Potential-induced nanoclustering of metallic catalysts during electrochemical CO2 reduction

Jianfeng Huang, Nicolas Hörmann, Emad Oveisi, Anna Loiudice, Gian Luca De Gregorio, Oliviero Andreussi, Nicola Marzari and Raffaella Buonsanti ()
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Jianfeng Huang: École Polytechnique Fédérale de Lausanne
Nicolas Hörmann: École Polytechnique Fédérale de Lausanne
Emad Oveisi: École Polytechnique Fédérale de Lausanne
Anna Loiudice: École Polytechnique Fédérale de Lausanne
Gian Luca De Gregorio: École Polytechnique Fédérale de Lausanne
Oliviero Andreussi: École Polytechnique Fédérale de Lausanne
Nicola Marzari: École Polytechnique Fédérale de Lausanne
Raffaella Buonsanti: École Polytechnique Fédérale de Lausanne

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract In catalysis science stability is as crucial as activity and selectivity. Understanding the degradation pathways occurring during operation and developing mitigation strategies will eventually improve catalyst design, thus facilitating the translation of basic science to technological applications. Herein, we reveal the unique and general degradation mechanism of metallic nanocatalysts during electrochemical CO2 reduction, exemplified by different sized copper nanocubes. We follow their morphological evolution during operation and correlate it with the electrocatalytic performance. In contrast with the most common coalescence and dissolution/precipitation mechanisms, we find a potential-driven nanoclustering to be the predominant degradation pathway. Grand-potential density functional theory calculations confirm the role of the negative potential applied to reduce CO2 as the main driving force for the clustering. This study offers a novel outlook on future investigations of stability and degradation reaction mechanisms of nanocatalysts in electrochemical CO2 reduction and, more generally, in electroreduction reactions.

Date: 2018
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-05544-3

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DOI: 10.1038/s41467-018-05544-3

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