skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on July 15, 2020

Title: A Hierarchical Nanoporous Diamondoid Superstructure

Abstract

Sophisticated architectures assembled from a single class of subunits by cooperative interactions are ubiquitous in nature. The construction of their artificial mimics, however, remains one of the most formidable challenges facing synthetic chemists. In this work, we introduce a hierarchical diamondoid superstructure—namely, a supramolecular diamond—that is constructed from the multiple-level self-assembly of a highly symmetrical salt, hexakis[(4,4'-bipyridin-1-ium)methylene]benzene hexafluorophosphate. The uniform octahedral single crystals, with 96 cationic organic fragments and 96 counteranions in a unit cell, can be prepared quantitatively in a controllable one-step procedure within seconds at ambient conditions. The sizes of the resulting samples are modulated from 280 nm to 660 μm. The mechanism of the self-assembly was elucidated at the atomic level. As proof of its intrinsically cationic superstructure with mobile anions, the three-dimensional nanoporous framework can exchange efficiently with metal oxoanions. This research demonstrates that precisely tunable hierarchical assemblies can translate charged molecules into complicated architectures.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [1];  [1];  [1];  [1];  [4];  [1];  [1];  [1];  [1];  [1];  [5]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Westlake Univ., Hangzhou (China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Northwestern Univ., Evanston, IL (United States); Nanjing Univ. (China)
  5. Northwestern Univ., Evanston, IL (United States); Tianjin Polytechnic Univ., (China); Univ. of New South Wales, Sydney, NSW (Australia)
Publication Date:
Research Org.:
Univ. of Notre Dame, IN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1544424
Alternate Identifier(s):
OSTI ID: 1561650
Grant/Contract Number:  
[NA0003763; FG02-08ER15967; AC02-05CH11231; AC05-00OR22725]
Resource Type:
Accepted Manuscript
Journal Name:
Chem
Additional Journal Information:
[ Journal Volume: 5; Journal Issue: 9]; Journal ID: ISSN 2451-9294
Publisher:
Cell Press, Elsevier
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; supramolecular diamond; diamondoid architecture; hierarchical self-assembly; nanoporous framework; metal oxoanion removal

Citation Formats

Guo, Qing-Hui, Liu, Zhichang, Li, Peng, Shen, Dengke, Xu, Yaobin, Ryder, Matthew R., Chen, Haoyuan, Stern, Charlotte L., Malliakas, Christos D., Zhang, Xuan, Zhang, Lin, Qiu, Yunyan, Shi, Yi, Snurr, Randall Q., Philp, Douglas, Farha, Omar K., and Stoddart, J. Fraser. A Hierarchical Nanoporous Diamondoid Superstructure. United States: N. p., 2019. Web. doi:10.1016/j.chempr.2019.06.011.
Guo, Qing-Hui, Liu, Zhichang, Li, Peng, Shen, Dengke, Xu, Yaobin, Ryder, Matthew R., Chen, Haoyuan, Stern, Charlotte L., Malliakas, Christos D., Zhang, Xuan, Zhang, Lin, Qiu, Yunyan, Shi, Yi, Snurr, Randall Q., Philp, Douglas, Farha, Omar K., & Stoddart, J. Fraser. A Hierarchical Nanoporous Diamondoid Superstructure. United States. doi:10.1016/j.chempr.2019.06.011.
Guo, Qing-Hui, Liu, Zhichang, Li, Peng, Shen, Dengke, Xu, Yaobin, Ryder, Matthew R., Chen, Haoyuan, Stern, Charlotte L., Malliakas, Christos D., Zhang, Xuan, Zhang, Lin, Qiu, Yunyan, Shi, Yi, Snurr, Randall Q., Philp, Douglas, Farha, Omar K., and Stoddart, J. Fraser. Mon . "A Hierarchical Nanoporous Diamondoid Superstructure". United States. doi:10.1016/j.chempr.2019.06.011.
@article{osti_1544424,
title = {A Hierarchical Nanoporous Diamondoid Superstructure},
author = {Guo, Qing-Hui and Liu, Zhichang and Li, Peng and Shen, Dengke and Xu, Yaobin and Ryder, Matthew R. and Chen, Haoyuan and Stern, Charlotte L. and Malliakas, Christos D. and Zhang, Xuan and Zhang, Lin and Qiu, Yunyan and Shi, Yi and Snurr, Randall Q. and Philp, Douglas and Farha, Omar K. and Stoddart, J. Fraser},
abstractNote = {Sophisticated architectures assembled from a single class of subunits by cooperative interactions are ubiquitous in nature. The construction of their artificial mimics, however, remains one of the most formidable challenges facing synthetic chemists. In this work, we introduce a hierarchical diamondoid superstructure—namely, a supramolecular diamond—that is constructed from the multiple-level self-assembly of a highly symmetrical salt, hexakis[(4,4'-bipyridin-1-ium)methylene]benzene hexafluorophosphate. The uniform octahedral single crystals, with 96 cationic organic fragments and 96 counteranions in a unit cell, can be prepared quantitatively in a controllable one-step procedure within seconds at ambient conditions. The sizes of the resulting samples are modulated from 280 nm to 660 μm. The mechanism of the self-assembly was elucidated at the atomic level. As proof of its intrinsically cationic superstructure with mobile anions, the three-dimensional nanoporous framework can exchange efficiently with metal oxoanions. This research demonstrates that precisely tunable hierarchical assemblies can translate charged molecules into complicated architectures.},
doi = {10.1016/j.chempr.2019.06.011},
journal = {Chem},
number = [9],
volume = [5],
place = {United States},
year = {2019},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on July 15, 2020
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share: