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Hierarchical NiCo2Se4 Arrays Composed of Atomically Thin Nanosheets: Simultaneous Improvements in Thermodynamics and Kinetics for Electrocatalytic Water Splitting in Neutral Media

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Title: Hierarchical NiCo2Se4 Arrays Composed of Atomically Thin Nanosheets: Simultaneous Improvements in Thermodynamics and Kinetics for Electrocatalytic Water Splitting in Neutral Media
Authors: Hongyu Chen, Yongsheng Xu, Xiaojie Li, Qing Ma, Delong Xie, Yi Mei, Guojing Wang, Yuanzhi Zhu
Source: Advanced Science, Vol 11, Iss 31, Pp n/a-n/a (2024)
Publisher Information: Wiley, 2024.
Publication Year: 2024
Collection: LCC:Science
Subject Terms: hierarchical ultrathin nanosheets, selenide, structural reconstruction, vacancies, water splitting, Science
More Details: Abstract The inefficiency of electrocatalysts for water splitting in neutral media stems from a comprehensive impact of poor intrinsic activity, a limited number of active sites, and inadequate mass transport. Herein, hierarchical ultrathin NiCo2Se4 nanosheets are synthesized by the selenization of NiCo2O4 porous nanoneedles. Theoretical and experimental investigations reveal that the intrinsic hydrogen evolution reaction (HER) activity primarily originate from the NiCo2Se4, whereas the high oxygen evolution reaction (OER) performance is related to the NiCoOOH due to the structural reconstruction. The abundant Se and O vacancies introduced by atomically thin nanostructure modulate the electronic structure of NiCo2Se4 and NiCoOOH, thereby improving the intrinsic HER and OER activities, respectively. COMSOL simulation demonstrate the edges of extended nanosheets from the main body significantly promote the charge aggregation, boosting the reduction and oxidation current during HER/OER process. This charge aggregation effect notably exceeds the tip effect for the nanoneedle, highlighting the unique advantage of the hierarchical nanosheet structure. Benefiting from abundant vacancies and unique nanostructure, the hierarchical ultrathin nanosheet simultaneously improve the thermodynamics and kinetics of the electrocatalyst. The optimized samples display an overpotential of 92 mV for HER and 214 mV for OER at 100 mA cm−2, significantly surpassing the performance of currently reported HER/OER catalysts in neutral media.
Document Type: article
File Description: electronic resource
Language: English
ISSN: 2198-3844
Relation: https://doaj.org/toc/2198-3844
DOI: 10.1002/advs.202402889
Access URL: https://doaj.org/article/abc838d3bf6a4db48d348cc35b1d59d2
Accession Number: edsdoj.bc838d3bf6a4db48d348cc35b1d59d2
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  Data: Hierarchical NiCo2Se4 Arrays Composed of Atomically Thin Nanosheets: Simultaneous Improvements in Thermodynamics and Kinetics for Electrocatalytic Water Splitting in Neutral Media
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  Data: <searchLink fieldCode="AR" term="%22Hongyu+Chen%22">Hongyu Chen</searchLink><br /><searchLink fieldCode="AR" term="%22Yongsheng+Xu%22">Yongsheng Xu</searchLink><br /><searchLink fieldCode="AR" term="%22Xiaojie+Li%22">Xiaojie Li</searchLink><br /><searchLink fieldCode="AR" term="%22Qing+Ma%22">Qing Ma</searchLink><br /><searchLink fieldCode="AR" term="%22Delong+Xie%22">Delong Xie</searchLink><br /><searchLink fieldCode="AR" term="%22Yi+Mei%22">Yi Mei</searchLink><br /><searchLink fieldCode="AR" term="%22Guojing+Wang%22">Guojing Wang</searchLink><br /><searchLink fieldCode="AR" term="%22Yuanzhi+Zhu%22">Yuanzhi Zhu</searchLink>
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  Data: Advanced Science, Vol 11, Iss 31, Pp n/a-n/a (2024)
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  Data: Abstract The inefficiency of electrocatalysts for water splitting in neutral media stems from a comprehensive impact of poor intrinsic activity, a limited number of active sites, and inadequate mass transport. Herein, hierarchical ultrathin NiCo2Se4 nanosheets are synthesized by the selenization of NiCo2O4 porous nanoneedles. Theoretical and experimental investigations reveal that the intrinsic hydrogen evolution reaction (HER) activity primarily originate from the NiCo2Se4, whereas the high oxygen evolution reaction (OER) performance is related to the NiCoOOH due to the structural reconstruction. The abundant Se and O vacancies introduced by atomically thin nanostructure modulate the electronic structure of NiCo2Se4 and NiCoOOH, thereby improving the intrinsic HER and OER activities, respectively. COMSOL simulation demonstrate the edges of extended nanosheets from the main body significantly promote the charge aggregation, boosting the reduction and oxidation current during HER/OER process. This charge aggregation effect notably exceeds the tip effect for the nanoneedle, highlighting the unique advantage of the hierarchical nanosheet structure. Benefiting from abundant vacancies and unique nanostructure, the hierarchical ultrathin nanosheet simultaneously improve the thermodynamics and kinetics of the electrocatalyst. The optimized samples display an overpotential of 92 mV for HER and 214 mV for OER at 100 mA cm−2, significantly surpassing the performance of currently reported HER/OER catalysts in neutral media.
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        Value: 10.1002/advs.202402889
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      – Text: English
    Subjects:
      – SubjectFull: hierarchical ultrathin nanosheets
        Type: general
      – SubjectFull: selenide
        Type: general
      – SubjectFull: structural reconstruction
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      – SubjectFull: vacancies
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      – TitleFull: Hierarchical NiCo2Se4 Arrays Composed of Atomically Thin Nanosheets: Simultaneous Improvements in Thermodynamics and Kinetics for Electrocatalytic Water Splitting in Neutral Media
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            NameFull: Hongyu Chen
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