Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts

Zhiwen Jiang, Carine Clavaguéra, Changjiang Hu, Sergey A. Denisov, Shuning Shen, Feng Hu, Jun Ma () and Mehran Mostafavi ()
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Zhiwen Jiang: University of Science and Technology of China
Carine Clavaguéra: CNRS, Institut de Chimie Physique
Changjiang Hu: Nanjing University of Aeronautics and Astronautics
Sergey A. Denisov: CNRS, Institut de Chimie Physique
Shuning Shen: Nanjing University of Aeronautics and Astronautics
Feng Hu: Nanjing University of Aeronautics and Astronautics
Jun Ma: University of Science and Technology of China
Mehran Mostafavi: CNRS, Institut de Chimie Physique

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Time-resolved identification of surface-bound intermediates on metallic nanocatalysts is imperative to develop an accurate understanding of the elementary steps of CO2 reduction. Direct observation on initial electron transfer to CO2 to form surface-bound CO2•− radicals is lacking due to the technical challenges. Here, we use picosecond pulse radiolysis to generate CO2•− via aqueous electron attachment and observe the stabilization processes toward well-defined nanoscale metallic sites. The time-resolved method combined with molecular simulations identifies surface-bound intermediates with characteristic transient absorption bands and distinct kinetics from nanosecond to the second timescale for three typical metallic nanocatalysts: Cu, Au, and Ni. The interfacial interactions are further investigated by varying the important factors, such as catalyst size and the presence of cation in the electrolyte. This work highlights fundamental ultrafast spectroscopy to clarify the critical initial step in the CO2 catalytic reduction mechanism.

Date: 2023
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DOI: 10.1038/s41467-023-42936-6

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