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

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作者
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
Yimei Zhu
机构
[1] SEU-FEI Nano-Pico Center,Condensed Matter Physics & Materials Science Department
[2] Key Laboratory of MEMS of the Ministry of Education,Department of Physics and Astronomy
[3] Southeast University,Department of Chemistry
[4] Brookhaven National Laboratory,Department of Materials Science and Engineering
[5] Stony Brook University,undefined
[6] Stony Brook University,undefined
[7] Institute for Advanced Computational Science,undefined
[8] Stony Brook University,undefined
[9] Stony Brook University,undefined
[10] Energy Sciences Directorate,undefined
[11] Brookhaven National Laboratory,undefined
[12] Center for Functional Nanomaterials,undefined
[13] Brookhaven National Laboratory,undefined
来源
Nature Communications | / 8卷
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摘要
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.
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