A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH

The electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) offers an energy-saving and environmentally friendly approach to producing hydrocarbon fuels. The use of a gas diffusion electrode (GDE) flow cell has generally improved the rate of CO<sub>2</s...

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Bibliographic Details
Main Authors: Liqun Wu, Xiaojun He, Jian Zhou
Format: Article
Language:English
Published: MDPI AG 2025-07-01
Series:Applied Sciences
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Online Access:https://www.mdpi.com/2076-3417/15/14/8095
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Summary:The electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) offers an energy-saving and environmentally friendly approach to producing hydrocarbon fuels. The use of a gas diffusion electrode (GDE) flow cell has generally improved the rate of CO<sub>2</sub>RR, while the gas diffusion layer (GDL) remains a significant challenge. In this study, we successfully engineered a novel metal–organic framework (MOF) heterojunction through the controlled coating of zeolitic imidazolate framework (ZIF-L) on ultrathin nickel—metal–organic framework (Ni-MOF) nanosheets. This innovative architecture simultaneously integrates GDL functionality and exposes abundant solid–liquid–gas triple-phase boundaries. The resulting Ni-MOF@ZIF-L heterostructure demonstrates exceptional performance, achieving a formate Faradaic efficiency of 92.4% while suppressing the hydrogen evolution reaction (HER) to 6.7%. Through computational modeling of the optimized heterojunction configuration, we further elucidated its competitive adsorption behavior and electronic modulation effects. The experimental and theoretical results demonstrate an improvement in electrochemical CO<sub>2</sub> reduction activity with suppressed hydrogen evolution for the heterojunction because of its hydrophobic interface, good electron transfer capability, and high CO<sub>2</sub> adsorption at the catalyst interface. This work provides a new insight into the rational design of porous crystalline materials in electrocatalytic CO<sub>2</sub>RR.
ISSN:2076-3417