Probing the Charge Storage Mechanism of a Pseudocapacitive MnO2 Electrode Using in Operando Raman Spectroscopy
Abstract
Although manganese oxide (MnO2) has been extensively studied as an electrode material for pseudocapacitors, a clear understanding of its charge storage mechanism is still lacking. Here we report our findings in probing the structural changes of a thin-film model MnO2 electrode during cycling using in operando Raman spectroscopy. The spectral features (e.g., band position, intensity, and width) are correlated quantitatively with the size (Li+, Na+, and K+) of cations in different electrolytes and with the degree of discharge to gain better understanding of the cation-incorporation mechanism into the interlayers of pseudocapacitive MnO2. Also, theoretical calculations of phonon energy associated with the models of interlayer cation-incorporated MnO2 agree with the experimental observations of cation-size effect on the positions of Raman bands. Additionally, the cation-size effects on spectral features at different potentials of MnO2 electrode are correlated quantitatively with the amount of charge stored in the MnO2 electrode. The understanding of the structural changes associated with charge storage gained from Raman spectroscopy provides valuable insights into the cation-size effects on the electrochemical performances of the MnO2 electrode.
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Heterogeneous Functional Materials Center (HeteroFoaM)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1370164
- Grant/Contract Number:
- SC0001061
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 27; Journal Issue: 19; Related Information: HeteroFoaM partners with University of South Carolina (lead); University of California, Santa Barbara; University of Connecticut; Georgia Institute of Technology; Princeton University; Rochester Institute of Technology; Savannah River National Laboratory; University of South Carolina; University of Utah; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Pseudocapacitor; manganese oxides (MnO2); operando; Raman spectroscopy; cation incorporation
Citation Formats
Chen, Dongchang, Ding, Dong, Li, Xiaxi, Waller, Gordon Henry, Xiong, Xunhui, El-Sayed, Mostafa A., and Liu, Meilin. Probing the Charge Storage Mechanism of a Pseudocapacitive MnO2 Electrode Using in Operando Raman Spectroscopy. United States: N. p., 2015.
Web. doi:10.1021/acs.chemmater.5b03118.
Chen, Dongchang, Ding, Dong, Li, Xiaxi, Waller, Gordon Henry, Xiong, Xunhui, El-Sayed, Mostafa A., & Liu, Meilin. Probing the Charge Storage Mechanism of a Pseudocapacitive MnO2 Electrode Using in Operando Raman Spectroscopy. United States. https://doi.org/10.1021/acs.chemmater.5b03118
Chen, Dongchang, Ding, Dong, Li, Xiaxi, Waller, Gordon Henry, Xiong, Xunhui, El-Sayed, Mostafa A., and Liu, Meilin. Thu .
"Probing the Charge Storage Mechanism of a Pseudocapacitive MnO2 Electrode Using in Operando Raman Spectroscopy". United States. https://doi.org/10.1021/acs.chemmater.5b03118. https://www.osti.gov/servlets/purl/1370164.
@article{osti_1370164,
title = {Probing the Charge Storage Mechanism of a Pseudocapacitive MnO2 Electrode Using in Operando Raman Spectroscopy},
author = {Chen, Dongchang and Ding, Dong and Li, Xiaxi and Waller, Gordon Henry and Xiong, Xunhui and El-Sayed, Mostafa A. and Liu, Meilin},
abstractNote = {Although manganese oxide (MnO2) has been extensively studied as an electrode material for pseudocapacitors, a clear understanding of its charge storage mechanism is still lacking. Here we report our findings in probing the structural changes of a thin-film model MnO2 electrode during cycling using in operando Raman spectroscopy. The spectral features (e.g., band position, intensity, and width) are correlated quantitatively with the size (Li+, Na+, and K+) of cations in different electrolytes and with the degree of discharge to gain better understanding of the cation-incorporation mechanism into the interlayers of pseudocapacitive MnO2. Also, theoretical calculations of phonon energy associated with the models of interlayer cation-incorporated MnO2 agree with the experimental observations of cation-size effect on the positions of Raman bands. Additionally, the cation-size effects on spectral features at different potentials of MnO2 electrode are correlated quantitatively with the amount of charge stored in the MnO2 electrode. The understanding of the structural changes associated with charge storage gained from Raman spectroscopy provides valuable insights into the cation-size effects on the electrochemical performances of the MnO2 electrode.},
doi = {10.1021/acs.chemmater.5b03118},
journal = {Chemistry of Materials},
number = 19,
volume = 27,
place = {United States},
year = {Thu Sep 24 00:00:00 EDT 2015},
month = {Thu Sep 24 00:00:00 EDT 2015}
}
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