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Title: SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes

Abstract

Carboxylated polythiophenes, such as poly[3-(potassium-4-butanoate) thiophene] (PPBT), play a critical role in securely connecting single-walled carbon nanotube (SWNT) electrical networks onto the surface of carbon-coated silicon monoxide (c-SiO x). These connections are a function of the materials’ surface chemistries and resultant physical/chemical bonding through favorable molecular interactions. Specifically, the PPBT $π$-conjugated backbone and alkyl side chain carboxylate moieties (COO-), respectively, physically interact with the SWNT and c-SiO x carbon layer $π$-electron-rich surfaces, and chemically bind to surface hydroxyl (-OH) species of the c-SiO x electroactive materials to form a carboxylate bond. This approach effectively captured pulverized particles that form during battery operation and beneficially suppressed the thickness change that electrodes typically undergo. The resultant electrodes exhibited superior electrochemical performance, which was ascribed to stable SEI layer formation, reduced electrode resistance, and improved electrode kinetics. Moreover, electrodes fabricated by blending 30 wt % of c-SiO x with graphite using <3 wt % binder exhibited remarkable performance in both coin-type half-cell and pouch-type full-cell systems. Finally, the concept that introduces robust SWNT electrical networks with PPBT carboxylate linkages suggests a feasible approach for the design of practical, high-performance, and high-capacity anodes for battery applications.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Energy Frontier Research Center (EFRC), Washington, DC (United States). Center for Mesoscale Transport Properties; Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1567228
Grant/Contract Number:  
SC0012673
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 2574-0962
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; poly[3-(potassium-4-butanoate) thiophene] (PPBT); single-walled carbon nanotube networks; silicon monoxide; electrical linkage; carboxylate bond; π−π interaction; surface chemistry

Citation Formats

Kwon, Yo Han, Minnici, Krysten, Lee, Sujin R., Zhang, Guoyan, Takeuchi, Esther S., Takeuchi, Kenneth J., Marschilok, Amy C., and Reichmanis, Elsa. SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes. United States: N. p., 2018. Web. doi:10.1021/acsaem.8b00522.
Kwon, Yo Han, Minnici, Krysten, Lee, Sujin R., Zhang, Guoyan, Takeuchi, Esther S., Takeuchi, Kenneth J., Marschilok, Amy C., & Reichmanis, Elsa. SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes. United States. doi:10.1021/acsaem.8b00522.
Kwon, Yo Han, Minnici, Krysten, Lee, Sujin R., Zhang, Guoyan, Takeuchi, Esther S., Takeuchi, Kenneth J., Marschilok, Amy C., and Reichmanis, Elsa. Mon . "SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes". United States. doi:10.1021/acsaem.8b00522. https://www.osti.gov/servlets/purl/1567228.
@article{osti_1567228,
title = {SWNT Networks with Polythiophene Carboxylate Links for High-Performance Silicon Monoxide Electrodes},
author = {Kwon, Yo Han and Minnici, Krysten and Lee, Sujin R. and Zhang, Guoyan and Takeuchi, Esther S. and Takeuchi, Kenneth J. and Marschilok, Amy C. and Reichmanis, Elsa},
abstractNote = {Carboxylated polythiophenes, such as poly[3-(potassium-4-butanoate) thiophene] (PPBT), play a critical role in securely connecting single-walled carbon nanotube (SWNT) electrical networks onto the surface of carbon-coated silicon monoxide (c-SiOx). These connections are a function of the materials’ surface chemistries and resultant physical/chemical bonding through favorable molecular interactions. Specifically, the PPBT $π$-conjugated backbone and alkyl side chain carboxylate moieties (COO-), respectively, physically interact with the SWNT and c-SiOx carbon layer $π$-electron-rich surfaces, and chemically bind to surface hydroxyl (-OH) species of the c-SiOx electroactive materials to form a carboxylate bond. This approach effectively captured pulverized particles that form during battery operation and beneficially suppressed the thickness change that electrodes typically undergo. The resultant electrodes exhibited superior electrochemical performance, which was ascribed to stable SEI layer formation, reduced electrode resistance, and improved electrode kinetics. Moreover, electrodes fabricated by blending 30 wt % of c-SiOx with graphite using <3 wt % binder exhibited remarkable performance in both coin-type half-cell and pouch-type full-cell systems. Finally, the concept that introduces robust SWNT electrical networks with PPBT carboxylate linkages suggests a feasible approach for the design of practical, high-performance, and high-capacity anodes for battery applications.},
doi = {10.1021/acsaem.8b00522},
journal = {ACS Applied Energy Materials},
issn = {2574-0962},
number = 6,
volume = 1,
place = {United States},
year = {2018},
month = {6}
}

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