Prasad, R.R.R. orcid.org/0000-0002-8724-6358, Boyadjieva, S.S., Zhou, G. et al. (7 more authors) (2024) Modulated self-assembly of catalytically active metal–organic nanosheets containing Zr6 clusters and dicarboxylate ligands. ACS Applied Materials & Interfaces, 16 (14). pp. 17812-17820. ISSN 1944-8244
Abstract
Two-dimensional metal-organic nanosheets (MONs) have emerged as attractive alternatives to their three-dimensional metal-organic framework (MOF) counterparts for heterogeneous catalysis due to their greater external surface areas and higher accessibility of catalytically active sites. Zr MONs are particularly prized because of their chemical stability and high Lewis and Brønsted acidities of the Zr clusters. Herein, we show that careful control over modulated self-assembly and exfoliation conditions allows the isolation of the first example of a two-dimensional nanosheet wherein Zr6 clusters are linked by dicarboxylate ligands. The hxl topology MOF, termed GUF-14 (GUF = Glasgow University Framework), can be exfoliated into monolayer thickness hns topology MONs, and acid-induced removal of capping modulator units yields MONs with enhanced catalytic activity toward the formation of imines and the hydrolysis of an organophosphate nerve agent mimic. The discovery of GUF-14 serves as a valuable example of the undiscovered MOF/MON structural diversity extant in established metal-ligand systems that can be accessed by harnessing the power of modulated self-assembly protocols.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2024 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0 (https://creativecommons.org/licenses/by/4.0/). |
Keywords: | catalysis; coordination modulation; detoxification; metal−organic frameworks; nanosheets; nerve agents; organophosphorus compounds; two-dimensional materials |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Science (Sheffield) > Department of Chemistry (Sheffield) |
Funding Information: | Funder Grant number ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL EP/S021124/1 Engineering and Physical Sciences Research Council EP/X035859/1 |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 15 Apr 2024 14:13 |
Last Modified: | 15 Apr 2024 14:13 |
Status: | Published |
Publisher: | American Chemical Society (ACS) |
Refereed: | Yes |
Identification Number: | 10.1021/acsami.4c00604 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:211509 |