TY - JOUR
T1 - Potential-induced nanoclustering of metallic catalysts during electrochemical CO2 reduction
AU - Huang, Jianfeng
AU - Hörmann, Nicolas
AU - Oveisi, Emad
AU - Loiudice, Anna
AU - De Gregorio, Gian Luca
AU - Andreussi, Oliviero
AU - Marzari, Nicola
AU - Buonsanti, Raffaella
N1 - Publisher Copyright:
© 2018, The Author(s).
PY - 2018/12/1
Y1 - 2018/12/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85051220571&partnerID=8YFLogxK
U2 - 10.1038/s41467-018-05544-3
DO - 10.1038/s41467-018-05544-3
M3 - Article
C2 - 30082872
AN - SCOPUS:85051220571
VL - 9
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 3117
ER -