Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni0.8Co0.1Mn0.1)O2 Cathode Materials

Mingyao Mou; Arjun Patel; Sourav Mallick; K. Jayanthi; Xiao Guang Sun; Mariappan Parans Paranthaman; Sophie Kothe; Ena Baral; Selma Saleh; Jethrine H. Mugumya; Michael L. Rasche; Ram B. Gupta; Herman Lopez; Mo Jiang

doi:10.1021/acsaem.2c03563

Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials

Mingyao Mou, Arjun Patel, Sourav Mallick, K. Jayanthi, Xiao Guang Sun, Mariappan Parans Paranthaman, Sophie Kothe, Ena Baral, Selma Saleh, Jethrine H. Mugumya, Michael L. Rasche, Ram B. Gupta, Herman Lopez, Mo Jiang

Nanomaterials Chemistry Group

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

7 Scopus citations

Abstract

The microparticle quality and reproducibility of Li(Ni_0.8Co_0.1Mn_0.1)O₂ (NCM811) cathode materials are important for Li-ion battery performance but can be challenging to control directly from synthesis. Here, a scalable reproducible synthesis process is designed based on slug flow to rapidly generate uniform micron-size spherical-shape NCM oxalate precursor microparticles at 25-34 °C. The whole process takes only 10 min, from solution mixing to precursor microparticle generation, without needing aging that typically takes hours. These oxalate precursors are convertible to spherical-shape NCM811 oxide microparticles, through a preliminary design of low heating rates (e.g., 0.1 and 0.8 °C/min) for calcination and lithiation. The outcome oxide cathode particles also demonstrate improved tap density (e.g., 2.4 g mL^-1 for NCM811) and good specific capacity (202 mAh g^-1 at 0.1 C) in coin cells and reasonably good cycling performance with LiF coating.

Original language	English
Pages (from-to)	3213-3224
Number of pages	12
Journal	ACS Applied Energy Materials
Volume	6
Issue number	6
DOIs	https://doi.org/10.1021/acsaem.2c03563
State	Published - Mar 27 2023

Funding

This material is based upon work supported by Virginia Commonwealth University and the National Science Foundation (Grant No. CMMI-1940948) and U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office (award DE-EE0009110). K.J and M.P.P. were supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office. X.-G.S. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This material is based upon work supported by Virginia Commonwealth University and the National Science Foundation (Grant No. CMMI-1940948) and U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office (award DE-EE0009110). K.J and M.P.P. were supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office. X.-G.S. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Funders	Funder number
Advanced Materials and Manufacturing Technologies Office	DE-EE0009110
DOE Public Access Plan
United States Government
National Science Foundation	CMMI-1940948
U.S. Department of Energy
Office of Science
Office of Energy Efficiency and Renewable Energy
Basic Energy Sciences
Virginia Commonwealth University
Division of Materials Sciences and Engineering	DE-AC05-00OR22725

Keywords

NCM811
coprecipitation
lithium-ion battery
slug flow
tap density

UN SDGs

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

Access to Document

10.1021/acsaem.2c03563

Cite this

Mou, M., Patel, A., Mallick, S., Jayanthi, K., Sun, X. G., Paranthaman, M. P., Kothe, S., Baral, E., Saleh, S., Mugumya, J. H., Rasche, M. L., Gupta, R. B., Lopez, H., & Jiang, M. (2023). Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials. ACS Applied Energy Materials, 6(6), 3213-3224. https://doi.org/10.1021/acsaem.2c03563

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title = "Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni0.8Co0.1Mn0.1)O2 Cathode Materials",

abstract = "The microparticle quality and reproducibility of Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) cathode materials are important for Li-ion battery performance but can be challenging to control directly from synthesis. Here, a scalable reproducible synthesis process is designed based on slug flow to rapidly generate uniform micron-size spherical-shape NCM oxalate precursor microparticles at 25-34 °C. The whole process takes only 10 min, from solution mixing to precursor microparticle generation, without needing aging that typically takes hours. These oxalate precursors are convertible to spherical-shape NCM811 oxide microparticles, through a preliminary design of low heating rates (e.g., 0.1 and 0.8 °C/min) for calcination and lithiation. The outcome oxide cathode particles also demonstrate improved tap density (e.g., 2.4 g mL-1 for NCM811) and good specific capacity (202 mAh g-1 at 0.1 C) in coin cells and reasonably good cycling performance with LiF coating.",

keywords = "NCM811, coprecipitation, lithium-ion battery, slug flow, tap density",

author = "Mingyao Mou and Arjun Patel and Sourav Mallick and K. Jayanthi and Sun, {Xiao Guang} and Paranthaman, {Mariappan Parans} and Sophie Kothe and Ena Baral and Selma Saleh and Mugumya, {Jethrine H.} and Rasche, {Michael L.} and Gupta, {Ram B.} and Herman Lopez and Mo Jiang",

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year = "2023",

month = mar,

day = "27",

doi = "10.1021/acsaem.2c03563",

language = "English",

volume = "6",

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Mou, M, Patel, A, Mallick, S, Jayanthi, K, Sun, XG , Paranthaman, MP, Kothe, S, Baral, E, Saleh, S, Mugumya, JH, Rasche, ML, Gupta, RB, Lopez, H & Jiang, M 2023, 'Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials', ACS Applied Energy Materials, vol. 6, no. 6, pp. 3213-3224. https://doi.org/10.1021/acsaem.2c03563

Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials. / Mou, Mingyao; Patel, Arjun; Mallick, Sourav et al.
In: ACS Applied Energy Materials, Vol. 6, No. 6, 27.03.2023, p. 3213-3224.

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

TY - JOUR

T1 - Slug Flow Coprecipitation Synthesis of Uniformly-Sized Oxalate Precursor Microparticles for Improved Reproducibility and Tap Density of Li(Ni0.8Co0.1Mn0.1)O2 Cathode Materials

AU - Mou, Mingyao

AU - Patel, Arjun

AU - Mallick, Sourav

AU - Jayanthi, K.

AU - Sun, Xiao Guang

AU - Paranthaman, Mariappan Parans

AU - Kothe, Sophie

AU - Baral, Ena

AU - Saleh, Selma

AU - Mugumya, Jethrine H.

AU - Rasche, Michael L.

AU - Gupta, Ram B.

AU - Lopez, Herman

AU - Jiang, Mo

PY - 2023/3/27

Y1 - 2023/3/27

N2 - The microparticle quality and reproducibility of Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) cathode materials are important for Li-ion battery performance but can be challenging to control directly from synthesis. Here, a scalable reproducible synthesis process is designed based on slug flow to rapidly generate uniform micron-size spherical-shape NCM oxalate precursor microparticles at 25-34 °C. The whole process takes only 10 min, from solution mixing to precursor microparticle generation, without needing aging that typically takes hours. These oxalate precursors are convertible to spherical-shape NCM811 oxide microparticles, through a preliminary design of low heating rates (e.g., 0.1 and 0.8 °C/min) for calcination and lithiation. The outcome oxide cathode particles also demonstrate improved tap density (e.g., 2.4 g mL-1 for NCM811) and good specific capacity (202 mAh g-1 at 0.1 C) in coin cells and reasonably good cycling performance with LiF coating.

AB - The microparticle quality and reproducibility of Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) cathode materials are important for Li-ion battery performance but can be challenging to control directly from synthesis. Here, a scalable reproducible synthesis process is designed based on slug flow to rapidly generate uniform micron-size spherical-shape NCM oxalate precursor microparticles at 25-34 °C. The whole process takes only 10 min, from solution mixing to precursor microparticle generation, without needing aging that typically takes hours. These oxalate precursors are convertible to spherical-shape NCM811 oxide microparticles, through a preliminary design of low heating rates (e.g., 0.1 and 0.8 °C/min) for calcination and lithiation. The outcome oxide cathode particles also demonstrate improved tap density (e.g., 2.4 g mL-1 for NCM811) and good specific capacity (202 mAh g-1 at 0.1 C) in coin cells and reasonably good cycling performance with LiF coating.

KW - NCM811

KW - coprecipitation

KW - lithium-ion battery

KW - slug flow

KW - tap density

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U2 - 10.1021/acsaem.2c03563

DO - 10.1021/acsaem.2c03563

M3 - Article

AN - SCOPUS:85149830572

SN - 2574-0962

VL - 6

SP - 3213

EP - 3224

JO - ACS Applied Energy Materials

JF - ACS Applied Energy Materials

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