Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.233
Publication date: 18th December 2023
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. Thus, significant effort must be dedicated to the development of low cost, efficient, selective and durable electro-catalysts that can operate under mild reaction conditions. This requires fundamental understanding of their structure and surface composition under reaction conditions, keeping in mind that even morphologically and chemically well-defined pre-catalysts will be susceptible to drastic modifications under operation, especially when the reaction conditions themselves change dynamically.
This talk will address the transformations that Metal-N-C catalysts (M=Cu, Ni, Co, Fe, Sn, Zn) experience during static and pulsed CO2RR using operando quick X-ray absorption spectroscopy (XAS) and Raman spectroscopy. In particular, I will illustrate the remarkable behavior displayed by Cu-N-C catalysts during CO2RR, featuring reversible transformations from single atom sites towards Cu nanoparticles. The switchable nature of these species that can be achieved by applying potential pulses holds the key for the on-demand control of the distribution of CO2RR products. The latter is key for the wide-spread adoption of this process.
Moreover, I will shed light on the nature of the ligands forming under CO2RR at singly dispersed Ni sites in a Ni-N-C catalysts, which are currently drawing great attention for their high performances in the CO formation. This will be achieved by a synergistic combination of conventional XAS, high energy resolution fluorescence detected X-ray absorption near edge structure (HERFD-XANES) spectroscopy, and X-ray emission spectroscopy (XES) coupled with unsupervised and supervised machine learning methodologies and density functional theory.
Overall, my lecture will feature the importance of operando characterization of electrocatalysts in order to unveil structure/composition-reactivity correlations during CO2RR.
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