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Title: Reversible and selective ion intercalation through the top surface of few-layer MoS2

Abstract

Electrochemical intercalation of ions into the van der Waals gap of two-dimensional (2D) layered materials is a promising low-temperature synthesis strategy to tune their physical and chemical properties. It is widely believed that ions prefer intercalation into the van der Waals gap through the edges of the 2D flake, which generally causes wrinkling and distortion. Here we demonstrate that the ions can also intercalate through the top surface of few-layer MoS2 and this type of intercalation is more reversible and stable compared to the intercalation through the edges. Density functional theory calculations show that this intercalation is enabled by the existence of natural defects in exfoliated MoS2 flakes. Furthermore, we reveal that sealed-edge MoS2 allows intercalation of small alkali metal ions (e.g., Li+ and Na+) and rejects large ions (e.g., K+). Lastly, these findings imply potential applications in developing functional 2D-material-based devices with high tunability and ion selectivity.

Authors:
 [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [2];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [2];  [5];  [2]; ORCiD logo [3]; ORCiD logo [5]
+ Show Author Affiliations
  1. Stanford Univ., Stanford, CA (United States); Tsinghua Univ., Beijing (People's Republic of China)
  2. Stanford Univ., Stanford, CA (United States)
  3. Tsinghua Univ., Shenzhen (People's Republic of China)
  4. Tsinghua Univ., Beijing (People's Republic of China)
  5. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490649
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhang, Jinsong, Yang, Ankun, Wu, Xi, van de Groep, Jorik, Tang, Peizhe, Li, Shaorui, Liu, Bofei, Shi, Feifei, Wan, Jiayu, Li, Qitong, Sun, Yongming, Lu, Zhiyi, Zheng, Xueli, Zhou, Guangmin, Wu, Chun -Lan, Zhang, Shou -Cheng, Brongersma, Mark L., Li, Jia, and Cui, Yi. Reversible and selective ion intercalation through the top surface of few-layer MoS2. United States: N. p., 2018. Web. doi:10.1038/s41467-018-07710-z.
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Zhang, Jinsong, Yang, Ankun, Wu, Xi, van de Groep, Jorik, Tang, Peizhe, Li, Shaorui, Liu, Bofei, Shi, Feifei, Wan, Jiayu, Li, Qitong, Sun, Yongming, Lu, Zhiyi, Zheng, Xueli, Zhou, Guangmin, Wu, Chun -Lan, Zhang, Shou -Cheng, Brongersma, Mark L., Li, Jia, & Cui, Yi. Reversible and selective ion intercalation through the top surface of few-layer MoS2. United States. https://doi.org/10.1038/s41467-018-07710-z
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Zhang, Jinsong, Yang, Ankun, Wu, Xi, van de Groep, Jorik, Tang, Peizhe, Li, Shaorui, Liu, Bofei, Shi, Feifei, Wan, Jiayu, Li, Qitong, Sun, Yongming, Lu, Zhiyi, Zheng, Xueli, Zhou, Guangmin, Wu, Chun -Lan, Zhang, Shou -Cheng, Brongersma, Mark L., Li, Jia, and Cui, Yi. Tue . "Reversible and selective ion intercalation through the top surface of few-layer MoS2". United States. https://doi.org/10.1038/s41467-018-07710-z. https://www.osti.gov/servlets/purl/1490649.
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@article{osti_1490649,
title = {Reversible and selective ion intercalation through the top surface of few-layer MoS2},
author = {Zhang, Jinsong and Yang, Ankun and Wu, Xi and van de Groep, Jorik and Tang, Peizhe and Li, Shaorui and Liu, Bofei and Shi, Feifei and Wan, Jiayu and Li, Qitong and Sun, Yongming and Lu, Zhiyi and Zheng, Xueli and Zhou, Guangmin and Wu, Chun -Lan and Zhang, Shou -Cheng and Brongersma, Mark L. and Li, Jia and Cui, Yi},
abstractNote = {Electrochemical intercalation of ions into the van der Waals gap of two-dimensional (2D) layered materials is a promising low-temperature synthesis strategy to tune their physical and chemical properties. It is widely believed that ions prefer intercalation into the van der Waals gap through the edges of the 2D flake, which generally causes wrinkling and distortion. Here we demonstrate that the ions can also intercalate through the top surface of few-layer MoS2 and this type of intercalation is more reversible and stable compared to the intercalation through the edges. Density functional theory calculations show that this intercalation is enabled by the existence of natural defects in exfoliated MoS2 flakes. Furthermore, we reveal that sealed-edge MoS2 allows intercalation of small alkali metal ions (e.g., Li+ and Na+) and rejects large ions (e.g., K+). Lastly, these findings imply potential applications in developing functional 2D-material-based devices with high tunability and ion selectivity.},
doi = {10.1038/s41467-018-07710-z},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Tue Dec 11 00:00:00 EST 2018},
month = {Tue Dec 11 00:00:00 EST 2018}
}
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https://doi.org/10.1038/s41467-018-07710-z
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Figures / Tables:

Fig. 1 Fig. 1: Schematic representation of the material and of the experimental setup. a Li+, Na+, and K+ intercalation into MoS2 through top and edge channels. b An electrochemical cell used to perform intercalation of Li+, Na+, and K+ into MoS2 with sealed and open edge. c-d AFM and optical microscopymore » images of typical MoS2 flakes designed for sealed edge measurement and open edge measurement, respectively. The thicknesses are typically < 10 nm, measured across three edges indicated by the dash lines. Scale bars in c and d, 5 µm« less
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