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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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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author Liqun Wu
Xiaojun He
Jian Zhou
author_facet Liqun Wu
Xiaojun He
Jian Zhou
author_sort Liqun Wu
collection DOAJ
description 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.
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spelling doaj-art-1ee1cdaf6a964c3198ecf1d7b1b9e8bf2025-08-20T03:58:27ZengMDPI AGApplied Sciences2076-34172025-07-011514809510.3390/app15148095A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOHLiqun Wu0Xiaojun He1Jian Zhou2School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, ChinaSchool of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, ChinaSchool of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, ChinaThe 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.https://www.mdpi.com/2076-3417/15/14/8095electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR)gas diffusion electrode (GDE)metal–organic framework (MOF)heterojunctionhydrophobic interface
spellingShingle Liqun Wu
Xiaojun He
Jian Zhou
A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
Applied Sciences
electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR)
gas diffusion electrode (GDE)
metal–organic framework (MOF)
heterojunction
hydrophobic interface
title A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
title_full A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
title_fullStr A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
title_full_unstemmed A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
title_short A Hierarchically Structured Ni-NOF@ZIF-L Heterojunction Using Van Der Waals Interactions for Electrocatalytic Reduction of CO<sub>2</sub> to HCOOH
title_sort hierarchically structured ni nof zif l heterojunction using van der waals interactions for electrocatalytic reduction of co sub 2 sub to hcooh
topic electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR)
gas diffusion electrode (GDE)
metal–organic framework (MOF)
heterojunction
hydrophobic interface
url https://www.mdpi.com/2076-3417/15/14/8095
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