Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices

Abstract Conductive 2D nanosheets have evoked tremendous scientific efforts because of their high efficiency as hybridization matrices for improving diverse functionalities of nanostructured materials. To address the problems posed by previously reported conductive nanosheets like poorly‐interacting...

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Main Authors: Nam Hee Kwon, Se‐Jun Kim, Tae‐Ha Gu, Jang Mee Lee, Myung Hwa Kim, Dooam Paik, Xiaoyan Jin, Hyungjun Kim, Seong‐Ju Hwang
Format: Article
Language:English
Published: Wiley 2024-11-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202408948
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author Nam Hee Kwon
Se‐Jun Kim
Tae‐Ha Gu
Jang Mee Lee
Myung Hwa Kim
Dooam Paik
Xiaoyan Jin
Hyungjun Kim
Seong‐Ju Hwang
author_facet Nam Hee Kwon
Se‐Jun Kim
Tae‐Ha Gu
Jang Mee Lee
Myung Hwa Kim
Dooam Paik
Xiaoyan Jin
Hyungjun Kim
Seong‐Ju Hwang
author_sort Nam Hee Kwon
collection DOAJ
description Abstract Conductive 2D nanosheets have evoked tremendous scientific efforts because of their high efficiency as hybridization matrices for improving diverse functionalities of nanostructured materials. To address the problems posed by previously reported conductive nanosheets like poorly‐interacting graphene and cost‐ineffective RuO2 nanosheets, economically feasible noble‐metal‐free conductive [MnxCo1−2xNix]O2 oxide nanosheets are synthesized with outstanding interfacial interaction capability. The surface‐optimized [Mn1/4Co1/2Ni1/4]O2 nanosheets outperformed RuO2/graphene nanosheets as hybridization matrices in exploring high‐performance visible‐light‐active (λ >420 nm) photocatalysts. The most efficient g‐C3N4–[Mn1/4Co1/2Ni1/4]O2 nanohybrid exhibited unusually high photocatalytic activity (NH4+ formation rate: 1.2 mmol g−1 h−1), i.e., one of the highest N2 reduction efficiencies. The outstanding hybridization effect of the defective [Mn1/4Co1/2Ni1/4]O2 nanosheets is attributed to the optimization of surface bonding character and electronic structure, allowing for improved interfacial coordination bonding with g‐C3N4 at the defect sites. Results from spectroscopic measurements and theoretical calculations reveal that hybridization helps optimize the bandgap energy, and improves charge separation, N2 adsorptivity, and surface reactivity. The universality of the [Mn1/4Co1/2Ni1/4]O2 nanosheet as versatile hybridization matrices is corroborated by the improvement in the electrocatalytic activity of hybridized Co−Fe‐LDH as well as the photocatalytic hydrogen production ability of hybridized CdS.
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spelling doaj-art-217a8945bd9c40b5bbc847ec0788f3852025-08-20T01:52:38ZengWileyAdvanced Science2198-38442024-11-011144n/an/a10.1002/advs.202408948Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization MatricesNam Hee Kwon0Se‐Jun Kim1Tae‐Ha Gu2Jang Mee Lee3Myung Hwa Kim4Dooam Paik5Xiaoyan Jin6Hyungjun Kim7Seong‐Ju Hwang8Department of Materials Science and Engineering College of Engineering Yonsei University Seoul 03722 Republic of KoreaDepartment of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of KoreaDepartment of Chemistry and Nanoscience College of Natural Science Ewha Womans University Seoul 03760 Republic of KoreaCentre for Advanced Materials and Industrial Chemistry (CAMIC) School of Science Royal Melbourne Institute of Technology (RMIT) University Melbourne VIC 3001 AustraliaDepartment of Chemistry and Nanoscience College of Natural Science Ewha Womans University Seoul 03760 Republic of KoreaDepartment of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of KoreaDepartment of Applied Chemistry College of Natural Science University of Seoul Seoul 02504 Republic of KoreaDepartment of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of KoreaDepartment of Materials Science and Engineering College of Engineering Yonsei University Seoul 03722 Republic of KoreaAbstract Conductive 2D nanosheets have evoked tremendous scientific efforts because of their high efficiency as hybridization matrices for improving diverse functionalities of nanostructured materials. To address the problems posed by previously reported conductive nanosheets like poorly‐interacting graphene and cost‐ineffective RuO2 nanosheets, economically feasible noble‐metal‐free conductive [MnxCo1−2xNix]O2 oxide nanosheets are synthesized with outstanding interfacial interaction capability. The surface‐optimized [Mn1/4Co1/2Ni1/4]O2 nanosheets outperformed RuO2/graphene nanosheets as hybridization matrices in exploring high‐performance visible‐light‐active (λ >420 nm) photocatalysts. The most efficient g‐C3N4–[Mn1/4Co1/2Ni1/4]O2 nanohybrid exhibited unusually high photocatalytic activity (NH4+ formation rate: 1.2 mmol g−1 h−1), i.e., one of the highest N2 reduction efficiencies. The outstanding hybridization effect of the defective [Mn1/4Co1/2Ni1/4]O2 nanosheets is attributed to the optimization of surface bonding character and electronic structure, allowing for improved interfacial coordination bonding with g‐C3N4 at the defect sites. Results from spectroscopic measurements and theoretical calculations reveal that hybridization helps optimize the bandgap energy, and improves charge separation, N2 adsorptivity, and surface reactivity. The universality of the [Mn1/4Co1/2Ni1/4]O2 nanosheet as versatile hybridization matrices is corroborated by the improvement in the electrocatalytic activity of hybridized Co−Fe‐LDH as well as the photocatalytic hydrogen production ability of hybridized CdS.https://doi.org/10.1002/advs.202408948hybridization matrixinterfacial coordination bondingnoble‐metal‐free conductive oxide nanosheetphoto‐/electro‐catalystsurface optimization
spellingShingle Nam Hee Kwon
Se‐Jun Kim
Tae‐Ha Gu
Jang Mee Lee
Myung Hwa Kim
Dooam Paik
Xiaoyan Jin
Hyungjun Kim
Seong‐Ju Hwang
Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
Advanced Science
hybridization matrix
interfacial coordination bonding
noble‐metal‐free conductive oxide nanosheet
photo‐/electro‐catalyst
surface optimization
title Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
title_full Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
title_fullStr Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
title_full_unstemmed Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
title_short Surface Optimization of Noble‐Metal‐Free Conductive [Mn1/4Co1/2Ni1/4]O2 Nanosheets for Boosting Their Efficacy as Hybridization Matrices
title_sort surface optimization of noble metal free conductive mn1 4co1 2ni1 4 o2 nanosheets for boosting their efficacy as hybridization matrices
topic hybridization matrix
interfacial coordination bonding
noble‐metal‐free conductive oxide nanosheet
photo‐/electro‐catalyst
surface optimization
url https://doi.org/10.1002/advs.202408948
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