Universiteit Leiden

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Dissertation

Electrocatalysis of CO2/CO interconversion and Hydrogen Evolution in Bicarbonate Buffers

Bicarbonate buffer is largely found in nature due to its ability to regulate pH variations around neutral values. As the pH changes, so does the speciation of the buffer.

Author
Marcandalli, G.
Date
03 February 2022
Links
Thesis in Leiden Repository

Bicarbonate buffer is largely found in nature due to its ability to regulate pH variations around neutral values. As the pH changes, so does the speciation of the buffer. At low pH the main buffer species is carbon dioxide, which for increasing pH transforms into bicarbonate, and then into carbonate. Besides the acid-base reactions in solution, the buffer species may react at the electrified interface to be reduced or oxidized.Given the importance of storing intermittent renewable electricity into chemical bonds using abundant reactants, such as carbon dioxide, it is crucial to understand the interplay of electrochemical and homogeneous reactions. Hence, in this PhD thesis we studied how the presence of a buffer in the electrolytes affects relevant electrocatalytic reactions, i.e. CO2 electrochemical reduction (Chapter 2 and 4), hydrogen evolution reaction (Chapter 4 and 5) and CO electrooxidation (Chapter 3). A special focus is placed on the employment of well-defined mass transport techniques in combination with digital simulations.

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