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Kinetic Stability and Propellant Performance of Green Energetic Materials
KTH, Skolan för kemivetenskap (CHE), Kemi, Fysikalisk kemi.
KTH, Skolan för kemivetenskap (CHE), Kemi, Fysikalisk kemi.ORCID-id: 0000-0003-2673-075X
2010 (Engelska)Ingår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 16, s. 6590-6600Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

A thorough theoretical investigation of four promising green energetic materials is presented. The kinetic stability of the dinitramide, trinitrogen dioxide, pentazole, and oxopentazole anions has been evaluated in the gas phase and in solution by using high-level ab initio and DFT calculations. Theoretical UV spectra, solid-state heats of formation, density, as well as propellant performance for the corresponding ammonium salts are reported. All calculated properties for dinitramide are in excellent agreement with experimental data. The stability of the trinitrogen dioxide anion is deemed sufficient to enable synthesis at low temperature, with a barrier for decomposition of approximately 27.5 kcal mol(-1) in solution. Oxopentazolate is expected to be approximately 1200 times more stable than pentazolate in solution, with a barrier exceeding 30 kcal mol(-1), which should enable handling at room temperature. All compounds are predicted to provide high specific impulses when combined with aluminum fuel and a polymeric binder, and rival or surpass the performance of a corresponding ammonium perchlorate based propellant. The investigated substances are also excellent monopropellant candidates. Further study and attempted synthesis of these materials is merited.

Ort, förlag, år, upplaga, sidor
Weinheim: Wiley-VCH Verlag GmbH & Co. KGaA , 2010. Vol. 16, s. 6590-6600
Nyckelord [en]
density functional calculations, energetic materials, green chemistry, kinetics, propellants
Nationell ämneskategori
Fysikalisk kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-25830DOI: 10.1002/chem.201000413ISI: 000279445400022Scopus ID: 2-s2.0-77953163809OAI: oai:DiVA.org:kth-25830DiVA, id: diva2:360015
Anmärkning
QC 20101103Tillgänglig från: 2010-11-01 Skapad: 2010-11-01 Senast uppdaterad: 2017-12-12Bibliografiskt granskad
Ingår i avhandling
1. Green Propellants
Öppna denna publikation i ny flik eller fönster >>Green Propellants
2010 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

To enable future environmentally friendly access to space by means of solid rocket propulsion a viable replacement to the hazardous ammonium perchlorate oxidizer is needed. Ammonium dinitramide (ADN) is one of few such compounds currently known. Unfortunately compatibility issues with many polymer binder systems and unexplained solid-state behavior have thus far hampered the development of ADN-based propellants.

Chapters one, two and three offer a general introduction to the thesis, and into relevant aspects of quantum chemistry and polymer chemistry.

Chapter four of this thesis presents extensive quantum chemical and spectroscopic studies that explain much of ADN’s anomalous reactivity, solid-state behavior and thermal stability. Polarization of surface dinitramide anions has been identified as the main reason for the decreased stability of solid ADN, and theoretical models have been developed to explain and predict the solid-state stability of general dinitramide salts. Experimental decomposition characteristics for ADN, such as activation energy and decomposition products, have been explained for different physical conditions. The reactivity of ADN towards many chemical groups is explained by ammonium-mediated conjugate addition reactions. It is predicted that ADN can be stabilized by changing the surface chemistry with additives, for example by using hydrogen bond donors, and by trapping radical intermediates using suitable amine-functionalities.

Chapter five presents several conceptual green energetic materials (GEMs), including different pentazolate derivatives, which have been subjected to thorough theoretical studies. One of these, trinitramide (TNA), has been synthesized and characterized by vibrational and nuclear magnetic resonance spectroscopy.

Finally, chapter six covers the synthesis of several polymeric materials based on polyoxetanes, which have been tested for compatibility with ADN. Successful formation of polymer matrices based on the ADN-compatible polyglycidyl azide polymer (GAP) has been demonstrated using a novel type of macromolecular curing agent. In light of these results further work towards ADN-propellants is strongly encouraged.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH, 2010. s. 77
Serie
Trita-CHE-Report, ISSN 1654-1081 ; 2010:43
Nyckelord
Quantum chemistry, reaction kinetics, ammonium dinitramide, high energy density materials, rocket propellants, chemical spectroscopy, polymer synthesis
Nationell ämneskategori
Teoretisk kemi Fysikalisk kemi
Identifikatorer
urn:nbn:se:kth:diva-25835 (URN)978-91-7415-758-1 (ISBN)
Disputation
2010-11-23, F1, Lindstedtsvägen 22, KTH, Stockholm, 09:30 (Engelska)
Opponent
Handledare
Anmärkning
QC 20101103Tillgänglig från: 2010-11-03 Skapad: 2010-11-02 Senast uppdaterad: 2011-03-21Bibliografiskt granskad

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