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Title: Direct observation of active material interactions in flowable electrodes using X-ray tomography

Abstract

Understanding electrical percolation and charging mechanisms in electrochemically active biphasic flowable electrodes is critical for enabling scalable deionization (desalination) and energy storage. Flowable electrodes are dynamic material systems which store charge (remove ions) and have the ability to flow. This flow process can induce structural changes in the underlying material arrangement and result in transient and non-uniform material properties. Carbon-based suspensions are opaque, multi-phase, and three dimensional, and thus prior characterization of the structural properties has been limited to indirect methods (electrochemical and rheology). Herein, a range of mixed electronic and ionically conducting suspensions are evaluated to determine their static structure, function, and properties, utilizing synchrotron radiation X-ray tomographic microscopy (SRXTM). The high brilliance of the synchrotron light enables deconvolution of the liquid and solid phases. Reconstruction of the solid phase reveals agglomeration cluster volumes between 10 μm 3and 10 3μm 3(1 pL) for low loaded samples (5 wt% carbon). The largest agglomeration cluster in the low loaded sample (5 wt%) occupied only 3% of the reconstructed volume whereas samples loaded with 10 wt% activated carbon demonstrated electrically connected clusters that occupied 22% of the imaged region. The highly loaded samples (20 wt%) demonstrated clusters of the order of amore » microliter, which accounted for 63–85% of the imaged region. These results demonstrate a capability for discerning the structural properties of biphasic systems utilizing SRXTM techniques, and show that discontinuity in the carbon particle networks induces decreased material utilization in low-loaded flowable electrodes.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [3]; ORCiD logo [4]
  1. Department of Mechanical Engineering; Department of Chemical and Biomolecular Engineering; Vanderbilt University; Nashville; USA
  2. Paul Scherrer Institute; Villigen PSI; Switzerland
  3. Department of Chemical and Biological Engineering; Drexel University; Philadelphia; USA
  4. Department of Material Science and Engineering; A.J. Drexel Nanomaterials Institute; Drexel University; Philadelphia; USA
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1388641
DOE Contract Number:  
ERKCC61
Resource Type:
Journal Article
Journal Name:
Faraday Discussions
Additional Journal Information:
Journal Volume: 199; Related Information: FIRST partners with Oak Ridge National Laboratory (lead); Argonne National Laboratory; Drexel University; Georgia State University; Northwestern University; Pennsylvania State University; Suffolk University; Vanderbilt University; University of Virginia; Journal ID: ISSN 1359-6640
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
catalysis (heterogeneous), solar (fuels), energy storage (including batteries and capacitors), hydrogen and fuel cells, electrodes - solar, mechanical behavior, charge transport, materials and chemistry by design, synthesis (novel materials)

Citation Formats

Hatzell, Kelsey B., Eller, Jens, Morelly, Samantha L., Tang, Maureen H., Alvarez, Nicolas J., and Gogotsi, Yury. Direct observation of active material interactions in flowable electrodes using X-ray tomography. United States: N. p., 2017. Web. doi:10.1039/C6FD00243A.
Hatzell, Kelsey B., Eller, Jens, Morelly, Samantha L., Tang, Maureen H., Alvarez, Nicolas J., & Gogotsi, Yury. Direct observation of active material interactions in flowable electrodes using X-ray tomography. United States. doi:10.1039/C6FD00243A.
Hatzell, Kelsey B., Eller, Jens, Morelly, Samantha L., Tang, Maureen H., Alvarez, Nicolas J., and Gogotsi, Yury. Sun . "Direct observation of active material interactions in flowable electrodes using X-ray tomography". United States. doi:10.1039/C6FD00243A.
@article{osti_1388641,
title = {Direct observation of active material interactions in flowable electrodes using X-ray tomography},
author = {Hatzell, Kelsey B. and Eller, Jens and Morelly, Samantha L. and Tang, Maureen H. and Alvarez, Nicolas J. and Gogotsi, Yury},
abstractNote = {Understanding electrical percolation and charging mechanisms in electrochemically active biphasic flowable electrodes is critical for enabling scalable deionization (desalination) and energy storage. Flowable electrodes are dynamic material systems which store charge (remove ions) and have the ability to flow. This flow process can induce structural changes in the underlying material arrangement and result in transient and non-uniform material properties. Carbon-based suspensions are opaque, multi-phase, and three dimensional, and thus prior characterization of the structural properties has been limited to indirect methods (electrochemical and rheology). Herein, a range of mixed electronic and ionically conducting suspensions are evaluated to determine their static structure, function, and properties, utilizing synchrotron radiation X-ray tomographic microscopy (SRXTM). The high brilliance of the synchrotron light enables deconvolution of the liquid and solid phases. Reconstruction of the solid phase reveals agglomeration cluster volumes between 10 μm3and 103μm3(1 pL) for low loaded samples (5 wt% carbon). The largest agglomeration cluster in the low loaded sample (5 wt%) occupied only 3% of the reconstructed volume whereas samples loaded with 10 wt% activated carbon demonstrated electrically connected clusters that occupied 22% of the imaged region. The highly loaded samples (20 wt%) demonstrated clusters of the order of a microliter, which accounted for 63–85% of the imaged region. These results demonstrate a capability for discerning the structural properties of biphasic systems utilizing SRXTM techniques, and show that discontinuity in the carbon particle networks induces decreased material utilization in low-loaded flowable electrodes.},
doi = {10.1039/C6FD00243A},
journal = {Faraday Discussions},
issn = {1359-6640},
number = ,
volume = 199,
place = {United States},
year = {2017},
month = {1}
}

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