Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry

doi:10.1021/acsami.8b21273

Title: Deliberate Modification of Fe₃O₄ Anode Surface Chemistry: Impact on Electrochemistry

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Abstract

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 agentsmore »« less

Authors:

^[1]; Housel, Lisa M. ^[1]; Bock, David C. ^[2]; Abraham, Alyson ^[1]; Dunkin, Mikaela R. ^[1]; McCarthy, Alison H. ^[1]; Wu, Qiyuan ^[2]; Kiss, Andrew ^[1]; Thieme, Juergen ^[1];

^[3];

^[1]

State Univ. of New York, Stony Brook, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States); State Univ. of New York, Stony Brook, NY (United States)

Publication Date:: 2019-05-01

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); 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.

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                    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.

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                    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.  https://www.osti.gov/servlets/purl/1557118.

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@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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DOI: 10.1021/acsami.8b21273

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Title: Deliberate Modification of Fe3O4 Anode Surface Chemistry: Impact on Electrochemistry

Abstract

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Title: Deliberate Modification of Fe₃O₄ Anode Surface Chemistry: Impact on Electrochemistry