Charge effects regulate reversible CO2 reduction catalysis

Abstract

Modular but geometrically constrained ligands were used to investigate the impact of key ligand design parameters (charge and bite angle) on CO₂ hydrogenation and formic acid dehydrogenation activity. These studies yielded an optimized catalyst that achieved over 118 000 turnovers in CO₂ hydrogenation, 247 000 turnovers in HCO₂H dehydrogenation, was applied in a hydrogen storage device used for 6 cycles of hydrogen storage/release without requiring changes in pH or solvent, and generated H₂/CO₂ gas at a pressure of 190 atm from formic acid.