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

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

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., 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. 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., and Laskin, Julia. 2016. "Rational design of efficient electrode–electrolyte interfaces for solid-state energy storage using ion soft landing". United States. doi: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},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {4}
}