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Characterization of Electrode Materials for Lithium Ion and Sodium Ion Batteries Using Synchrotron Radiation Techniques

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Published on: November 11, 2013

Evaluating pristine and modified SnS2 as a lithium-ion battery anode: a first-principles study.

Zhixiao Liu¹, Huiqiu Deng, Partha P Mukherjee

¹Department of Mechanical Engineering, Texas A&M University , College Station, Texas 77843, United States.

ACS Applied Materials & Interfaces

|January 29, 2015

Summary

Lithium intercalation and diffusion in tin disulfide (SnS2) are optimized by expanding interlayer spacing, which lowers energy barriers. However, cerium doping hinders lithium diffusion despite optimizing spacing.

Keywords:

first-principles calculation interlayer diffusion tin disulfide anode two-dimensional nanostructure volume expansion

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Area of Science:

Materials Science
Computational Chemistry
Electrochemistry

Background:

Tin disulfide (SnS2) is a promising material for lithium-ion batteries.
Understanding lithium ion intercalation and diffusion is crucial for optimizing battery performance.

Purpose of the Study:

Investigate lithium intercalation and diffusion mechanisms in pristine and modified SnS2 interlayers.
Elucidate the impact of interlayer spacing and cerium doping on lithium dynamics.
Analyze lithiation-induced volume expansion and structural changes in LixSnS2.

Main Methods:

First-principles calculations.
Climbing image nudged elastic band (CI-NEB) method for diffusion pathway analysis.
Geometric structure analysis of lithiated SnS2 (LixSnS2).

Main Results:

Octahedral interstitial sites are energetically favored for lithium intercalation in SnS2.
Lithium diffusion occurs between octahedral sites via tetrahedral sites, with expanded interlayer spacing reducing the diffusion barrier.
Cerium doping negatively affects lithium diffusivity.
Lithiation proceeds in two stages: initial volume expansion with electron transfer to sulfur, followed by Sn(4+) reduction, S-Sn-S trilayer decomposition, and formation of LixS2 layers for higher lithium content.

Conclusions:

Expanding interlayer spacing is beneficial for enhancing lithium diffusion in SnS2.
Cerium doping presents a trade-off between interlayer spacing optimization and lithium diffusivity.
The two-stage lithiation mechanism explains the volume expansion and structural evolution in SnS2 during battery operation.