<p>Understanding the dynamic heterogeneity of the hydrogen evolution reaction (HER) at electrochemical interfaces is crucial for advancing HER electrocatalysis. However, conventional electrochemical imaging methods offer limited simultaneous spatial and temporal resolution, hindering capture of dynamic electrocatalytic current distributions. Here we introduce interferometric electro-optical microscopy to in situ map electrocatalytic current with simultaneous nanometre and millisecond resolution. We validate interferometric electro-optical microscopy with Au and Pt electrocatalysts and apply it to investigate the HER activity of bilayer MoS<sub>2</sub>. The spatial evolution of HER currents reveals sequential activation of HER sites along trajectories aligned with the zigzag or armchair directions of MoS<sub>2</sub>. Correlative atomic-level structural analysis and simulations reveal that the directional chain electrocatalytic reaction dynamics originate from the more favourable adsorption free energy along nanoscale strain stripes. This method for uncovering dynamically evolving structure relationships at nanoscopic electrochemical interfaces and identifying strain-related electrocatalytic performance holds promise for advancing the rational design of electrocatalysts.</p>

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Imaging dynamic electrocatalytic processes on nano-strained MoS2 using interferometric electro-optical microscopy

  • Kaijie Ma,
  • Yu Cui,
  • Yizhang Ren,
  • Qiunan Liu,
  • Song Luo,
  • Jiaxin Mao,
  • Guopeng Li,
  • Yueshao Zheng,
  • Kazu Suenaga,
  • Jiang Zeng,
  • Yung-Chang Lin,
  • Song Liu,
  • Rui Hao

摘要

Understanding the dynamic heterogeneity of the hydrogen evolution reaction (HER) at electrochemical interfaces is crucial for advancing HER electrocatalysis. However, conventional electrochemical imaging methods offer limited simultaneous spatial and temporal resolution, hindering capture of dynamic electrocatalytic current distributions. Here we introduce interferometric electro-optical microscopy to in situ map electrocatalytic current with simultaneous nanometre and millisecond resolution. We validate interferometric electro-optical microscopy with Au and Pt electrocatalysts and apply it to investigate the HER activity of bilayer MoS2. The spatial evolution of HER currents reveals sequential activation of HER sites along trajectories aligned with the zigzag or armchair directions of MoS2. Correlative atomic-level structural analysis and simulations reveal that the directional chain electrocatalytic reaction dynamics originate from the more favourable adsorption free energy along nanoscale strain stripes. This method for uncovering dynamically evolving structure relationships at nanoscopic electrochemical interfaces and identifying strain-related electrocatalytic performance holds promise for advancing the rational design of electrocatalysts.