Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 3, Pages 765-770Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1817286116
Keywords
supercooled liquids; liquid sulfur droplets; in situ optical microscopy; Li-S batteries; crystallization
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Funding
- Moore Foundation
- Stanford University
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy under the Battery Materials Research Program
- Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering [DE-AC02-76SF00515]
- Battery500 Consortium
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Supercooled liquid sulfur microdroplets were directly generated from polysulfide electrochemical oxidation on various metal-containing electrodes. The sulfur droplets remain liquid at 155 degrees C below sulfur's melting point (T-m = 115 degrees C), with fractional supercooling change (T-m - T-sc)/T-m larger than 0.40. In operando light microscopy captured the rapid merging and shape relaxation of sulfur droplets, indicating their liquid nature. Micropatterned electrode and electrochemical current allow precise control of the location and size of supercooled microdroplets, respectively. Using this platform, we initiated and observed the rapid solidification of supercooled sulfur microdroplets upon crystalline sulfur touching, which confirms supercooled sulfur's metastability at room temperature. In addition, the formation of liquid sulfur in electrochemical cell enriches lithium-sulfur-electrolyte phase diagram and potentially may create new opportunities for high-energy Li-S batteries.
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