Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

X-ray Nanocomputed Tomography in Zernike Phase Contrast for Studying 3D Morphology of Li–O2 Battery Electrode

Journal Article · · ACS Applied Energy Materials
 [1];  [2];  [3];  [1];  [2];  [4];  [5]
  1. Univ. de Picardie Jules Verne, Amiens (France). Lab. de Reactivite et Chimie des Solides (LRCS); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Univ. de Picardie Jules Verne, Amiens (France). Lab. de Reactivite et Chimie des Solides (LRCS); Nanyang Technological Univ. (Singapore)
  4. Univ. de Picardie Jules Verne, Amiens (France). Lab. de Reactivite et Chimie des Solides (LRCS); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France); Inst. Univ. de France, Paris (France); ALISTORE-European Research Inst., Amiens (France)
  5. Univ. de Picardie Jules Verne, Amiens (France). Lab. de Reactivite et Chimie des Solides (LRCS); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France); ALISTORE-European Research Inst., Amiens (France)

In this work, we investigated the lithium peroxide (Li2O2) and pore size distribution in lithium-O2 battery electrodes at different states of charge using transmission X-ray microscopy coupled with Zernike phase contrast to carry out nano-Computed Tomography. We report that such technique enables, at the nanoscale, to distinguish light elements such as carbon and Li2O2 in Li-O2 battery cathode electrodes. We verified by wave-propagation simulation that this approach efficiently improves the contrast of images in comparison with the pure absorption. The Li2O2 distribution and thickness, interphases, and pore network are visualized and quantified, which give a valuable insight into our cathode architecture. From this 3D analysis, we highlight modifications of the air-cathode morphology and the Li2O2 spatial organization as well as their potential implication in terms of carbon surface passivation and pore-clogging. After the full recharge process, this technique can also reveal the spatial distribution of the residual Li2O2 and other byproducts.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1785721
Journal Information:
ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 5 Vol. 3; ISSN 2574-0962
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (37)

Redox Mediators for Li-O 2 Batteries: Status and Perspectives journal November 2017
Tortuosity Anisotropy in Lithium-Ion Battery Electrodes journal October 2013
Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity journal January 2018
Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Direct Detection of Discharge Products in Lithium-Oxygen Batteries by Solid-State NMR Spectroscopy journal July 2012
Superior Rechargeability and Efficiency of Lithium-Oxygen Batteries: Hierarchical Air Electrode Architecture Combined with a Soluble Catalyst journal March 2014
Identifying Reactive Sites and Transport Limitations of Oxygen Reactions in Aprotic Lithium-O 2 Batteries at the Stage of Sudden Death journal March 2016
Defect Chemistry in Discharge Products of Li-O 2 Batteries journal November 2018
Investigation of bi-porous electrodes for lithium oxygen batteries journal July 2018
In situ investigation of pore clogging during discharge of a Li/O2 battery by electrochemical impedance spectroscopy journal March 2015
Three-dimensional phase segregation of micro-porous layers for fuel cells by nano-scale X-ray computed tomography journal April 2016
Operando liquid cell electron microscopy of discharge and charge kinetics in lithium-oxygen batteries journal July 2018
In situ characterization of Si-based anodes by coupling synchrotron X-ray tomography and diffraction journal February 2019
The application of phase contrast X-ray techniques for imaging Li-ion battery electrodes journal April 2014
Relative merits and limiting factors for x-ray and electron microscopy of thick, hydrated organic materials journal January 2018
Discharge Performance of Li–O 2 Batteries Using a Multiscale Modeling Approach journal June 2015
Stochasticity of Pores Interconnectivity in Li–O 2 Batteries and its Impact on the Variations in Electrochemical Performance journal February 2018
Four-Dimensional Studies of Morphology Evolution in Lithium–Sulfur Batteries journal August 2018
Decoupling Energy Storage from Electrochemical Reactions in Li–Air Batteries toward Achieving Continuous Discharge journal February 2017
Enhanced Cyclability of Li–O 2 Batteries Based on TiO 2 Supported Cathodes with No Carbon or Binder journal April 2014
Aprotic and Aqueous Li–O2 Batteries journal April 2014
The Carbon Electrode in Nonaqueous Li–O2 Cells
  • Ottakam Thotiyl, Muhammed M.; Freunberger, Stefan A.; Peng, Zhangquan
  • Journal of the American Chemical Society, Vol. 135, Issue 1, p. 494-500 https://doi.org/10.1021/ja310258x
journal December 2012
Anomalous Discharge Product Distribution in Lithium-Air Cathodes journal April 2012
Lithium−Air Battery: Promise and Challenges journal June 2010
Probing the Reaction Kinetics of the Charge Reactions of Nonaqueous Li–O 2 Batteries journal December 2012
In Situ Transmission Electron Microscopy Observations of Electrochemical Oxidation of Li 2 O 2 journal April 2013
Erratum: Li–O2 and Li–S batteries with high energy storage journal December 2011
Three-dimensional localization of nanoscale battery reactions using soft X-ray tomography journal March 2018
Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging journal June 2018
Reaction chemistry in rechargeable Li–O 2 batteries journal January 2017
Current density dependence of peroxide formation in the Li–O2 battery and its effect on charge journal January 2013
Free-standing, hierarchically porous carbon nanotube film as a binder-free electrode for high-energy Li–O2 batteries journal January 2013
Full-field transmission x-ray microscopy for bio-imaging journal September 2009
TomoPy: a framework for the analysis of synchrotron tomographic data journal August 2014
Integration of TomoPy and the ASTRA toolbox for advanced processing and reconstruction of tomographic synchrotron data journal April 2016
Issues and challenges facing rechargeable lithium batteries book October 2010
Impact of the Cathode Microstructure on the Discharge Performance of Lithium Air Batteries: A Multiscale Model journal January 2014