Abstract
Ammonium perchlorate (AP) is an oxidizer material that is widely employed in applications ranging from rocketry to airbags. Previous research has suggested that efficient electron transfer plays a critical role in determining the kinetics of catalyzed AP decomposition reactions. Consequently, intimate contact between AP crystals and electron acceptors has the potential to accelerate decomposition kinetics, which motivates the development of conformal coatings with suitably tailored electronic structures. Here, we demonstrate a scalable method for conformally coating AP crystals with two atomically well-defined 2D materials with orthogonal electronic properties─namely, pristine graphene, which is a zero-band gap semiconductor that has been shown to be an effective electron acceptor in diverse heterojunctions and hexagonal boron nitride (hBN), which is a wide-band gap electrical insulator. Consistent with an electron transfer mechanism, graphene-coated AP undergoes accelerated decomposition kinetics compared to uncoated (neat) or hBN-coated AP. Through extensive structural characterization including electron microscopy and X-ray diffraction, the effects of AP crystal size and crystallinity are examined. In addition, the accelerated decomposition kinetics of graphene-coated AP are quantified through thermogravimetric analysis, gas chromatography mass spectrometry, and kinetic modeling. Overall, this work establishes pristine graphene as an effective coating for promoting accelerated decomposition of AP, which enhances its utility in various applications.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 9608-9617 |
| Number of pages | 10 |
| Journal | Chemistry of Materials |
| Volume | 33 |
| Issue number | 24 |
| DOIs | |
| State | Published - Dec 28 2021 |
Funding
A.J.B. thanks the in-house laboratory independent research (ILIR) program for funding support. The authors also thank the Office of Naval Research for funding under contract number N0001420WX02135. This work was further supported by the Air Force Research Laboratory under agreement number FA8650-15-2-5518 in addition to the U.S. Department of Commerce, National Institute of Standards and Technology (Award 70NANB19H005) as part of the Center for Hierarchical Materials Design (CHiMaD). Decomposition product analysis made use of the IMSERC X-RAY facility at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633) and Northwestern University. S.G.W. also gratefully thanks Prof. Christos Malliakas for extensive discussions and help with decomposition analysis. The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of the sponsors.
ASJC Scopus subject areas
- General Chemistry
- General Chemical Engineering
- Materials Chemistry