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

DOI: 10.1016/j.apmt.2024.102466

Authors: Nivetha Jeyachandran (Queen Mary University of London) , Wangchao Yuan (Queen Mary University of London) , Xiang Li (Queen Mary University of London) , Akshayini Muthuperiyanayagam (Queen Mary University of London) , Stefania Gardoni (Queen Mary University of London) , Jiye Feng (Jinan University) , Qingsheng Gao (Jinan University) , Martin Wilding (Research Complex at Harwell) , Peter Wells (University of Southampton; Catalysis Hub, Research Complex at Harwell) , Devis Di Tommaso (Queen Mary University of London) , Cristina Giordano (Queen Mary University of London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Applied Materials Today , VOL 41

State: Published (Approved)
Published: December 2024
Diamond Proposal Number(s): 29721

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.

Subject Areas: Materials, Chemistry, Environment


Instruments: B18-Core EXAFS

Added On: 16/10/2024 09:44

Documents:
1-s2.0-S2352940724004116-main.pdf

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Materials Science Chemical Engineering Engineering & Technology Nanoscience/Nanotechnology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)