Highly Stable Nanoparticle Supercrystals Formed by the Aldol Reaction in Conjunction with Slow Solvent Evaporation

Jiwhan Kim; Jahar Dey; Aminah Umar; Jae Min Ha; Sang Jo Lee; Jehan Kim; Sung Min Choi

doi:10.1021/acs.chemmater.2c00672

Highly Stable Nanoparticle Supercrystals Formed by the Aldol Reaction in Conjunction with Slow Solvent Evaporation

Jiwhan Kim, Jahar Dey, Aminah Umar, Jae Min Ha, Sang Jo Lee, Jehan Kim, Sung Min Choi

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

Abstract

The nanoparticle supercrystals (NPSCs) have been of great interest for their collective emergent properties. While various NPSCs have been successfully fabricated using intermolecular forces, the limited structural stability of NPSCs due to the weak nature of the intermolecular forces often limits their practical applications. Herein, we report a new method to fabricate highly stable three-dimensional NPSCs by using aldol reaction, a model covalent bond-forming reaction, in conjunction with slow solvent evaporation. Gold nanoparticles functionalized with formyl poly-ethylene glycol thiol are linked to each other by carbon-carbon covalent bonds formed by the aldol reaction as the particle dispersion in aqueous NaOH solution is slowly evaporated, resulting in highly faceted three-dimensional NPSCs. The as-synthesized NPSCs show excellent structural stability in solvents of different polarities as well as the dried condition and at temperature up to 160 °C, which is far superior to NPSCs stabilized by intermolecular forces such as hydrogen bonding and van der Waals interactions. A new covalent bonding approach opens up new opportunities in the synthesis of NPSCs and their applications.

Original language	English
Pages (from-to)	6744-6752
Number of pages	9
Journal	Chemistry of Materials
Volume	34
Issue number	15
DOIs	https://doi.org/10.1021/acs.chemmater.2c00672
Publication status	Published - 9 Aug 2022

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10.1021/acs.chemmater.2c00672

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title = "Highly Stable Nanoparticle Supercrystals Formed by the Aldol Reaction in Conjunction with Slow Solvent Evaporation",

abstract = "The nanoparticle supercrystals (NPSCs) have been of great interest for their collective emergent properties. While various NPSCs have been successfully fabricated using intermolecular forces, the limited structural stability of NPSCs due to the weak nature of the intermolecular forces often limits their practical applications. Herein, we report a new method to fabricate highly stable three-dimensional NPSCs by using aldol reaction, a model covalent bond-forming reaction, in conjunction with slow solvent evaporation. Gold nanoparticles functionalized with formyl poly-ethylene glycol thiol are linked to each other by carbon-carbon covalent bonds formed by the aldol reaction as the particle dispersion in aqueous NaOH solution is slowly evaporated, resulting in highly faceted three-dimensional NPSCs. The as-synthesized NPSCs show excellent structural stability in solvents of different polarities as well as the dried condition and at temperature up to 160 °C, which is far superior to NPSCs stabilized by intermolecular forces such as hydrogen bonding and van der Waals interactions. A new covalent bonding approach opens up new opportunities in the synthesis of NPSCs and their applications.",

author = "Jiwhan Kim and Jahar Dey and Aminah Umar and Ha, {Jae Min} and Lee, {Sang Jo} and Jehan Kim and Choi, {Sung Min}",

note = "Funding Information: This work was supported by the NRF grants funded by the Ministry of Science and ICT of the Korean Government (NRF-2017R1A2A1A05001425, NRF-2017M2A2A6A01021366, NRF-2020M2D8A2069134, and NRF-2020M2D6A1069222) and the KUSTAR-KAIST Institute, KAIST, Korea. The authors thank the Pohang Accelerator Laboratory (PAL) for providing access to the beamlines 3C and 4C used in this study. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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AU - Dey, Jahar

AU - Umar, Aminah

AU - Ha, Jae Min

AU - Lee, Sang Jo

AU - Kim, Jehan

AU - Choi, Sung Min

N1 - Funding Information: This work was supported by the NRF grants funded by the Ministry of Science and ICT of the Korean Government (NRF-2017R1A2A1A05001425, NRF-2017M2A2A6A01021366, NRF-2020M2D8A2069134, and NRF-2020M2D6A1069222) and the KUSTAR-KAIST Institute, KAIST, Korea. The authors thank the Pohang Accelerator Laboratory (PAL) for providing access to the beamlines 3C and 4C used in this study. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/8/9

Y1 - 2022/8/9

N2 - The nanoparticle supercrystals (NPSCs) have been of great interest for their collective emergent properties. While various NPSCs have been successfully fabricated using intermolecular forces, the limited structural stability of NPSCs due to the weak nature of the intermolecular forces often limits their practical applications. Herein, we report a new method to fabricate highly stable three-dimensional NPSCs by using aldol reaction, a model covalent bond-forming reaction, in conjunction with slow solvent evaporation. Gold nanoparticles functionalized with formyl poly-ethylene glycol thiol are linked to each other by carbon-carbon covalent bonds formed by the aldol reaction as the particle dispersion in aqueous NaOH solution is slowly evaporated, resulting in highly faceted three-dimensional NPSCs. The as-synthesized NPSCs show excellent structural stability in solvents of different polarities as well as the dried condition and at temperature up to 160 °C, which is far superior to NPSCs stabilized by intermolecular forces such as hydrogen bonding and van der Waals interactions. A new covalent bonding approach opens up new opportunities in the synthesis of NPSCs and their applications.

AB - The nanoparticle supercrystals (NPSCs) have been of great interest for their collective emergent properties. While various NPSCs have been successfully fabricated using intermolecular forces, the limited structural stability of NPSCs due to the weak nature of the intermolecular forces often limits their practical applications. Herein, we report a new method to fabricate highly stable three-dimensional NPSCs by using aldol reaction, a model covalent bond-forming reaction, in conjunction with slow solvent evaporation. Gold nanoparticles functionalized with formyl poly-ethylene glycol thiol are linked to each other by carbon-carbon covalent bonds formed by the aldol reaction as the particle dispersion in aqueous NaOH solution is slowly evaporated, resulting in highly faceted three-dimensional NPSCs. The as-synthesized NPSCs show excellent structural stability in solvents of different polarities as well as the dried condition and at temperature up to 160 °C, which is far superior to NPSCs stabilized by intermolecular forces such as hydrogen bonding and van der Waals interactions. A new covalent bonding approach opens up new opportunities in the synthesis of NPSCs and their applications.

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Highly Stable Nanoparticle Supercrystals Formed by the Aldol Reaction in Conjunction with Slow Solvent Evaporation

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