Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
Publication date: 28th August 2024
The global primary energy consumption reached around 604 exajoules in 2022. The main energy fuel used in the world was oil, followed by other fossil fuels (like coal and natural gas) leading to 36.8 Gt of CO2 emitted globally due to energy reasons. [https://www.statista.com/statistics/265598/consumption-of-primary-energy-
worldwide/statisticContainer.]
Achieving a CO2-neutral world economy is a formidable task that requires multiple approaches. One of them is converting the emitted and captured CO2 into value-added chemicals. This is possible through electrochemical CO2 conversion powered by renewable energy sources.
In this method electrical energy is supplied to establish a potential difference between two electrodes, enabling the reduction of CO2 reduction into value-added chemicals. Even if this technology seems promising, there are many challenges that are due to the low energy content in CO2, high reaction energy barrier, slow kinetics for CO2 electroreduction reaction (CO2RR), and low selectivity toward a specific target product.
These problems can be overcome by improving the catalyst, cell design and other chemical components. The catalytic activity of a given metal or metal alloy in the CO2RR depends on its electronic structure (oxidation and spin state), local coordination, and elemental distribution. These aspects can be studied by in situ/operando x-ray absorption and emission spectroscopy (XAS-XES).
Herein, we designed a flow cell able to perform CO2RR and whose geometry is adapted to carry out XAS-XES measurements. This cell allows a sample (GDE, gas diffusion electrode, layered with a copper (Cu) catalyst) to be in contact with the CO2 on the GDE hydrophobic side and with the electrolyte (KOH) on the layered one.
It was used at the high brilliance spectroscopy beamline ID26 of the ESRF, European Synchrotron Radiation Facility. We operated at the Cu absorption K-edge first ex situ, then in situ with and without potential applied and then again in ex situ condition. By exploiting high-energy-resolution fluorescence-detected (HERFD) XAS, we identified transition from 1s into the Cu 3d orbital providing direct information about the Cu oxidation state.
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