Allying cobalt nanoclusters with carbon nanofibers for selectively electrocatalytic hydrogenation of unsaturated aldehyde with water as hydrogen source

The electrocatalytic hydrogenation of α, β-unsaturated aldehydes has attracted significant attention, yet the design of electrocatalysts with selective adsorption over CC or CO bond remaining a challenging task. In this study, the Co nanoclusters anchored onto the nitrogen-doped porous carbon nano...

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Bibliographic Details
Main Authors: Xinyu Yang, Sheng-Hua Zhou, Xiaofang Li, Xin-Tao Wu, Qi-Long Zhu
Format: Article
Language:English
Published: Elsevier 2025-06-01
Series:Materials Today Catalysis
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Online Access:http://www.sciencedirect.com/science/article/pii/S2949754X25000171
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Summary:The electrocatalytic hydrogenation of α, β-unsaturated aldehydes has attracted significant attention, yet the design of electrocatalysts with selective adsorption over CC or CO bond remaining a challenging task. In this study, the Co nanoclusters anchored onto the nitrogen-doped porous carbon nanofibers were elaborately fabricated for efficient electrocatalytic hydrogenation. A kinetically driven mono-micelle-oriented self-assembly method was applied to synthesize the polymer nanofibers as the accommodation for Co2 +. The stepwise pyrolysis of Co2+/polymer nanofibers with dicyandiamide yielded the evenly distributed Co nanoclusters with an average size of ∼4 nm over the nitrogen-doped porous carbon nanofibers. Benefited from the high activity of the Co nanoclusters and their rapid electron communication with the nitrogen-doped porous carbon nanofibers, this electrocatalyst demonstrated excellent performance in the selectively electrocatalytic hydrogenation of cinnamaldehyde to hydrocinnamaldehyde, achieving a high selectivity of 90.9 % and a conversion of 68.2 % at 12 mA cm−2. The further in-situ spectroscopy analysis and density functional theory calculations revealed the more preferred adsorption of CC bond and easier water dissociation to give the active H atoms over the Co nanoclusters, which shed light on the hydrogenation mechanism over this electrocatalyst. Our study can provide a new insight in catalyst design for electrocatalytic hydrogenation reaction.
ISSN:2949-754X