Kinetically-Driven Phase Transformation during Lithiation in Copper Sulfide Nanoflakes

He, Kai; Yao, Zhenpeng; Hwang, Sooyeon; Li, Na; Sun, Ke; Gan, Hong; Du, Yaping; Zhang, Hua; Wolverton, Chris; Su, Dong

doi:10.1021/acs.nanolett.7b02694

Kinetically-Driven Phase Transformation during Lithiation in Copper Sulfide Nanoflakes

Journal Article · Fri Aug 11 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b02694· OSTI ID:1376191

^[1]; Yao, Zhenpeng ^[2]; Hwang, Sooyeon ^[3]; Li, Na ^[4]; Sun, Ke ^[5]; Gan, Hong ^[5]; ^[4]; ^[6]; ^[2]; ^[3]

Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Xi'an Jiaotong Univ., Xi'an (China). Frontier Inst. of Science and Technology jointly with College of Science, State Key Lab. for Mechanical Behavior of Materials
Brookhaven National Lab. (BNL), Upton, NY (United States)
Nanyang Technological Univ. (Singapore). Center for Programmable Materials, School of Materials Science and Engineering

Two-dimensional (2D) transition metal chalcogenides have been widely studied and utilized as electrode materials for lithium ion batteries due to their unique layered structures to accommodate reversible lithium insertion. Real-time observation and mechanistic understanding of the phase transformations during lithiation of these materials are critically important for improving battery performance by controlling structures and reaction pathways. Here, we use in situ transmission electron microscopy methods to study the structural, morphological, and chemical evolutions in individual copper sulfide (CuS) nanoflakes during lithiation. We report a highly kinetically driven phase transformation in which lithium ions rapidly intercalate into the 2D van der Waals-stacked interlayers in the initial stage, and further lithiation induces the Cu extrusion via a displacement reaction mechanism that is different from the typical conversion reactions. Density functional theory calculations have confirmed both the thermodynamically favored and the kinetically driven reaction pathways. Lastly, our findings elucidate the reaction pathways of the Li/CuS system under nonequilibrium conditions and provide valuable insight into the atomistic lithiation mechanisms of transition metal sulfides in general.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0012704

OSTI ID:: 1376191

Report Number(s):: BNL--114187-2017-JA; KC0403020

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 9 Vol. 17; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
36 MATERIALS SCIENCE
Center for Functional Nanomaterials
CuS
Nanoflake
copper sulfide
electrochemistry kinetics
in situ TEM
lithium ion battery

Kinetically-Driven Phase Transformation during Lithiation in Copper Sulfide Nanoflakes

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