Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure

Chang An Lo; Yixian Wang; Varun R. Kankanallu; Aditya Singla; Dean Yen; Xiaoyin Zheng; Kaustubh G. Naik; Bairav S. Vishnugopi; Callum Campbell; Vikalp Raj; Chonghang Zhao; Lu Ma; Jianming Bai; Feipeng Yang; Ruipeng Li; Mingyuan Ge; John Watt; Partha P. Mukherjee; David Mitlin; Yu chen Karen Chen-Wiegart

doi:10.1002/anie.202412550

Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure

Chang An Lo, Yixian Wang, Varun R. Kankanallu, Aditya Singla, Dean Yen, Xiaoyin Zheng, Kaustubh G. Naik, Bairav S. Vishnugopi, Callum Campbell, Vikalp Raj, Chonghang Zhao, Lu Ma, Jianming Bai, Feipeng Yang, Ruipeng Li, Mingyuan Ge, John Watt, Partha P. Mukherjee, David Mitlin, Yu chen Karen Chen-Wiegart

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

2 Scopus citations

Abstract

This study examines how current collector support chemistry (sodiophilic intermetallic Na₂Te vs. sodiophobic baseline Cu) and electrodeposition rate affect microstructure of sodium metal and its solid electrolyte interphase (SEI). Capacity and current (6 mAh cm⁻², 0.5–3 mA cm⁻²) representative of commercially relevant mass loading in anode-free sodium metal battery (AF-SMBs) are analyzed. Synchrotron X-ray nanotomography and grazing-incidence wide-angle X-ray scattering (GIWAXS) are combined with cryogenic ion beam (cryo-FIB) microscopy. Highlighted are major differences in film morphology, internal porosity, and crystallographic preferred orientation e.g. (110) vs. (100) and (211) with support and deposition rate. Within the SEI, sodium fluoride (NaF) is more prevalent with Te−Cu versus sodium hydride (NaH) and sodium hydroxide (NaOH) with baseline Cu. Due to competitive grain growth the preferred orientation of sodium crystallites depends on film thickness. Mesoscale modeling delineates the role of SEI (ionic conductivity, morphology) on electrodeposit growth and onset of electrochemical instability.

Original language	English
Article number	e202412550
Journal	Angewandte Chemie - International Edition
Volume	64
Issue number	8
DOIs	https://doi.org/10.1002/anie.202412550
State	Published - Feb 17 2025
Externally published	Yes

Funding

We gratefully acknowledge support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award# DE-SC0023260. This research used resources, Full Field X-ray Imaging (FXI) beamline (18-ID), Complex Materials Scattering (CMS) beamline (11-BM), and Quick X-ray Absorption and Scattering (QAS) beamline (7-BM) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used scanning electron microscopy capabilities of the Center for Functional Nanomaterials (CFN), which is a U.S. DOE Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704. Cryo-EM was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. The Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under contract 89233218CNA000001. This work was supported by The Welch Foundation (F-2206). We gratefully acknowledge support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award# DE‐SC0023260. This research used resources, Full Field X‐ray Imaging (FXI) beamline (18‐ID), Complex Materials Scattering (CMS) beamline (11‐BM), and Quick X‐ray Absorption and Scattering (QAS) beamline (7‐BM) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. This research used scanning electron microscopy capabilities of the Center for Functional Nanomaterials (CFN), which is a U.S. DOE Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE‐SC0012704. Cryo‐EM was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. The Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under contract 89233218CNA000001. This work was supported by The Welch Foundation (F‐2206).

Keywords

fiber texture
film growth
sodium metal anode
sodium metal battery
solid electrolyte interphase (SEI)

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10.1002/anie.202412550

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Lo, C. A., Wang, Y., Kankanallu, V. R., Singla, A., Yen, D., Zheng, X., Naik, K. G., Vishnugopi, B. S., Campbell, C., Raj, V., Zhao, C., Ma, L., Bai, J., Yang, F., Li, R., Ge, M., Watt, J., Mukherjee, P. P., Mitlin, D., & Karen Chen-Wiegart, Y. C. (2025). Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure. Angewandte Chemie - International Edition, 64(8), Article e202412550. https://doi.org/10.1002/anie.202412550

@article{ccc481de63554a8fb9601d3eaaa238bd,

title = "Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure",

abstract = "This study examines how current collector support chemistry (sodiophilic intermetallic Na2Te vs. sodiophobic baseline Cu) and electrodeposition rate affect microstructure of sodium metal and its solid electrolyte interphase (SEI). Capacity and current (6 mAh cm−2, 0.5–3 mA cm−2) representative of commercially relevant mass loading in anode-free sodium metal battery (AF-SMBs) are analyzed. Synchrotron X-ray nanotomography and grazing-incidence wide-angle X-ray scattering (GIWAXS) are combined with cryogenic ion beam (cryo-FIB) microscopy. Highlighted are major differences in film morphology, internal porosity, and crystallographic preferred orientation e.g. (110) vs. (100) and (211) with support and deposition rate. Within the SEI, sodium fluoride (NaF) is more prevalent with Te−Cu versus sodium hydride (NaH) and sodium hydroxide (NaOH) with baseline Cu. Due to competitive grain growth the preferred orientation of sodium crystallites depends on film thickness. Mesoscale modeling delineates the role of SEI (ionic conductivity, morphology) on electrodeposit growth and onset of electrochemical instability.",

keywords = "fiber texture, film growth, sodium metal anode, sodium metal battery, solid electrolyte interphase (SEI)",

author = "Lo, \{Chang An\} and Yixian Wang and Kankanallu, \{Varun R.\} and Aditya Singla and Dean Yen and Xiaoyin Zheng and Naik, \{Kaustubh G.\} and Vishnugopi, \{Bairav S.\} and Callum Campbell and Vikalp Raj and Chonghang Zhao and Lu Ma and Jianming Bai and Feipeng Yang and Ruipeng Li and Mingyuan Ge and John Watt and Mukherjee, \{Partha P.\} and David Mitlin and \{Karen Chen-Wiegart\}, \{Yu chen\}",

note = "Publisher Copyright: {\textcopyright} 2024 Wiley-VCH GmbH.",

year = "2025",

month = feb,

day = "17",

doi = "10.1002/anie.202412550",

language = "English",

volume = "64",

journal = "Angewandte Chemie - International Edition",

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Lo, CA, Wang, Y, Kankanallu, VR, Singla, A, Yen, D, Zheng, X, Naik, KG, Vishnugopi, BS, Campbell, C, Raj, V, Zhao, C, Ma, L, Bai, J, Yang, F, Li, R, Ge, M, Watt, J, Mukherjee, PP, Mitlin, D & Karen Chen-Wiegart, YC 2025, 'Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure', Angewandte Chemie - International Edition, vol. 64, no. 8, e202412550. https://doi.org/10.1002/anie.202412550

TY - JOUR

T1 - Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure

AU - Lo, Chang An

AU - Wang, Yixian

AU - Kankanallu, Varun R.

AU - Singla, Aditya

AU - Yen, Dean

AU - Zheng, Xiaoyin

AU - Naik, Kaustubh G.

AU - Vishnugopi, Bairav S.

AU - Campbell, Callum

AU - Raj, Vikalp

AU - Zhao, Chonghang

AU - Ma, Lu

AU - Bai, Jianming

AU - Yang, Feipeng

AU - Li, Ruipeng

AU - Ge, Mingyuan

AU - Watt, John

AU - Mukherjee, Partha P.

AU - Mitlin, David

AU - Karen Chen-Wiegart, Yu chen

PY - 2025/2/17

Y1 - 2025/2/17

N2 - This study examines how current collector support chemistry (sodiophilic intermetallic Na2Te vs. sodiophobic baseline Cu) and electrodeposition rate affect microstructure of sodium metal and its solid electrolyte interphase (SEI). Capacity and current (6 mAh cm−2, 0.5–3 mA cm−2) representative of commercially relevant mass loading in anode-free sodium metal battery (AF-SMBs) are analyzed. Synchrotron X-ray nanotomography and grazing-incidence wide-angle X-ray scattering (GIWAXS) are combined with cryogenic ion beam (cryo-FIB) microscopy. Highlighted are major differences in film morphology, internal porosity, and crystallographic preferred orientation e.g. (110) vs. (100) and (211) with support and deposition rate. Within the SEI, sodium fluoride (NaF) is more prevalent with Te−Cu versus sodium hydride (NaH) and sodium hydroxide (NaOH) with baseline Cu. Due to competitive grain growth the preferred orientation of sodium crystallites depends on film thickness. Mesoscale modeling delineates the role of SEI (ionic conductivity, morphology) on electrodeposit growth and onset of electrochemical instability.

AB - This study examines how current collector support chemistry (sodiophilic intermetallic Na2Te vs. sodiophobic baseline Cu) and electrodeposition rate affect microstructure of sodium metal and its solid electrolyte interphase (SEI). Capacity and current (6 mAh cm−2, 0.5–3 mA cm−2) representative of commercially relevant mass loading in anode-free sodium metal battery (AF-SMBs) are analyzed. Synchrotron X-ray nanotomography and grazing-incidence wide-angle X-ray scattering (GIWAXS) are combined with cryogenic ion beam (cryo-FIB) microscopy. Highlighted are major differences in film morphology, internal porosity, and crystallographic preferred orientation e.g. (110) vs. (100) and (211) with support and deposition rate. Within the SEI, sodium fluoride (NaF) is more prevalent with Te−Cu versus sodium hydride (NaH) and sodium hydroxide (NaOH) with baseline Cu. Due to competitive grain growth the preferred orientation of sodium crystallites depends on film thickness. Mesoscale modeling delineates the role of SEI (ionic conductivity, morphology) on electrodeposit growth and onset of electrochemical instability.

KW - fiber texture

KW - film growth

KW - sodium metal anode

KW - sodium metal battery

KW - solid electrolyte interphase (SEI)

UR - https://www.scopus.com/pages/publications/85208592188

U2 - 10.1002/anie.202412550

DO - 10.1002/anie.202412550

M3 - Article

C2 - 39278827

AN - SCOPUS:85208592188

SN - 1433-7851

VL - 64

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 8

M1 - e202412550

ER -

Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure

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Funding

Keywords

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