电子显微镜研究,ACS Energy Letters

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金属单分子层命令：纳米晶体表面的欠电位沉积：定量操作电化学透射电子显微镜研究
ACS Energy Letters ( IF 19.3 ) Pub Date : 2022-03-09 , DOI: 10.1021/acsenergylett.2c00209
Yao Yang ₁ , Yu-Tsun Shao ₂ , Francis J. DiSalvo ₁ , David A. Muller _{2,

3} , Héctor D. Abruña ₁

Affiliation

欠电位沉积 (UPD) 能够生成金属单分子层，其电子特性可能与本体显着不同。虽然对体电极进行了广泛研究，但由于局部电场分布的明显差异，单个纳米粒子的 UPD 动力学可能会偏离其体电极。由于在接口处缺乏纳米级时间分辨操作/原位技术，UPD 的性质在很大程度上仍未被探索。本研究基于对电化学结果和高分辨率化学绘图的相关分析，对模型系统进行了研究，即单层 Cu 在单晶 Au 纳米立方体表面的 UPD。操作电化学液体细胞扫描透射电子显微镜 (EC-STEM) 直接可视化电位依赖性和空间分辨的铜电沉积动力学，分为平面、岛形或树枝状生长。Operando EC-STEM 通过定量电化学和定量成像分析揭示了在亚微米厚液体中铜电沉积过程中明确定义的扩散控制过程。4D-STEM 显示 Cu 电沉积由 Au 基板的晶体取向引导。这种用于定量电化学的操作EC-STEM 方法可以作为一个通用平台来促进对（电）化学反应动力学的基本理解。

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Metal Monolayers on Command: Underpotential Deposition at Nanocrystal Surfaces: A Quantitative Operando Electrochemical Transmission Electron Microscopy Study

Underpotential deposition (UPD) enables the generation of metal monolayers whose electronic properties can be significantly different from the bulk. While studied extensively for bulk electrodes, UPD kinetics for individual nanoparticles can deviate from their bulk counterparts due to the distinct differences in the distribution of local electric fields. UPD’s nature remains largely unexplored due to the lack of nanoscale time-resolved operando/in situ techniques at interfaces. This study presents an investigation on a model system, the UPD of monolayer Cu at single-crystal Au nanocube surfaces, based on a correlative analysis of electrochemical results and high-resolution chemical mapping. Operando electrochemical liquid-cell scanning transmission electron microscopy (EC-STEM) directly visualizes the potential-dependent and spatially resolved Cu electrodeposition kinetics, classified as planar, island-shaped, or dendritic growth. Operando EC-STEM reveals the well-defined diffusion-controlled processes during Cu electrodeposition in sub-μm thick liquid with both quantitative electrochemistry and quantitative imaging analysis. 4D-STEM shows that the Cu electrodeposition is guided by the crystallographic orientation of the Au substrate. This methodology of operando EC-STEM for quantitative electrochemistry can serve as a generalized platform to advance fundamental understanding of (electro)chemical reaction dynamics.

更新日期：2022-03-09

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