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Title: General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX3 Peroskite Nanocrystals

Abstract

The potential optoelectronic applications of perovskite nanocrystals (NCs) are primarily limited by major material instability arising from the ionic nature of the NC lattice. Herein, we introduce a facile and effective strategy to prepare extremely stable CsPbX3 NC-polymer composites. NC surfaces are passivated with reactive methacrylic acid (MA) ligands, resulting in the formation of homogeneous nanocubes (abbreviated as MA-NCs) with a size of 14-17 nm and a photoluminescence quantum yield above 80%. The free double bonds on the surface then serve as chemically addressable synthetic handles, enabling UV-induced radical polymerization. Critically, a bromide-rich environment is developed to prevent NC sintering. The composites obtained from copolymerizing MA-NCs with hydrophobic methyl methacrylate and methacrylisobutyl polyhedral oligomeric silsesquioxane monomers exhibit enhanced properties compared to previously reported encapsulated NCs, including higher quantum yields, remarkable chemical stability toward water, and much enhanced thermal stability. The good solubility of the composite in organic solvent further enables its use as a solution-processable luminescent ink, used here for fabrication of white-light-emitting diodes with high luminous efficiency and excellent color-rendering index. The resulting fluorescent and stable NC ink opens the door to potential scalable and robust optoelectronic applications.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [1];  [3];  [1];  [1];  [1]; ORCiD logo [2]
  1. Xi’an Jiaotong Univ., Xi'an (China)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Xi’an Jiaotong Univ., Shaanxi (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1530353
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 8; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Pan, Aizhao, Wang, Jianli, Jurow, Matthew J., Jia, Mengjun, Liu, Ya, Wu, Youshen, Zhang, Yanfeng, He, Ling, and Liu, Yi. General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX3 Peroskite Nanocrystals. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.8b00587.
Pan, Aizhao, Wang, Jianli, Jurow, Matthew J., Jia, Mengjun, Liu, Ya, Wu, Youshen, Zhang, Yanfeng, He, Ling, & Liu, Yi. General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX3 Peroskite Nanocrystals. United States. https://doi.org/10.1021/acs.chemmater.8b00587
Pan, Aizhao, Wang, Jianli, Jurow, Matthew J., Jia, Mengjun, Liu, Ya, Wu, Youshen, Zhang, Yanfeng, He, Ling, and Liu, Yi. Wed . "General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX3 Peroskite Nanocrystals". United States. https://doi.org/10.1021/acs.chemmater.8b00587. https://www.osti.gov/servlets/purl/1530353.
@article{osti_1530353,
title = {General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX3 Peroskite Nanocrystals},
author = {Pan, Aizhao and Wang, Jianli and Jurow, Matthew J. and Jia, Mengjun and Liu, Ya and Wu, Youshen and Zhang, Yanfeng and He, Ling and Liu, Yi},
abstractNote = {The potential optoelectronic applications of perovskite nanocrystals (NCs) are primarily limited by major material instability arising from the ionic nature of the NC lattice. Herein, we introduce a facile and effective strategy to prepare extremely stable CsPbX3 NC-polymer composites. NC surfaces are passivated with reactive methacrylic acid (MA) ligands, resulting in the formation of homogeneous nanocubes (abbreviated as MA-NCs) with a size of 14-17 nm and a photoluminescence quantum yield above 80%. The free double bonds on the surface then serve as chemically addressable synthetic handles, enabling UV-induced radical polymerization. Critically, a bromide-rich environment is developed to prevent NC sintering. The composites obtained from copolymerizing MA-NCs with hydrophobic methyl methacrylate and methacrylisobutyl polyhedral oligomeric silsesquioxane monomers exhibit enhanced properties compared to previously reported encapsulated NCs, including higher quantum yields, remarkable chemical stability toward water, and much enhanced thermal stability. The good solubility of the composite in organic solvent further enables its use as a solution-processable luminescent ink, used here for fabrication of white-light-emitting diodes with high luminous efficiency and excellent color-rendering index. The resulting fluorescent and stable NC ink opens the door to potential scalable and robust optoelectronic applications.},
doi = {10.1021/acs.chemmater.8b00587},
journal = {Chemistry of Materials},
number = 8,
volume = 30,
place = {United States},
year = {Wed Mar 28 00:00:00 EDT 2018},
month = {Wed Mar 28 00:00:00 EDT 2018}
}

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Cited by: 90 works
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Figures / Tables:

Scheme 1 Scheme 1: The design of PMPOPNC by co-polymerization with chemically addressable NCs

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