期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 43, 页码 18261-18271出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c08356
关键词
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资金
- Army Installations and Operations Environments Research Program (U.S. Army Engineer Research and Development Center, ERDC) [489630]
- University of California San Diego, UCSD [W912HZ-18-BAA-01]
- National Science Foundation [ECCS-1542148]
- Army Research Office, Department of Army Material command [W911NF-20-2-0143]
- Department of Defense (DoD) through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program
- Achievement Rewards for College Scientists (ARCS) Foundation Fellowship
This study introduces a new, green, thermally stable, and biocompatible zirconium metal-organic framework (Zr-MOF) catalyst for rapid and efficient detection of nerve agent threats. The catalytic degradation of diisopropylfluorophosphate (DFP) by the MIP-202(Zr) catalyst showed exceptional performance at near-neutral pH, as validated by various analytical techniques. The MIP-202(Zr)/F-ISE sensor demonstrated high thermal and storage stability, paving the way for remote or wearable field detection of G-type nerve agents in real-world environments.
Rapid and robust sensing of nerve agent (NA) threats is necessary for real-time field detection to facilitate timely countermeasures. Unlike conventional phosphotriesterases employed for biocatalytic NA detection, this work describes the use of a new, green, thermally stable, and biocompatible zirconium metal-organic framework (Zr-MOF) catalyst, MIP-202(Zr). The biomimetic Zr-MOF-based catalytic NA recognition layer was coupled with a solid-contact fluoride ion-selective electrode (F-ISE) transducer, for potentiometric detection of diisopropylfluorophosphate (DFP), a F-containing G-type NA simulant. Catalytic DFP degradation by MIP-202(Zr) was evaluated and compared to the established UiO-66-NH2 catalyst. The efficient catalytic DFP degradation with MIP-202(Zr) at near-neutral pH was validated by P-31 NMR and FT-IR spectroscopy and potentiometric F-ISE and pH-ISE measurements. Activation of MIP-202(Zr) using Soxhlet extraction improved the DFP conversion rate and afforded a 2.64-fold improvement in total percent conversion over UiO-66-NH2. The exceptional thermal and storage stability of the MIP-202/F-ISE sensor paves the way toward remote/wearable field detection of G-type NAs in real-world environments. Overall, the green, sustainable, highly scalable, and biocompatible nature of MIP-202(Zr) suggests the unexploited scope of such MOF catalysts for on-body sensing applications toward rapid on-site detection and detoxification of NA threats.
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