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Title: Size-controlled Intercalation to Conversion Transition in Lithiation of Transition-Metal Chalcogenides – NbSe3

Abstract

Transition metal chalcogenides (TMCs) can either be used as intercalation cathodes or as conversion type anodes for lithium ion batteries, for which two distinctively different lithiation reaction mechanisms govern the electrochemical performance of TMCs. However, it remains elusive that what controls the transition of lithiation mechanisms. Herein, we investigated the lithiation process of NbSe3 ribbons using in situ transmission electron microscopy (TEM) and observed a size dependent transition from intercalation to conversion reaction. The large NbSe3 ribbons can accommodate high concentration of Li+ through intercalation by relaxing its internal spacing, while lithiation of small NbSe3 ribbons proceeds readily to full conversion reaction. We find that the size dependent variation of lithiation mechanism is attributed to the Li+ diffusion in NbSe3 and the accommodation of newly formed phases, i.e., insufficient Li+ diffusion and limited space for accommodating the volume expansion induced by forming new phases in large size ribbons both impede the intercalation-to-conversion transition. These results demonstrate the inherent structural instability of NbSe3 as an intercalation cathode and fast lithiation rate as a promising conversion type anode.

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1240219
Report Number(s):
PNNL-SA-114163
Journal ID: ISSN 1936-0851; 48379; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Luo, Langli, Zhao, Benliang, Xiang, Bin, and Wang, Chong M. Size-controlled Intercalation to Conversion Transition in Lithiation of Transition-Metal Chalcogenides – NbSe3. United States: N. p., 2016. Web. doi:10.1021/acsnano.5b06614.
Luo, Langli, Zhao, Benliang, Xiang, Bin, & Wang, Chong M. Size-controlled Intercalation to Conversion Transition in Lithiation of Transition-Metal Chalcogenides – NbSe3. United States. doi:10.1021/acsnano.5b06614.
Luo, Langli, Zhao, Benliang, Xiang, Bin, and Wang, Chong M. Sat . "Size-controlled Intercalation to Conversion Transition in Lithiation of Transition-Metal Chalcogenides – NbSe3". United States. doi:10.1021/acsnano.5b06614.
@article{osti_1240219,
title = {Size-controlled Intercalation to Conversion Transition in Lithiation of Transition-Metal Chalcogenides – NbSe3},
author = {Luo, Langli and Zhao, Benliang and Xiang, Bin and Wang, Chong M.},
abstractNote = {Transition metal chalcogenides (TMCs) can either be used as intercalation cathodes or as conversion type anodes for lithium ion batteries, for which two distinctively different lithiation reaction mechanisms govern the electrochemical performance of TMCs. However, it remains elusive that what controls the transition of lithiation mechanisms. Herein, we investigated the lithiation process of NbSe3 ribbons using in situ transmission electron microscopy (TEM) and observed a size dependent transition from intercalation to conversion reaction. The large NbSe3 ribbons can accommodate high concentration of Li+ through intercalation by relaxing its internal spacing, while lithiation of small NbSe3 ribbons proceeds readily to full conversion reaction. We find that the size dependent variation of lithiation mechanism is attributed to the Li+ diffusion in NbSe3 and the accommodation of newly formed phases, i.e., insufficient Li+ diffusion and limited space for accommodating the volume expansion induced by forming new phases in large size ribbons both impede the intercalation-to-conversion transition. These results demonstrate the inherent structural instability of NbSe3 as an intercalation cathode and fast lithiation rate as a promising conversion type anode.},
doi = {10.1021/acsnano.5b06614},
journal = {ACS Nano},
issn = {1936-0851},
number = 1,
volume = 10,
place = {United States},
year = {2016},
month = {1}
}