CO₂ electroreduction reaction offers an attractive approach to global carbon neutrality. Industrial CO₂ electrolysis towards formate requires stepped-up current densities, which is limited by the difficulty of precisely reconciling the competing intermediates (COOH* and HCOO*). Herein, nano-crumples induced Sn-Bi bimetallic interface-rich materials are in situ designed by tailored electrodeposition under CO₂ electrolysis conditions, significantly expediting formate production. Compared with Sn-Bi bulk alloy and pure Sn, this Sn-Bi interface pattern delivers optimum upshift of Sn p-band center, accordingly the moderate valence electron depletion, which leads to weakened Sn-C hybridization of competing COOH* and suitable Sn-O hybridization of HCOO*. Superior partial current density up to 140 mA/cm² for formate is achieved. High Faradaic efficiency (>90%) is maintained at a wide potential window with a durability of 160 h. In this work, we elevate the interface design of highly active and stable materials for efficient CO₂ electroreduction.

This study reports the preparation of pyrrolic-structure enriched nitrogen doped graphene by hydrothermal synthesis at varied temperature. The morphology, structure and composition of the prepared nitrogen doped graphene were confirmed with SEM, XRD, XPS and Raman spectroscopy. The material was tested for supercapacitive behavior. It was found that doping graphene with nitrogen increased the electrical double layer supercapacitance to as high as 194 F g⁻¹. Furthermore, density functional theory (DFT) calculations showed the proper level of binding energy found between the pyrrolic-nitrogen structure and the electrolyte ions, which may be used to explain the highest contribution of the pyrrolic-structure to the capacitance.