Wrinkled Graphene Cages as Hosts for High-Capacity Li Metal Anodes Shown by Cryogenic Electron Microscopy

Journal Article · Thu Jan 24 00:00:00 EST 2019 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.8b04906· OSTI ID:1507152

Wang, Hansen ^[1]; Li, Yuzhang ^[1]; Li, Yanbin ^[1]; Liu, Yayuan ^[1]; Lin, Dingchang ^[1]; Zhu, Cheng ^[1]; Chen, Guangxu ^[1]; Yang, Ankun ^[1]; Yan, Kai ^[1]; Chen, Hao ^[1]; Zhu, Yangying ^[1]; Li, Jun ^[1]; Xie, Jin ^[1]; Xu, Jinwei ^[1]; Zhang, Zewen ^[1]; Vilá, Rafael ^[1]; Pei, Allen ^[1]; Wang, Kecheng ^[1]; Cui, Yi ^[2]

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1. Stanford Univ., Stanford, CA (United States)
2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Lithium (Li) metal has long been considered the “holy grail” of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection. At low areal capacities, Li metal is preferentially deposited inside the graphene cage. Cryogenic electron microscopy characterization shows that a uniform and stable SEI forms on the WGC surface that can shield the Li metal from direct exposure to electrolyte. With increased areal capacities, Li metal is plated densely and homogeneously into the outer pore spaces between graphene cages with no dendrite growth or volume change. As a result, a high Coulombic efficiency (CE) of ~98.0% was achieved under 0.5 mA/cm² and 1–10 mAh/cm² in commercial carbonate electrolytes, and a CE of 99.1% was realized with high-concentration electrolytes under 0.5 mA/cm² and 3 mAh/cm². Full cells using WGC electrodes with prestored Li paired with Li iron phosphate showed greatly improved cycle lifetime. With 10 mAh/cm² Li metal deposition, the WGC/Li composite anode was able to provide a high specific capacity of ~2785 mAh/g. Furthermore, with its roll-to-roll compatible fabrication procedure, WGC serves as a highly promising material for the practical realization of Li metal anodes in next-generation high energy density secondary batteries.

• Research Organization: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
• Grant/Contract Number: AC02-76SF00515
• OSTI ID: 1507152
• Journal Information: Nano Letters, Journal Name: Nano Letters Journal Issue: 2 Vol. 19; ISSN 1530-6984
• Publisher: American Chemical Society
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
Coulombic efficiency
Li metal anode
cryo-EM
wrinkled graphene cage