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Interfacial Electric Field Sharping by Non‐Ionic Halogens Enables Selective CO <sub>2</sub> ‐to C <sub>2+</sub> Electroreduction

Jing Zhou, Dongge Wang, Ying Wang, Minghua Guo, Kewei Zhai, Jing Xu, Yao Wang, Ying Zhang, Chengsi Pan, Bingling He, Yang Lou, Hongwen Huang, Jiawei Zhang, Yongfa Zhu

2025Advanced Energy Materials6 citationsDOI

Abstract

ABSTRACT Halide ions are widely employed to accelerate the electrochemical CO 2 reduction reaction (CO 2 RR), but their practical application is hampered by site blocking and electrode corrosion. Here we present an organic‐inorganic hybrid (OIH) strategy that embeds non‐ionic halogenated molecules (C 8 H 17 X, X = Cl, Br, I) into the Cu 2 O matrix to shape interfacial electric fields. This design preserves the kinetic benefits of halides while eliminating instability from ionic incorporation. The optimized C 8 H 17 Cl‐Cu 2 O OIHs delivers an outstanding C 2+ Faradaic efficiency of 80.6% with a partial current density of 161.2 mA cm −2 . Spectroscopic and theoretical analyses reveal that non‐ionic halogens act as molecular “field shapers,” generating strong interfacial electric fields that strengthen *CO adsorption and balance atop/bridge configurations. This tailored *CO landscape promotes efficient C–C coupling by simultaneously increasing coverage and dimerization kinetics. Our findings establish non‐ionic halogen modifiers as a robust platform for stabilizing and steering interfacial electric fields in CO 2 RR, offering a general strategy for designing selective and durable electrocatalysts.

Topics & Concepts

HalideHalogenMaterials scienceElectric fieldElectrochemistryIonic bondingMoleculeChemical physicsCoupling (piping)Faraday efficiencyIonElectrodeAdsorptionKinetic energyDensity functional theoryMatrix (chemical analysis)Inorganic chemistryIonic liquidNanotechnologyCurrent densityChemical engineeringField (mathematics)InstabilityCatalysisCO2 Reduction Techniques and CatalystsAmmonia Synthesis and Nitrogen ReductionCarbon dioxide utilization in catalysis
Interfacial Electric Field Sharping by Non‐Ionic Halogens Enables Selective CO <sub>2</sub> ‐to C <sub>2+</sub> Electroreduction | Litcius