Nanoscale Heterogeneity of Multilayered Si Anodes with Embedded Nanoparticle Scaffolds for Li-Ion Batteries

Marta Haro; Vidyadhar Singh; Stephan Steinhauer; Evropi Toulkeridou; Panagiotis Grammatikopoulos; Mukhles Sowwan

doi:10.1002/advs.201700180

Nanoscale Heterogeneity of Multilayered Si Anodes with Embedded Nanoparticle Scaffolds for Li-Ion Batteries

Marta Haro, Vidyadhar Singh, Stephan Steinhauer, Evropi Toulkeridou, Panagiotis Grammatikopoulos, Mukhles Sowwan^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

30 Scopus citations

Abstract

A new approach on the synthesis of Si anodes for Li-ion batteries is reported, combining advantages of both nanoparticulated and continuous Si films. A multilayered configuration prototype is proposed, comprising amorphous Si arranged in nanostructured, mechanically heterogeneous films, interspersed with Ta nanoparticle scaffolds. Particular structural features such as increased surface roughness, nanogranularity, and porosity are dictated by the nanoparticle scaffolds, boosting the lithiation process due to fast Li diffusion and low electrode polarization. Consequently, a remarkable charge/discharge speed is reached with the proposed anode, in the order of minutes (1200 mAh g⁻¹ at 10 C). Moreover, nanomechanical heterogeneity self-limits the capacity at intermediate charge/discharge rates; as a consequence, exceptional cycleability is observed at 0.5 C, with 100% retention over 200 cycles with 700 mAh g⁻¹. Higher capacity can be obtained when the first cycles are performed at 0.2 C, due to the formation of microislands, which facilitate the swelling of the active Si. This study indicates a method to tune the mechanical, morphological, and electrochemical properties of Si electrodes via engineering nanoparticle scaffolds, paving the way for a novel design of nanostructured Si electrodes for high-performance energy storage devices.

Original language	English
Article number	1700180
Journal	Advanced Science
Volume	4
Issue number	10
DOIs	https://doi.org/10.1002/advs.201700180
State	Published - Oct 2017
Externally published	Yes

Keywords

Li-ion batteries
Si anodes
cluster beam deposition
hybrid materials
nanoparticles

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10.1002/advs.201700180

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title = "Nanoscale Heterogeneity of Multilayered Si Anodes with Embedded Nanoparticle Scaffolds for Li-Ion Batteries",

abstract = "A new approach on the synthesis of Si anodes for Li-ion batteries is reported, combining advantages of both nanoparticulated and continuous Si films. A multilayered configuration prototype is proposed, comprising amorphous Si arranged in nanostructured, mechanically heterogeneous films, interspersed with Ta nanoparticle scaffolds. Particular structural features such as increased surface roughness, nanogranularity, and porosity are dictated by the nanoparticle scaffolds, boosting the lithiation process due to fast Li diffusion and low electrode polarization. Consequently, a remarkable charge/discharge speed is reached with the proposed anode, in the order of minutes (1200 mAh g−1 at 10 C). Moreover, nanomechanical heterogeneity self-limits the capacity at intermediate charge/discharge rates; as a consequence, exceptional cycleability is observed at 0.5 C, with 100% retention over 200 cycles with 700 mAh g−1. Higher capacity can be obtained when the first cycles are performed at 0.2 C, due to the formation of microislands, which facilitate the swelling of the active Si. This study indicates a method to tune the mechanical, morphological, and electrochemical properties of Si electrodes via engineering nanoparticle scaffolds, paving the way for a novel design of nanostructured Si electrodes for high-performance energy storage devices.",

keywords = "Li-ion batteries, Si anodes, cluster beam deposition, hybrid materials, nanoparticles",

author = "Marta Haro and Vidyadhar Singh and Stephan Steinhauer and Evropi Toulkeridou and Panagiotis Grammatikopoulos and Mukhles Sowwan",

note = "Publisher Copyright: {\textcopyright} 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2017",

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AU - Haro, Marta

AU - Singh, Vidyadhar

AU - Steinhauer, Stephan

AU - Toulkeridou, Evropi

AU - Grammatikopoulos, Panagiotis

AU - Sowwan, Mukhles

PY - 2017/10

Y1 - 2017/10

N2 - A new approach on the synthesis of Si anodes for Li-ion batteries is reported, combining advantages of both nanoparticulated and continuous Si films. A multilayered configuration prototype is proposed, comprising amorphous Si arranged in nanostructured, mechanically heterogeneous films, interspersed with Ta nanoparticle scaffolds. Particular structural features such as increased surface roughness, nanogranularity, and porosity are dictated by the nanoparticle scaffolds, boosting the lithiation process due to fast Li diffusion and low electrode polarization. Consequently, a remarkable charge/discharge speed is reached with the proposed anode, in the order of minutes (1200 mAh g−1 at 10 C). Moreover, nanomechanical heterogeneity self-limits the capacity at intermediate charge/discharge rates; as a consequence, exceptional cycleability is observed at 0.5 C, with 100% retention over 200 cycles with 700 mAh g−1. Higher capacity can be obtained when the first cycles are performed at 0.2 C, due to the formation of microislands, which facilitate the swelling of the active Si. This study indicates a method to tune the mechanical, morphological, and electrochemical properties of Si electrodes via engineering nanoparticle scaffolds, paving the way for a novel design of nanostructured Si electrodes for high-performance energy storage devices.

AB - A new approach on the synthesis of Si anodes for Li-ion batteries is reported, combining advantages of both nanoparticulated and continuous Si films. A multilayered configuration prototype is proposed, comprising amorphous Si arranged in nanostructured, mechanically heterogeneous films, interspersed with Ta nanoparticle scaffolds. Particular structural features such as increased surface roughness, nanogranularity, and porosity are dictated by the nanoparticle scaffolds, boosting the lithiation process due to fast Li diffusion and low electrode polarization. Consequently, a remarkable charge/discharge speed is reached with the proposed anode, in the order of minutes (1200 mAh g−1 at 10 C). Moreover, nanomechanical heterogeneity self-limits the capacity at intermediate charge/discharge rates; as a consequence, exceptional cycleability is observed at 0.5 C, with 100% retention over 200 cycles with 700 mAh g−1. Higher capacity can be obtained when the first cycles are performed at 0.2 C, due to the formation of microislands, which facilitate the swelling of the active Si. This study indicates a method to tune the mechanical, morphological, and electrochemical properties of Si electrodes via engineering nanoparticle scaffolds, paving the way for a novel design of nanostructured Si electrodes for high-performance energy storage devices.

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Nanoscale Heterogeneity of Multilayered Si Anodes with Embedded Nanoparticle Scaffolds for Li-Ion Batteries

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Keywords

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