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Title: In situ study of nucleation and growth dynamics of Au nanoparticles on MoS 2 nanoflakes

Two-dimensional (2D) substrates decorated with metal nanoparticles offer new opportunities to achieve high-performance catalytic behavior. However, little is known on how the substrates control the nucleation and growth processes of the nanoparticles. This paper presents the visualization of dynamic nucleation and growth processes of gold nanoparticles on ultrathin MoS 2 nanoflakes by in situ liquid-cell transmission electron microscopy (TEM). The galvanic displacement resulting in Au nuclei formation on MoS 2 was observed in real time inside the liquid cell. We found that the growth mechanism of Au particles on pristine MoS 2 is in between diffusion-limited and reaction-limited, possibly due to the presence of electrochemical Ostwald ripening. A larger size distribution and more orientation variation is observed for the Au particles along the MoS 2 edge than on the interior. Differing from pristine MoS 2, sulfur vacancies on MoS 2 induce Au particle diffusion and coalescence during the growth process. Density functional theory (DFT) calculations show that the size difference is because the exposed molybdenum atoms at the edge with dangling bonds can strongly interact with Au atoms, whereas sulfur atoms on the MoS 2 interior have no dangling bonds and weakly interact with gold atoms. In addition, S vacanciesmore » on MoS 2 generate strong nucleation centers that can promote diffusion and coalescence of Au nanoparticles. Furthermore, the present work provides key insights into the role of 2D materials in controlling the size and orientation of noble metal nanoparticles vital to the design of next generation catalysts.« less
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [1] ; ORCiD logo [1] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [1]
  1. Univ. of Illinois at Chicago, Chicago, IL (United States)
  2. Univ. of Illinois at Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of Pittsburgh, Pittsburgh, PA (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; 4J-30361
Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 10; Journal Issue: 33; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Science Foundation (NSF); University of Pittsburgh; USDOE
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 2D materials; DFT simulation; coalescence; electrochemical Ostwald ripening; galvanic displacement; in situ TEM; kinetic modeling; nucleation and growth
OSTI Identifier:
1472115
Alternate Identifier(s):
OSTI ID: 1464297

Song, Boao, He, Kun, Yuan, Yifei, Sharifi-Asl, Soroosh, Cheng, Meng, Lu, Jun, Saidi, Wissam A., and Shahbazian-Yassar, Reza. In situ study of nucleation and growth dynamics of Au nanoparticles on MoS2 nanoflakes. United States: N. p., Web. doi:10.1039/C8NR03519A.
Song, Boao, He, Kun, Yuan, Yifei, Sharifi-Asl, Soroosh, Cheng, Meng, Lu, Jun, Saidi, Wissam A., & Shahbazian-Yassar, Reza. In situ study of nucleation and growth dynamics of Au nanoparticles on MoS2 nanoflakes. United States. doi:10.1039/C8NR03519A.
Song, Boao, He, Kun, Yuan, Yifei, Sharifi-Asl, Soroosh, Cheng, Meng, Lu, Jun, Saidi, Wissam A., and Shahbazian-Yassar, Reza. 2018. "In situ study of nucleation and growth dynamics of Au nanoparticles on MoS2 nanoflakes". United States. doi:10.1039/C8NR03519A.
@article{osti_1472115,
title = {In situ study of nucleation and growth dynamics of Au nanoparticles on MoS2 nanoflakes},
author = {Song, Boao and He, Kun and Yuan, Yifei and Sharifi-Asl, Soroosh and Cheng, Meng and Lu, Jun and Saidi, Wissam A. and Shahbazian-Yassar, Reza},
abstractNote = {Two-dimensional (2D) substrates decorated with metal nanoparticles offer new opportunities to achieve high-performance catalytic behavior. However, little is known on how the substrates control the nucleation and growth processes of the nanoparticles. This paper presents the visualization of dynamic nucleation and growth processes of gold nanoparticles on ultrathin MoS2 nanoflakes by in situ liquid-cell transmission electron microscopy (TEM). The galvanic displacement resulting in Au nuclei formation on MoS2 was observed in real time inside the liquid cell. We found that the growth mechanism of Au particles on pristine MoS2 is in between diffusion-limited and reaction-limited, possibly due to the presence of electrochemical Ostwald ripening. A larger size distribution and more orientation variation is observed for the Au particles along the MoS2 edge than on the interior. Differing from pristine MoS2, sulfur vacancies on MoS2 induce Au particle diffusion and coalescence during the growth process. Density functional theory (DFT) calculations show that the size difference is because the exposed molybdenum atoms at the edge with dangling bonds can strongly interact with Au atoms, whereas sulfur atoms on the MoS2 interior have no dangling bonds and weakly interact with gold atoms. In addition, S vacancies on MoS2 generate strong nucleation centers that can promote diffusion and coalescence of Au nanoparticles. Furthermore, the present work provides key insights into the role of 2D materials in controlling the size and orientation of noble metal nanoparticles vital to the design of next generation catalysts.},
doi = {10.1039/C8NR03519A},
journal = {Nanoscale},
number = 33,
volume = 10,
place = {United States},
year = {2018},
month = {7}
}

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