In-situ Multimodal Imaging and Spectroscopy of Mg Electrodeposition at Electrode-Electrolyte Interfaces
Abstract
We report the study of Mg cathodic electrochemical deposition on Ti and Au electrode using a multimodal approach by examining the sample area in-situ using liquid cell transmission electron microscopy (TEM), scanning transmission X-ray microscopy (STXM) and X-ray absorption spectroscopy (XAS). Magnesium Aluminum Chloride Complex was synthesized and utilized as electrolyte, where non-reversible features during in situ charging-discharging cycles were observed. During charging, a uniform Mg film was deposited on the electrode, which is consistent with the intrinsic non-dendritic nature of Mg deposition in Mg ion batteries. The Mg thin film was not dissolvable during the following discharge process. We found that such Mg thin film is hexacoordinated Mg compounds by in-situ STXM and XAS. This study provides insights on the non-reversibility issue and failure mechanism of Mg ion batteries. Also, our method provides a novel generic method to understand the in situ battery chemistry without any further sample processing, which can preserve the original nature of battery materials or electrodeposited materials. This multimodal in situ imaging and spectroscopy provides many opportunities to attack complex problems that span orders of magnitude in length and time scale, which can be applied to a broad range of the energy storage systems.
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Sciences and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Xiamen Univ. (China). College of Energy
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source; Univ. of Illinois, Chicago, IL (United States). Dept. of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Xiamen Univ. (China). College of Chemistry and Chemical Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; National Chiao Tung Univ., Hsinchu (Taiwan). Dept. of Materials Science and Engineering
- National Chiao Tung Univ., Hsinchu (Taiwan). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1379730
- Grant/Contract Number:
- AC02-05CH11231; SC0012583
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemistry; nanofluidics
Citation Formats
Wu, Yimin A., Yin, Zuwei, Farmand, Maryam, Yu, Young-Sang, Shapiro, David A., Liao, Hong-Gang, Liang, Wen-I, Chu, Ying-Hao, and Zheng, Haimei. In-situ Multimodal Imaging and Spectroscopy of Mg Electrodeposition at Electrode-Electrolyte Interfaces. United States: N. p., 2017.
Web. doi:10.1038/srep42527.
Wu, Yimin A., Yin, Zuwei, Farmand, Maryam, Yu, Young-Sang, Shapiro, David A., Liao, Hong-Gang, Liang, Wen-I, Chu, Ying-Hao, & Zheng, Haimei. In-situ Multimodal Imaging and Spectroscopy of Mg Electrodeposition at Electrode-Electrolyte Interfaces. United States. https://doi.org/10.1038/srep42527
Wu, Yimin A., Yin, Zuwei, Farmand, Maryam, Yu, Young-Sang, Shapiro, David A., Liao, Hong-Gang, Liang, Wen-I, Chu, Ying-Hao, and Zheng, Haimei. Fri .
"In-situ Multimodal Imaging and Spectroscopy of Mg Electrodeposition at Electrode-Electrolyte Interfaces". United States. https://doi.org/10.1038/srep42527. https://www.osti.gov/servlets/purl/1379730.
@article{osti_1379730,
title = {In-situ Multimodal Imaging and Spectroscopy of Mg Electrodeposition at Electrode-Electrolyte Interfaces},
author = {Wu, Yimin A. and Yin, Zuwei and Farmand, Maryam and Yu, Young-Sang and Shapiro, David A. and Liao, Hong-Gang and Liang, Wen-I and Chu, Ying-Hao and Zheng, Haimei},
abstractNote = {We report the study of Mg cathodic electrochemical deposition on Ti and Au electrode using a multimodal approach by examining the sample area in-situ using liquid cell transmission electron microscopy (TEM), scanning transmission X-ray microscopy (STXM) and X-ray absorption spectroscopy (XAS). Magnesium Aluminum Chloride Complex was synthesized and utilized as electrolyte, where non-reversible features during in situ charging-discharging cycles were observed. During charging, a uniform Mg film was deposited on the electrode, which is consistent with the intrinsic non-dendritic nature of Mg deposition in Mg ion batteries. The Mg thin film was not dissolvable during the following discharge process. We found that such Mg thin film is hexacoordinated Mg compounds by in-situ STXM and XAS. This study provides insights on the non-reversibility issue and failure mechanism of Mg ion batteries. Also, our method provides a novel generic method to understand the in situ battery chemistry without any further sample processing, which can preserve the original nature of battery materials or electrodeposited materials. This multimodal in situ imaging and spectroscopy provides many opportunities to attack complex problems that span orders of magnitude in length and time scale, which can be applied to a broad range of the energy storage systems.},
doi = {10.1038/srep42527},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {2017},
month = {2}
}
Web of Science
Works referenced in this record:
Probing the Degradation Mechanisms in Electrolyte Solutions for Li-Ion Batteries by in Situ Transmission Electron Microscopy
journal, February 2014
- Abellan, Patricia; Mehdi, B. Layla; Parent, Lucas R.
- Nano Letters, Vol. 14, Issue 3
A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries
journal, September 2010
- Verma, Pallavi; Maire, Pascal; Novák, Petr
- Electrochimica Acta, Vol. 55, Issue 22, p. 6332-6341
Magnesium Borohydride: From Hydrogen Storage to Magnesium Battery
journal, August 2012
- Mohtadi, Rana; Matsui, Masaki; Arthur, Timothy S.
- Angewandte Chemie International Edition, Vol. 51, Issue 39, p. 9780-9783
Electrodeposition of magnesium from halide melts—charge transfer and diffusion kinetics
journal, January 1997
- Børresen, B.; Haarberg, G. M.; Tunold, R.
- Electrochimica Acta, Vol. 42, Issue 10
Highly active electrolytes for rechargeable Mg batteries based on a [Mg 2 (μ-Cl) 2 ] 2+ cation complex in dimethoxyethane
journal, January 2015
- Cheng, Yingwen; Stolley, Ryan M.; Han, Kee Sung
- Physical Chemistry Chemical Physics, Vol. 17, Issue 20
Grain Size Refinements of Au-Mg Alloy by Hydrogen Absorption/Desorption Treatments
journal, January 2009
- Takeda, Yugo; Kuriiwa, Takahiro; Kamegawa, Atsunori
- MATERIALS TRANSACTIONS, Vol. 50, Issue 3
Low-dimensional systems investigated by x-ray absorption spectroscopy: a selection of 2D, 1D and 0D cases
journal, September 2013
- Mino, Lorenzo; Agostini, Giovanni; Borfecchia, Elisa
- Journal of Physics D: Applied Physics, Vol. 46, Issue 42
Lithium Electrode Morphology during Cycling in Lithium Cells
journal, January 1988
- Yoshimatsu, Isamu
- Journal of The Electrochemical Society, Vol. 135, Issue 10
Electrolyte Solutions for Rechargeable Magnesium Batteries Based on Organomagnesium Chloroaluminate Complexes
journal, January 2002
- Aurbach, Doron; Gizbar, Haim; Schechter, Alex
- Journal of The Electrochemical Society, Vol. 149, Issue 2, p. A115-A121
The Solvation Structure of Mg Ions in Dichloro Complex Solutions from First-Principles Molecular Dynamics and Simulated X-ray Absorption Spectra
journal, October 2014
- Wan, Liwen F.; Prendergast, David
- Journal of the American Chemical Society, Vol. 136, Issue 41
Mg deposition observed by in situ electrochemical Mg K-edge X-ray absorption spectroscopy
journal, October 2012
- Arthur, Timothy S.; Glans, Per-Anders; Matsui, Masaki
- Electrochemistry Communications, Vol. 24
Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte
journal, February 2014
- Holtz, Megan E.; Yu, Yingchao; Gunceler, Deniz
- Nano Letters, Vol. 14, Issue 3
Nonaqueous magnesium electrochemistry and its application in secondary batteries
journal, January 2003
- Aurbach, Doron; Weissman, Idit; Gofer, Yosef
- The Chemical Record, Vol. 3, Issue 1, p. 61-73
Structure and compatibility of a magnesium electrolyte with a sulphur cathode
journal, August 2011
- Kim, Hee Soo; Arthur, Timothy S.; Allred, Gary D.
- Nature Communications, Vol. 2, Article No. 427
Structural Analysis of Electrolyte Solutions for Rechargeable Mg Batteries by Stereoscopic Means and DFT Calculations
journal, April 2011
- Pour, Nir; Gofer, Yossi; Major, Dan T.
- Journal of the American Chemical Society, Vol. 133, Issue 16
Highly Reversible Mg Insertion in Nanostructured Bi for Mg Ion Batteries
journal, December 2013
- Shao, Yuyan; Gu, Meng; Li, Xiaolin
- Nano Letters, Vol. 14, Issue 1
Room Temperature Magnesium Electrodeposition from Glyme-Coordinated Ammonium Amide Electrolytes
journal, January 2015
- Kitada, Atsushi; Kang, Yuu; Matsumoto, Kazuhiko
- Journal of The Electrochemical Society, Vol. 162, Issue 8
Progress in Rechargeable Magnesium Battery Technology
journal, December 2007
- Aurbach, D.; Suresh, G. S.; Levi, E.
- Advanced Materials, Vol. 19, Issue 23
Suppression of Lithium Dendrite Growth Using Cross-Linked Polyethylene/Poly(ethylene oxide) Electrolytes: A New Approach for Practical Lithium-Metal Polymer Batteries
journal, May 2014
- Khurana, Rachna; Schaefer, Jennifer L.; Archer, Lynden A.
- Journal of the American Chemical Society, Vol. 136, Issue 20
Sulfur Speciation in Li–S Batteries Determined by Operando X-ray Absorption Spectroscopy
journal, September 2013
- Cuisinier, Marine; Cabelguen, Pierre-Etienne; Evers, Scott
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 19
Rechargeable Mg Batteries with Graphene-like MoS2 Cathode and Ultrasmall Mg Nanoparticle Anode
journal, December 2010
- Liang, Yanliang; Feng, Rujun; Yang, Siqi
- Advanced Materials, Vol. 23, Issue 5
In Situ Observation of the Electrochemical Lithiation of a Single SnO2 Nanowire Electrode
journal, December 2010
- Huang, J. Y.; Zhong, L.; Wang, C. M.
- Science, Vol. 330, Issue 6010, p. 1515-1520
Room-Temperature Electrodeposition of Mg Metal from Amide Salts Dissolved in Glyme-Ionic Liquid Mixture
journal, December 2013
- Kitada, Atsushi; Kang, Yuu; Uchimoto, Yoshiharu
- Journal of The Electrochemical Society, Vol. 161, Issue 3
Evaluation of (CF 3 SO 2 ) 2 N − (TFSI) Based Electrolyte Solutions for Mg Batteries
journal, January 2015
- Shterenberg, Ivgeni; Salama, Michael; Yoo, Hyun Deog
- Journal of The Electrochemical Society, Vol. 162, Issue 13
Prototype systems for rechargeable magnesium batteries
journal, October 2000
- Aurbach, D.; Lu, Z.; Schechter, A.
- Nature, Vol. 407, Issue 6805, p. 724-727
Novel transmetalation reaction for electrolyte synthesis for rechargeable magnesium batteries
journal, January 2014
- Zhao-Karger, Zhirong; Mueller, Jonathan E.; Zhao, Xiangyu
- RSC Adv., Vol. 4, Issue 51
A facile approach using MgCl2 to formulate high performance Mg2+ electrolytes for rechargeable Mg batteries
journal, January 2014
- Liu, Tianbiao; Shao, Yuyan; Li, Guosheng
- Journal of Materials Chemistry A, Vol. 2, Issue 10
Magnesium(II) Bis(trifluoromethane sulfonyl) Imide-Based Electrolytes with Wide Electrochemical Windows for Rechargeable Magnesium Batteries
journal, March 2014
- Ha, Se-Young; Lee, Yong-Won; Woo, Sang Won
- ACS Applied Materials & Interfaces, Vol. 6, Issue 6, p. 4063-4073
Study of the electrochemical deposition of Mg in the atomic level: Why it prefers the non-dendritic morphology
journal, August 2012
- Ling, Chen; Banerjee, Debasish; Matsui, Masaki
- Electrochimica Acta, Vol. 76
Mg rechargeable batteries: an on-going challenge
journal, January 2013
- Yoo, Hyun Deog; Shterenberg, Ivgeni; Gofer, Yosef
- Energy & Environmental Science, Vol. 6, Issue 8, p. 2265-2279
The challenge of developing rechargeable magnesium batteries
journal, May 2014
- Shterenberg, Ivgeni; Salama, Michael; Gofer, Yossi
- MRS Bulletin, Vol. 39, Issue 5
Novel, electrolyte solutions comprising fully inorganic salts with high anodic stability for rechargeable magnesium batteries
journal, January 2014
- Doe, Robert E.; Han, Ruoban; Hwang, Jaehee
- Chemical Communications, Vol. 50, Issue 2, p. 243-245
High Areal Capacity Hybrid Magnesium–Lithium-Ion Battery with 99.9% Coulombic Efficiency for Large-Scale Energy Storage
journal, March 2015
- Yoo, Hyun Deog; Liang, Yanliang; Li, Yifei
- ACS Applied Materials & Interfaces, Vol. 7, Issue 12
High energy density rechargeable magnesium battery using earth-abundant and non-toxic elements
journal, July 2014
- Orikasa, Yuki; Masese, Titus; Koyama, Yukinori
- Scientific Reports, Vol. 4, Issue 1
Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes
journal, November 2013
- Harry, Katherine J.; Hallinan, Daniel T.; Parkinson, Dilworth Y.
- Nature Materials, Vol. 13, Issue 1
Visualization of Electrode–Electrolyte Interfaces in LiPF 6 /EC/DEC Electrolyte for Lithium Ion Batteries via in Situ TEM
journal, March 2014
- Zeng, Zhiyuan; Liang, Wen-I; Liao, Hong-Gang
- Nano Letters, Vol. 14, Issue 4
Interconnected hollow carbon nanospheres for stable lithium metal anodes
journal, July 2014
- Zheng, Guangyuan; Lee, Seok Woo; Liang, Zheng
- Nature Nanotechnology, Vol. 9, Issue 8
Investigating the Reversibility of in Situ Generated Magnesium Organohaloaluminates for Magnesium Deposition and Dissolution
journal, May 2014
- Barile, Christopher J.; Spatney, Russell; Zavadil, Kevin R.
- The Journal of Physical Chemistry C, Vol. 118, Issue 20
Coordination Chemistry in magnesium battery electrolytes: how ligands affect their performance
journal, November 2013
- Shao, Yuyan; Liu, Tianbiao; Li, Guosheng
- Scientific Reports, Vol. 3, Issue 1
Dynamics of Lithium Dendrite Growth and Inhibition: Pulse Charging Experiments and Monte Carlo Calculations
journal, May 2014
- Aryanfar, Asghar; Brooks, Daniel; Merinov, Boris V.
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 10
Structural and Morphological Evolution of Lead Dendrites during Electrochemical Migration
journal, November 2013
- Sun, Minghua; Liao, Hong-Gang; Niu, Kaiyang
- Scientific Reports, Vol. 3, Issue 1
Works referencing / citing this record:
In Situ Transmission Electron Microscopy Studies of Electrochemical Reaction Mechanisms in Rechargeable Batteries
journal, June 2019
- Wu, Xiaoyu; Li, Songmei; Yang, Bin
- Electrochemical Energy Reviews, Vol. 2, Issue 3
Simultaneous activity and surface area measurements on single mesoporous nanoparticle aggregates
journal, January 2018
- Jiao, Xue; Batchelor-McAuley, Christopher; Young, Neil P.
- Physical Chemistry Chemical Physics, Vol. 20, Issue 37