Affiliation:
1. Key Laboratory of Structure and Functional Regulation of Hybrid Materials Ministry of Education Institute of Energy Hefei Comprehensive National Science Center Anhui University Hefei 230601 P. R. China
Abstract
AbstractThe electrochemical reduction of nitrate to ammonia (NO3RR) has emerged as a promising but challenging orientation in sustainable development. Cu is one of the most effective NO3RR catalysts. However, the accumulation of NO2− on their surface has erected bars to the further improvement of NO3RR efficiency. Herein, Cu‐based electrocatalyst with low‐coordinated Cu atoms (Cu‐LC) is synthesized via the instantaneous ablation and rapid cooling of the Cu target by pulse laser and proposed as a new NO3RR electrocatalyst, which exhibits enhanced NO3RR activity with NH3 selectivity of 97.01%, yield rate of 0.624 mmol h−1 cm−2 at −0.8 V versus RHE and long‐term durability, superior to most reported Cu‐based catalysts. The introduction of low‐coordinated Cu sites upshifts the Cu d‐band center to near the Fermi Level, enhancing the adsorption of key intermediates (*NO2, *NO) in NO3RR, and also effectively regulating the generation of *NO2 and hydrogenation process, inhibiting the accumulation of NO2− on the Cu‐LC surface, thus achieving efficient NH3 production. Furthermore, when evaluated as cathode material in Zn–NO3− battery, an open circuit voltage of 1.3 V and a power density of 3.1 mW cm−2 are achieved by the Cu‐LC‐based battery, highlighting a promising multifunctional system for ammonia production and energy supply.
Funder
National Natural Science Foundation of China
National Key Research and Development Program of China
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials