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Title: Design Rules for Self-Assembly of 2D Nanocrystal/Metal–Organic Framework Superstructures

Abstract

Here, we demonstrate the guiding principles behind simple two dimensional self-assembly of MOF nanoparticles (NPs) and oleic acid capped iron oxide (Fe3O4) NCs into a uniform two-dimensional bi-layered superstructure. This self-assembly process can be controlled by the energy of ligand–ligand interactions between surface ligands on Fe3O4 NCs and Zr6O4(OH)4(fumarate)6 MOF NPs. Scanning transmission electron microscopy (TEM)/energy-dispersive X-ray spectroscopy and TEM tomography confirm the hierarchical co-assembly of Fe3O4 NCs with MOF NPs as ligand energies are manipulated to promote facile diffusion of the smaller NCs. First-principles calculations and event-driven molecular dynamics simulations indicate that the observed patterns are dictated by combination of ligand–surface and ligand–ligand interactions. This study opens a new avenue for design and self-assembly of MOFs and NCs into high surface area assemblies, mimicking the structure of supported catalyst architectures, and provides a thorough fundamental understanding of the self-assembly process, which could be a guide for designing functional materials with desired structure.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division (SC-22.3)
OSTI Identifier:
1599783
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 130; Journal Issue: 40; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; dichtefunktionalrechnungen; metall-organische Geruste; molekuldynamiksimulationen; selbstorganisation; uberstrukturen

Citation Formats

Qiu, Fen, Edison, John R., Preisler, Zdenek, Zhang, Yan‐Fang, Li, Guo, Pan, Aizhao, Hsu, Chih‐Hao, Mattox, Tracy M., Ercius, Peter, Song, Chengyu, Bustillo, Karen, Brady, Michael A., Zaia, Edmond W., Jeong, Sohee, Neaton, Jeffrey B., Du, Shixuan, Whitelam, Stephen, and Urban, Jeffrey J. Design Rules for Self-Assembly of 2D Nanocrystal/Metal–Organic Framework Superstructures. United States: N. p., 2018. Web. doi:10.1002/ange.201807776.
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Qiu, Fen, Edison, John R., Preisler, Zdenek, Zhang, Yan‐Fang, Li, Guo, Pan, Aizhao, Hsu, Chih‐Hao, Mattox, Tracy M., Ercius, Peter, Song, Chengyu, Bustillo, Karen, Brady, Michael A., Zaia, Edmond W., Jeong, Sohee, Neaton, Jeffrey B., Du, Shixuan, Whitelam, Stephen, & Urban, Jeffrey J. Design Rules for Self-Assembly of 2D Nanocrystal/Metal–Organic Framework Superstructures. United States. https://doi.org/10.1002/ange.201807776
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Qiu, Fen, Edison, John R., Preisler, Zdenek, Zhang, Yan‐Fang, Li, Guo, Pan, Aizhao, Hsu, Chih‐Hao, Mattox, Tracy M., Ercius, Peter, Song, Chengyu, Bustillo, Karen, Brady, Michael A., Zaia, Edmond W., Jeong, Sohee, Neaton, Jeffrey B., Du, Shixuan, Whitelam, Stephen, and Urban, Jeffrey J. Wed . "Design Rules for Self-Assembly of 2D Nanocrystal/Metal–Organic Framework Superstructures". United States. https://doi.org/10.1002/ange.201807776. https://www.osti.gov/servlets/purl/1599783.
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@article{osti_1599783,
title = {Design Rules for Self-Assembly of 2D Nanocrystal/Metal–Organic Framework Superstructures},
author = {Qiu, Fen and Edison, John R. and Preisler, Zdenek and Zhang, Yan‐Fang and Li, Guo and Pan, Aizhao and Hsu, Chih‐Hao and Mattox, Tracy M. and Ercius, Peter and Song, Chengyu and Bustillo, Karen and Brady, Michael A. and Zaia, Edmond W. and Jeong, Sohee and Neaton, Jeffrey B. and Du, Shixuan and Whitelam, Stephen and Urban, Jeffrey J.},
abstractNote = {Here, we demonstrate the guiding principles behind simple two dimensional self-assembly of MOF nanoparticles (NPs) and oleic acid capped iron oxide (Fe3O4) NCs into a uniform two-dimensional bi-layered superstructure. This self-assembly process can be controlled by the energy of ligand–ligand interactions between surface ligands on Fe3O4 NCs and Zr6O4(OH)4(fumarate)6 MOF NPs. Scanning transmission electron microscopy (TEM)/energy-dispersive X-ray spectroscopy and TEM tomography confirm the hierarchical co-assembly of Fe3O4 NCs with MOF NPs as ligand energies are manipulated to promote facile diffusion of the smaller NCs. First-principles calculations and event-driven molecular dynamics simulations indicate that the observed patterns are dictated by combination of ligand–surface and ligand–ligand interactions. This study opens a new avenue for design and self-assembly of MOFs and NCs into high surface area assemblies, mimicking the structure of supported catalyst architectures, and provides a thorough fundamental understanding of the self-assembly process, which could be a guide for designing functional materials with desired structure.},
doi = {10.1002/ange.201807776},
journal = {Angewandte Chemie},
number = 40,
volume = 130,
place = {United States},
year = {Wed Aug 22 00:00:00 EDT 2018},
month = {Wed Aug 22 00:00:00 EDT 2018}
}
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