skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Atomic-scale combination of germanium-zinc nanofibers for structural and electrochemical evolution

Abstract

Alloy materials have been emerged to achieve compatible properties in various applications. The structural manipulation, however, requires sensitive and complicated synthetic process. Herein, we report atomic-scale combination of germanium-zinc distorted alloy exhibiting uncertain eutectic point in a phase diagram can imply a great potential to form atomically collaborated array via a simple fabrication method. When interconnected together, it prevents a fatal sublimation of germanium/germanium oxide during gas-solid phase reduction reaction and allows outstanding electronic conductivity as well as high available capacity in lithium-ion batteries, leading to structural and electrochemical evolution of germanium/zinc distorted array. Further, the unique features are clearly confirmed through in situ analysis. Besides, as-prepared battery anodes remarkably highlights outstanding rate capabilities (capacity retention of ~50% at 20 C compared to 0.2 C-rate) and cycle retention (73% at 3.0 C-rate) with a capacity of 546 mAh g-1 even after 1000 cycles. Even when assembled in a full cell, it notably facilitates considerable energy density during 400 cycles with 99.4% of average coulombic efficiency, which is suitable for a large-scale energy storage system.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [1]; ORCiD logo [5];  [5]; ORCiD logo [1];  [5];  [1]; ORCiD logo [4]; ORCiD logo [3];  [5]
  1. Ulsan National Institute of Science and Technology (UNIST), Ulsan (Republic of Korea)
  2. Korea Advanced Institute of Science and Technology, Daejeon (Republic of Korea)
  3. Korea Institute of Industrial Technology, Jeju-do (Republic of Korea)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Pohang Univ. of Science and Technology (POSTECH), Pohang (Republic of Korea)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1543296
Report Number(s):
PNNL-SA-135597
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Song, Gyujin, Cheong, Jun Young, Kim, Chanhoon, Luo, Langli, Hwang, Chihyun, Choi, Sungho, Ryu, Jaegeon, Kim, Sungho, Song, Woo -Jin, Song, Hyun -Kon, Wang, Chongmin, Kim, Il -Doo, and Park, Soojin. Atomic-scale combination of germanium-zinc nanofibers for structural and electrochemical evolution. United States: N. p., 2019. Web. doi:10.1038/s41467-019-10305-x.
Song, Gyujin, Cheong, Jun Young, Kim, Chanhoon, Luo, Langli, Hwang, Chihyun, Choi, Sungho, Ryu, Jaegeon, Kim, Sungho, Song, Woo -Jin, Song, Hyun -Kon, Wang, Chongmin, Kim, Il -Doo, & Park, Soojin. Atomic-scale combination of germanium-zinc nanofibers for structural and electrochemical evolution. United States. doi:10.1038/s41467-019-10305-x.
Song, Gyujin, Cheong, Jun Young, Kim, Chanhoon, Luo, Langli, Hwang, Chihyun, Choi, Sungho, Ryu, Jaegeon, Kim, Sungho, Song, Woo -Jin, Song, Hyun -Kon, Wang, Chongmin, Kim, Il -Doo, and Park, Soojin. Thu . "Atomic-scale combination of germanium-zinc nanofibers for structural and electrochemical evolution". United States. doi:10.1038/s41467-019-10305-x. https://www.osti.gov/servlets/purl/1543296.
@article{osti_1543296,
title = {Atomic-scale combination of germanium-zinc nanofibers for structural and electrochemical evolution},
author = {Song, Gyujin and Cheong, Jun Young and Kim, Chanhoon and Luo, Langli and Hwang, Chihyun and Choi, Sungho and Ryu, Jaegeon and Kim, Sungho and Song, Woo -Jin and Song, Hyun -Kon and Wang, Chongmin and Kim, Il -Doo and Park, Soojin},
abstractNote = {Alloy materials have been emerged to achieve compatible properties in various applications. The structural manipulation, however, requires sensitive and complicated synthetic process. Herein, we report atomic-scale combination of germanium-zinc distorted alloy exhibiting uncertain eutectic point in a phase diagram can imply a great potential to form atomically collaborated array via a simple fabrication method. When interconnected together, it prevents a fatal sublimation of germanium/germanium oxide during gas-solid phase reduction reaction and allows outstanding electronic conductivity as well as high available capacity in lithium-ion batteries, leading to structural and electrochemical evolution of germanium/zinc distorted array. Further, the unique features are clearly confirmed through in situ analysis. Besides, as-prepared battery anodes remarkably highlights outstanding rate capabilities (capacity retention of ~50% at 20 C compared to 0.2 C-rate) and cycle retention (73% at 3.0 C-rate) with a capacity of 546 mAh g-1 even after 1000 cycles. Even when assembled in a full cell, it notably facilitates considerable energy density during 400 cycles with 99.4% of average coulombic efficiency, which is suitable for a large-scale energy storage system.},
doi = {10.1038/s41467-019-10305-x},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Graphene balls for lithium rechargeable batteries with fast charging and high volumetric energy densities
journal, November 2017


Li-ion battery materials: present and future
journal, June 2015


State-of-the-art characterization techniques for advanced lithium-ion batteries
journal, March 2017


Nanostructured materials for advanced energy conversion and storage devices
journal, May 2005

  • Aricò, Antonino Salvatore; Bruce, Peter; Scrosati, Bruno
  • Nature Materials, Vol. 4, Issue 5, p. 366-377
  • DOI: 10.1038/nmat1368

Lithium metal protection enabled by in-situ olefin polymerization for high-performance secondary lithium sulfur batteries
journal, September 2017


Vacuum distillation derived 3D porous current collector for stable lithium–metal batteries
journal, May 2018


Ultrafine TiO 2 Confined in Porous-Nitrogen-Doped Carbon from Metal–Organic Frameworks for High-Performance Lithium Sulfur Batteries
journal, March 2017

  • An, Yongling; Zhang, Zhen; Fei, Huifang
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 14
  • DOI: 10.1021/acsami.6b16699

A titanium-based metal–organic framework as an ultralong cycle-life anode for PIBs
journal, January 2017

  • An, Yongling; Fei, Huifang; Zhang, Zhen
  • Chemical Communications, Vol. 53, Issue 59
  • DOI: 10.1039/C7CC03606J

Germanium Nanotubes Prepared by Using the Kirkendall Effect as Anodes for High-Rate Lithium Batteries
journal, August 2011

  • Park, Mi-Hee; Cho, YongHyun; Kim, Kitae
  • Angewandte Chemie International Edition, Vol. 50, Issue 41
  • DOI: 10.1002/anie.201103062

Carbon-Coated Germanium Nanowires on Carbon Nanofibers as Self-Supported Electrodes for Flexible Lithium-Ion Batteries
journal, February 2015


Mesoporous Ge/GeO 2 /Carbon Lithium-Ion Battery Anodes with High Capacity and High Reversibility
journal, April 2015


Preparation of nanostructured Ge/GeO 2 composite in carbon matrix as an anode material for lithium-ion batteries
journal, January 2016


Amorphous Hierarchical Porous GeO x as High-Capacity Anodes for Li Ion Batteries with Very Long Cycling Life
journal, December 2011

  • Wang, Xiao-Liang; Han, Wei-Qiang; Chen, Haiyan
  • Journal of the American Chemical Society, Vol. 133, Issue 51
  • DOI: 10.1021/ja208880f

Catalytic Role of Ge in Highly Reversible GeO 2 /Ge/C Nanocomposite Anode Material for Lithium Batteries
journal, February 2013

  • Seng, Kuok Hau; Park, Mi-hee; Guo, Zai Ping
  • Nano Letters, Vol. 13, Issue 3
  • DOI: 10.1021/nl304716e

Ge/C Nanowires as High-Capacity and Long-Life Anode Materials for Li-Ion Batteries
journal, June 2014

  • Liu, Jun; Song, Kepeng; Zhu, Changbao
  • ACS Nano, Vol. 8, Issue 7
  • DOI: 10.1021/nn501945f

A New Strategy for Achieving a High Performance Anode for Lithium Ion Batteries-Encapsulating Germanium Nanoparticles in Carbon Nanoboxes
journal, December 2015

  • Li, Dan; Wang, Hongqiang; Liu, Hua Kun
  • Advanced Energy Materials, Vol. 6, Issue 5
  • DOI: 10.1002/aenm.201501666

Preparation of Ge nanotube arrays from an ionic liquid for lithium ion battery anodes with improved cycling stability
journal, January 2015

  • Liu, Xusong; Hao, Jian; Liu, Xiaoxu
  • Chemical Communications, Vol. 51, Issue 11
  • DOI: 10.1039/C4CC08722D

Electrolytic Formation of Crystalline Silicon/Germanium Alloy Nanotubes and Hollow Particles with Enhanced Lithium-Storage Properties
journal, May 2016

  • Xiao, Wei; Zhou, Jing; Yu, Le
  • Angewandte Chemie International Edition, Vol. 55, Issue 26
  • DOI: 10.1002/anie.201602653

Three-dimensional interconnected network GeO x /multi-walled CNT composite spheres as high-performance anodes for lithium ion batteries
journal, January 2015

  • He, Wei; Tian, Huajun; Wang, Xiaoliang
  • Journal of Materials Chemistry A, Vol. 3, Issue 38
  • DOI: 10.1039/C5TA04456A

A germanium nanoparticles/molybdenum disulphide (MoS 2 ) nanocomposite as a high-capacity, high-rate anode material for lithium-ion batteries
journal, January 2017

  • Hsieh, Meng-Hsun; Li, Guo-An; Chang, Wei-Chung
  • Journal of Materials Chemistry A, Vol. 5, Issue 8
  • DOI: 10.1039/C6TA08455A

Hybridizing germanium anodes with polysaccharide-derived nitrogen-doped carbon for high volumetric capacity of Li-ion batteries
journal, January 2017

  • Ryu, Jaegeon; Hong, Dongki; Shin, Sunghee
  • Journal of Materials Chemistry A, Vol. 5, Issue 30
  • DOI: 10.1039/C7TA04028H

A novel strategy to prepare Ge@C/rGO hybrids as high-rate anode materials for lithium ion batteries
journal, February 2017


ZnO decorated germanium nanoparticles as anode materials in Li-ion batteries
journal, January 2017


Quinary wurtzite Zn-Ga-Ge-N-O solid solutions and their photocatalytic properties under visible light irradiation
journal, January 2016

  • Xie, Yinghao; Wu, Fangfang; Sun, Xiaoqin
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep19060

Zn x Ge 1– x O 3D Micronano Structures with Excellent Performance as Anode Material in Lithium Ion Battery
journal, July 2015

  • Sun, Y.; Yang, G. Z.; Cui, H.
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 28
  • DOI: 10.1021/acsami.5b02518

In Situ Synthesis and Characterization of Ge Embedded Electrospun Carbon Nanostructures as High Performance Anode Material for Lithium-Ion Batteries
journal, March 2016

  • Lee, Young-Woo; Kim, Da-Mi; Kim, Si-Jin
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 11
  • DOI: 10.1021/acsami.5b12284

Synthesis and optical properties of Zn2GeO4 microrods
journal, February 2016


Correction: Core–shell Zn 2 GeO 4 nanorods and their size-dependent photoluminescence properties
journal, January 2016

  • Wu, Songping; Wang, Zhuolin; Ouyang, Xin
  • Nanoscale, Vol. 8, Issue 12
  • DOI: 10.1039/C6NR90026G

Electronic structure and optical properties of Zn(OH) 2 : LDA+U calculations and intense yellow luminescence
journal, January 2015

  • Wang, Mingsong; Jiang, Lingxia; Kim, Eui Jung
  • RSC Advances, Vol. 5, Issue 106
  • DOI: 10.1039/C5RA17024A

Orange Zinc Germanate with Metallic GeGe Bonds as a Chromophore-Like Center for Visible-Light-Driven Water Splitting
journal, August 2015

  • Qian, Ling; Chen, Jian Fu; Li, Yu Hang
  • Angewandte Chemie International Edition, Vol. 54, Issue 39
  • DOI: 10.1002/anie.201505988

Au–ZnO bullet-like heterodimer nanoparticles: synthesis and use for enhanced nonenzymatic electrochemical determination of glucose
journal, January 2014

  • Kumar, Deivasigamani Ranjith; Manoj, Devaraj; Santhanalakshmi, Jayadevan
  • RSC Advances, Vol. 4, Issue 18
  • DOI: 10.1039/c3ra45269g

Zinc-Zinc Double Bonds: A Theoretical Study
journal, July 2017

  • Echeverría, Jorge; Falceto, Andrés; Alvarez, Santiago
  • Angewandte Chemie International Edition, Vol. 56, Issue 34
  • DOI: 10.1002/anie.201702171

Reduced GeO2 Nanoparticles: Electronic Structure of a Nominal GeOx Complex and Its Stability under H2 Annealing
journal, December 2015

  • Zhao, Jia; Yang, Linju; McLeod, John A.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep17779

In situ analyses for ion storage materials
journal, January 2016

  • Yang, Junghoon; Muhammad, Shoaib; Jo, Mi Ru
  • Chemical Society Reviews, Vol. 45, Issue 20
  • DOI: 10.1039/C5CS00734H

High-performance silicon-based multicomponent battery anodes produced via synergistic coupling of multifunctional coating layers
journal, January 2015

  • Lee, Jung-In; Ko, Younghoon; Shin, Myoungsoo
  • Energy & Environmental Science, Vol. 8, Issue 7
  • DOI: 10.1039/C5EE01493J

Study of the surface reaction mechanism of Li4Ti5O12 anode for lithium-ion cells
journal, April 2015


Surface Modification of Over-Lithiated Layered Oxides with PEDOT:PSS Conducting Polymer in Lithium-Ion Batteries
journal, January 2015

  • Lee, Jieun; Choi, Wonchang
  • Journal of The Electrochemical Society, Vol. 162, Issue 4
  • DOI: 10.1149/2.0801504jes

Conductivity and NMR study of ionic mobility in lithium oxide
journal, January 1990

  • Strange, J. H.; Rageb, S. M.; Chadwick, A. V.
  • Journal of the Chemical Society, Faraday Transactions, Vol. 86, Issue 8
  • DOI: 10.1039/ft9908601239

Defect structures and ionic transport in lithium oxide
journal, September 1988


Lithium carbonate as a solid electrolyte
journal, July 1992


Understanding Phase Transformation in Crystalline Ge Anodes for Li-Ion Batteries
journal, June 2014

  • Lim, Linda Y.; Liu, Nian; Cui, Yi
  • Chemistry of Materials, Vol. 26, Issue 12
  • DOI: 10.1021/cm501233k

Understanding materials challenges for rechargeable ion batteries with in situ transmission electron microscopy
journal, August 2017

  • Yuan, Yifei; Amine, Khalil; Lu, Jun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15806

Reversible Nanopore Formation in Ge Nanowires during Lithiation–Delithiation Cycling: An In Situ Transmission Electron Microscopy Study
journal, September 2011

  • Liu, Xiao Hua; Huang, Shan; Picraux, S. Tom
  • Nano Letters, Vol. 11, Issue 9
  • DOI: 10.1021/nl2024118