Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Runming Tao; Boman Su; Santosh Thapa; Kübra Uzun; Haidar Alolaywi; Xiang Lyu; Bryan Steinhoff; Kahla Sardo; Zhijia Du; Yang Tse Cheng; Chris Yuan; Krzysztof Z. Pupek; Georgios Polizos; Jianlin Li

doi:10.1016/j.cej.2024.157194

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Runming Tao, Boman Su, Santosh Thapa, Kübra Uzun, Haidar Alolaywi, Xiang Lyu, Bryan Steinhoff, Kahla Sardo, Zhijia Du, Yang Tse Cheng, Chris Yuan, Krzysztof Z. Pupek, Georgios Polizos, Jianlin Li

Research output: Contribution to journal › Article › peer-review

Abstract

Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. The results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g⁻¹ at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g⁻¹ and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.

Original language	English
Article number	157194
Journal	Chemical Engineering Journal
Volume	500
DOIs	https://doi.org/10.1016/j.cej.2024.157194
State	Published - Nov 15 2024

Funding

The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (\u201CArgonne\u201D). Argonne, a U.S. Department of Energy (DOE) Office of Science laboratory, is operated under Contract DE-AC02-06CH11357. Part of this research was conducted at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, and was sponsored by the DOE Advanced Materials & Manufacturing Technologies Office (DE-EE0009109). The SEM characterization was conducted at the Center for Nanophase Materials Sciences at ORNL, which is a DOE Office of Science User Facility. B. S. was funded by the Institute for Smart, Secure and Connected Systems (ISSACS) at Case Western Reserve University. The authors thank Cabot Corporation and Arkema for their material and technical assistance. The authors also thank Ben La Riviere at ORNL for experimental assistance. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

Funders	Funder number
United States Government
Institute for Smart, Secure and Connected Systems
DOE Public Access Plan
Oak Ridge National Laboratory
Case Western Reserve University
Argonne National Laboratory
ISSACS
Office of Science
U.S. Department of Energy	DE-AC02-06CH11357
U.S. Department of Energy
UT-Battelle	DE-AC05-00OR22725
UT-Battelle
Advanced Materials and Manufacturing Technologies Office	DE-EE0009109
Advanced Materials and Manufacturing Technologies Office

Keywords

Dry processing
Electrode engineering
High-loading electrodes
Lithium-ion batteries
Single crystal

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.cej.2024.157194

Cite this

Tao, R., Su, B., Thapa, S., Uzun, K., Alolaywi, H., Lyu, X., Steinhoff, B., Sardo, K., Du, Z., Cheng, Y. T., Yuan, C., Pupek, K. Z., Polizos, G., & Li, J. (2024). Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries. Chemical Engineering Journal, 500, Article 157194. https://doi.org/10.1016/j.cej.2024.157194

@article{e7c9e81f24454ec0bdac27e70cb88f6e,

title = "Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries",

abstract = "Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. The results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g−1 at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g−1 and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.",

keywords = "Dry processing, Electrode engineering, High-loading electrodes, Lithium-ion batteries, Single crystal",

author = "Runming Tao and Boman Su and Santosh Thapa and K{\"u}bra Uzun and Haidar Alolaywi and Xiang Lyu and Bryan Steinhoff and Kahla Sardo and Zhijia Du and Cheng, {Yang Tse} and Chris Yuan and Pupek, {Krzysztof Z.} and Georgios Polizos and Jianlin Li",

note = "Publisher Copyright: {\textcopyright} 2024 Elsevier B.V.",

year = "2024",

month = nov,

day = "15",

doi = "10.1016/j.cej.2024.157194",

language = "English",

volume = "500",

journal = "Chemical Engineering Journal",

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Tao, R, Su, B, Thapa, S, Uzun, K, Alolaywi, H, Lyu, X, Steinhoff, B, Sardo, K, Du, Z, Cheng, YT, Yuan, C, Pupek, KZ, Polizos, G & Li, J 2024, 'Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries', Chemical Engineering Journal, vol. 500, 157194. https://doi.org/10.1016/j.cej.2024.157194

TY - JOUR

T1 - Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

AU - Tao, Runming

AU - Su, Boman

AU - Thapa, Santosh

AU - Uzun, Kübra

AU - Alolaywi, Haidar

AU - Lyu, Xiang

AU - Steinhoff, Bryan

AU - Sardo, Kahla

AU - Du, Zhijia

AU - Cheng, Yang Tse

AU - Yuan, Chris

AU - Pupek, Krzysztof Z.

AU - Polizos, Georgios

AU - Li, Jianlin

PY - 2024/11/15

Y1 - 2024/11/15

N2 - Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. The results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g−1 at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g−1 and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.

AB - Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. The results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g−1 at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g−1 and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.

KW - Dry processing

KW - Electrode engineering

KW - High-loading electrodes

KW - Lithium-ion batteries

KW - Single crystal

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U2 - 10.1016/j.cej.2024.157194

DO - 10.1016/j.cej.2024.157194

M3 - Article

AN - SCOPUS:85208174318

SN - 1385-8947

VL - 500

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 157194

ER -

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Abstract

Funding

Keywords

UN SDGs

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