NDLI: Influence of Li<sub>2</sub>O<sub>2</sub> morphology on oxygen reduction and evolution kinetics in Li

Content Provider	Royal Society of Chemistry (RSC)
Author	Kwabi, David G. Shao-Horn, Yang Thompson, Carl V. Mitchell, Robert R. Gallant, Betar M. Zhou, Jigang
Copyright Year	2013
Abstract	Understanding the origins of high overpotentials required for Li2O2 oxidation in Li–O2 batteries is critical for developing practical devices with improved round-trip efficiency. While a number of studies have reported different Li2O2 morphologies formed during discharge, the influence of the morphology and structure of Li2O2 on the oxygen evolution reaction (OER) kinetics and pathways is not known. Here, we show that two characteristic Li2O2 morphologies are formed in carbon nanotube (CNT) electrodes in a 1,2-dimethoxyethane (DME) electrolyte: discs/toroids (50–200 nm) at low rates/overpotentials (10 mA gC−1 or E > 2.7 V vs. Li), or small particles (<20 nm) at higher rates/overpotentials. Upon galvanostatic charging, small particles exhibit a sloping profile with low overpotential (<4 V) while discs exhibit a two-stage process involving an initially sloping region followed by a voltage plateau. Potentiostatic intermittent titration technique (PITT) measurements reveal that charging in the sloping region corresponds to solid solution-like delithiation, whereas the voltage plateau (E = 3.4 V vs. Li) corresponds to two-phase oxidation. The marked differences in charging profiles are attributed to differences in surface structure, as supported by X-ray absorption near edge structure (XANES) data showing that oxygen anions on disc surfaces have LiO2-like electronic features while those on the particle surfaces are more bulk Li2O2-like with modified electronic structure compared to commercial Li2O2. Such an integrated structural, chemical, and morphological approach to understanding the OER kinetics provides new insights into the desirable discharge product structure for charging at lower overpotentials.
Starting Page	2518
Ending Page	2528
Page Count	11
File Format	HTM / HTML PDF
ISSN	17545692
Volume Number	6
Issue Number	8
Journal	Energy & Environmental Science
DOI	10.1039/c3ee40998h
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	CNT PITT Li Oxygen evolution Carbon nanotube Dimethoxyethane Electrolyte Overpotential Plateau Titration X-ray absorption spectroscopy X-ray absorption near edge structure Oxygen
Content Type	Text
Resource Type	Article
Subject	Environmental Chemistry Pollution Renewable Energy, Sustainability and the Environment Nuclear Energy and Engineering

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