Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.082
Publication date: 18th December 2023
It is well known that climate change is one of the main challenges of our generation. The large CO2 emissions generated by anthropogenic activities are the main contributor to the so-called greenhouse effect. Therefore, the decarbonisation of industries and energy sources is of utmost importance. In this context, the electrochemical CO2 reduction reaction (CO2RR) is a promising way of reutilising the emitted CO2 to form value-added chemicals. Amongst the broad spectrum of species that can be obtained, CO is arguably one of the most industrially relevant products.[1] In addition, CO is a more reactive molecule than CO2 and can therefore be activated to form more reduced carbon products, such as formate or ethanol. Hence, it can be employed in a tandem-catalyst system to convert CO2 into C2+ species in a more controlled manner.[2] Regarding the selective conversion of CO2 into CO, there are only a few candidates. Au-based catalysts, and in particular Au nanoparticles (NPs), have been shown to achieve high efficiencies and current densities at low overpotentials for this reaction. Furthermore, it has been demonstrated in a number of studies how the functionalisation of the surface of these NPs with different ligands, such as amines or thiols, can enhance the activity and selectivity of Au catalysts for the CO2RR.[3] In this work, ligand-capped Au NPs have been synthesised by a novel organometallic approach using hexadecylamine (HDA) and tetradecanethiol (TDT) as stabilisers. The NPs obtained with both ligands present the same size around 1 nm and show no significant aggregation in TEM micrographs. However, electrochemical studies showed that the TDT-capped Au NPs had a poor catalytic performance in comparison with its HDA-capped analogue. Interestingly, these two systems of identical size, showed a shift in their plasmon resonance peaks as seen by in the UV-vis spectroscopy. Hence, this unusual behaviour was explored in order to get to the root of the surprising differences in their catalytic activities.
I would like to acknowledge the funding from the research proyects PID2019-104171RB-I00-, PID2021-128197NA-I00, TED2021-129237B-I00 and the PhD scholarship from AGAUR.