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Title: High-Performance Capacitive Deionization via Manganese Oxide-Coated, Vertically Aligned Carbon Nanotubes

Abstract

Discovering electrode materials with exceptional capacitance, an indicator of the ability of a material to hold charge, is critical for developing capacitive deionization devices for water desalination. Maganese oxides (MnOx) have shown promise as capacitive electrode materials, but they exhibit a tradeoff where higher loading of the active MnOx comes at a cost of lower conductivity. To address this challenge and achieve high salt adsorption, we fabricated electrodes comprising vertically aligned core-shell nanostructures using atomic layer deposition (ALD) to coat thin films of MnOx onto vertically aligned carbon nanotubes (VACNTs). The inherently hierarchical, anisotropic, three-dimensional macroporous structure of VACNTs and the tunable coating, a hallmark of ALD, enabled co-optimization of the hybrid material’s specific capacitance with respect to mass and geometric area. The specific capacitance was optimized in this study to 215 ± 7 F/g and 1.1 ± 0.1 F/cm2 in 1 M NaCl electrolyte at 5 mV/s scan rate, respectively. This material exhibited remarkable sodium ion adsorption capacity of 489 ± 25 μmol Na /g material (two-fold higher than pristine VACNTs) at a functioning voltage of 1.2 V, which may ultimately enable expanded desalination applications of capacitive deionization.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Civil and Environmental Engineering, Massachusetts Institute of Technology; Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
  2. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering, and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT)
  3. Key Laboratory of Advanced Technologies of Materials (Ministry of Education), School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu 610031, P. R. China
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
  5. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; New York Univ. (NYU), NY (United States). Dept. of Chemical and Biomolecular Engineering
  6. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering, and Energy Sciences Inst.
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1560981
Report Number(s):
LLNL-JRNL-755914
Journal ID: ISSN 2328-8930; 943204
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science & Technology Letters (Online)
Additional Journal Information:
Journal Name: Environmental Science & Technology Letters (Online); Journal Volume: 5; Journal Issue: 11; Journal ID: ISSN 2328-8930
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Shi, Wenbo, Zhou, Xuechen, Li, Jinyang, Meshot, Eric R., Taylor, André D., Hu, Shu, Kim, Jae-Hong, Elimelech, Menachem, and Plata, Desiree L. High-Performance Capacitive Deionization via Manganese Oxide-Coated, Vertically Aligned Carbon Nanotubes. United States: N. p., 2018. Web. doi:10.1021/acs.estlett.8b00397.
Shi, Wenbo, Zhou, Xuechen, Li, Jinyang, Meshot, Eric R., Taylor, André D., Hu, Shu, Kim, Jae-Hong, Elimelech, Menachem, & Plata, Desiree L. High-Performance Capacitive Deionization via Manganese Oxide-Coated, Vertically Aligned Carbon Nanotubes. United States. doi:https://doi.org/10.1021/acs.estlett.8b00397
Shi, Wenbo, Zhou, Xuechen, Li, Jinyang, Meshot, Eric R., Taylor, André D., Hu, Shu, Kim, Jae-Hong, Elimelech, Menachem, and Plata, Desiree L. Fri . "High-Performance Capacitive Deionization via Manganese Oxide-Coated, Vertically Aligned Carbon Nanotubes". United States. doi:https://doi.org/10.1021/acs.estlett.8b00397. https://www.osti.gov/servlets/purl/1560981.
@article{osti_1560981,
title = {High-Performance Capacitive Deionization via Manganese Oxide-Coated, Vertically Aligned Carbon Nanotubes},
author = {Shi, Wenbo and Zhou, Xuechen and Li, Jinyang and Meshot, Eric R. and Taylor, André D. and Hu, Shu and Kim, Jae-Hong and Elimelech, Menachem and Plata, Desiree L.},
abstractNote = {Discovering electrode materials with exceptional capacitance, an indicator of the ability of a material to hold charge, is critical for developing capacitive deionization devices for water desalination. Maganese oxides (MnOx) have shown promise as capacitive electrode materials, but they exhibit a tradeoff where higher loading of the active MnOx comes at a cost of lower conductivity. To address this challenge and achieve high salt adsorption, we fabricated electrodes comprising vertically aligned core-shell nanostructures using atomic layer deposition (ALD) to coat thin films of MnOx onto vertically aligned carbon nanotubes (VACNTs). The inherently hierarchical, anisotropic, three-dimensional macroporous structure of VACNTs and the tunable coating, a hallmark of ALD, enabled co-optimization of the hybrid material’s specific capacitance with respect to mass and geometric area. The specific capacitance was optimized in this study to 215 ± 7 F/g and 1.1 ± 0.1 F/cm2 in 1 M NaCl electrolyte at 5 mV/s scan rate, respectively. This material exhibited remarkable sodium ion adsorption capacity of 489 ± 25 μmol Na /g material (two-fold higher than pristine VACNTs) at a functioning voltage of 1.2 V, which may ultimately enable expanded desalination applications of capacitive deionization.},
doi = {10.1021/acs.estlett.8b00397},
journal = {Environmental Science & Technology Letters (Online)},
number = 11,
volume = 5,
place = {United States},
year = {2018},
month = {10}
}

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Figures / Tables:

Figure 1 Figure 1: Vertically aligned coaxial CNT-MnOx hybrid synthesis and characterization. (a) Schematic illustration of MnOx coating strategy on VACNTs via ALD and proposed model of electrosorption of ions on the coated VACNTs. (b) Cross-sectional SEM image demonstrating the alignment of pristine VACNTs. (c) Increase in VACNT diameter after 150 ALDmore » cycles. (d, e) TEM images demonstrating the tunable MnOx coating via changing ALD cycle number at (d) 75 and (e) 150 cycles. (f) STEM image (high-angle annular dark-field imaging, HAADF) of VACNT-MnOx with 75 ALD cycles and (g) corresponding EDX elemental mapping confirming the presence of MnOx coating (Mn shown in blue and O shown in red).« less

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