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Tuning Amorphous Surface Microenvironments for Accelerated *OH Adsorption toward Efficient CO2 Electrocatalysis.

Zejiang Huang1, Jianming Gu2, Hang Zhou1

  • 1Physics Department & Shanghai Key Laboratory of Magnetic Resonance, School of Physics, Institute of Magnetic Resonance and Molecular Imaging in Medicine, East China Normal University, North Zhongshan Road 3663, Shanghai 200062, P. R. China.

The Journal of Physical Chemistry Letters
|April 16, 2026
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Engineered amorphous copper tin oxide (a-CuSnOx) catalysts enhance carbon dioxide electroreduction to formate. This novel catalyst design optimizes hydroxyl (*OH) adsorption, boosting efficiency for CO2RR applications.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • The electrocatalytic reduction of carbon dioxide (CO2RR) is crucial for sustainable energy.
  • Copper-based catalysts are promising for CO2RR but controlling their surface is difficult.
  • Surface microenvironments, especially hydroxyl (*OH) adsorption, significantly impact CO2RR performance.

Purpose of the Study:

  • To design and synthesize amorphous copper tin oxide (a-CuSnOx) catalysts with tailored surface microenvironments.
  • To investigate the role of *OH adsorption in CO2 electroreduction to formate.
  • To establish a structure-activity relationship for high-performance CO2RR catalysts.

Main Methods:

  • Synthesis of amorphous CuSnOx catalysts via strategic Cu-Sn integration.
  • Electrochemical testing across a range of current densities to determine Faradaic efficiency.
  • Operando 1H and 17O NMR spectroscopy to probe surface species and reaction mechanisms.

Main Results:

  • Achieved >90% formate Faradaic efficiency with a-CuSnOx catalysts over a broad current density range.
  • Demonstrated that the amorphous structure provides abundant undercoordinated Cu and Sn sites, enhancing *OH adsorption.
  • NMR studies confirmed the direct involvement of *OH in formate production through a water-assisted pathway.

Conclusions:

  • Amorphous CuSnOx catalysts with engineered microenvironments offer a new strategy for efficient CO2 electroreduction.
  • Optimized *OH adsorption is key to high formate selectivity in CO2RR.
  • This work deepens the understanding of structure-activity relationships in CO2RR catalysis.