Wrinkled Graphene Cages as Hosts for High-Capacity Li Metal Anodes Shown by Cryogenic Electron Microscopy
Top Cited Papers
- 31 January 2019
- journal article
- research article
- Published by American Chemical Society (ACS) in Nano Letters
- Vol. 19 (2), 1326-1335
- https://doi.org/10.1021/acs.nanolett.8b04906
Abstract
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 similar to 98.0% was achieved under 0.5 mA/cm(2) and 1-10 mAh/cm(2) in commercial carbonate electrolytes, and a CE of 99.1% was realized with high-concentration electrolytes under 0.5 mA/cm(2) and 3 mAh/cm(2). Full cells using WGC electrodes with prestored Li paired with Li iron phosphate showed greatly improved cycle lifetime. With 10 mAh/cm(2) Li metal deposition, the WGC/Li composite anode was able to provide a high specific capacity of similar to 2785 mAh/g. 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.Funding Information
- Intelligence Community Postdoctoral Research Fellowship Program
- Vehicle Technologies Program
This publication has 51 references indexed in Scilit:
- High rate and stable cycling of lithium metal anodeNature Communications, 2015
- Ultrathin Two-Dimensional Atomic Crystals as Stable Interfacial Layer for Improvement of Lithium Metal AnodeNano Letters, 2014
- Stable lithium electrodeposition in liquid and nanoporous solid electrolytesNature Materials, 2014
- Interconnected hollow carbon nanospheres for stable lithium metal anodesNature Nanotechnology, 2014
- A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteriesNature Communications, 2013
- Opportunities and challenges for a sustainable energy futureNature, 2012
- Synthesis of Multilayer Graphene Balls by Carbon Segregation from Nickel NanoparticlesACS Nano, 2012
- Microstructural Characterization of Lithiated GraphiteJournal of the Electrochemical Society, 1996
- Formation of Lithium-Graphite Intercalation Compounds in Nonaqueous Electrolytes and Their Application as a Negative Electrode for a Lithium Ion (Shuttlecock) CellJournal of the Electrochemical Society, 1993
- Suppression of staging in lithium-intercalated carbon by disorder in the hostPhysical Review B, 1990