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Title: Ultrahigh–current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF 3 framework

Abstract

Lithium (Li) metal is the ultimate solution for next-generation high–energy density batteries but is plagued from commercialization by infinite relative volume change, low Coulombic efficiency due to side reactions, and safety issues caused by dendrite growth. These hazardous issues are further aggravated under high current densities needed by the increasing demand for fast charging/discharging. We report a one-step fabricated Li/Al 4Li 9-LiF nanocomposite (LAFN) through an “overlithiation” process of a mesoporous AlF 3 framework, which can simultaneously mitigate the abovementioned problems. Reaction-produced Al 4Li 9-LiF nanoparticles serve as the ideal skeleton for Li metal infusion, helping to achieve a near-zero volume change during stripping/plating and suppressed dendrite growth. As a result, the LAFN electrode is capable of working properly under an ultrahigh current density of 20 mA cm –2 in symmetric cells and manifests highly improved rate capability with increased Coulombic efficiency in full cells. Here, the simple fabrication process and its remarkable electrochemical performances enable LAFN to be a promising anode candidate for next-generation lithium metal batteries.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1389865
Grant/Contract Number:
AC02-76SF00515; award343944; BMR program and Battery 500 Consortium
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wang, Hansen, Lin, Dingchang, Liu, Yayuan, Li, Yuzhang, and Cui, Yi. Ultrahigh–current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF3 framework. United States: N. p., 2017. Web. doi:10.1126/sciadv.1701301.
Wang, Hansen, Lin, Dingchang, Liu, Yayuan, Li, Yuzhang, & Cui, Yi. Ultrahigh–current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF3 framework. United States. doi:10.1126/sciadv.1701301.
Wang, Hansen, Lin, Dingchang, Liu, Yayuan, Li, Yuzhang, and Cui, Yi. 2017. "Ultrahigh–current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF3 framework". United States. doi:10.1126/sciadv.1701301. https://www.osti.gov/servlets/purl/1389865.
@article{osti_1389865,
title = {Ultrahigh–current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF3 framework},
author = {Wang, Hansen and Lin, Dingchang and Liu, Yayuan and Li, Yuzhang and Cui, Yi},
abstractNote = {Lithium (Li) metal is the ultimate solution for next-generation high–energy density batteries but is plagued from commercialization by infinite relative volume change, low Coulombic efficiency due to side reactions, and safety issues caused by dendrite growth. These hazardous issues are further aggravated under high current densities needed by the increasing demand for fast charging/discharging. We report a one-step fabricated Li/Al4Li9-LiF nanocomposite (LAFN) through an “overlithiation” process of a mesoporous AlF3 framework, which can simultaneously mitigate the abovementioned problems. Reaction-produced Al4Li9-LiF nanoparticles serve as the ideal skeleton for Li metal infusion, helping to achieve a near-zero volume change during stripping/plating and suppressed dendrite growth. As a result, the LAFN electrode is capable of working properly under an ultrahigh current density of 20 mA cm–2 in symmetric cells and manifests highly improved rate capability with increased Coulombic efficiency in full cells. Here, the simple fabrication process and its remarkable electrochemical performances enable LAFN to be a promising anode candidate for next-generation lithium metal batteries.},
doi = {10.1126/sciadv.1701301},
journal = {Science Advances},
number = 9,
volume = 3,
place = {United States},
year = 2017,
month = 9
}

Journal Article:
Free Publicly Available Full Text
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  • We report that lithium (Li) metal batteries (LMBs) have recently attracted extensive interest in the energy-storage field after silence from the public view for several decades. However, many challenges still need to be overcome before their practical application, especially those that are related to the interfacial instability of Li metal anodes. Here, we reveal for the first time that the thickness of the degradation layer on the metallic Li anode surface shows a linear relationship with Li areal capacity utilization up to 4.0 mAh cm -2 in a practical LMB system. The increase in Li capacity utilization in each cyclemore » causes variations in the morphology and composition of the degradation layer on the Li anode. Under high Li capacity utilization, the current density for charge (i.e., Li deposition) is identified to be a key factor controlling the corrosion of the Li metal anode. Lastly, these fundamental findings provide new perspectives for the development of rechargeable LMBs.« less
  • Lithium (Li) metal batteries (LMBs) are regarded as the most promising power sources for electric vehicles. Besides the Li dendrite growth and low Li Coulombic efficiency, how to well match Li metal anode with a high loading (normally over 3.0 mAh cm-2) cathode is another key challenge to achieve the real high energy density battery. In this work, we systematically investigate the effects of the Li metal capacity usage in each cycle, manipulated by varying the cathode areal loading, on the stability of Li metal anode and the cycling performance of LMBs using the LiNi1/3Mn1/3Co1/3O2 (NMC) cathode and an additive-containingmore » dual-salt/carbonate-solvent electrolyte. It is demonstrated that the Li||NMC cells show decent long-term cycling performance even with NMC areal capacity loading up to ca. 4.0 mAh cm-2 and at a charge current density of 1.0 mA cm-2. The increase of the Li capacity usage in each cycle causes variation in the components of the solid electrolyte interphase (SEI) layer on Li metal anode and generates more ionic conductive species from this electrolyte. Further study reveals for the first time that the degradation of Li metal anode and the thickness of SEI layer on Li anode show linear relationship with the areal capacity of NMC cathode. Meanwhile, the expansion rate of consumed Li and the ratio of SEI thickness to NMC areal loading are kept almost the same value with increasing cathode loading, respectively. These fundamental findings provide new perspectives on the rational evaluation of Li metal anode stability for the development of rechargeable LMBs.« less
  • A collaboration has been established between the All-Russian Scientific Research Institute of Experimental Physics (VNIIEF) and the Los Alamos National Laboratory (LANL). In 1992, when emerging governmental policy in the US and Russia began to encourage lab-to-lab interactions, the two institutes quickly recognized a common interest in the technology and applications of magnetic flux compression, the technique for converting the chemical energy released by high-explosives into intense electrical pulses and intensely concentrated magnetic energy. In a period of just over three years, the two institutes have performed more than fifteen joint experiments covering research areas ranging from basic pulsed powermore » technology to solid-state physics to controlled thermonuclear fusion. Using magnetic flux compression generators, electrical currents ranging from 20 to 100 MA were delivered to loads of interest in high-energy-density physics. A 20-MA pulse was delivered to an imploding liner load with a 10--90% rise time of 0.7 {micro}s. A new, high-energy concept for soft X-ray generation was tested at 65 MA. More than 20 MJ of implosion kinetic energy was delivered to a condensed matter imploding liner by a 100-MA current pulse. Magnetic flux compressors were used to determine the upper critical field of a high-temperature superconductor and to create pressure high enough that the transition from single particle behavior to quasimolecular behavior was observed in solid argon. A major step was taken toward the achievement of controlled thermonuclear fusion by a relatively unexplored approach known in Russia as MAGO (MAGnitnoye Obzhatiye, or magnetic compression) and in the US as MTF (Magnetized Target Fusion). Many of the characteristics of a target plasma that produced 10{sup 13} fusion neutrons have been evaluated. Computational models of the target plasma suggest that the plasma is suitable for subsequent compression to fusion conditions by an imploding pusher.« less