GC-DFT-Based Dynamic Product Distribution Reveals Enhanced CO₂-to-Methanol Electrocatalysis Durability by Heterogeneous CoPc

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 16(1), P. 294 - 307

Published: Dec. 26, 2024

Heterogeneous cobalt phthalocyanine has emerged as a promising molecular catalyst for electrochemical reduction of CO2 to methanol. Boosting both electrocatalytic durability and selectivity remains great challenge, which is more difficult with unknown regulation factors the HER side reaction. Herein, discover key balancing selectivity, well regulation, we carried out GC-DFT calculations, based on dynamic product distribution modeling was conducted visually present variation within applied voltage range. The strongly electron-donating NMe2-substituted CoPc found be an excellent candidate. reveals that balance regulate potential highest methanol Faradaic efficiency corresponding energy barrier selectivity-determining step hydrogenated CoPc. pivotal factor in stems from hindered H adsorption due ligand hydrogenation, arising decreased Co-to-H charge transfer. analysis provides intuitive theoretical guidance highly selective durable electroreduction.

Language: Английский

Metal Complexes with Redox-Active Ligands in the Indirect Electrosynthesis of Organic Sulfur Compounds

Russian Journal of Coordination Chemistry, Journal Year: 2023, Volume and Issue: 49(S2), P. S128 - S158

Published: Dec. 1, 2023

Language: Английский