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. 2022 Aug 27;12(17):2965.
doi: 10.3390/nano12172965.

Nano-Sheet-like Morphology of Nitrogen-Doped Graphene-Oxide-Grafted Manganese Oxide and Polypyrrole Composite for Chemical Warfare Agent Simulant Detection

Sanjeeb Lama  1 , Bong-Gyu Bae  1 , Sivalingam Ramesh  2 , Young-Jun Lee  1 , Namjin Kim  3 , Joo-Hyung Kim  1
Affiliations

Nano-Sheet-like Morphology of Nitrogen-Doped Graphene-Oxide-Grafted Manganese Oxide and Polypyrrole Composite for Chemical Warfare Agent Simulant Detection

Sanjeeb Lama et al. Nanomaterials (Basel). .

Abstract

Chemical warfare agents (CWAs) have inflicted monumental damage to human lives from World War I to modern warfare in the form of armed conflict, terrorist attacks, and civil wars. Is it possible to detect the CWAs early and prevent the loss of human lives? To answer this research question, we synthesized hybrid composite materials to sense CWAs using hydrothermal and thermal reduction processes. The synthesized hybrid composite materials were evaluated with quartz crystal microbalance (QCM) and surface acoustic wave (SAW) sensors as detectors. The main findings from this study are: (1) For a low dimethyl methyl phosphonate (DMMP) concentration of 25 ppm, manganese dioxide nitrogen-doped graphene oxide (NGO@MnO2) and NGO@MnO2/Polypyrrole (PPy) showed the sensitivities of 7 and 51 Hz for the QCM sensor and 146 and 98 Hz for the SAW sensor. (2) NGO@MnO2 and NGO@MnO2/PPy showed sensitivities of more than 50-fold in the QCM sensor and 100-fold in the SAW sensor between DMMP and potential interferences. (3) NGO@MnO2 and NGO@MnO2/PPy showed coefficients of determination (R2) of 0.992 and 0.975 for the QCM sensor and 0.979 and 0.989 for the SAW sensor. (4) NGO@MnO2 and NGO@MnO2/PPy showed repeatability of 7.00 ± 0.55 and 47.29 ± 2.69 Hz in the QCM sensor and 656.37 ± 73.96 and 665.83 ± 77.50 Hz in the SAW sensor. Based on these unique findings, we propose NGO@MnO2 and NGO@MnO2/PPy as potential candidate materials that could be used to detect CWAs.

Keywords: chemical warfare agents (CWAs); dimethyl methyl phosphonate (DMMP); quartz crystal microbalance (QCM); surface acoustic wave (SAW); volatile compounds (VOCs).

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
The synthesis process of NGO@MnO2/PPy.
Figure 2
Figure 2
Vaporization system. (a) Bubbler flask used in the presented study. (b) Schematic diagram of the vapor generating process in the bubbler.
Figure 3
Figure 3
(a–f) High-resolution SEM images of NGO@MnO2 under different magnification levels. (g–i) EDX profile.
Figure 4
Figure 4
(a–f) High-resolution SEM images of NGO@MnO2/PPy under different magnification levels. (g–i) EDX profile.
Figure 5
Figure 5
Frequency shifts of (a) NGO@MnO2, (b) NGO@MnO2/PPy in the QCM sensor (T = 20 °C, R.H. = 25–30%) and 3D computed graphics of hydrogen bond formation between (c) PPy and DMMP, and (d) PPy and Sarin. Figure (c,d) are not to scale.
Figure 6
Figure 6
Selectivity of (a) NGO@MnO2, and (b) NGO@MnO2/PPy in the QCM sensor, and (c) the polar plot of response ratio (R1/R2) between the NGO@MnO2/PPy-coated and NGO@MnO2-coated QCM (T = 20 °C, R.H. = 25–30%).
Figure 7
Figure 7
Linearity of (a) NGO@MnO2 and (b) NGO@MnO2/PPy in the QCM sensor (T = 20 °C, R.H. = 25–30%).
Figure 8
Figure 8
Frequency shifts of (a) NGO@MnO2 and (b) NGO@MnO2/PPy in the SAW sensor (T = 20 °C, R.H. = 25–30%).
Figure 9
Figure 9
Selectivity of (a) NGO@MnO2, (b) NGO@MnO2/PPy in the SAW sensor, and (c) the polar plot of response ratios (R3/R4) between the NGO@MnO2/PPy-coated and NGO@MnO2-coated SAW (T = 20 °C, R.H. = 25–30%).
Figure 10
Figure 10
Linearity of (a) NGO@MnO2 and (b) NGO@MnO2/PPy in the SAW sensor (T = 20 °C, R.H. = 25–30%).
Figure 11
Figure 11
The proposed mechanism of DMMP adsorption on the NGO@MnO2/PPy composites with a Bronsted acid site, Lewis acid site, and hydrogen bonding or van der Waals force. The figure is not to scale.
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