April 21, 2016
Journal Article

Rational Design of Efficient Electrode-Electrolyte Interfaces for Solid-State Energy Storage Using Ion Soft-Landing

Abstract

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.

Revised: March 21, 2017 | Published: April 21, 2016

Citation

Prabhakaran V., B.L. Mehdi, J.J. Ditto, M.H. Engelhard, B. Wang, K.D. Gunaratne, and D.C. Johnson, et al. 2016. Rational Design of Efficient Electrode-Electrolyte Interfaces for Solid-State Energy Storage Using Ion Soft-Landing. Nature Communications 7. PNNL-SA-113159. doi:10.1038/ncomms11399