Visualization of lithium-ion transport and phase evolution within and between manganese oxide nanorods

Feng Xu, Lijun Wu, Qingping Meng, Merzuk Kaltak, Jianping Huang, Jessica L. Durham, Marivi Fernandez-Serra, Litao Sun, Amy C. Marschilok, Esther S. Takeuchi, Kenneth J. Takeuchi, Mark S. Hybertsen and Yimei Zhu ()
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Feng Xu: SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of the Ministry of Education, Southeast University
Lijun Wu: Brookhaven National Laboratory
Qingping Meng: Brookhaven National Laboratory
Merzuk Kaltak: Stony Brook University
Jianping Huang: Stony Brook University
Jessica L. Durham: Stony Brook University
Marivi Fernandez-Serra: Stony Brook University
Litao Sun: SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of the Ministry of Education, Southeast University
Amy C. Marschilok: Stony Brook University
Esther S. Takeuchi: Stony Brook University
Kenneth J. Takeuchi: Stony Brook University
Mark S. Hybertsen: Center for Functional Nanomaterials, Brookhaven National Laboratory
Yimei Zhu: Brookhaven National Laboratory

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract Multiple lithium-ion transport pathways and local phase changes upon lithiation in silver hollandite are revealed via in situ microscopy including electron diffraction, imaging and spectroscopy, coupled with density functional theory and phase field calculations. We report unexpected inter-nanorod lithium-ion transport, where the reaction fronts and kinetics are maintained within the neighbouring nanorod. Notably, this is the first time-resolved visualization of lithium-ion transport within and between individual nanorods, where the impact of oxygen deficiencies is delineated. Initially, fast lithium-ion transport is observed along the long axis with small net volume change, resulting in two lithiated silver hollandite phases distinguishable by orthorhombic distortion. Subsequently, a slower reaction front is observed, with formation of polyphase lithiated silver hollandite and face-centred-cubic silver metal with substantial volume expansion. These results indicate lithium-ion transport is not confined within a single nanorod and may provide a paradigm shift for one-dimensional tunnelled materials, particularly towards achieving high-rate capability.

Date: 2017
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DOI: 10.1038/ncomms15400

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