TY - JOUR
T1 - Enhanced Decomposition of Ammonium Perchlorate-Ethyl Cellulose-Molybdenum Disulfide Nanocomposites
AU - Baca, Alfred J.
AU - Garrison, Michael D.
AU - Kuo, Lidia
AU - Xu, Feiyu
AU - Baldwin, Lawrence C.
AU - Hyla, Alexander S.
AU - Zachariah, Michael R.
AU - Hersam, Mark C.
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/6/7
Y1 - 2023/6/7
N2 - Ammonium perchlorate (AP) is commonly used in propulsion technology. Recent studies have demonstrated that two-dimensional (2D) nanomaterials such as graphene (Gr) and hexagonal boron nitride (hBN) dispersed with nitrocellulose (NC) can conformally coat the surface of AP particles and enhance the reactivity of AP. In this work, the effectiveness of ethyl cellulose (EC) as an alternative to NC was studied. Using a similar encapsulation procedure as in recent work, Gr and hBN dispersed with EC were used to synthesize the composite materials Gr-EC-AP and hBN-EC-AP. Additionally, EC was used because the polymer can be used to disperse other 2D nanomaterials, specifically molybdenum disulfide (MoS2), which has semiconducting properties. While Gr and hBN dispersed in EC had a minimal effect on the reactivity of AP, MoS2 dispersed in EC significantly enhanced the decomposition behavior of AP compared to the control and other 2D nanomaterials, as evidenced by a pronounced low-temperature decomposition event (LTD) centered at 300 °C and then complete high-temperature decomposition (HTD) below 400 °C. Moreover, thermogravimetric analysis (TGA) showed a 5% mass loss temperature (Td5%) of 291 °C for the MoS2-coated AP, which was 17 °C lower than the AP control. The kinetic parameters for the three encapsulated AP samples were calculated using the Kissinger equation and confirmed a lower activation energy pathway for the MoS2 (86 kJ/mol) composite compared to pure AP (137 kJ/mol). This unique behavior of MoS2 is likely due to enhanced oxidation-reduction of AP during the initial stages of the reaction via a transition metal-catalyzed pathway. Density functional theory (DFT) calculations showed that the interactions between AP and MoS2 were stronger than AP on the Gr or hBN surfaces. Overall, this study complements previous work on NC-wrapped AP composites and demonstrates the unique roles of the disperagent and 2D nanomaterial in tuning the thermal decomposition of AP.
AB - Ammonium perchlorate (AP) is commonly used in propulsion technology. Recent studies have demonstrated that two-dimensional (2D) nanomaterials such as graphene (Gr) and hexagonal boron nitride (hBN) dispersed with nitrocellulose (NC) can conformally coat the surface of AP particles and enhance the reactivity of AP. In this work, the effectiveness of ethyl cellulose (EC) as an alternative to NC was studied. Using a similar encapsulation procedure as in recent work, Gr and hBN dispersed with EC were used to synthesize the composite materials Gr-EC-AP and hBN-EC-AP. Additionally, EC was used because the polymer can be used to disperse other 2D nanomaterials, specifically molybdenum disulfide (MoS2), which has semiconducting properties. While Gr and hBN dispersed in EC had a minimal effect on the reactivity of AP, MoS2 dispersed in EC significantly enhanced the decomposition behavior of AP compared to the control and other 2D nanomaterials, as evidenced by a pronounced low-temperature decomposition event (LTD) centered at 300 °C and then complete high-temperature decomposition (HTD) below 400 °C. Moreover, thermogravimetric analysis (TGA) showed a 5% mass loss temperature (Td5%) of 291 °C for the MoS2-coated AP, which was 17 °C lower than the AP control. The kinetic parameters for the three encapsulated AP samples were calculated using the Kissinger equation and confirmed a lower activation energy pathway for the MoS2 (86 kJ/mol) composite compared to pure AP (137 kJ/mol). This unique behavior of MoS2 is likely due to enhanced oxidation-reduction of AP during the initial stages of the reaction via a transition metal-catalyzed pathway. Density functional theory (DFT) calculations showed that the interactions between AP and MoS2 were stronger than AP on the Gr or hBN surfaces. Overall, this study complements previous work on NC-wrapped AP composites and demonstrates the unique roles of the disperagent and 2D nanomaterial in tuning the thermal decomposition of AP.
KW - 2D nanomaterials
KW - ammonium perchlorate
KW - crystallinity
KW - ethyl cellulose
KW - graphene
KW - hexagonal boron nitride
KW - molybdenum disulfide
KW - morphology
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U2 - 10.1021/acsami.3c04021
DO - 10.1021/acsami.3c04021
M3 - Article
C2 - 37218169
AN - SCOPUS:85162777819
SN - 1944-8244
VL - 15
SP - 26799
EP - 26811
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 22
ER -