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Title: Electrochemical Reaction Mechanism of the MoS2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy

Journal Article · · Nano Letters
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)

As a typical transition metal dichalcogenide, MoS2 offers numerous advantages for nanoelectronics and electrochemical energy storage due to its unique layered structure and tunable electronic properties. When used as the anode in lithium-ion cells, MoS2 undergoes intercalation and conversion reactions in sequence upon lithiation, and the reversibility of the conversion reaction is an important but still controversial topic. Here, we clarify unambiguously that the conversion reaction of MoS2 is not reversible, and the formed Li2S is converted to sulfur in the first charge process. Li2S/sulfur becomes the main redox couple in the subsequent cycles and the main contributor to the reversible capacity. In addition, due to the insulating nature of both Li2S and sulfur, a strong relaxation effect is observed during the cycling process. This study clearly reveals the electrochemical lithiation-delithiation mechanism of MoS2, which can facilitate further developments of high-performance MoS2-based electrodes.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1530338
Journal Information:
Nano Letters, Vol. 18, Issue 2; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 124 works
Citation information provided by
Web of Science

References (57)

Phase engineering of transition metal dichalcogenides journal January 2015
Recent Advances in Ultrathin Two-Dimensional Nanomaterials journal March 2017
Fast kinetics of magnesium monochloride cations in interlayer-expanded titanium disulfide for magnesium rechargeable batteries journal August 2017
Lithium ion battery applications of molybdenum disulfide (MoS 2 ) nanocomposites journal January 2014
MoS 2 -Based Nanocomposites for Electrochemical Energy Storage journal December 2016
Electrochemical tuning of vertically aligned MoS2 nanofilms and its application in improving hydrogen evolution reaction journal November 2013
Single-layer MoS2 transistors journal January 2011
Solution-Processed Two-Dimensional MoS 2 Nanosheets: Preparation, Hybridization, and Applications journal June 2016
Interface strain in vertically stacked two-dimensional heterostructured carbon-MoS2 nanosheets controls electrochemical reactivity journal June 2016
Synthesis of Highly Uniform Molybdenum-Glycerate Spheres and Their Conversion into Hierarchical MoS 2 Hollow Nanospheres for Lithium-Ion Batteries journal April 2016
Rational Design of Three-Layered TiO 2 @Carbon@MoS 2 Hierarchical Nanotubes for Enhanced Lithium Storage journal July 2017
Single-Layered Ultrasmall Nanoplates of MoS 2 Embedded in Carbon Nanofibers with Excellent Electrochemical Performance for Lithium and Sodium Storage journal January 2014
MoS 2 Nanoplates Consisting of Disordered Graphene-like Layers for High Rate Lithium Battery Anode Materials journal November 2011
Intercalation chemistry of molybdenum disulfide journal January 2002
In Situ Visualization of Lithium Ion Intercalation into MoS 2 Single Crystals using Differential Optical Microscopy with Atomic Layer Resolution journal March 2016
Atomic Mechanism of Dynamic Electrochemical Lithiation Processes of MoS 2 Nanosheets journal April 2014
In Situ Study of Lithiation and Delithiation of MoS 2 Nanosheets Using Electrochemical Liquid Cell Transmission Electron Microscopy journal July 2015
The lithium intercalates of the transition metal dichalcogenides journal May 1975
Lithium electrochemical cells at low voltage: Decomposition of Mo and W dichalcogenides journal February 1987
Superior stability and high capacity of restacked molybdenum disulfide as anode material for lithium ion batteries journal January 2010
In situ synthesis of MoS2/graphene nanosheet composites with extraordinarily high electrochemical performance for lithium ion batteries journal January 2011
l -Cysteine-Assisted Synthesis of Layered MoS 2 /Graphene Composites with Excellent Electrochemical Performances for Lithium Ion Batteries journal May 2011
Hierarchical MoS 2 /Polyaniline Nanowires with Excellent Electrochemical Performance for Lithium-Ion Batteries journal December 2012
Mechanism of Lithium Storage in MoS2 and the Feasibility of Using Li2S/Mo Nanocomposites as Cathode Materials for Lithium-Sulfur Batteries journal February 2012
Lithium storage in commercial MoS2 in different potential ranges journal October 2012
Electrochemically Induced High Capacity Displacement Reaction of PEO/MoS2/Graphene Nanocomposites with Lithium journal May 2011
Exfoliated MoS 2 Nanocomposite as an Anode Material for Lithium Ion Batteries journal August 2010
Nanosized Li2S-based cathodes derived from MoS2 for high-energy density Li–S cells and Si–Li2S full cells in carbonate-based electrolyte journal July 2017
Facilitated Lithium Storage in MoS 2 Overlayers Supported on Coaxial Carbon Nanotubes journal February 2007
Self-assembled MoS2–carbon nanostructures: influence of nanostructuring and carbon on lithium battery performance journal January 2012
An experimental and computational study to understand the lithium storage mechanism in molybdenum disulfide journal January 2014
Lithium storage in nitrogen-rich mesoporous carbon materials journal January 2012
Origin of the Phase Transition in Lithiated Molybdenum Disulfide journal November 2014
In Situ Investigations of Li-MoS 2 with Planar Batteries journal November 2014
Conversion Reaction Mechanisms in Lithium Ion Batteries: Study of the Binary Metal Fluoride Electrodes journal November 2011
Phase evolution for conversion reaction electrodes in lithium-ion batteries journal February 2014
Nano-sized transition-metal oxides as negative-electrode materials for lithium-ion batteries journal September 2000
High-Capacity Micrometer-Sized Li2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries journal September 2012
Structure of single-molecular-layer MoS 2 journal May 1991
Characterization of few-layer 1T-MoSe 2 and its superior performance in the visible-light induced hydrogen evolution reaction journal September 2014
Epitaxial growth of a monolayer WSe2-MoS2 lateral p-n junction with an atomically sharp interface journal July 2015
Erratum: Corrigendum: Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies journal February 2016
Chemical Bonding in Restacked Single-Layer MoS2 by X-ray Absorption Spectroscopy journal May 1994
The capacity fading mechanism and improvement of cycling stability in MoS 2 -based anode materials for lithium-ion batteries journal January 2016
Structural Transitions in Monolayer MoS 2 by Lithium Adsorption journal May 2015
Sulfur K -Edge X-Ray-Absorption Study of the Charge Transfer upon Lithium Intercalation into Titanium Disulfide journal September 1996
Revealing the Electrochemical Charging Mechanism of Nanosized Li 2 S by in Situ and Operando X-ray Absorption Spectroscopy journal July 2017
Operando Characterization of Intermediates Produced in a Lithium-Sulfur Battery journal January 2015
Sulfiphilic Nickel Phosphosulfide Enabled Li 2 S Impregnation in 3D Graphene Cages for Li-S Batteries journal January 2017
High-Performance Lithium-Sulfur Batteries with a Self-Supported, 3D Li 2 S-Doped Graphene Aerogel Cathodes journal November 2015
Designing high-energy lithium–sulfur batteries journal January 2016
Rechargeable Lithium–Sulfur Batteries journal July 2014
Catalytic oxidation of Li 2 S on the surface of metal sulfides for Li−S batteries journal January 2017
Slurryless Li 2 S/Reduced Graphene Oxide Cathode Paper for High-Performance Lithium Sulfur Battery journal February 2015
Safe and Durable High-Temperature Lithium–Sulfur Batteries via Molecular Layer Deposited Coating journal May 2016
Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries journal August 2014
Burning lithium in CS2 for high-performing compact Li2S–graphene nanocapsules for Li–S batteries journal June 2017

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Approaching the Lithiation Limit of MoS 2 While Maintaining Its Layered Crystalline Structure to Improve Lithium Storage journal February 2019
Unsaturated Sulfur Edge Engineering of Strongly Coupled MoS 2 Nanosheet-Carbon Macroporous Hybrid Catalyst for Enhanced Hydrogen Generation journal October 2018
Electrode Materials for High-Performance Sodium-Ion Batteries journal June 2019
Approaching the Lithiation Limit of MoS 2 While Maintaining Its Layered Crystalline Structure to Improve Lithium Storage journal February 2019
Chemical Mass Production of MoS 2 /Graphene van der Waals Heterostructure as a High‐Performance Li‐ion Intercalation Host journal July 2019
Fibrous Network of C@MoS 2 Nanocapsule‐Decorated Cotton Linters Interconnected by Bacterial Cellulose for Lithium‐ and Sodium‐Ion Batteries journal October 2019
Understanding the electrochemical reaction mechanism of VS 2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy journal September 2018
Multiple roles of a heterointerface in two-dimensional van der Waals heterostructures: insights into energy-related applications journal January 2019
Unraveling the Formation of Amorphous MoS 2 Nanograins during the Electrochemical Delithiation Process journal August 2019
Reversible and selective ion intercalation through the top surface of few-layer MoS2 journal December 2018
MoS 2 Nanosheets Vertically Aligned on Hierarchically Porous Graphitic Carbon for High-Performance Lithium Storage journal January 2018
Enhanced high rate capability of Li intercalation in planar and edge defect-rich MoS 2 nanosheets journal January 2019
3D Metal‐Rich Cu 7.2 S 4 /Carbon‐Supported MoS 2 Nanosheets for Enhanced Lithium‐Storage Performance journal January 2019
In situ formation of a bifunctional interlayer enabled by a conversion reaction to initiatively prevent lithium dendrites in a garnet solid electrolyte journal January 2019
A Pseudolayered MoS 2 as Li-Ion Intercalation Host with Enhanced Rate Capability and Durability journal October 2018
Ultra-thin solid electrolyte interphase evolution and wrinkling processes in molybdenum disulfide-based lithium-ion batteries journal July 2019
Rational design of two-dimensional nanomaterials for lithium–sulfur batteries journal January 2020
Unlocking Few‐Layered Ternary Chalcogenides for High‐Performance Potassium‐Ion Storage journal June 2019
Reviving bulky MoS 2 as an advanced anode for lithium-ion batteries journal January 2019
How does Molybdenum Disulfide Store Charge: A Minireview journal March 2020
Deciphering the Reaction Mechanism of Lithium–Sulfur Batteries by In Situ/Operando Synchrotron‐Based Characterization Techniques journal March 2019
Bilayer MoS 2 quantum dots with tunable magnetism and spin journal November 2018
Conversion-type Anode Materials for Alkali-Ion Batteries: State of the Art and Possible Research Directions journal April 2018

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