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Title:Non-covalent ligand-oxide interaction promotes oxygen evolution
Authors:ID Wu, Qianbao (Author)
ID Liang, Junwu (Author)
ID Xiao, Mengjun (Author)
ID Long, Chang (Author)
ID Li, Lei (Author)
ID Zeng, Zhenhua (Author)
ID Mavrič, Andraž (Author)
ID Zheng, Xia (Author)
ID Zhu, Jing (Author)
ID Valant, Matjaž (Author), et al.
Files:.pdf RAZ_Wu_Qianbao_2023.pdf (1,77 MB)
MD5: E4F79C241FB1DD40A54149C271260491
 
Language:English
Work type:Unknown
Typology:1.01 - Original Scientific Article
Organization:UNG - University of Nova Gorica
Abstract:Strategies to generate high-valence metal species capable of oxidizing water often employ composition and coordination tuning of oxide-based catalysts, where strong covalent interactions with metal sites are crucial. However, it remains unexplored whether a relatively weak “non-bonding” interaction between ligands and oxides can mediate the electronic states of metal sites in oxides. Here we present an unusual non-covalent phenanthroline-CoO2 interaction that substantially elevates the population of Co4+ sites for improved water oxidation. We find that phenanthroline only coordinates with Co2+ forming soluble Co(phenanthroline)2(OH)2 complex in alkaline electrolytes, which can be deposited as amorphous CoOxHy film containing non-bonding phenanthroline upon oxidation of Co2+ to Co3+/4+. This in situ deposited catalyst demonstrates a low overpotential of 216 mV at 10 mA cm−2 and sustainable activity over 1600 h with Faradaic efficiency above 97%. Density functional theory calculations reveal that the presence of phenanthroline can stabilize CoO2 through the non-covalent interaction and generate polaron-like electronic states at the Co-Co center.
Keywords:water oxidation, cobalt hydroxide, ligand-metal interactions
Publication status:Published
Publication version:Version of Record
Publication date:01.01.2023
Year of publishing:2023
Number of pages:str. 1-12
Numbering:Vol. 14, article no. 997
PID:20.500.12556/RUNG-7997-ba085eca-51ea-1c45-6b79-1b60410f164f New window
COBISS.SI-ID:142729475 New window
UDC:54
ISSN on article:2041-1723
DOI:10.1038/s41467-023-36718-3 New window
NUK URN:URN:SI:UNG:REP:TFCI9DZW
Publication date in RUNG:23.02.2023
Views:1606
Downloads:15
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Record is a part of a journal

Title:Nature communications
Shortened title:Nat. Commun.
Publisher:Nature Publishing Group
ISSN:2041-1723
COBISS.SI-ID:2315876 New window

Document is financed by a project

Funder:ARRS - Slovenian Research Agency
Project number:J2-2498
Name:Redukcija ogljikovega dioksida na katalizatorju z izoliranimi atomi za tvorbo spojin z dodano vrednostjo

Funder:ARIS - Slovenian Research and Innovation Agency
Project number:P2-0412
Name:Heterogeni procesi na površinah trdnin za trajnostne tehnologije

Licences

License:CC BY 4.0, Creative Commons Attribution 4.0 International
Link:http://creativecommons.org/licenses/by/4.0/
Description:This is the standard Creative Commons license that gives others maximum freedom to do what they want with the work as long as they credit the author.
Licensing start date:23.02.2023

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