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Title: Deliberate Modification of Fe 3O 4 Anode Surface Chemistry: Impact on Electrochemistry

Abstract

Fe 3O 4 nanoparticles (NPs) with an average size of 8-10 nm have been successfully functionalized with various surface-treatment agents to serve as model systems for probing surface chemistry-dependent electrochemistry of the resulting electrodes. The surface-treatment agents used for the functionalization of Fe 3O 4 anode materials were systematically varied to include aromatic or aliphatic structures: 4-mercaptobenzoic acid (MBA), benzoic acid (BA), 3-mercaptopropionic acid (MPA), and propionic acid (PA). Both structural and electrochemical characterizations have been used to systematically correlate the electrode functionality with the corresponding surface chemistry. Surface treatment with ligands led to better Fe 3O 4 dispersion, especially with the aromatic ligands. Electrochemistry was impacted where the PA and BA-treated Fe 3O 4 systems without the -SH group demonstrated higher rate capability than their thiol-containing counterparts and the pristine Fe 3O 4. Specifically, the PA system delivered the highest capacity and cycling stability amongst all samples tested. Notably, the aromatic BA system outperformed the aliphatic PA counterpart during extended cycling under high current density, due to the improved charge transfer and ion transport kinetics as well as better dispersion of Fe 3O 4 NPs, induced by the conjugated system. Our surface engineering of the Fe 3O 4 electrodemore » presented herein, highlights the importance of modifying the structure and chemistry of surface-treatment agents as a plausible means of enhancing interfacial charge transfer within metal oxide composite electrodes without hampering the resulting tap density of the resulting electrode.« less

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [1];  [1];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. State Univ. of New York, Stony Brook, NY (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States); State Univ. of New York, Stony Brook, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1557118
Report Number(s):
BNL-211954-2019-JAAM
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 22; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Fe3O4; Surface Chemistry; Surface-treatment ligands; Anodes; Li-ion Batteries

Citation Formats

Wang, Lei, Housel, Lisa M., Bock, David C., Abraham, Alyson, Dunkin, Mikaela R., McCarthy, Alison H., Wu, Qiyuan, Kiss, Andrew, Thieme, Juergen, Takeuchi, Esther S., Marschilok, Amy C., and Takeuchi, Kenneth J. Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry. United States: N. p., 2019. Web. doi:10.1021/acsami.8b21273.
Wang, Lei, Housel, Lisa M., Bock, David C., Abraham, Alyson, Dunkin, Mikaela R., McCarthy, Alison H., Wu, Qiyuan, Kiss, Andrew, Thieme, Juergen, Takeuchi, Esther S., Marschilok, Amy C., & Takeuchi, Kenneth J. Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry. United States. doi:10.1021/acsami.8b21273.
Wang, Lei, Housel, Lisa M., Bock, David C., Abraham, Alyson, Dunkin, Mikaela R., McCarthy, Alison H., Wu, Qiyuan, Kiss, Andrew, Thieme, Juergen, Takeuchi, Esther S., Marschilok, Amy C., and Takeuchi, Kenneth J. Wed . "Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry". United States. doi:10.1021/acsami.8b21273.
@article{osti_1557118,
title = {Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry},
author = {Wang, Lei and Housel, Lisa M. and Bock, David C. and Abraham, Alyson and Dunkin, Mikaela R. and McCarthy, Alison H. and Wu, Qiyuan and Kiss, Andrew and Thieme, Juergen and Takeuchi, Esther S. and Marschilok, Amy C. and Takeuchi, Kenneth J.},
abstractNote = {Fe3O4 nanoparticles (NPs) with an average size of 8-10 nm have been successfully functionalized with various surface-treatment agents to serve as model systems for probing surface chemistry-dependent electrochemistry of the resulting electrodes. The surface-treatment agents used for the functionalization of Fe3O4 anode materials were systematically varied to include aromatic or aliphatic structures: 4-mercaptobenzoic acid (MBA), benzoic acid (BA), 3-mercaptopropionic acid (MPA), and propionic acid (PA). Both structural and electrochemical characterizations have been used to systematically correlate the electrode functionality with the corresponding surface chemistry. Surface treatment with ligands led to better Fe3O4 dispersion, especially with the aromatic ligands. Electrochemistry was impacted where the PA and BA-treated Fe3O4 systems without the -SH group demonstrated higher rate capability than their thiol-containing counterparts and the pristine Fe3O4. Specifically, the PA system delivered the highest capacity and cycling stability amongst all samples tested. Notably, the aromatic BA system outperformed the aliphatic PA counterpart during extended cycling under high current density, due to the improved charge transfer and ion transport kinetics as well as better dispersion of Fe3O4 NPs, induced by the conjugated system. Our surface engineering of the Fe3O4 electrode presented herein, highlights the importance of modifying the structure and chemistry of surface-treatment agents as a plausible means of enhancing interfacial charge transfer within metal oxide composite electrodes without hampering the resulting tap density of the resulting electrode.},
doi = {10.1021/acsami.8b21273},
journal = {ACS Applied Materials and Interfaces},
number = 22,
volume = 11,
place = {United States},
year = {2019},
month = {5}
}

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This content will become publicly available on May 1, 2020
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