The development of the asymmetric variant of decarboxylative electrocatalytic NHK took place in a bifurcated fashion as outlined in Table on substrates 1 and 2. Thus, parallel optimizations were carried out to maximize reactivity in an electrochemical setting and to maximize ee in a purely chemical system. By separating the challenges of maximizing electrochemical reactivity and ee, the research teams could cover ground more rapidly as it was practically simpler to explore >50 chiral ligands using superstoichiometric Cr loading under low yielding chemical conditions as only the ee measurement was relevant. At the same time, a variety of electrochemical parameters (>150 conditions screened) were explored such as solvent, electrolyte, additives, current density, concentration, and electrode material (see SI for complete summary of both endeavors). Early in those studies it was verified that the ee measurements observed using purely chemical conditions could be translated to non-optimized electrochemical conditions. With relatively optimized conditions and chiral ligand candidates identified, final reaction development commenced with