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Title: Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing

Abstract

Here, the rational design of improved electrode-electrolyte interfaces (EEI) for energy storage is critically dependent on a molecular-level understanding of ionic interactions and nanoscale phenomena. The presence of non-redox active species at EEI has been shown to strongly influence Faradaic efficiency and long-term operational stability during energy storage processes. Herein, we achieve substantially higher performance and long-term stability of EEI prepared with highly-dispersed discrete redox-active cluster anions (50 ng of pure ~0.7 nm size molybdenum polyoxometalate anions (POM) anions on 25 mg (≈ 0.2 wt%) carbon nanotube (CNT) electrodes) by complete elimination of strongly coordinating non-redox species through ion soft-landing (SL). For the first time, electron microscopy provides atomically-resolved images of individual POM species directly on complex technologically relevant CNT electrodes. In this context, SL is established as a versatile approach for the controlled design of novel surfaces for both fundamental and applied research in energy storage.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [2];  [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Univ. of Oregon, Eugene, OR (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1253857
Report Number(s):
PNNL-SA-113159
Journal ID: ISSN 2041-1723; ncomms11399
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Prabhakaran, Venkateshkumar, Mehdi, B. Layla, Ditto, Jeffrey J., Engelhard, Mark H., Wang, Bingbing, Gunaratne, K. Don D., Johnson, David C., Browning, Nigel D., Johnson, Grant E., and Laskin, Julia. Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing. United States: N. p., 2016. Web. doi:10.1038/ncomms11399.
Prabhakaran, Venkateshkumar, Mehdi, B. Layla, Ditto, Jeffrey J., Engelhard, Mark H., Wang, Bingbing, Gunaratne, K. Don D., Johnson, David C., Browning, Nigel D., Johnson, Grant E., & Laskin, Julia. Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing. United States. https://doi.org/10.1038/ncomms11399
Prabhakaran, Venkateshkumar, Mehdi, B. Layla, Ditto, Jeffrey J., Engelhard, Mark H., Wang, Bingbing, Gunaratne, K. Don D., Johnson, David C., Browning, Nigel D., Johnson, Grant E., and Laskin, Julia. 2016. "Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing". United States. https://doi.org/10.1038/ncomms11399. https://www.osti.gov/servlets/purl/1253857.
@article{osti_1253857,
title = {Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing},
author = {Prabhakaran, Venkateshkumar and Mehdi, B. Layla and Ditto, Jeffrey J. and Engelhard, Mark H. and Wang, Bingbing and Gunaratne, K. Don D. and Johnson, David C. and Browning, Nigel D. and Johnson, Grant E. and Laskin, Julia},
abstractNote = {Here, the rational design of improved electrode-electrolyte interfaces (EEI) for energy storage is critically dependent on a molecular-level understanding of ionic interactions and nanoscale phenomena. The presence of non-redox active species at EEI has been shown to strongly influence Faradaic efficiency and long-term operational stability during energy storage processes. Herein, we achieve substantially higher performance and long-term stability of EEI prepared with highly-dispersed discrete redox-active cluster anions (50 ng of pure ~0.7 nm size molybdenum polyoxometalate anions (POM) anions on 25 mg (≈ 0.2 wt%) carbon nanotube (CNT) electrodes) by complete elimination of strongly coordinating non-redox species through ion soft-landing (SL). For the first time, electron microscopy provides atomically-resolved images of individual POM species directly on complex technologically relevant CNT electrodes. In this context, SL is established as a versatile approach for the controlled design of novel surfaces for both fundamental and applied research in energy storage.},
doi = {10.1038/ncomms11399},
url = {https://www.osti.gov/biblio/1253857}, journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 7,
place = {United States},
year = {Thu Apr 21 00:00:00 EDT 2016},
month = {Thu Apr 21 00:00:00 EDT 2016}
}

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Cited by: 71 works
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Works referencing / citing this record:

Flexible Li-CO 2 Batteries with Liquid-Free Electrolyte
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Von isolierten Ionen zu mehrschichtigen funktionellen Materialien durch sanfte Landung von Ionen
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From Isolated Ions to Multilayer Functional Materials Using Ion Soft Landing
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