Metal-Organic Frameworks for the CO2 Reduction Reaction
A Selectivity Study
K. Roohi (TU Delft - Team Peyman Taheri)
J.M.C. Mol – Promotor (TU Delft - Team Arjan Mol)
P. Taheri – Promotor (TU Delft - Team Peyman Taheri)
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Abstract
The electrochemical reduction of carbon dioxide (CO2RR) offers a sustainable route to convert CO2 into value-added chemicals and fuels, contributing to both carbon management and renewable energy storage. However, the competing intermediates of the reaction often results in poor selectivity and energy inefficiency. This thesis explores metal–organic frameworks (MOFs) as a tunable platform for studying and improving selectivity in CO2RR through atomically precise control of catalytic environments. By systematically tailoring the local coordination, geometry, and composition of Cu-based MOFs, this work establishes direct relationships between structure, intermediate stabilization, and product distribution, thereby advancing the rational design of selective CO2RR electrocatalysts. Overally, this thesis demonstrates that the local coordination environment and electronic structure of Cu-based MOFs dictate CO2RR selectivity. By integrating synthesis, operando spectroscopy, and DFT modeling, this work establishes coordination engineering as a powerful strategy for rationally designing selective and efficient MOF-based electrocatalysts for CO2 conversion.