Deactivation of copper electrocatalysts during CO [sub] 2 reduction occurs via dissolution and selective redeposition mechanism

Blaž Tomc (Author), Marjan Bele (Author), Mohammed Azeezulla Nazrulla (Author), Primož Šket (Author), Matjaž Finšgar (Author), Angela Šurca Vuk (Author), Ana Rebeka Kamšek (Author), Martin Šala (Author), Jan Šiler Hudoklin (Author), Matej Huš (Author), Blaž Likozar (Author), Nejc Hodnik (Author)

Abstract

As electrochemical CO2 reduction (ECR) nears industrialisation levels, addressing the uncontrolled stability, restructuring, and deactivation of copper (Cu) catalysts during operation becomes as crucial as achieving high activity and selectivity for a single product. This study used a high-surface area Cu catalyst that exhibited changes in ECR product selectivity over prolonged operation. The detection of dissolved Cu species during electrolysis confirmed an intermediates-mediated Cu dissolution mechanism at ECR potentials (−0.8 to −1.1 V vs. reversible hydrogen electrode). The findings suggest that the electrodeposition of dissolved Cu species is biased towards Cu catalyst sites with lower reaction intermediates coverage, e.g. adsorbed CO (*CO). A dynamic equilibrium between dissolution and subsequent selective redeposition gradually led to morphological restructuring, resulting in a shift in selectivity away from ECR and towards hydrogen production. With the obtained extensive experimental results, theoretical modelling, and literature data, four interconnected parameters governing restructuring and selectivity shifts were recognised: (i) size and (ii) crystallographic orientation of facets rsc.li/materials-a Introduction of the nanoparticles, (iii) *CO coverage and (iv) CObridge vs. COatop ratio.

Keywords

elektrokemija;katalizatorji;baker;proizvodnja vodika;electrochemistry;catalysts;copper;hydrogen production;

Data

Language:	English
Year of publishing:	2025
Typology:	1.01 - Original Scientific Article
Organization:	KI - National Institute of Chemistry
Publisher:	RSC Publications
UDC:	544.5/.6
COBISS:	221109763
ISSN:	2050-7496
Views:	0
Downloads:	2
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Other data

Secondary language:	Slovenian
Secondary keywords:	elektrokemija;katalizatorji;baker;proizvodnja vodika;
Type (COBISS):	Article
Source comment:	Nasl. z nasl. zaslona; Soavtorji: Marjan Bele, Mohammed Azeezulla Nazrulla, Primož Šket, Matjaž Finšgar, Angelja Kjara Surca, Ana Rebeka Kamšek, Martin Šala, Jan Šiler Hudoklin, Matej Huš, Blaž Likozar and Nejc Hodnik; Opis vira z dne 7. 1. 2025;
Pages:	str. 4119-4128
Volume:	ǂVol. ǂ13
Issue:	ǂiss. ǂ6
Chronology:	2025
DOI:	10.1039/d4ta06466f
ID:	25859550