In Situ Reconstruction of a Hierarchical Sn‐Cu/SnOx Core/Shell Catalyst for High‐Performance CO2 Electroreduction. (4th February 2020)

• Record Type: Journal Article
• Authors: Ye, Ke; Zhou, Zhiwen; Shao, Jiaqi; Lin, Long; Gao, Dunfeng; Ta, Na; Si, Rui; Wang, Guoxiong; Bao, Xinhe
• Is Part Of: Angewandte Chemie. Volume 132:Number 12(2020)
• Page Start: 4844
• Page End: 4851
• Publication Date: 2020-02-04
• Subjects: Elektrochemie -- Grenzflächen -- Hierarchische Strukturen -- Kohlendioxidreduktion -- Zinnoxid; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201916538
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: The electrochemical CO2 reduction reaction (CO2 RR) to give C1 (formate and CO) products is one of the most techno‐economically achievable strategies for alleviating CO2 emissions. Now, it is demonstrated that the SnO x shell in Sn2.7 Cu catalyst with a hierarchical Sn‐Cu core can be reconstructed in situ under cathodic potentials of CO2 RR. The resulting Sn2.7 Cu catalyst achieves a high current density of 406.7±14.4 mA cm −2 with C1 Faradaic efficiency of 98.0±0.9 % at −0.70 V vs. RHE, and remains stable at 243.1±19.2 mA cm −2 with a C1 Faradaic efficiency of 99.0±0.5 % for 40 h at −0.55 V vs. RHE. DFT calculations indicate that the reconstructed Sn/SnO x interface facilitates formic acid production by optimizing binding of the reaction intermediate HCOO* while promotes Faradaic efficiency of C1 products by suppressing the competitive hydrogen evolution reaction, resulting in high Faradaic efficiency, current density, and stability of CO2 RR at low overpotentials. Abstract : CO2 zu Ameisensäure : Eine in situ rekonstruierte Sn/SnO x ‐Grenzfläche ermöglicht die Ameisensäurebildung durch Optimieren der Bindung des Intermediats HCOO* und Förderung des Faradayschen Wirkungsgrads von C1 ‐Produkten, indem die konkurrierende Wasserstoffentwicklung unterdrückt wird. Dies ergibt einen hohen Faradayschen Wirkungsgrad, eine hohe Stromdichte und eine hohe Stabilität der elektrochemischen CO2 ‐Reduktion bei niedriger Überspannung.