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Title: Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets

Abstract

Synthesizing concave-structured nanoparticles (NP) with high-index surfaces offers a viable method to significantly enhance the catalytic activity of NPs. Current approaches for fabricating concave NPs, however, are limited. Exploring novel synthesis methods requires a thorough understanding of the competing mechanisms that contribute to the evolution of surface structures during NP growth. Here, by tracking the evolution of Pd nanocubes into concave NPs at atomic scale using in situ liquid cell transmission electron microscopy, our study reveals that concave-structured Pd NPs can be formed by the cointroduction of surface capping agents and halogen ions. These two chemicals jointly create a new surface energy landscape of Pd NPs, leading to the morphological transformation. In particular, Pd atoms dissociate from the {100} surfaces with the aid of Cl -ions and preferentially redeposit to the corners and edges of the nanocubes when the capping agent polyvinylpyrrolidone is introduced, resulting in the formation of concave Pd nanocubes with distinctive high-index facets. Our work not only demonstrates a potential route for synthesizing NPs with well-defined high-index facets but also reveals the detailed atomic-scale kinetics during their formation, providing insight for future predictive synthesis.

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [5];  [2]; ORCiD logo [6];  [7]; ORCiD logo [5]
  1. Univ. of California, Irvine, CA (United States). Dept. of Materials Science and Engineering
  2. Univ. of California, Irvine, CA (United States). Dept. of Physics and Astronomy
  3. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
  4. Georgia Inst. of Technology, Atlanta, GA (United States). Wallace H. Coulter Dept. of Biomedical Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  6. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry, Wallace H. Coulter Dept. of Biomedical Engineering, and School of Chemical and Biomolecular Engineering
  7. Univ. of California, Irvine, CA (United States). Dept. of Materials Science and Engineering; Univ. of California, Irvine, CA (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1476371
Alternate Identifier(s):
OSTI ID: 1508748
Grant/Contract Number:  
FG02-05ER46237
Resource Type:
Journal Article: Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 11; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst; high index; in situ transmission electron microscopy; Liquid cell; nanoparticle

Citation Formats

Gao, Wenpei, Hou, Yusheng, Hood, Zachary D., Wang, Xue, More, Karren, Wu, Ruqian, Xia, Younan, Pan, Xiaoqing, and Chi, Miaofang. Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b02953.
Gao, Wenpei, Hou, Yusheng, Hood, Zachary D., Wang, Xue, More, Karren, Wu, Ruqian, Xia, Younan, Pan, Xiaoqing, & Chi, Miaofang. Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets. United States. doi:10.1021/acs.nanolett.8b02953.
Gao, Wenpei, Hou, Yusheng, Hood, Zachary D., Wang, Xue, More, Karren, Wu, Ruqian, Xia, Younan, Pan, Xiaoqing, and Chi, Miaofang. Fri . "Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets". United States. doi:10.1021/acs.nanolett.8b02953.
@article{osti_1476371,
title = {Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets},
author = {Gao, Wenpei and Hou, Yusheng and Hood, Zachary D. and Wang, Xue and More, Karren and Wu, Ruqian and Xia, Younan and Pan, Xiaoqing and Chi, Miaofang},
abstractNote = {Synthesizing concave-structured nanoparticles (NP) with high-index surfaces offers a viable method to significantly enhance the catalytic activity of NPs. Current approaches for fabricating concave NPs, however, are limited. Exploring novel synthesis methods requires a thorough understanding of the competing mechanisms that contribute to the evolution of surface structures during NP growth. Here, by tracking the evolution of Pd nanocubes into concave NPs at atomic scale using in situ liquid cell transmission electron microscopy, our study reveals that concave-structured Pd NPs can be formed by the cointroduction of surface capping agents and halogen ions. These two chemicals jointly create a new surface energy landscape of Pd NPs, leading to the morphological transformation. In particular, Pd atoms dissociate from the {100} surfaces with the aid of Cl-ions and preferentially redeposit to the corners and edges of the nanocubes when the capping agent polyvinylpyrrolidone is introduced, resulting in the formation of concave Pd nanocubes with distinctive high-index facets. Our work not only demonstrates a potential route for synthesizing NPs with well-defined high-index facets but also reveals the detailed atomic-scale kinetics during their formation, providing insight for future predictive synthesis.},
doi = {10.1021/acs.nanolett.8b02953},
journal = {Nano Letters},
issn = {1530-6984},
number = 11,
volume = 18,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acs.nanolett.8b02953

Citation Metrics:
Cited by: 4 works
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Figures / Tables:

Figure 1 Figure 1: Diffusion of Pd atoms from center of sides/facets to corners on the surfaces of Pd nanocube. (a) Sequential BF-TEM images of a Pd nanocube showing the morphological change with time during electron irradiation in liquid cell. The particle shape became concave as highlighted by the arrows. (b−d) Schematicsmore » show the formation of concave nanocubes at different times during electron beam irradiation (0−150 s).« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.