Covalently Interlayer-Confined Organic–Inorganic Heterostructures for Aqueous Potassium Ion Supercapacitors

Jianping Chen; Bin Liu; Hang Cai; Shude Liu; Yusuke Yamauchi; Seong Chan Jun

doi:10.1002/smll.202204275

Covalently Interlayer-Confined Organic–Inorganic Heterostructures for Aqueous Potassium Ion Supercapacitors

Jianping Chen, Bin Liu, Hang Cai, Shude Liu, Yusuke Yamauchi, Seong Chan Jun

Department of Mechanical Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

Artificial assembly of organic–inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer-confined organic (polyaniline [PANI])–inorganic (MoS₂) hybrid with a dual charge-storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS₂, expands the interlayer spacing of MoS₂, and increases the hydrophilicity. More in-depth insights from the synchrotron radiation-based X-ray technique illustrate that the covalent grafting of PANI to MoS₂ induces the formation of Mo-N bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross-layer electron transfer and decreases the diffusion barrier of K⁺ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic–inorganic heterostructures for superior K-ion storage. The K-ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X-ray photoelectron spectroscopy.

Original language	English
Article number	2204275
Journal	Small
Volume	19
Issue number	4
DOIs	https://doi.org/10.1002/smll.202204275
Publication status	Published - 2023 Jan 25

Bibliographical note

Funding Information:
J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF-2019R1A2C2090443) ‘20013621', and Technology Innovation Program (‘20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers.

Funding Information:
J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF‐2019R1A2C2090443) ‘20013621', and Technology Innovation Program (‘20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST‐ERATO Yamauchi Materials Space‐Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers.

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

Biotechnology
Chemistry(all)
Biomaterials
Materials Science(all)

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10.1002/smll.202204275

Cite this

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title = "Covalently Interlayer-Confined Organic–Inorganic Heterostructures for Aqueous Potassium Ion Supercapacitors",

abstract = "Artificial assembly of organic–inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer-confined organic (polyaniline [PANI])–inorganic (MoS2) hybrid with a dual charge-storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS2, expands the interlayer spacing of MoS2, and increases the hydrophilicity. More in-depth insights from the synchrotron radiation-based X-ray technique illustrate that the covalent grafting of PANI to MoS2 induces the formation of Mo-N bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross-layer electron transfer and decreases the diffusion barrier of K+ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic–inorganic heterostructures for superior K-ion storage. The K-ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X-ray photoelectron spectroscopy.",

author = "Jianping Chen and Bin Liu and Hang Cai and Shude Liu and Yusuke Yamauchi and Jun, {Seong Chan}",

note = "Funding Information: J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF-2019R1A2C2090443) {\textquoteleft}20013621', and Technology Innovation Program ({\textquoteleft}20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers. Funding Information: J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF‐2019R1A2C2090443) {\textquoteleft}20013621', and Technology Innovation Program ({\textquoteleft}20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST‐ERATO Yamauchi Materials Space‐Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers. Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH.",

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doi = "10.1002/smll.202204275",

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AU - Cai, Hang

AU - Liu, Shude

AU - Yamauchi, Yusuke

AU - Jun, Seong Chan

N1 - Funding Information: J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF-2019R1A2C2090443) ‘20013621', and Technology Innovation Program (‘20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers. Funding Information: J.C. and B.L. contributed equally to this work. The authors acknowledge financial support from the Henan Provincial Science and Technology Research Project (No. 212102210585). S. Liu and S.C. Jun gratefully acknowledge the financial support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (MIST) (No. NRF‐2019R1A2C2090443) ‘20013621', and Technology Innovation Program (‘20013621', Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). S. Liu and Y. Yamauchi would like to gratefully acknowledge the financial support from the JST‐ERATO Yamauchi Materials Space‐Tectonics Project (JPMJER2003). This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers. Publisher Copyright: © 2022 Wiley-VCH GmbH.

PY - 2023/1/25

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N2 - Artificial assembly of organic–inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer-confined organic (polyaniline [PANI])–inorganic (MoS2) hybrid with a dual charge-storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS2, expands the interlayer spacing of MoS2, and increases the hydrophilicity. More in-depth insights from the synchrotron radiation-based X-ray technique illustrate that the covalent grafting of PANI to MoS2 induces the formation of Mo-N bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross-layer electron transfer and decreases the diffusion barrier of K+ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic–inorganic heterostructures for superior K-ion storage. The K-ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X-ray photoelectron spectroscopy.

AB - Artificial assembly of organic–inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer-confined organic (polyaniline [PANI])–inorganic (MoS2) hybrid with a dual charge-storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS2, expands the interlayer spacing of MoS2, and increases the hydrophilicity. More in-depth insights from the synchrotron radiation-based X-ray technique illustrate that the covalent grafting of PANI to MoS2 induces the formation of Mo-N bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross-layer electron transfer and decreases the diffusion barrier of K+ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic–inorganic heterostructures for superior K-ion storage. The K-ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X-ray photoelectron spectroscopy.

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Covalently Interlayer-Confined Organic–Inorganic Heterostructures for Aqueous Potassium Ion Supercapacitors

Abstract

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