Journal
CHEMISTRY OF MATERIALS
Volume 34, Issue 11, Pages 4983-4991Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c00262
Keywords
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Funding
- Defense Threat Reduction Agency [HDTRA1-19-1-0010]
- Army Research Office [W911NF-181-0359]
- NSF [CHE-1048773]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-2025633]
- Int. Institute of Nanotechnology
- North-western University
- SHyNE Resource [NSF ECCS-2025633]
- IIN
- Northwestern's MRSEC program [NSF DMR-1720139]
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In this study, we encapsulated reactive hexa-nuclear zirconium (Zr-6) clusters in processable polymers to improve the hydrolysis performance of a nerve agent simulant. The loading of Zr-6 clusters in the polymer matrices was controlled by adjusting the amount of clusters. The resulting composites can also be electrospun into reactive nanofibers.
We describe a composite in which reactive hexa-nuclear zirconium (Zr-6) clusters were encapsulated in the micropores of processable polymers of intrinsic microporosity (PIMs). By varying the amount of Zr-6 clusters in PIMs, it was possible to tune the loading of Zr-6 in two polymer matrices: the pristine PIM-1 and the amidoxime-functionalized PIM (PIM-1-AO). Aggregation of Zr-6 clusters was suppressed in both Zr-6@PIM composites to achieve improved hydrolysis performance of a nerve agent simulant, dimethyl 4-nitrophenylphosphate (DMNP). Low-loading Zr-6@PIM-1-AO was found to be the best catalyst, with a DMNP hydrolysis half-life of less than 1 h, which is comparable to some zirconium metal-organic frameworks (Zr-MOFs) at higher catalyst loading. Further, these composites can be electrospun into reactive nanofibers. This demonstrates a new route to apply porous polymers as matrices to encapsulate, stabilize, and utilize the reactivity of soluble Zr-6 clusters, which could act as effective candidate materials for the fabrication of personal protective equipment (PPE) against nerve agents.
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