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];
[4];
[3]
- School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
- The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30332, United States
- The Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
- School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States, The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30332, United States, School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
- 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)
- OSTI Identifier:
- 1476371
- Alternate Identifier(s):
- OSTI ID: 1508748
- Grant/Contract Number:
- FG02-05ER46237
- Resource Type:
- Published Article
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Name: Nano Letters 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. https://doi.org/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. https://doi.org/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},
number = 11,
volume = 18,
place = {United States},
year = {Fri Oct 05 00:00:00 EDT 2018},
month = {Fri Oct 05 00:00:00 EDT 2018}
}
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https://doi.org/10.1021/acs.nanolett.8b02953
https://doi.org/10.1021/acs.nanolett.8b02953
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Cited by: 31 works
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Figures / Tables:
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 »
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Works referencing / citing this record:
Self‐Assembly in Hopper‐Shaped Crystals
journal, December 2019
- Yang, Zeda; Zhang, Jingyi; Zhang, Lifu
- Advanced Functional Materials, Vol. 30, Issue 26
In Situ Transmission Electron Microscopy on Energy‐Related Catalysis
journal, December 2019
- Hwang, Sooyeon; Chen, Xiaobo; Zhou, Guangwen
- Advanced Energy Materials
In Situ Transmission Electron Microscopy Study of Nanocrystal Formation for Electrocatalysis
journal, October 2019
- Shi, Fenglei; Li, Fan; Ma, Yanling
- ChemNanoMat, Vol. 5, Issue 12
Tailoring the Size and Shape of Colloidal Noble Metal Nanocrystals as a Valuable Tool in Catalysis
journal, April 2019
- Navlani-García, Miriam; Salinas-Torres, David; Mori, Kohsuke
- Catalysis Surveys from Asia, Vol. 23, Issue 3
Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.