Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis

Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis

© 2023 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 18 vom: 21. Mai, Seite e2300020
1. Verfasser: Wei, Xiaoxiao (VerfasserIn)
Weitere Verfasser: Liu, Yingying, Zhu, Xiaorong, Bo, Shuowen, Xiao, Lei, Chen, Chen, Nga, Ta Thi Thuy, He, Yuanqing, Qiu, Mengyi, Xie, Chao, Wang, Dongdong, Liu, Qinghua, Dong, Fan, Dong, Chung-Li, Fu, Xian-Zhu, Wang, Shuangyin
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article active sites clusters copper single atoms dynamic reconstitutions urea synthesis
Beschreibung
Zusammenfassung:© 2023 Wiley-VCH GmbH.
Electrocatalytic CN coupling between carbon dioxide and nitrate has emerged to meet the comprehensive demands of carbon footprint closing, valorization of waste, and sustainable manufacture of urea. However, the identification of catalytic active sites and the design of efficient electrocatalysts remain a challenge. Herein, the synthesis of urea catalyzed by copper single atoms decorated on a CeO2 support (denoted as Cu1 -CeO2 ) is reported. The catalyst exhibits an average urea yield rate of 52.84 mmol h-1 gcat. -1 at -1.6 V versus reversible hydrogen electrode. Operando X-ray absorption spectra demonstrate the reconstitution of copper single atoms (Cu1 ) to clusters (Cu4 ) during electrolysis. These electrochemically reconstituted Cu4 clusters are real active sites for electrocatalytic urea synthesis. Favorable CN coupling reactions and urea formation on Cu4 are validated using operando synchrotron-radiation Fourier transform infrared spectroscopy and theoretical calculations. Dynamic and reversible transformations of clusters to single-atom configurations occur when the applied potential is switched to an open-circuit potential, endowing the catalyst with superior structural and electrochemical stabilities
Beschreibung:Date Completed 07.05.2023
Date Revised 07.05.2023
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202300020