An Exceptionally Stable Metal–Organic Framework Constructed from Chelate-Based Metal–Organic Polyhedra
Abstract
We report the rational design and synthesis of a water-stable metal–organic framework (MOF), Fe-HAF-1, constructed from supramolecular, Fe3+-hydroxamate-based polyhedra with mononuclear metal nodes. Owing to its chelate-based construction, Fe-HAF-1 displays exceptional chemical stability in organic and aqueous solvents over a wide pH range (pH 1–14), including in the presence of 5 M NaOH. Despite the charge neutrality of the Fe3+-tris(hydroxamate) centers, Fe-HAF-1 crystals are negatively charged above pH 4. This unexpected property is attributed to the formation of defects during crystallization that results in uncoordinated hydroxamate ligands or hydroxide-coordinated Fe centers. The anionic nature of Fe-HAF-1 crystals enables selective adsorption of positively charged ions in aqueous solution, resulting in efficient separation of organic dyes and other charged species in a size-selective fashion. Fe-HAF-1 presents a new addition to a small group of chelate-based MOFs and provides a rare framework whose 3D connectivity is exclusively formed by metal–hydroxamate coordination.
- Authors:
-
- Univ. of California, San Diego, CA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); University of California, San Diego, La Jolla, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Institutes of Health (NIH); National Science Foundation (NSF)
- OSTI Identifier:
- 1656873
- Alternate Identifier(s):
- OSTI ID: 1668315
- Grant/Contract Number:
- AC02-06CH11357; SC0003844; T32GM112584; CHE-1661655; CHE-1338173
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 15; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; Design; reticular chemistry; dyes and pigments; metals; ligands; metal organic frameworks; cluster chemistry
Citation Formats
Chiong, Jerika A., Zhu, Jie, Bailey, Jake B., Kalaj, Mark, Subramanian, Rohit H., Xu, Wenqian, Cohen, Seth M., and Tezcan, F. Akif. An Exceptionally Stable Metal–Organic Framework Constructed from Chelate-Based Metal–Organic Polyhedra. United States: N. p., 2020.
Web. doi:10.1021/jacs.0c01626.
Chiong, Jerika A., Zhu, Jie, Bailey, Jake B., Kalaj, Mark, Subramanian, Rohit H., Xu, Wenqian, Cohen, Seth M., & Tezcan, F. Akif. An Exceptionally Stable Metal–Organic Framework Constructed from Chelate-Based Metal–Organic Polyhedra. United States. https://doi.org/10.1021/jacs.0c01626
Chiong, Jerika A., Zhu, Jie, Bailey, Jake B., Kalaj, Mark, Subramanian, Rohit H., Xu, Wenqian, Cohen, Seth M., and Tezcan, F. Akif. Sat .
"An Exceptionally Stable Metal–Organic Framework Constructed from Chelate-Based Metal–Organic Polyhedra". United States. https://doi.org/10.1021/jacs.0c01626. https://www.osti.gov/servlets/purl/1656873.
@article{osti_1656873,
title = {An Exceptionally Stable Metal–Organic Framework Constructed from Chelate-Based Metal–Organic Polyhedra},
author = {Chiong, Jerika A. and Zhu, Jie and Bailey, Jake B. and Kalaj, Mark and Subramanian, Rohit H. and Xu, Wenqian and Cohen, Seth M. and Tezcan, F. Akif},
abstractNote = {We report the rational design and synthesis of a water-stable metal–organic framework (MOF), Fe-HAF-1, constructed from supramolecular, Fe3+-hydroxamate-based polyhedra with mononuclear metal nodes. Owing to its chelate-based construction, Fe-HAF-1 displays exceptional chemical stability in organic and aqueous solvents over a wide pH range (pH 1–14), including in the presence of 5 M NaOH. Despite the charge neutrality of the Fe3+-tris(hydroxamate) centers, Fe-HAF-1 crystals are negatively charged above pH 4. This unexpected property is attributed to the formation of defects during crystallization that results in uncoordinated hydroxamate ligands or hydroxide-coordinated Fe centers. The anionic nature of Fe-HAF-1 crystals enables selective adsorption of positively charged ions in aqueous solution, resulting in efficient separation of organic dyes and other charged species in a size-selective fashion. Fe-HAF-1 presents a new addition to a small group of chelate-based MOFs and provides a rare framework whose 3D connectivity is exclusively formed by metal–hydroxamate coordination.},
doi = {10.1021/jacs.0c01626},
journal = {Journal of the American Chemical Society},
number = 15,
volume = 142,
place = {United States},
year = {Sat Mar 28 00:00:00 EDT 2020},
month = {Sat Mar 28 00:00:00 EDT 2020}
}
Web of Science
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