Controllable CO₂ electroreduction to pure syngas and ethanol on CuZn-LDH surface with tunable intermediates affinity

Electrochemical CO2 reduction (ECR) towards pure syngas (CO/H-2 = 0.33-3.3) and ethanol as single gas-liquid products is highly desirable and challenging, which could achieve maximized CO2 utilization and avoid subsequent separation and purification processes. Herein, a series of Cu/Zn layered double hydroxides (CuZn-LDHs) nanosheets with various Cu/Zn ratios were fabricated for ECR to produce pure syngas and ethanol. The formation of uniformly dispersed Cu/Zn sites in CuZn-LDHs finely modulated the adsorption strength of *CO(2)(center dot-)and *H intermediates. Combined with the large electrochemical active surface area (ECSA) and small charge transfer resistance, the obtained optimal Cu3Zn3-LDH catalyst with appropriate *CO2 center dot- and *H binding affinity exhibited high Faraday efficiency (FE) for pure syngas (74.7%) and ethanol (15.0 %). Notably, the Cu3Zn3-LDH showed a good durability with a FE of 82.1% for 5 h at -1.25 V vs RHE. This work put forward a promising candidate of LDHs-based electrocatalysts for ECR to prepare single gas-liquid products.