Reconstruction-induced NiCu-based catalysts towards paired electrochemical refining

A paired electrochemical refinery toward the cathodic nitrate reduction reaction (NO 3 RR) and anodic glycerol oxidation reaction (GOR) driven by renewable electricity could generate high value-added ammonia and formic acid simultaneously. However, both cathode and anode electrocatalysts often suffer from low efficiency and unclear reconstruction. Herein, we prepare a non-noble NiCuOH nanocomposite precatalyst composed of crystalline Cu 2 (OH) 3 (NO 3 ) and amorphous Ni(OH) 2 , which can be reconstructed into high-activity and stable cathodic NO 3 RR and anodic GOR electrocatalysts under operating conditions. Various in situ and ex situ experiments demonstrate that NiCuOH could convert into active Cu nanoparticles coupled with amorphous Ni(OH) 2 under cathodic NO 3 RR conditions. Meanwhile, under anodic GOR conditions, NiCuOH-derived bimetal oxide (NiCuO) changes into active NiOOH species composited with Cu vacancy-rich CuO. Furthermore, an actual paired electrochemical refinery with the reconstructed NiCu-based catalysts toward the NO 3 RR and GOR shows a low potential of 1.37 V at a current density of 100 mA cm 2 to continuously produce ammonium and formate. This study provides a new paradigm for the design of an electrochemical refinery with reconstructed non-noble electrocatalysts toward chemical upgradation. A paired electrochemical refinery for simultaneously producing value-added ammonium and formate is successfully demonstrated using reconstruction-induced NiCu-based nanocomposites as both cathode and anode electrocatalysts.