Tuning the crystallinity of Cu-based electrocatalysts: Synthesis, structure, and activity towards the CO2 reduction reaction

Jeyachandran, Nivetha, Yuan, Wangchao, Li, Xiang, Muthuperiyanayagam, Akshayini, Gardoni, Stefania, Feng, Jiye, Gao, Qingsheng, Wilding, Martin, Wells, Peter, Tommaso, Devis Di and Giordano, Cristina 2024. Tuning the crystallinity of Cu-based electrocatalysts: Synthesis, structure, and activity towards the CO2 reduction reaction. Applied Materials Today 41 , 102466. 10.1016/j.apmt.2024.102466

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Abstract

The rising levels of CO2 have spurred growing concerns for our environment, and curbing CO2 emissions may not be practically viable with the expanding human population. One attractive strategy is the electrochemical CO2 reduction (CO2RR) into value added chemicals but because of the chemical inertness of the CO2 molecule, the electrochemical reduction requires a suitable catalyst. Cu-based catalysts have been largely investigated for CO2RR, however, the difficulty achieving a high selectivity and faradaic efficiency towards specific products, especially hydrocarbons, is still a challenge, alongside the concern over cost, stability and scarcity of the metal catalyst. The present research focuses on tuning the crystallinity of Cu nanoparticles via a green, cost-friendly, and facile method, called the urea glass route. Remarkably, the incorporation of a selected nitrogen-carbon rich source (namely, 4,5 dicyanoimidazole) at low temperatures allow the formation of an oxidized derived amorphous Cu system, whilst a second thermal treatment enables the transformation to crystalline Cu0. We found that the combination of surface Cu0 and Cu1+ (observed via XPS studies) present in our amorphous and crystalline Cu nanoparticles leads to interesting differences in the final catalytic activity when tested under CO2 reaction conditions. The combination of extended X-ray absorption fine structure (EXAFS) experiments and molecular dynamics simulations provides compelling evidence for the amorphous and metallic nature of Cu nanoparticles.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Publisher:	Elsevier
ISSN:	2352-9407
Date of First Compliant Deposit:	4 February 2025
Date of Acceptance:	1 October 2024
Last Modified:	04 Feb 2025 10:15
URI:	https://orca.cardiff.ac.uk/id/eprint/175860

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