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Title: Strain Effect in Palladium Nanostructures as Nanozymes

Abstract

While various effects of physicochemical parameters (e.g., size, facet, composition, and internal structure) on the catalytic efficiency of nanozymes (i.e., nanoscale enzyme mimics) have been studied, the strain effect has never been reported and understood before. Herein, we demonstrate the strain effect in nanozymes by using Pd octahedra and icosahedra with peroxidase-like activities as a model system. Strained Pd icosahedra were found to display 2-fold higher peroxidase-like catalytic efficiency than unstrained Pd octahedra. Theoretical analysis suggests that tensile strain is more beneficial to OH radical (a key intermediate for the catalysis) generation than compressive strain. Pd icosahedra are more active than Pd octahedra because icosahedra amplify the surface strain field. As a proof-of-concept demonstration, the strained Pd icosahedra were applied to an immunoassay of biomarkers, outperforming both unstrained Pd octahedra and natural peroxidases. The findings in this research may serve as a strong foundation to guide the design of high-performance nanozymes.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [3];  [3];  [1];  [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Central Florida, Orlando, FL (United States)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
  3. Brown Univ., Providence, RI (United States)
Publication Date:
Research Org.:
Louisiana State Univ., Baton Rouge, LA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1594049
Alternate Identifier(s):
OSTI ID: 1656777
Grant/Contract Number:  
SC0018408
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 20; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Palladium nanostructures; strain effect; enzyme mimic; catalysis; immunoassay

Citation Formats

Xi, Zheng, Cheng, Xun, Gao, Zhuangqiang, Wang, Mengjing, Cai, Tong, Muzzio, Michelle, Davidson, Edwin, Chen, Ou, Jung, Yeonwoong, Sun, Shouheng, Xu, Ye, and Xia, Xiaohu. Strain Effect in Palladium Nanostructures as Nanozymes. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.nanolett.9b03782.
Xi, Zheng, Cheng, Xun, Gao, Zhuangqiang, Wang, Mengjing, Cai, Tong, Muzzio, Michelle, Davidson, Edwin, Chen, Ou, Jung, Yeonwoong, Sun, Shouheng, Xu, Ye, & Xia, Xiaohu. Strain Effect in Palladium Nanostructures as Nanozymes. United States. https://doi.org/10.1021/acs.nanolett.9b03782
Xi, Zheng, Cheng, Xun, Gao, Zhuangqiang, Wang, Mengjing, Cai, Tong, Muzzio, Michelle, Davidson, Edwin, Chen, Ou, Jung, Yeonwoong, Sun, Shouheng, Xu, Ye, and Xia, Xiaohu. Tue . "Strain Effect in Palladium Nanostructures as Nanozymes". United States. https://doi.org/10.1021/acs.nanolett.9b03782. https://www.osti.gov/servlets/purl/1594049.
@article{osti_1594049,
title = {Strain Effect in Palladium Nanostructures as Nanozymes},
author = {Xi, Zheng and Cheng, Xun and Gao, Zhuangqiang and Wang, Mengjing and Cai, Tong and Muzzio, Michelle and Davidson, Edwin and Chen, Ou and Jung, Yeonwoong and Sun, Shouheng and Xu, Ye and Xia, Xiaohu},
abstractNote = {While various effects of physicochemical parameters (e.g., size, facet, composition, and internal structure) on the catalytic efficiency of nanozymes (i.e., nanoscale enzyme mimics) have been studied, the strain effect has never been reported and understood before. Herein, we demonstrate the strain effect in nanozymes by using Pd octahedra and icosahedra with peroxidase-like activities as a model system. Strained Pd icosahedra were found to display 2-fold higher peroxidase-like catalytic efficiency than unstrained Pd octahedra. Theoretical analysis suggests that tensile strain is more beneficial to OH radical (a key intermediate for the catalysis) generation than compressive strain. Pd icosahedra are more active than Pd octahedra because icosahedra amplify the surface strain field. As a proof-of-concept demonstration, the strained Pd icosahedra were applied to an immunoassay of biomarkers, outperforming both unstrained Pd octahedra and natural peroxidases. The findings in this research may serve as a strong foundation to guide the design of high-performance nanozymes.},
doi = {10.1021/acs.nanolett.9b03782},
journal = {Nano Letters},
number = 1,
volume = 20,
place = {United States},
year = {2019},
month = {12}
}

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