Oxygen‐Bridged Copper–Iron Atomic Pair as Dual‐Metal Active Sites for Boosting Electrocatalytic NO Reduction

Abstract

Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH3) is a promising approach to NH3 synthesis. However, due to the lack of efficient electrocatalysts, the performance of electrocatalytic NO reduction reaction (NORR) is far from satisfactory. Herein, it is reported that an atomic copper–iron dual‐site electrocatalyst bridged by an axial oxygen atom (OFeN6Cu) is anchored on nitrogen‐doped carbon (CuFe DS/NC) for NORR. The CuFe DS/NC can significantly enhance the electrocatalytic NH3 synthesis performance (Faraday efficiency, 90%; yield rate, 112.52 µmol cm−2 h−1) at −0.6 V versus RHE, which is dramatically higher than the corresponding Cu single‐atom, Fe single‐atom and all NORR single‐atom catalysts in the literature so far. Moreover, an assembled proof‐of‐concept Zn–NO battery using CuFe DS/NC as the cathode outputs a power density of 2.30 mW cm−2 and an NH3 yield of 45.52 µg h−1 mgcat−1. The theoretical calculation result indicates that bimetallic sites can promote electrocatalytic NORR by changing the rate‐determining step and accelerating the protonation process. This work provides a flexible strategy for efficient sustainable NH3 synthesis.

Emerging single-atom catalysts in the detection and purification of contaminated gases

“…13a ), which has attracted significant interest in the scientific community. 201 Fig. 13b shows the relationship between the calculated Δ G for NO adsorption on transition metal (TM)-N 4 /graphene and the d-band center of the central TM, demonstrating a clear linear correlation.…”

Research progress of dual-atom site catalysts for photocatalysis

“…In addition to the NRR to NH 3 , the reduction of nitrate (NO 3 − ) or NO to NH 3 using DASCs has attracted attention due to their high conversion efficiency and low cost. 152,153 Shu et al studied the NO 3 RR performance by using a series of graphitic carbon nitride (g-CN)-supported diatomic catalysts. 154 The reaction pathway of the NO 3 RR is shown in Fig.…”

Copper-based electro-catalytic nitrate reduction to ammonia from water: Mechanism, preparation, and research directions

“…Based on density functional theory (DFT) calculations of Gibbs free energies on intermediates, the most common reaction pathways for NO 3 RR can be deduced [ 31 , 32 ]. And DFT calculations were widely used in the NO 3 RR-related mechanism study [ [33] , [34] , [35] ]. Researchers also used software such as VASP, Gaussian, and Materials Studio et al.…”