The built-in electric field across FeN/Fe3N interface for efficient electrochemical reduction of CO2 to CO

Abstract

Nanostructured metal-nitrides have attracted tremendous interest as a new generation of catalysts for electroreduction of CO2, but these structures have limited activity and stability in the reduction condition. Herein, we report a method of fabricating FeN/Fe3N nanoparticles with FeN/Fe3N interface exposed on the NP surface for efficient electrochemical CO2 reduction reaction (CO2RR). The FeN/Fe3N interface is populated with Fe−N4 and Fe−N2 coordination sites respectively that show the desired catalysis synergy to enhance the reduction of CO2 to CO. The CO Faraday efficiency reaches 98% at −0.4 V vs. reversible hydrogen electrode, and the FE stays stable from −0.4 to −0.9 V during the 100 h electrolysis time period. This FeN/Fe3N synergy arises from electron transfer from Fe3N to FeN and the preferred CO2 adsorption and reduction to *COOH on FeN. Our study demonstrates a reliable interface control strategy to improve catalytic efficiency of the Fe–N structure for CO2RR.

Ultra-fast synthesis of three-dimensional porous Cu/Zn heterostructures for enhanced carbon dioxide electroreduction

“…4e, it is clear that the Cu-CP-1-30 electrode exhibits the highest energy barrier (0.92 eV) at the rst hydrogenation step, and this energy barrier is lowered to 0.82 eV on the Zn-CP-1-30 electrode. In particular, the Cu/Zn-CP-1-30 electrode reduces the energy barrier to 0.66 eV, because the heterostructure sites can improve the adsorption of the *COOH intermediate and facilitate the formation of CO. 50 Taken together, our control experiments and DFT calculations provide compelling evidence certifying that the porous and selfsupported architecture is crucial for fast mass/ion diffusion and the Cu/Zn heterostructures can produce an interfacial bonding effect, offering more active sites for ECR to CO.…”

Mechanistic Insights into the Phase Formation of an Atypical Iron Oxynitride (FexOyNz) System and Its Multifunctional Photocatalytic Applications

“…Conventionally, the magnetic property of photocatalysts is often exploited for their separation from the reaction medium. However, it is reported that the superparamagnetic property of photocatalysts augments the photocatalytic reactions in the presence of a magnetic field owing to the spin alignment of electrons, which influences the charge recombination and electron transfer dynamics in the photocatalytic systems. − …”

Asymmetric Chemical Potential Activated Nanointerfacial Electric Field for Efficient Vanadium Redox Flow Batteries

“…The reason for this lack of efficiency is the low-grade intrinsic catalytic activity at the active sites, where the charge-transfer process and adsorption behavior of active species at the intrinsic activity-dominated region is sluggish (Figure a) and hence unable to cater for fast kinetics. Some emerging strategies, such as electric fields based on semiconductor heterojunctions, can effectively optimize the charge transfer and adsorption processes of reactant species by modulating the coordination and electronic band structures within heterojunctions. − Bearing validations to the point are the recent studies on hydrogen evolution reaction (HER) and CO 2 reduction reaction (CO 2 RR) lying in the heterogeneous interfaces with superior intrinsic activity. , Sun et al developed a FeN/Fe 3 N heterojunction for electrochemical CO 2 RR with a modified interfacial environment for preferential adsorption and reduction of CO 2 , resulting in a dramatically improved catalytic efficiency . However, there remains a gap on the explanation of the chemical and physical origins of redox reactions catalyzed by heterojunction sites in VRFB, let alone unraveling its structure–property-function correlation.…”