Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes
Abstract
Dendrites and dead lithium formation over prolonged cycling have long been challenges that hinder the safe implementation of metallic Li anodes. In this study, we employ polymer-stabilized liquid metal nanoparticles (LM-P NPs) of eutectic gallium indium (EGaIn) to create uniform Li nucleation sites enabling homogeneous lithium electrodeposition. Block copolymers of poly(ethylene oxide) and poly(acrylic acid) (PEO-b-PAA) were grafted onto the EGaIn surface, forming stabilized, well-dispersed NPs. Using a scalable spray coating approach, LM-P NPs were fabricated on copper current collectors, providing lithiophilic PEO sites and interactive carboxyl groups to guide Li deposition. The Li-EGaIn alloying process greatly reduced the Li+ diffusion barrier, enabling fast Li transport through the coating layer, resulting in decreased nucleation overpotential. Therefore, about five times lower Li nucleation overpotential was obtained on the LM-P modified Cu with an optimal composition of the polymers than the bare Cu substrates. DFT computations was used to reveal the binding properties between the LM-P layer and Li. Due to the regulated Li plating/stripping process, as-obtained 30 μm Li anodes paired with LiNi0.8Co0.1Mn0.1O2 (NCM811) with a negative/positive electrode capacity (N/P) ratio ~ 10 exhibited stable cycling performance at 0.5C for over 250 cycles, with an average Coulombic efficiency of 99.55%. Ultrathinmore »
- Authors:
-
[1];
[1];
[1];
[2];
[2];
[1];
[1]
- Carnegie Mellon Univ., Pittsburgh, PA (United States)
- Univ. of Pittsburgh, PA (United States)
- Publication Date:
- Research Org.:
- Univ. of Pittsburgh, PA (United States)
- Sponsoring Org.:
- USDOE; National Science Foundation (NSF); Carnegie Mellon University
- OSTI Identifier:
- 1869217
- Grant/Contract Number:
- FG02-07ER46430; 1501324; 2202747; MCF677785
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Energy Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 3; Journal ID: ISSN 2574-0962
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lithium metal anode; eutectic alloys; block copolymers; ATRP; EGaln; cu current collector; liquid metal
Citation Formats
Liu, Tong, Wu, Xinsheng, Zhu, Shang, Lorandi, Francesca, Ni, Longchang, Li, Sipei, Sun, Mingkang, Bloom, Brian P., Waldeck, David H., Viswanathan, Venkatasubramanian, Whitacre, Jay F., and Matyjaszewski, Krzysztof. Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes. United States: N. p., 2022.
Web. doi:10.1021/acsaem.1c04106.
Liu, Tong, Wu, Xinsheng, Zhu, Shang, Lorandi, Francesca, Ni, Longchang, Li, Sipei, Sun, Mingkang, Bloom, Brian P., Waldeck, David H., Viswanathan, Venkatasubramanian, Whitacre, Jay F., & Matyjaszewski, Krzysztof. Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes. United States. https://doi.org/10.1021/acsaem.1c04106
Liu, Tong, Wu, Xinsheng, Zhu, Shang, Lorandi, Francesca, Ni, Longchang, Li, Sipei, Sun, Mingkang, Bloom, Brian P., Waldeck, David H., Viswanathan, Venkatasubramanian, Whitacre, Jay F., and Matyjaszewski, Krzysztof. Mon .
"Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes". United States. https://doi.org/10.1021/acsaem.1c04106. https://www.osti.gov/servlets/purl/1869217.
@article{osti_1869217,
title = {Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes},
author = {Liu, Tong and Wu, Xinsheng and Zhu, Shang and Lorandi, Francesca and Ni, Longchang and Li, Sipei and Sun, Mingkang and Bloom, Brian P. and Waldeck, David H. and Viswanathan, Venkatasubramanian and Whitacre, Jay F. and Matyjaszewski, Krzysztof},
abstractNote = {Dendrites and dead lithium formation over prolonged cycling have long been challenges that hinder the safe implementation of metallic Li anodes. In this study, we employ polymer-stabilized liquid metal nanoparticles (LM-P NPs) of eutectic gallium indium (EGaIn) to create uniform Li nucleation sites enabling homogeneous lithium electrodeposition. Block copolymers of poly(ethylene oxide) and poly(acrylic acid) (PEO-b-PAA) were grafted onto the EGaIn surface, forming stabilized, well-dispersed NPs. Using a scalable spray coating approach, LM-P NPs were fabricated on copper current collectors, providing lithiophilic PEO sites and interactive carboxyl groups to guide Li deposition. The Li-EGaIn alloying process greatly reduced the Li+ diffusion barrier, enabling fast Li transport through the coating layer, resulting in decreased nucleation overpotential. Therefore, about five times lower Li nucleation overpotential was obtained on the LM-P modified Cu with an optimal composition of the polymers than the bare Cu substrates. DFT computations was used to reveal the binding properties between the LM-P layer and Li. Due to the regulated Li plating/stripping process, as-obtained 30 μm Li anodes paired with LiNi0.8Co0.1Mn0.1O2 (NCM811) with a negative/positive electrode capacity (N/P) ratio ~ 10 exhibited stable cycling performance at 0.5C for over 250 cycles, with an average Coulombic efficiency of 99.55%. Ultrathin Li (1 μm) anodes with an N/P ratio ~ 0.6 were also demonstrated in Li|LiFePO4 cells, which examined the stabilization of Li by LM-P NPs and monitored practical loadings of Li anodes that are close to anode-free systems.},
doi = {10.1021/acsaem.1c04106},
journal = {ACS Applied Energy Materials},
number = 3,
volume = 5,
place = {United States},
year = {Mon Mar 14 00:00:00 EDT 2022},
month = {Mon Mar 14 00:00:00 EDT 2022}
}
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