Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction

Abstract

Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO₂RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO₂) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FE_CO) values exceeding 90% across a broad potential range of −0.55 to −0.9 V (vs. RHE), and attains the maximum FE_CO of 95.6% at −0.75 V (vs. RHE) in 0.5 M NaHCO₃. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm⁻² is achieved in a flow cell at −0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO₂ activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO₂ reduction across a wide potential window.