Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO3/MnO2@NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors
Abstract
High-performance energy storage devices (HPEDs) play a critical role in the realization of clean energy and thus enable the overarching pursuit of nonpolluting, green technologies. Supercapacitors are one class of such lucrative HPEDs; however, a serious limiting factor of supercapacitor technology is its sub-par energy density. Here, this report presents hitherto unchartered pathway of physical deformation, chemical dealloying, and microstructure engineering to produce ultrahigh-capacitance, energy-dense NiMn alloy electrodes. The activated electrode delivered an ultrahigh specific-capacitance of 2700 F/cm3 at 0.5 A/cm3. The symmetric device showcased an excellent energy density of 96.94 Wh/L and a remarkable cycle life of 95% retention after 10,000 cycles. Transmission electron microscopy and atom probe tomography studies revealed the evolution of a unique hierarchical microstructure comprising fine Ni/NiMnO3 nanoligaments within MnO2-rich nanoflakes. Theoretical analysis using density functional theory showed semimetallic nature of the nanoscaled oxygen-vacancy-rich NiMnO3 structure, highlighting enhanced carrier concentration and electronic conductivity of the active region. Furthermore, the geometrical model of NiMnO3 crystals revealed relatively large voids, likely providing channels for the ion intercalation/de-intercalation. The current processing approach is highly adaptable and can be applied to a wide range of material systems for designing highly efficient electrodes for energy-storage devices.
- Authors:
-
- Shiv Nadar University (India)
- University of Petroleum and Energy Studies (India)
- Colorado State Univ., Fort Collins, CO (United States)
- Univ. of North Texas, Denton, TX (United States)
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); North Carolina State University, Raleigh, NC (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1975262
- Report Number(s):
- PNNL-SA-181415
Journal ID: ISSN 1944-8244
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 4; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; oxygen vacancies; physical deformation; atom probe tomography; density functional theory; hierarchical microstructures; defects in solids; electrical properties; electrodes; ions; transition metals
Citation Formats
Thomas, Arpit, Kumar, Ambrish, Perumal, Gopinath, Sharma, Ram Kumar, Manivasagam, Vignesh, Popat, Ketul C., Ayyagari, Aditya, Yu, Anqi, Tripathi, Shalini, Buck, Edgar C., Gwalani, Bharat, Bhogra, Meha, and Arora, Harpreet Singh. Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO3/MnO2@NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors. United States: N. p., 2023.
Web. doi:10.1021/acsami.2c16818.
Thomas, Arpit, Kumar, Ambrish, Perumal, Gopinath, Sharma, Ram Kumar, Manivasagam, Vignesh, Popat, Ketul C., Ayyagari, Aditya, Yu, Anqi, Tripathi, Shalini, Buck, Edgar C., Gwalani, Bharat, Bhogra, Meha, & Arora, Harpreet Singh. Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO3/MnO2@NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors. United States. https://doi.org/10.1021/acsami.2c16818
Thomas, Arpit, Kumar, Ambrish, Perumal, Gopinath, Sharma, Ram Kumar, Manivasagam, Vignesh, Popat, Ketul C., Ayyagari, Aditya, Yu, Anqi, Tripathi, Shalini, Buck, Edgar C., Gwalani, Bharat, Bhogra, Meha, and Arora, Harpreet Singh. Fri .
"Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO3/MnO2@NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors". United States. https://doi.org/10.1021/acsami.2c16818. https://www.osti.gov/servlets/purl/1975262.
@article{osti_1975262,
title = {Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO3/MnO2@NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors},
author = {Thomas, Arpit and Kumar, Ambrish and Perumal, Gopinath and Sharma, Ram Kumar and Manivasagam, Vignesh and Popat, Ketul C. and Ayyagari, Aditya and Yu, Anqi and Tripathi, Shalini and Buck, Edgar C. and Gwalani, Bharat and Bhogra, Meha and Arora, Harpreet Singh},
abstractNote = {High-performance energy storage devices (HPEDs) play a critical role in the realization of clean energy and thus enable the overarching pursuit of nonpolluting, green technologies. Supercapacitors are one class of such lucrative HPEDs; however, a serious limiting factor of supercapacitor technology is its sub-par energy density. Here, this report presents hitherto unchartered pathway of physical deformation, chemical dealloying, and microstructure engineering to produce ultrahigh-capacitance, energy-dense NiMn alloy electrodes. The activated electrode delivered an ultrahigh specific-capacitance of 2700 F/cm3 at 0.5 A/cm3. The symmetric device showcased an excellent energy density of 96.94 Wh/L and a remarkable cycle life of 95% retention after 10,000 cycles. Transmission electron microscopy and atom probe tomography studies revealed the evolution of a unique hierarchical microstructure comprising fine Ni/NiMnO3 nanoligaments within MnO2-rich nanoflakes. Theoretical analysis using density functional theory showed semimetallic nature of the nanoscaled oxygen-vacancy-rich NiMnO3 structure, highlighting enhanced carrier concentration and electronic conductivity of the active region. Furthermore, the geometrical model of NiMnO3 crystals revealed relatively large voids, likely providing channels for the ion intercalation/de-intercalation. The current processing approach is highly adaptable and can be applied to a wide range of material systems for designing highly efficient electrodes for energy-storage devices.},
doi = {10.1021/acsami.2c16818},
journal = {ACS Applied Materials and Interfaces},
number = 4,
volume = 15,
place = {United States},
year = {Fri Jan 20 00:00:00 EST 2023},
month = {Fri Jan 20 00:00:00 EST 2023}
}
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