Efficient Electrosynthesis of Syngas with Tunable CO/H2 Ratios over Znx Cd1-x S-Amine Inorganic-Organic Hybrids.

Efficient electrochemical reduction of CO2 and H2 O into industrial syngas with tunable CO/H2 ratios, especially integrated with anodic organic synthesis to replace the low-value oxygen evolution reaction (OER), is highly desirable. Here, integration of controllable partial substitution of zinc (Zn) with amine incorporation into CdS-amine inorganic-organic hybrids is used to generate highly efficient electrocatalysts for synthesizing syngas with tunable CO/H2 ratios (0-19.7), which are important feedstocks for the Fischer-Tropsch process. Diethylenetriamine could enhance the adsorption and accelerate the activation of CO2 to form the key intermediate COOH* for CO formation. Zn substitution promoted the hydrogen evolution reaction (HER), leading to tunable CO/H2 ratios. Importantly, syngas and dihydroisoquinoline can be simultaneously synthesized by pairing with anodic semi-oxidation of tetrahydroisoquinoline in a Znx Cd1-x S-Amine ∥ Ni2 P two-electrode electrolyzer.