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Modulated Self-Assembly of Catalytically Active Metal–Organic Nanosheets Containing Zr6 Clusters and Dicarboxylate Ligands

Prasad, Ram R. R.; Boyadjieva, Sophia S.; Zhou, Guojun; Tan, Jiangtian; Firth, Francesca C. N.; Ling, Sanliang; Huang, Zhehao; Cliffe, Matthew J.; Foster, Jonathan A.; Forgan, Ross S.

Modulated Self-Assembly of Catalytically Active Metal–Organic Nanosheets Containing Zr6 Clusters and Dicarboxylate Ligands Thumbnail


Authors

Ram R. R. Prasad

Sophia S. Boyadjieva

Guojun Zhou

Jiangtian Tan

Francesca C. N. Firth

Zhehao Huang

Jonathan A. Foster

Ross S. Forgan



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.

Citation

Prasad, R. R. R., Boyadjieva, S. S., Zhou, G., Tan, J., Firth, F. C. N., Ling, S., …Forgan, R. S. (2024). Modulated Self-Assembly of Catalytically Active Metal–Organic Nanosheets Containing Zr6 Clusters and Dicarboxylate Ligands. ACS Applied Materials and Interfaces, 16(14), 17812–17820. https://doi.org/10.1021/acsami.4c00604

Journal Article Type Article
Acceptance Date Mar 13, 2024
Online Publication Date Apr 1, 2024
Publication Date Apr 10, 2024
Deposit Date May 2, 2024
Publicly Available Date May 2, 2024
Journal ACS Applied Materials and Interfaces
Print ISSN 1944-8244
Electronic ISSN 1944-8252
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 16
Issue 14
Pages 17812–17820
DOI https://doi.org/10.1021/acsami.4c00604
Public URL https://nottingham-repository.worktribe.com/output/33294629
Publisher URL https://pubs.acs.org/doi/10.1021/acsami.4c00604

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