Rare-earth neodymium single atom catalyst for efficient electrochemical CO2 reduction

Abstract

Electrochemical reduction of carbon dioxide (CO₂) to valuable fuels or feedstocks holds great promise for zero-emission carbon recycling and renewable energy storage. However, it remains a great challenge to prepare high-performance rare earth single-atom catalysts (SACs) for electroreduction of CO₂. In this work, we reported the facile synthesis of Nd SACs with atomically dispersed Nd-N₆ active sites by using g-C₃N₄ as support (Nd₁/NC) for efficient electroreduction of CO₂ to CO. Nd₁/NC exhibited a maximum FE of 83 % and a CO partial current density of 7.0 mA cm⁻², and a stability of 50 h at −0.8 V in an H-cell. Notably, a dramatically improved CO partial current density of 50.6 mA cm⁻² with FE_CO of up to 93 % was obtained in the flow cell. DFT calculations revealed that the Nd-N₆ sites facilitate the transfer of electrons from g-C₃N₄ to Nd, which strengthens the adsorption of the *COOH intermediate, contributing to the enhanced catalytic activity.