Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.280
Publication date: 16th December 2024
The re-utilization of CO2 via its electrocatalytic reduction (CO2RR) into value-added chemicals and fuels is a promising avenue to minimize the impact of existing technologies on the climate change. This requires the development of low cost, efficient, selective and durable electrocatalysts. However, their rational design requires in depth understanding of the modifications that structurally and chemically well-defined pre-catalysts undergo during operation, especially when the reaction conditions themselves change dynamically.
Here, the transformations that Metal-N-C catalysts (M=Cu, Ni, Co, Fe, Sn, Zn) experience during static and pulsed CO2RR will be unveiled. This will be achieved by a synergistic combination of operando quick X-ray absorption spectroscopy (XAS), high energy resolution fluorescence detected X-ray absorption near edge structure (HERFD-XANES) and X-ray emission spectroscopy (XES), coupled with unsupervised and supervised machine learning methodologies and density functional theory.
In particular, I will illustrate the astonishing behavior displayed by Cu-N-C catalysts during CO2RR, featuring reversible transformations from single atom sites towards small clusters and Cu nanoparticles. The switchable nature of these species, that can be achieved by applying different potential pulses, holds the key for the on-demand control of the distribution of the CO2RR products and thus, a wide-spread adoption of this process. Moreover, I will elucidate the nature of the ligands formed under CO2RR at singly dispersed Ni sites or Co sites in Ni- or Co-N-C catalysts, which are currently drawing great attention for their excellent CO yields.
Overall, my lecture will feature the importance of operando characterization of electrocatalysts in order to elucidate structure/composition-reactivity correlations during CO2RR.
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