ABSTRACT It has recently been shown that sulfur, a solid material in its elementary form S8, can stay in a supercooled state as liquid sulfur in an electrochemical cell. We establish that

this newly discovered state could have implications for lithium–sulfur batteries. Here, through in situ studies of electrochemical sulfur generation, we show that liquid (supercooled) and

solid elementary sulfur possess very different areal capacities over the same charging period. To control the physical state of sulfur, we studied its growth on two-dimensional layered

materials. We found that on the basal plane, only liquid sulfur accumulates; by contrast, at the edge sites, liquid sulfur accumulates if the thickness of the two-dimensional material is

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* Log in * Learn about institutional subscriptions * Read our FAQs * Contact customer support SIMILAR CONTENT BEING VIEWED BY OTHERS HIGH-ENTROPY SULFOSELENIDE AS NEGATIVE ELECTRODES WITH

FAST KINETICS AND HIGH STABILITY FOR SODIUM-ION BATTERIES Article Open access 30 April 2025 A NEAR DIMENSIONALLY INVARIABLE HIGH-CAPACITY POSITIVE ELECTRODE MATERIAL Article 12 December 2022

REALIZING HIGH-CAPACITY ALL-SOLID-STATE LITHIUM-SULFUR BATTERIES USING A LOW-DENSITY INORGANIC SOLID-STATE ELECTROLYTE Article Open access 05 April 2023 DATA AVAILABILITY The data that

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monolayer to bulk. _npj 2D Mater. Appl._ 2, 4106 (2018). Article  Google Scholar  Download references ACKNOWLEDGEMENTS We acknowledge support from the Department of Energy, Office of Basic

Energy Sciences, Division of Materials Science and Engineering under contract DE-AC02-76SF00515. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF) and Stanford

Nanofabrication Facilities (SNF), supported by the National Science Foundation under award ECCS-1542152. R.A.V. acknowledges support from the National Academy of Sciences Ford Foundation

Fellowship and the National Science Foundation Graduate Research Fellowship Program (NSF GRFP, grant number: DGE – 1656518). We acknowledge C. Su and J. Li from MIT for performing the DFT

calculations. A.Y. acknowledges D. Zakhidov for his assistance with polarized Raman measurements and Y. Ye, Z. Wang and R. Xu for helpful discussions. AUTHOR INFORMATION Author notes * Di

Chen Present address: The Future Laboratory, Tsinghua University, Beijing, China * These authors contributed equally: Ankun Yang, Guangmin Zhou. AUTHORS AND AFFILIATIONS * Department of

Materials Science and Engineering, Stanford University, Stanford, CA, USA Ankun Yang, Guangmin Zhou, Rafael A. Vilá, Allen Pei, Xiaoyun Yu, Xueli Zheng, Chun-Lan Wu, Bofei Liu, Hao Chen, Yan

Xu, Di Chen, Yanxi Li & Yi Cui * Department of Chemical Engineering, Stanford University, Stanford, CA, USA Xian Kong & Jian Qin * Department of Electrical Engineering, Stanford

University, Stanford, CA, USA Yecun Wu * Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA Sirine Fakra * Department of Applied Physics, Stanford University,

Stanford, CA, USA Harold Y. Hwang * Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA Harold Y. Hwang & Yi Cui * Department

of Physics, Stanford University, Stanford, CA, USA Steven Chu * Department of Molecular and Cellular Physiology, Stanford University, Stanford, CA, USA Steven Chu Authors * Ankun Yang View

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Google Scholar * Xiaoyun Yu View author publications You can also search for this author inPubMed Google Scholar * Xueli Zheng View author publications You can also search for this author

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author inPubMed Google Scholar * Hao Chen View author publications You can also search for this author inPubMed Google Scholar * Yan Xu View author publications You can also search for this

author inPubMed Google Scholar * Di Chen View author publications You can also search for this author inPubMed Google Scholar * Yanxi Li View author publications You can also search for this

author inPubMed Google Scholar * Sirine Fakra View author publications You can also search for this author inPubMed Google Scholar * Harold Y. Hwang View author publications You can also

search for this author inPubMed Google Scholar * Jian Qin View author publications You can also search for this author inPubMed Google Scholar * Steven Chu View author publications You can

also search for this author inPubMed Google Scholar * Yi Cui View author publications You can also search for this author inPubMed Google Scholar CONTRIBUTIONS A.Y. and Y.C. conceived and

designed the experiments. A.Y. and G.Z. carried out device fabrication, imaging and electrochemical measurements. X.K. and J.Q. performed MD simulations. R.A.V. performed TEM

characterizations. A.P. performed COMSOL simulations. X.Z. and S.F. performed in situ XAS measurements. Y.W., C.-L.W. and B.L. assisted in material preparation. X.Y., H.C., Y.X., D.C. and

Y.L. assisted in electrochemical measurements. H.Y.H., S.C. and Y.C. supervised the project and all authors contributed to data discussions. A.Y. and Y.C. analysed the data and wrote the

paper with input from all authors. CORRESPONDING AUTHOR Correspondence to Yi Cui. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing interests. ADDITIONAL INFORMATION

PEER REVIEW INFORMATION Nature Nanotechnology thanks Yuyan Shao, Guoxiu Wang and Reza Shahbazian-Yassar for their contribution to the peer review of this work. PUBLISHER’S NOTE Springer

Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations. SUPPLEMENTARY INFORMATION SUPPLEMENTARY INFORMATION Supplementary Figs. 1-21 and

Table 1. SUPPLEMENTARY VIDEO 1 Sulfur generation on MoS2 shows distinct growth behaviors on the basal plane and the edges. Specifically, liquid sulfur droplets were generated on the basal

plane of the MoS2 while solid sulfur crystal was generated on the edges of the MoS2 flake. Play speed is 3× of the actual speed. SUPPLEMENTARY VIDEO 2 Cryogenic electron microscopy (Cryo-EM)

Selected Area Electron Diffraction (SAED) of solid sulfur indicates its high crystallinity. The sample was tilted between -30° and 30°. Play speed is 5× of the actual speed. SUPPLEMENTARY

VIDEO 3 Liquid and solid sulfur generation on the edges of 2D flake. Liquid droplets were observed on the edges at the initial stage and quickly turned into solid by the emerging crystals

from the edges. Play speed is 5× of the actual speed. SUPPLEMENTARY VIDEO 4 Sulfur generation on monolayer MoS2. Liquid droplets were dynamically generated on monolayer MoS2 without

crystallization. The MoS2 flake in the middle was not connected to the Ti electrode, so no sulfur was generated. Play speed is 20× of the actual speed. SUPPLEMENTARY VIDEO 5 Liquid sulfur

generation on MoS2 window. The edges of the MoS2 flake were completely covered to suppress crystal growth. Play speed is 10× of the actual speed. SUPPLEMENTARY VIDEO 6 Solid sulfur

generation on MoS2 window. The edges of the MoS2 flake were partially left open to initiate crystal growth. Play speed is 10× of the actual speed. RIGHTS AND PERMISSIONS Reprints and

permissions ABOUT THIS ARTICLE CITE THIS ARTICLE Yang, A., Zhou, G., Kong, X. _et al._ Electrochemical generation of liquid and solid sulfur on two-dimensional layered materials with

distinct areal capacities. _Nat. Nanotechnol._ 15, 231–237 (2020). https://doi.org/10.1038/s41565-019-0624-6 Download citation * Received: 10 June 2019 * Accepted: 12 December 2019 *

Published: 27 January 2020 * Issue Date: March 2020 * DOI: https://doi.org/10.1038/s41565-019-0624-6 SHARE THIS ARTICLE Anyone you share the following link with will be able to read this

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