Title: Understanding Thickness-Dependent Transport Kinetics in Nanosheet-Based Battery Electrodes

Abstract

There is a growing need for thicker electrode designs to achieve high energy/power for ever-increasing power needs by electronic devices and electric automobiles. Though great efforts, such as structure optimization, have been devoted on fabricating thick electrodes, understanding of performance-limiting factors essential to electrode architecture design, has not been well established. In this study, the dependence of electrochemical behavior on electrode mass loading is comprehensively investigated in nanosheet-based electrodes. In particular, the effects of electrical conductivity and porosity are illustrated. In drop-casted electrodes, where nanosheets are highly stacked, ionic diffusion in the electrolyte has been determined to be the controlling step in electrodes with high thickness. To overcome the limitation of such sluggish ionic transport, a facile ice-templating strategy was employed to create vertically aligned channels, offering fast-diffusion pathways for the Li ion in the electrolyte. Impressively, the ice-templated electrodes exhibit a specific capacity of 144 mA h g^–1 at 0.2 C and retain 83 mA h g^–1 at 10 C with high mass loading ~10 mg cm^–2. The enhanced ion transport kinetics was verified by various electrochemical and structural characterizations. This work demonstrates the thickness scaling effect of nanosheet-based electrodes and highlights the importance of promoting ionic transport andmore » electrolyte access for designing thick electrodes.« less

Authors:

Ju, Zhengyu ^[1]; Zhu, Yue ^[1]; Zhang, Xiao  ^[1];

• Search DOE PAGES for author "Zhang, Xiao"
• Search DOE PAGES for ORCID "0000-0002-6596-9731"

Lutz, Diana M.  ^[2];

• Search DOE PAGES for author "Lutz, Diana M."
• Search DOE PAGES for ORCID "0000-0002-0358-8300"

Fang, Zhiwei  ^[1];

• Search DOE PAGES for author "Fang, Zhiwei"
• Search DOE PAGES for ORCID "0000-0001-8826-8834"

Takeuchi, Kenneth J.  ^[3];

• Search DOE PAGES for author "Takeuchi, Kenneth J."
• Search DOE PAGES for ORCID "0000-0001-8129-444X"

Takeuchi, Esther S.  ^[4];

• Search DOE PAGES for author "Takeuchi, Esther S."
• Search DOE PAGES for ORCID "0000-0001-8518-1047"

Marschilok, Amy C.  ^[4];

• Search DOE PAGES for author "Marschilok, Amy C."
• Search DOE PAGES for ORCID "0000-0001-9174-0474"

Yu, Guihua  ^[1]

• Search DOE PAGES for author "Yu, Guihua"
• Search DOE PAGES for ORCID "0000-0002-3253-0749"

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+ Show Author Affiliations

1. Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program, Texas Materials Inst.
2. Stony Brook Univ., NY (United States). Dept. of Chemistry
3. Stony Brook Univ., NY (United States). Dept. of Chemistry, and Dept. of Materials Science and Chemical Engineering
4. Stony Brook Univ., NY (United States). Dept. of Chemistry, and Dept. of Materials Science and Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:

Wed Jan 22 00:00:00 EST 2020

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1606183

Report Number(s):

BNL-213746-2020-JAAM
Journal ID: ISSN 0897-4756

Grant/Contract Number:  

SC0012704

Resource Type:

Accepted Manuscript

Journal Name:

Chemistry of Materials

Additional Journal Information:

Journal Volume: 32; Journal Issue: 4; Journal ID: ISSN 0897-4756

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE; Charge transport; Diffusion; Kinetics; Electrodes; Ions