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Title: Tailoring Surface Opening of Hollow Nanocubes and Their Application as Nanocargo Carriers

Abstract

Hollow nanoparticles (NPs) are of broad interest for biomedical, optical, and catalytic applications due to their unique geometry-related physicochemical properties. The ability to engineer hollow structures with surface openings is particularly attractive since emergent properties are promised by the design of shell porosity and encapsulation of guest materials. However, it still remains challenging to precisely control the opening of the hollow structure, in terms of shape, size, and location. Here in this paper, we report a facile one-step strategy to synthesize a hollow nanostructure with well-defined cubic-shape openings at the corners, by regulating nanoscale galvanic replacement processes with specific surface-capping agents. The final product is a single-crystalline AuAg alloy which morphologically features three “belts” orthogonally wrapping around a virtual cube, denoted by nanowrapper. We demonstrate a structural tunability of our synthetic method for tailoring nanowrapper and the corresponding tuning of its plasmonic band from the visible to near-infrared (NIR) range. Advanced electron tomography techniques provide unambiguous three-dimensional (3D) visualizations to reveal an unconventional transformation pathway of sharp-cornered Ag nanocube to nanowrapper and correlate its structure with measured and computed spectroscopic properties. Importantly, we find that the surfactant, i.e., cetylpyridinium chloride (CPC), is crucial for the openings to be localized atmore » the corners of the hollow cube and be tailored to a cubic shape in our one-step process. Furthermore, such a well-defined hollow architecture also allows a guest nano-object to be contained within, while the large openings at corners enable controlled loading/release of nanoscale cargo, a DNA-coated particle, using change of ionic conditions. This work expands our understanding of surface engineering in nanoscale galvanic replacement reactions and opens new ways toward the shape control of hollow NPs.« less

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2];  [3]; ORCiD logo [4];  [5]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN), Energy & Photon Sciences Directorate
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN), Energy & Photon Sciences Directorate
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II), Energy & Photon Sciences Directorate
  4. Chinese Academy of Sciences (CAS), Hefei (China). Key Lab. of Materials Physics, Anhui Key Lab. of Nanomaterials and Nanotechnology, Inst.of Solid State Physics; Univ. of Science and Technology of China, Hefei (China). Dept. of Materials Science and Engineering
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN), Energy & Photon Sciences Directorate; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1485522
Alternate Identifier(s):
OSTI ID: 1485776; OSTI ID: 1508815
Report Number(s):
BNL-209740-2018-JAAM
Journal ID: ISSN 2374-7943
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Lu, Fang, Xin, Huolin, Xia, Weiwei, Liu, Mingzhao, Zhang, Yugang, Cai, Weiping, and Gang, Oleg. Tailoring Surface Opening of Hollow Nanocubes and Their Application as Nanocargo Carriers. United States: N. p., 2018. Web. doi:10.1021/acscentsci.8b00778.
Lu, Fang, Xin, Huolin, Xia, Weiwei, Liu, Mingzhao, Zhang, Yugang, Cai, Weiping, & Gang, Oleg. Tailoring Surface Opening of Hollow Nanocubes and Their Application as Nanocargo Carriers. United States. doi:10.1021/acscentsci.8b00778.
Lu, Fang, Xin, Huolin, Xia, Weiwei, Liu, Mingzhao, Zhang, Yugang, Cai, Weiping, and Gang, Oleg. Wed . "Tailoring Surface Opening of Hollow Nanocubes and Their Application as Nanocargo Carriers". United States. doi:10.1021/acscentsci.8b00778.
@article{osti_1485522,
title = {Tailoring Surface Opening of Hollow Nanocubes and Their Application as Nanocargo Carriers},
author = {Lu, Fang and Xin, Huolin and Xia, Weiwei and Liu, Mingzhao and Zhang, Yugang and Cai, Weiping and Gang, Oleg},
abstractNote = {Hollow nanoparticles (NPs) are of broad interest for biomedical, optical, and catalytic applications due to their unique geometry-related physicochemical properties. The ability to engineer hollow structures with surface openings is particularly attractive since emergent properties are promised by the design of shell porosity and encapsulation of guest materials. However, it still remains challenging to precisely control the opening of the hollow structure, in terms of shape, size, and location. Here in this paper, we report a facile one-step strategy to synthesize a hollow nanostructure with well-defined cubic-shape openings at the corners, by regulating nanoscale galvanic replacement processes with specific surface-capping agents. The final product is a single-crystalline AuAg alloy which morphologically features three “belts” orthogonally wrapping around a virtual cube, denoted by nanowrapper. We demonstrate a structural tunability of our synthetic method for tailoring nanowrapper and the corresponding tuning of its plasmonic band from the visible to near-infrared (NIR) range. Advanced electron tomography techniques provide unambiguous three-dimensional (3D) visualizations to reveal an unconventional transformation pathway of sharp-cornered Ag nanocube to nanowrapper and correlate its structure with measured and computed spectroscopic properties. Importantly, we find that the surfactant, i.e., cetylpyridinium chloride (CPC), is crucial for the openings to be localized at the corners of the hollow cube and be tailored to a cubic shape in our one-step process. Furthermore, such a well-defined hollow architecture also allows a guest nano-object to be contained within, while the large openings at corners enable controlled loading/release of nanoscale cargo, a DNA-coated particle, using change of ionic conditions. This work expands our understanding of surface engineering in nanoscale galvanic replacement reactions and opens new ways toward the shape control of hollow NPs.},
doi = {10.1021/acscentsci.8b00778},
journal = {ACS Central Science},
number = 12,
volume = 4,
place = {United States},
year = {2018},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/acscentsci.8b00778

Figures / Tables:

Figure 1 Figure 1: Synthesis of AuAg alloy nanowrappers and the morphological and structural characterizations. (a) Schematic illustration of the one-step synthesis of AuAg nanowrapper using Ag nanocube as sacrificial template. (b) HAADF-STEM characterization and EDX elemental mapping of a single AuAg alloy nanowrapper obtained after 3 h of reaction (Au, green;more » Ag, red; scale bars are 30 nm). (c) HAADF-STEM image (scale bar is 30 nm), electron diffraction pattern along a [001] zone axis direction, and high-resolution TEM (HRTEM) images of local areas marked by different color frames (scale bars are 0.5 nm). (d) Typical large-area, (e) locally magnified, and (f) high-magnification SEM images of the as-prepared AuAg nanowrappers obtained after 3 h of reaction.« less

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