Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 30, Issue 32, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201910749
Keywords
2D materials; black phosphorous nanosheets; lithium batteries; polymer electrolytes
Categories
Funding
- NSF [CBET-1805938, 1625061]
- Robert A. Welch Foundation [F1599]
- National Science Foundation [CBET-17069698, DMR-1721512]
- US Army Research Laboratory [W911NF-16-2-0189]
- National Science Foundation Extreme Science and Engineering Discovery Environment (XSEDE) [TG-DMR180106]
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Despite significant interest toward solid-state electrolytes owing to their superior safety in comparison to liquid-based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high-power density batteries. Here, a novel quasi-solid Li+ ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm(-2) at room temperature. The cycling overpotential is dropped by 75% in comparison to BP-free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li+ ions around (trifluoromethanesulfonyl)imide (TFSI-) pairs and ethylene-oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li+ transport through the polymer host. Density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li+ ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid-state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long-life cycling.
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