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Title: Lithiation of multilayer Ni/NiO electrodes: criticality of nickel layer thicknesses on conversion reaction kinetics

Abstract

X-ray reflectivity and transmission electron microscopy (TEM) were used to characterize the morphological changes in thin film electrodes with alternating Ni and NiO layers during lithiation as a function of the Ni buffer layer thickness. Complete lithiation of the active NiO layers occurs only when the thickness of the Ni/NiO bilayers are less than 75 Å – a threshold value that is determined by the sum of the Ni quantity in the Ni/NiO bilayer of the multilayer stack. Thicker Ni/NiO bilayers present a kinetic barrier for lithium ion diffusion inside the stack resulting in partial lithiation of the multilayer electrodes in which only the top NiO layer lithiates. Lithiation of NiO layers in a multilayer stack also leads to an interface-specific reaction that is observed to increase the thicknesses of adjacent Ni layers by 3–4 Å and is associated with the formation of a low-density Li 2O layer, corresponding to an interfacially-driven phase separation of the NiO. Rate dependent cyclic voltammetry studies reveal a linear relation between the peak current and scan rate suggesting that the lithiation kinetics are controlled by charge transfer resistance at the liquid–solid interface.

Authors:
 [1];  [2];  [1];  [3];  [3];  [4]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [5]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  3. Northwestern Univ., Evanston, IL (United States). EPIC, NUANCE Center
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering; Northwestern Univ., Evanston, IL (United States). EPIC, NUANCE Center
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering and Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566741
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 30; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
conversion reaction; lithium-ion battery; multilayer; nickel oxide; thin-film electrodes

Citation Formats

Evmenenko, Guennadi, Fister, Timothy T., Buchholz, D. Bruce, Castro, Fernando C., Li, Qianqian, Wu, Jinsong, Dravid, Vinayak P., Fenter, Paul, and Bedzyk, Michael J. Lithiation of multilayer Ni/NiO electrodes: criticality of nickel layer thicknesses on conversion reaction kinetics. United States: N. p., 2017. Web. doi:10.1039/C7CP02448G.
Evmenenko, Guennadi, Fister, Timothy T., Buchholz, D. Bruce, Castro, Fernando C., Li, Qianqian, Wu, Jinsong, Dravid, Vinayak P., Fenter, Paul, & Bedzyk, Michael J. Lithiation of multilayer Ni/NiO electrodes: criticality of nickel layer thicknesses on conversion reaction kinetics. United States. doi:10.1039/C7CP02448G.
Evmenenko, Guennadi, Fister, Timothy T., Buchholz, D. Bruce, Castro, Fernando C., Li, Qianqian, Wu, Jinsong, Dravid, Vinayak P., Fenter, Paul, and Bedzyk, Michael J. Tue . "Lithiation of multilayer Ni/NiO electrodes: criticality of nickel layer thicknesses on conversion reaction kinetics". United States. doi:10.1039/C7CP02448G. https://www.osti.gov/servlets/purl/1566741.
@article{osti_1566741,
title = {Lithiation of multilayer Ni/NiO electrodes: criticality of nickel layer thicknesses on conversion reaction kinetics},
author = {Evmenenko, Guennadi and Fister, Timothy T. and Buchholz, D. Bruce and Castro, Fernando C. and Li, Qianqian and Wu, Jinsong and Dravid, Vinayak P. and Fenter, Paul and Bedzyk, Michael J.},
abstractNote = {X-ray reflectivity and transmission electron microscopy (TEM) were used to characterize the morphological changes in thin film electrodes with alternating Ni and NiO layers during lithiation as a function of the Ni buffer layer thickness. Complete lithiation of the active NiO layers occurs only when the thickness of the Ni/NiO bilayers are less than 75 Å – a threshold value that is determined by the sum of the Ni quantity in the Ni/NiO bilayer of the multilayer stack. Thicker Ni/NiO bilayers present a kinetic barrier for lithium ion diffusion inside the stack resulting in partial lithiation of the multilayer electrodes in which only the top NiO layer lithiates. Lithiation of NiO layers in a multilayer stack also leads to an interface-specific reaction that is observed to increase the thicknesses of adjacent Ni layers by 3–4 Å and is associated with the formation of a low-density Li2O layer, corresponding to an interfacially-driven phase separation of the NiO. Rate dependent cyclic voltammetry studies reveal a linear relation between the peak current and scan rate suggesting that the lithiation kinetics are controlled by charge transfer resistance at the liquid–solid interface.},
doi = {10.1039/C7CP02448G},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 30,
volume = 19,
place = {United States},
year = {2017},
month = {7}
}

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Works referenced in this record:

Nano-sized transition-metal oxides as negative-electrode materials for lithium-ion batteries
journal, September 2000

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