Title: Direct electrochemical generation of supercooled sulfur microdroplets well below their melting temperature

Abstract

Supercooled liquid sulfur microdroplets were directly generated from polysulfide electrochemical oxidation on various metal-containing electrodes. The sulfur droplets remain liquid at 155 °C below sulfur’s melting point (T_m= 115 °C), with fractional supercooling change (T_m–T_sc)/T_mlarger 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. Furthermore, 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.

Authors:

Liu, Nian  ^[1];

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Zhou, Guangmin ^[2]; Yang, Ankun ^[2]; Yu, Xiaoyun ^[2]; Shi, Feifei ^[2]; Sun, Jie ^[2]; Zhang, Jinsong ^[2]; Liu, Bofei ^[2]; Wu, Chun-Lan ^[2]; Tao, Xinyong ^[3]; Sun, Yongming ^[2]; Cui, Yi ^[4]; Chu, Steven ^[5]

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+ Show Author Affiliations

1. Department of Physics, Stanford University, Stanford, CA 94305,, Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305,, School of Chemical &, Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332,
2. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305,
3. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305,, College of Materials Science and Engineering, Zhejiang University of Technology, 310014 Hangzhou, China,
4. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305,, SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, CA 94025,
5. Department of Physics, Stanford University, Stanford, CA 94305,, Department of Molecular and Cellular Physiology, Stanford University, Stanford, CA 94305

Publication Date:

2019-01-02

Research Org.:

SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:

USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

OSTI Identifier:

1489413

Alternate Identifier(s):

OSTI ID: 1493456

Grant/Contract Number:  

Battery Materials Research (BMR) Program; Battery500 Consortium; AC02-76SF00515

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 3; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; supercooled liquids; liquid sulfur droplets; in situ optical microscopy; Li-S; batteries; crystallization