Operando Grazing Incidence Small-Angle X-ray Scattering/X-ray Diffraction of Model Ordered Mesoporous Lithium-Ion Battery Anodes

Bhaway, Sarang M.; Qiang, Zhe; Xia, Yanfeng; Xia, Xuhui; Lee, Byeongdu; Yager, Kevin G.; Zhang, Lihua; Kisslinger, Kim; Chen, Yu-Ming; Liu, Kewei; Zhu, Yu; Vogt, Bryan D.

doi:10.1021/acsnano.6b06708

Title: Operando Grazing Incidence Small-Angle X-ray Scattering/X-ray Diffraction of Model Ordered Mesoporous Lithium-Ion Battery Anodes

Journal Article · Tue Feb 07 00:00:00 EST 2017 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.6b06708· OSTI ID:1344240

Bhaway, Sarang M. ^[1]; Qiang, Zhe ^[1]; Xia, Yanfeng ^[2]; Xia, Xuhui ^[1];

^[3]; Yager, Kevin G. ^[4]; Zhang, Lihua ^[4]; Kisslinger, Kim ^[4]; Chen, Yu-Ming ^[2]; Liu, Kewei ^[2]; Zhu, Yu ^[2];

^[1]

Univ. of Akron, OH (United States). Dept. of Polymer Engineering
Univ. of Akron, OH (United States). Dept. of Polymer Science
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Emergent lithium ion batteries commonly rely on nanostructuring of the active electrode materials to decrease the Li+ ion diffusion path length and to accommodate the strains associated with the insertion and de-insertion of Li+, but in many cases these nanostructures evolve during electrochemical charging-discharging. This change in the nanostructure can adversely impact performance, but challenges remain on how to control these changes from the perspective of morphological design. In order to start to address these questions, in-operando grazing incidence small angle x-ray scattering and x-ray diffraction (GISAXS/GIXD) were used to assess the structural evolution of a family of model ordered mesoporous NiCo2O4 anode films during battery operation. The pore dimensions were systematically varied and appear to impact the stability of the ordered nanostructure during the cycling. For the anodes with small mesopores (≈ 9 nm), the ordered nanostructure collapses during the first 2 charge-discharge cycles as determined from GISAXS. This collapse is accompanied by irreversible Li ion insertion within the oxide framework determined from GIXD and irreversible capacity loss. Conversely, anodes with larger ordered mesopores (17 nm - 28 nm) mostly maintained their nanostructure through the first 2 cycles with reversible Li ion insertion with small additional deformation of the mesostructure during the 2nd cycle. This preservation of the ordered structure lead to significant improvement in capacity retention during these first two cycles, however, a gradual loss in the ordered nanostructure from continuing deformation of the ordered structure during additional charge-discharge cycles leads to capacity decay in battery performance. These multiscale in-operando measurements provide insight into how changes at the atomic scale (lithium insertion and de-insertion) are translated to the nanostructure during battery operation. Moreover, small changes in the nanostructure can build up to significant morphological transformations that adversely impact battery performance through multiple charge-discharge cycles.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; AC02-98CH10886; AC02-06CH11357

OSTI ID:: 1344240

Alternate ID(s):: OSTI ID: 1374575

Report Number(s):: BNL-113558-2017-JA; KC0403020

Journal Information:: ACS Nano, Vol. 11, Issue 2; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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