EP3563111B1 - Green primary explosive - Google Patents

Green primary explosive Download PDF

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EP3563111B1
EP3563111B1 EP17908564.2A EP17908564A EP3563111B1 EP 3563111 B1 EP3563111 B1 EP 3563111B1 EP 17908564 A EP17908564 A EP 17908564A EP 3563111 B1 EP3563111 B1 EP 3563111B1
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dinitromethyl
nitro
imidazole
iii
solution
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German (de)
French (fr)
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EP3563111A4 (en
EP3563111A2 (en
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Seniz OZALP YAMAN
Zuhal GERCEK
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Atilim Universitesi
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Atilim Universitesi
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    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F42AMMUNITION; BLASTING
    • F42BEXPLOSIVE CHARGES, e.g. FOR BLASTING, FIREWORKS, AMMUNITION
    • F42B99/00Subject matter not provided for in other groups of this subclass
    • CCHEMISTRY; METALLURGY
    • C06EXPLOSIVES; MATCHES
    • C06BEXPLOSIVES OR THERMIC COMPOSITIONS; MANUFACTURE THEREOF; USE OF SINGLE SUBSTANCES AS EXPLOSIVES
    • C06B25/00Compositions containing a nitrated organic compound

Definitions

  • the invention relates to green primary explosive that can be used particularly at the defense industry and developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof.
  • the primary explosives are the explosives that burn in very short time under atmospheric pressure, causing explosion.
  • Lead azide or lead styphnate is used as primary explosive as they feature high thermal stability, offer ease of synthesizing and are cheap, but such lead containing explosives might cause environmental pollution as a consequence of long-term use. Furthermore, these explosives with high destructive power generates significant amount of energy, and has negative impacts with respect to human health. Due to the disadvantages arising from the lead, NATO decided to terminate use of primary explosives that contain lead, which, in turn, necessitated development of alternate compounds that can be used as primary explosive.
  • the application no. US2012125493A1 mentions about a primary explosive and oxidizing system that contain bismuth oxide
  • the application no. WO2016101057A1 mentions about a primary explosive and oxidizing system that contain tungsten oxide or tungstate compound, and mentions that said explosives are not toxic.
  • the application no. CN104130275 discloses synthesis method for Cu(NH 3 ) 4 ATZ.2H 2 O compound that can be used as primary explosive, and mentions that said compound is environmentally friendly.
  • environmentally friendly explosives are synthesized in aforementioned applications, said applications not only fail to achieve the efficiency and chemical properties of the primary explosives to the full extent, but also fails to produce explosives with required potency and stability.
  • US4028154 discloses that ammonium 2,4,5-trinitroimidazole has an explosive performance comparable to RDX.
  • US2008/091029 discloses lead-free primary explosives consisting of metal complexes with at least one 5-nitrotetrazolate as a ligand and iron (Fe) as a central atom.
  • TALAWAR MAHADEV et al., Journal of Scientific and Industrial Research, vol.63, pages 677-681 discloses bis-(5-nitro-2H tetrazolato-N2) tetraamino cobalt perchlorate (BNCP) as a potential replacement primary explosive for lead azide.
  • the objective of the invention is to develop green primary explosive compounds that can be used particularly at the defense industry and developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof.
  • Another objective of the invention is to is to ensure elimination of foreign dependency in the defense industry through use of our own resources in production of the primary explosive.
  • Yet another objective of the invention is to ensure that cobalt or iron and zinc or copper compounds that are free of toxic metals and heavy transition metals that can be used as alternates in lieu of lead styphnate or lead azide are obtained.
  • the invention is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II), tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II),
  • the cobalt or iron complex of the invention that can be used as primary explosive material is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II) which is characterized with formula II shown hereunder,
  • M which is a constituent of Formula II, can be cobalt(II) or iron(II) ions. If constituent "M” is cobalt(II), it is characterized as tetraaminebis (4-nitro-5(dinitromethyl) imidazole cobalt(II), and if constituent "M” is iron(II), then it is characterized as tetraaminebis (4-nitro-5(dinitromethyl) imidazole iron(II).
  • the cobalt or iron complexes of the invention are tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, which is characterized with formula III, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
  • M which is a constituent of Formula III, can be cobalt(III) or iron(III) ions, while “an” can be hexafluorophosphate (PF 6 - ) or carbonate (CO 3 -2 ). If constituent "M” is cobalt(III), "an” is either hexafluorophosphate or carbonate and can be characterized as 5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, respectively; If constituent "M” is iron(III), then “an” is either hexafluorophosphate or carbonate, and can be characterized as tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, respectively.
  • the cobalt or iron complexes of the invention are ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium (diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(diaminete
  • M which is a constituent of Formula IV, can be cobalt(II/III) or iron(II/III) ions, while “kat” can be ammonium (NH 4 + ) or sodium (Na + ). If constituent "M” is cobalt (II/III), then “kat” is ammonium or sodium, and is characterized as ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), respectively; If constituent "M” is iron (II/III), then "kat” is ammonium or sodium and is characterized as ammonium
  • the cobalt or iron complexes of the invention are ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), which is characterized with formula V, obtained using
  • M which is a constituent of Formula V, can be cobalt(II/III) or iron(II/III) ions, while “kat” can be ammonium (NH 4 + ) or sodium (Na + ). If constituent "M” is cobalt (II/III), then “kat” is ammonium or sodium, and is characterized as ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), respectively; if constituent "M” is iron(II/III), then “kat” is ammonium or sodium, and is characterized as ammonium(hexakis(4-nitro-5(dinitro)
  • the zinc or copper complexes of the invention are triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate, triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, which is characterized with formula VI, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
  • M which is a constituent of Formula VI, can be zinc(II) or copper(II) ions, while “an” can be hexafluorophosphate or carbonate. If constituent "M” is zinc(II), then “an” is hexafluorophosphate or carbonate, and is characterized as triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, respectively; if constituent "M” is copper(II), then “an” is hexafluorophosphate or carbonate, and is characterized as triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, respectively.
  • the zinc or copper complexes of the invention are ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II), which is characterized with formula VII, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
  • M which is a constituent of Formula VII, can be zinc(II) or copper(II) ions, while “kat” can be ammonium or sodium. If constituent "M” is zinc(II), then “kat” is ammonium or sodium, and is characterized as ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole) zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole) zincate(II), respectively; if constituent "M” is copper(II), then “kat” is ammonium or sodium, and is characterized as ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), respectively.
  • cobalt (II)nitrate (Co(NO 3 ) 2 .6H 2 O) is used in lieu of cobalt (III) nitrate in the synthesis method of (Co(NO 3 ) 3 .6H 2 O) Tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate and tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate.
  • ammonium carbonate (NH 4 ) 2 CO 3 ) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide
  • iron(II)nitrate Fe(NO 3 ) 2 .6H 2 O
  • iron(III)nitrate Fe(NO 3 ) 3 .6H 2 O
  • ammonium carbonate (NH 4 ) 2 CO 3 ) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide
  • the new generation primary explosive of the invention that can be used in lieu of lead styphnate and/or lead azide particularly at the defense industry, developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof, is capable of presenting superior characteristics than other primary explosives.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)

Description

    Technical Field
  • The invention relates to green primary explosive that can be used particularly at the defense industry and developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof.
  • State of the Art
  • The security environment that the countries are facing today necessitates possessing powerful and deterrent armed forces. Having the competence of being able to support such deterrence in all respective fields is possible by means of developing a national defense industry. In this respect, self-sufficiency of the countries and development of defense industry products, production of which bases on domestic sources, is of paramount importance.
  • The primary explosives are the explosives that burn in very short time under atmospheric pressure, causing explosion. Lead azide or lead styphnate is used as primary explosive as they feature high thermal stability, offer ease of synthesizing and are cheap, but such lead containing explosives might cause environmental pollution as a consequence of long-term use. Furthermore, these explosives with high destructive power generates significant amount of energy, and has negative impacts with respect to human health. Due to the disadvantages arising from the lead, NATO decided to terminate use of primary explosives that contain lead, which, in turn, necessitated development of alternate compounds that can be used as primary explosive.
  • In the state of the art, the application no. US2012125493A1 mentions about a primary explosive and oxidizing system that contain bismuth oxide, and the application no. WO2016101057A1 mentions about a primary explosive and oxidizing system that contain tungsten oxide or tungstate compound, and mentions that said explosives are not toxic. The application no. CN104130275 , on the other hand, discloses synthesis method for Cu(NH3)4ATZ.2H2O compound that can be used as primary explosive, and mentions that said compound is environmentally friendly. However, although environmentally friendly explosives are synthesized in aforementioned applications, said applications not only fail to achieve the efficiency and chemical properties of the primary explosives to the full extent, but also fails to produce explosives with required potency and stability.
  • US4028154 discloses that ammonium 2,4,5-trinitroimidazole has an explosive performance comparable to RDX. US2008/091029 discloses lead-free primary explosives consisting of metal complexes with at least one 5-nitrotetrazolate as a ligand and iron (Fe) as a central atom. TALAWAR, MAHADEV et al., Journal of Scientific and Industrial Research, vol.63, pages 677-681 discloses bis-(5-nitro-2H tetrazolato-N2) tetraamino cobalt perchlorate (BNCP) as a potential replacement primary explosive for lead azide.
  • The Problems that the Invention Aims to Solve
  • The objective of the invention is to develop green primary explosive compounds that can be used particularly at the defense industry and developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof.
  • Another objective of the invention is to is to ensure elimination of foreign dependency in the defense industry through use of our own resources in production of the primary explosive.
  • Yet another objective of the invention is to ensure that cobalt or iron and zinc or copper compounds that are free of toxic metals and heavy transition metals that can be used as alternates in lieu of lead styphnate or lead azide are obtained.
  • Description of the Invention
  • The invention is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II), tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III),ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate, triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) compounds, illustrated with formula II, III, IV, V, VI and VII, and that contain at least one of the cobalt, iron, zinc or copper metals that can be used as alternate primary explosive in lieu of lead styphnate or lead azide.
  • The cobalt or iron complex of the invention that can be used as primary explosive material is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II) which is characterized with formula II shown hereunder,
    Figure imgb0001
  • Which is obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I shown hereunder.
    Figure imgb0002
  • "M", which is a constituent of Formula II, can be cobalt(II) or iron(II) ions. If constituent "M" is cobalt(II), it is characterized as tetraaminebis (4-nitro-5(dinitromethyl) imidazole cobalt(II), and if constituent "M" is iron(II), then it is characterized as tetraaminebis (4-nitro-5(dinitromethyl) imidazole iron(II).
  • The cobalt or iron complexes of the invention are tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, which is characterized with formula III, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
    Figure imgb0003
  • "M", which is a constituent of Formula III, can be cobalt(III) or iron(III) ions, while "an" can be hexafluorophosphate (PF6 -) or carbonate (CO3 -2). If constituent "M" is cobalt(III), "an" is either hexafluorophosphate or carbonate and can be characterized as 5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, respectively; If constituent "M" is iron(III), then "an" is either hexafluorophosphate or carbonate, and can be characterized as tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, respectively.
  • The cobalt or iron complexes of the invention are ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), which is characterized with formula IV, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
    Figure imgb0004
    Figure imgb0005
  • "M", which is a constituent of Formula IV, can be cobalt(II/III) or iron(II/III) ions, while "kat" can be ammonium (NH4 +) or sodium (Na+). If constituent "M" is cobalt (II/III), then "kat" is ammonium or sodium, and is characterized as ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), respectively; If constituent "M" is iron (II/III), then "kat" is ammonium or sodium and is characterized as ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), respectively.
  • The cobalt or iron complexes of the invention are ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), which is characterized with formula V, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
    Figure imgb0006
  • "M", which is a constituent of Formula V, can be cobalt(II/III) or iron(II/III) ions, while "kat" can be ammonium (NH4 +) or sodium (Na+). If constituent "M" is cobalt (II/III), then "kat" is ammonium or sodium, and is characterized as ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), respectively; if constituent "M" is iron(II/III), then "kat" is ammonium or sodium, and is characterized as ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), respectively.
  • The zinc or copper complexes of the invention are triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate, triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, which is characterized with formula VI, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
    Figure imgb0007
  • "M", which is a constituent of Formula VI, can be zinc(II) or copper(II) ions, while "an" can be hexafluorophosphate or carbonate. If constituent "M" is zinc(II), then "an" is hexafluorophosphate or carbonate, and is characterized as triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, respectively; if constituent "M" is copper(II), then "an" is hexafluorophosphate or carbonate, and is characterized as triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, respectively.
  • The zinc or copper complexes of the invention are ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II), which is characterized with formula VII, obtained using 4-nitro-5(dinitromethyl)imidazole ligand characterized with formula I.
    Figure imgb0008
  • "M", which is a constituent of Formula VII, can be zinc(II) or copper(II) ions, while "kat" can be ammonium or sodium. If constituent "M" is zinc(II), then "kat" is ammonium or sodium, and is characterized as ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole) zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole) zincate(II), respectively; if constituent "M" is copper(II), then "kat" is ammonium or sodium, and is characterized as ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), respectively.
  • The synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) [Co(NH3)4(L)2] or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II) [Fe(NH3)4(L)2] (Formula II), one of the developed cobalt or iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving Cobalt(II)nitrate (Co(NO3)2.6H2O) or iron (II) nitrate (Fe(NO3)2.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting the tetraaminecarbonateocobalt(II) [Co(NH3)4CO3] complex or tetraaminecarbonateoiron(II) [Fe(NH3)4CO3] complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of ligand solution prepared in 2 equivalent mole of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraaminecobalt(II) perchlorate ([Co(NH3)4(H2O)2] (ClO4)2) solution or to diaquatetraamineiron(II) perchlorate ([Fe(NH3)4(H2O)2] (ClO4)2) solution so obtained,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • The synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III) hexafluorophosphate ([Co(NH)4(L)2]PF6) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III) carbonate ([Co(NH3)4(L)2]2CO3) (Formula III), one of the developed cobalt complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving Cobalt (III)nitrate in (Co(NO3)6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting tetraaminecarbonateocobalt(III)nitrate [Co(NH3)4CO3]NO3 complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the ligand solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraaminecobalt(III)perchlorate ([Co(NH3)4(H2O)2] (ClO4)3) solution so obtained,
    • Separating tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt (III)perchlorate ([Co(NH)4(L)2]ClO4) so obtained by filtering,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at an equivalent mole amount at minimum to [Co(NH)4(L)2]ClO4 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Agitating the solution for 1-3 hours at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • The same process steps can also be followed when cobalt (II)nitrate (Co(NO3)2.6H2O) is used in lieu of cobalt (III) nitrate in the synthesis method of (Co(NO3)3.6H2O) Tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate and tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate. When Cobalt(II)nitrate (Co (NO3)2.6H2O) is used, the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied, and then the process can proceed with the process step of refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium.
  • The synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate ([Fe(NH3)4(L)2]PF6) or tetraaminebis(4-nitro-5(dinitromethyl) imidazole iron (III) carbonate ([Fe(NH3)4(L)2]2CO3) (Formula III), one of the developed iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting tetraaminecarbonateoiron(III)nitrate [Fe(NH3)4CO3]NO3 complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the ligand solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraamineiron(II)perchlorate ([Fe(NH3)4(H2O)2](ClO4)3) solution so obtained,
    • Separating tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)perchlorate ([Fe(NH)4(L)2]ClO4) so obtained by filtering,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at an equivalent mole amount at minimum to [Fe(NH)4(L)2]ClO4 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Agitating the solution for 1-3 hours at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • The same process steps can also be followed when iron(II)nitrate (Fe(NO3)2.6H2O) is used in lieu of iron(III)nitrate (Fe(NO3)3.6H2O) at the synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate. When Iron(II)nitrate (Fe(NO3)6H2O) is used, the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied, and then the process can proceed with the process step of Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium.
  • The synthesis method of ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II) ((NH4)2[Co (NH3)2(L)4]), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) (NH4[Co(NH3)4(L)2]), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) ((NH4)2[Fe(NH3)2(L)4]) or ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) (NH4[Fe(NH3)4(L)2] (formula IV), one of the developed cobalt or iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving cobalt(II)nitrate (Co (NO3)2.6H2O), cobalt(III)nitrate (Co(NO3)3.6H2O), iron(II)nitrate (Fe(NO3)2.6H2O) or iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting ammonium(diaminedicarbonateo)cobaltate(II) ((NH4)2[Co(NH3)2(CO3)2]), ammonium(diaminedicarbonateo)cobaltate(II) (NH4)[Co(NH3)2(CO3)2], ammonium(diaminedicarbonateo)ferrate(II) (NH4)2[Fe(NH3)2(CO3)] or ammonium(diaminedicarbonateo)ferrate(II) (NH4)[Fe(NH3)2(CO3)2] complex so obtained with perchloric acid solution at room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the ligand solution prepared in 4 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the tetraaquadiaminecobalt(II)perchlorate ([Co(NH3)2(H2O)4](ClO4)2), tetraaquadiaminecobalt(III)perchlorate ([Co(NH3)2(H2O)4](ClO4)3), tetraaquadiamineiron(II)perchlorate ([Fe(NH3)2(H2O)4](ClO4)2) or tetraaquadiamineiron(III)perchlorate ([Fe(NH3)2(H2O)4](ClO4)3) solution so obtained,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • When cobalt(II)nitrate (Co(NO3)2.6H2O) or iron(II)nitrate (Fe (NO3)2.6H2O) in the synthesis method of Ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III)or ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) is used, the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by mixing with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied, and then the process can proceed with the process step of refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium.
  • The synthesis method of sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II) (Na2[Co(NH3)2(L)4]), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) (Na[Co(NH3)4(L)2]), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) (Na2[Fe(NH3)2(L)4]) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) (Na[Fe(NH3)4(L)2]) (formula IV), one of the developed cobalt or iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving cobalt(II)nitrate (Co(NO3)2.6H2O), cobalt(III)nitrate (Co(NO3)3.6H2O), iron(II)nitrate (Fe(NO3)2.6H2O) or iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting ammonium(diaminedicarbonateo)cobaltate(II) ((NH4)2[Co(NH3)2(CO3)2]), ammonium(diaminedicarbonateo)cobaltate(II) (NH4)[Co(NH3)2(CO3)2], ammonium(diaminedicarbonateo)ferrate(II) (NH4)2[Fe(NH3)2(CO3)2] or ammonium(diaminedicarbonateo)ferrate(II) (NH4)[Fe(NH3)2(CO3)2] complex so obtained with perchloric acid solution at room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the ligand solution prepared in 4 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the diaminetetraaquacobalt(II)perchlorate ([Co(NH3)2(H2O)4](ClO4)2), diaminetetraaquacobalt(III)perchlorate ([Co(NH3)2(H2O)4](ClO4)3), diaminetetraaquairon(II)perchlorate ([Fe(NH3)2(H2O)4](ClO4)2) or diaminetetraaquairon(III)perchlorate ([Fe(NH3)2(H2O)4](ClO4)3) solution so obtained,
    • Addition of sodium chloride (Nacl) to the mixture at an equivalent mole amount at minimum, and then agitation,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • When cobalt(II)nitrate (Co(NO3)2.6H2O) or iron(II)nitrate (Fe(NO3)2.6H2O) in the synthesis method of Sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobalt(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)iron(II) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) is used; the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by mixing with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied, and then the process can proceed with the process step of refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium.
  • The synthesis method of ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II) ((NH4)4[Co(L)6]), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) ((NH4)3[Co(L)6]), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) ((NH4)4[Fe(L)6]) or ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) ((NH4)3[Fe(L)6]) (formula V), one of the developed cobalt or iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving cobalt(II)chloride (CoCl2.6H2O), cobalt(III)chloride (CoCl3.6H2O), iron(II)chloride (FeCl2.6H2O) or iron(III)chloride (FeCl3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of the ligand solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution,
    • Refluxing the mixture for 2-3 at 50-90°C,
    • Addition of equivalent mole amount of ammonium chloride (NH4Cl) to the mixture,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • When the cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) in the synthesis method of ammonium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) is used; then the process step of oxidizing the solution in by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied after the process step of dissolving cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide can be applied, and then the process can proceed with the process step of dropwise addition of the ligand solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution.
  • The synthesis method of sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II) (Na4[Co(L)6]), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) (Na3[Co(L)6]), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II) (Na4[Fe(L)6]) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) (Na3[Fe(L)6]) (formula V), one of the developed cobalt or iron complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving cobalt(II)chloride (CoCl2.6H2O), cobalt(III)chloride (CoCl3.6H2O), iron(II)chloride (FeCl2.6H2O) or iron(III)chloride (FeCl3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of the ligand solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution,
    • Refluxing the mixture for 2-3 at 50-90°C,
    • Addition of equivalent mole amount of sodium chloride (NaCl) to the mixture,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • When the cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) in the synthesis method of sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) is used; then the process step of oxidizing the solution in by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied after the process step of dissolving cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide, and then the process can proceed with the process step of dropwise addition of the ligand solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution.
  • The synthesis method of triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate ([Cu(NH3)3(L)]PF6), triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate ([Cu(NH3)3(L)]2CO3), triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate ([Zn(NH3)3(L)]PF6) or triamine(4-nitro-5(dinitromethyl) imidazole zinc(II)carbonate ([Zn(NH3)3(L)]2CO3) (formula VI), one of the developed copper or zinc complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving copper(II)nitrate (Cu(NO3)2.5H2O) or zinc(II)nitrate (Zn(NO3)2) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting the triaminecarbonateocopper(II) ([Cu(NH3)3.(NH4)2CO3]NO3) or triaminecarbonateozinc(II) ([Zn(NH3)3.(NH4)2CO3]NO3) complexes with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the ligand solution prepared in equivalent amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the aquatriaminecopper(II)perchlorate/nitrate ([Cu(NH3)3(H2O)](ClO4)2 or [Cu(NH3)3(H2O)](NO3)2) or aquatriaminezinc(II)perchlorate/nitrate ([Zn(NH3)3(H2O)](ClO4)2 or [Zn(NH3)3(H2O)](NO3)2) solution so obtained,
    • Separating, by filtering, triamine(4-nitro-5(dinitromethyl)imidazole copper(II) perchlorate/nitrate ([Cu(NH4)3(L)]ClO4 or [Cu(NH4)3(L)]NO3) or triamine (4-nitro-5(dinitromethyl)imidazole zinc(II) perchlorate/nitrate ([Zn(NH4)3(L)]ClO4 or [Zn(NH4)3(L)]NO3) so obtained,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared in equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at minimum to [Cu(NH4)3(L)]ClO4, [Cu(NH4)3(L)]NO3, [Zn(NH4)3(L)]ClO4 or [Zn(NH4)3(L)]NO3 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Drying the product so obtained.
  • The synthesis method of ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II) ((NH4)2[Cu(L)4]), sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II) (Na2[Cu(L)4]), ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) ((NH4)2[Zn(L)4]) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) (Na2[Zn(L)4]) (formula VII), one of the developed copper or zinc complexes of the invention that can be used as primary explosive comprises the process steps set forth hereunder;
    • Dissolving 4 moles of ligand in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of copper chloride (CuCl2) or zinc chloride (ZnCl2) prepared in 1 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the mixture for 2-3 hours at 50-85°C,
    • Addition of ammonium chloride (NH4Cl) or sodium chloride (NaCl) at an equivalent mole amount at minimum to the solution at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  • The foreign dependency is eliminated in the defense industry through use of our own resources in production of the compounds of the invention. In addition, environmentally friendly compounds are obtained as toxic metals and heavy transition metals are not used in the compound.
  • Application Method of the Invention to the Industry:
  • The new generation primary explosive of the invention that can be used in lieu of lead styphnate and/or lead azide particularly at the defense industry, developed for the purpose of eliminating the environmental pollution and negative impact on the human health caused by lead containing explosives as a consequence of long-term use, and the synthesis method thereof, is capable of presenting superior characteristics than other primary explosives.

Claims (16)

  1. Compounds that can be used as primary explosive, and that allows elimination of the environmental pollution and negative impacts on the human health caused by lead containing explosives as a consequence of long-term use, and that contain one of the cobalt, iron, zinc or copper metals, characterized in that; said compounds are
    • the cobalt complex, shown with formula II; and in case M is cobalt (II), said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II), or
    • the iron complex, shown with formula II; and in case M is iron (II); said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II), or
    Figure imgb0009
    • the cobalt complex, shown with formula III; and in case M is cobalt (III) and if an is hexafluorophosphate; said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate, or
    • the cobalt complex, shown with formula III; and in case M is cobalt (III) and if an is carbonate; said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, or
    • the iron complex, shown with formula III; and in case M is iron (II) and if an is hexafluorophosphate; said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate, or
    • the iron complex, shown with formula III; and in case M is iron (III) and if an is carbonate; said compound is tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, or
    Figure imgb0010
    • cobalt complexes, shown with formula IV; and in case M is cobalt (II/III) and if kat is ammonium or sodium; said compound is ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), or ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), or
    • iron complexes, shown with formula IV; and in case M is iron (II/III) and if kat is ammonium or sodium; said compound is ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), or
    Figure imgb0011
    • cobalt complexes, shown with formula V; and in case M is cobalt (II/III) and if kat is ammonium or sodium ; said compound is ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), or
    • iron complexes, shown with formula V; and in case M is iron (II/III) and if kat is ammonium or sodium; said compound is ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), or
    Figure imgb0012
    • zinc complexes, shown with formula VI; and in case M is zinc (II) and if an is hexafluorophosphate or carbonate; said compound is triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, or
    • copper complexes, shown with formula VI; and in case M is copper (II) and if an is hexafluorophosphate or carbonate; said compound is triamine(4-nitro-5(dinitromethyl)imidazole copper(II)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole copper(II)carbonate, or
    Figure imgb0013
    • zinc complexes, shown with formula VII; and in case M is zinc (II) and if kat is ammonium or sodium; said compound is ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II), or
    • copper complexes, shown with formula VII; and in case M is copper (II) and if kat is ammonium or sodium ; said compound is ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), or
    Figure imgb0014
  2. A synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(II) or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(II), characterized in that it comprises process steps of;
    • Dissolving cobalt(II)nitrate (Co(NO3)2.6H2O) or iron(II)nitrate(Fe(NO3)2.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at 60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting tetraaminecarbonateocobalt(II) [Co(NH3)4CO3] complex or tetraaminecarbonateoiron(II) [Fe(NH3)4CO3] complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of 4-nitro-5(dinitromethyl)imidazole solution prepared in 2 equivalent mole of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraaminecobalt(II) perchlorate ([Co(NH3)4(H2O)2] (ClO4)2) solution or to diaquatetraamineiron(II) perchlorate ([Fe(NH3)4(H2O)2] (ClO4)2) solution so obtained,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  3. A synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)carbonate, characterized in that it comprises process steps of;
    • Dissolving cobalt(III)nitrate (Co(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting tetraaminecarbonateocobalt(III)nitrate [Co(NH3)4CO3]NO3 complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of 4-nitro-5(dinitromethyl)imidazole solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraaminecobalt(III)perchlorate ([Co(NH3)4(H2O)2](ClO4)3) solution so obtained,
    • Separating tetraaminebis(4-nitro-5(dinitromethyl)imidazole cobalt(III)perchlorate ([Co(NH)4(L)2]ClO4) so obtained by filtering,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at an equivalent mole amount at minimum to [Co(NH)4(L)2]ClO4 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Agitating the solution for 1-3 hours at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  4. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 3, characterized in that, when cobalt(II)nitrate (Co(NO3)2.6H2O) is used in lieu of cobalt(III)nitrate (Co(NO3)3.6H2O), the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied.
  5. A synthesis method of tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)hexafluorophosphate or tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)carbonate, characterized in that it comprises process steps of;
    • Dissolving iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting the tetraaminecarbonateocobalt(II) [Co(NH3)4CO3] complex or tetraaminecarbonateoiron(II) [Fe(NH3)4CO3] complex so obtained with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of 4-nitro-5(dinitromethyl)imidazole solution prepared in 2 equivalent mole of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to diaquatetraaminecobalt(II) perchlorate ([Co(NH3)4(H2O)2] (ClO4)2) solution or to diaquatetraamineiron(II) perchlorate ([Fe(NH3)4(H2O)2] (ClO4)2) solution so obtained,
    • Separating tetraaminebis(4-nitro-5(dinitromethyl)imidazole iron(III)perchlorate ([Fe(NH)4(L)2]ClO4) so obtained by filtering,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at an equivalent mole amount at minimum to [Fe(NH)4(L)2]ClO4 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Agitating the solution for 1-3 hours at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  6. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 5, characterized in that, when iron(II)nitrate (Fe(NO3)2.6H2O) is used in lieu of iron(III)nitrate (Fe(NO3)3.6H2O), the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation by mixing the same with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied.
  7. A synthesis method of ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) or ammonium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III) , characterized in that it comprises process steps of;
    • Dissolving cobalt(II)nitrate (Co(NO3)2.6H2O), cobalt(III)nitrate (Co(NO3)3.6H2O), iron(II)nitrate(Fe(NO3)2.6H2O) or iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the solution at60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting ammonium(diaminedicarbonateo)cobaltate(II) ((NH4)2[Co(NH3)2(CO3)2]), ammonium(diaminedicarbonateo)cobaltate(III) (NH4)[Co(NH3)2(CO3)2], ammonium(diaminedicarbonateo)ferrate(II) (NH4)2[Fe(NH3)2(CO3)] or ammonium(diaminedicarbonateo)ferrate(III) (NH4)[Fe(NH3)2(CO3)2] complex so obtained with perchloric acid solution at room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the 4-nitro-5(dinitromethyl)imidazole solution prepared in 4 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the tetraaquadiaminecobalt(II)perchlorate ([Co(NH3)2(H2O)4](ClO4)2), tetraaquadiaminecobalt(III)perchlorate ([Co(NH3)2(H2O)4](ClO4)3), tetraaquadiamineiron(II)perchlorate ([Fe(NH3)2(H2O)4](ClO4)2) or tetraaquadiaminecobaltiron(III)perchlorate ([Fe(NH3)2(H2O)4](ClO4)3) solution so obtained,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  8. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 7, characterized in that, when cobalt(II)nitrate (Co(NO3)2.6H2O) or iron(II)nitrate (Fe(NO3)2.6H2O) is used; the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by mixing with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied.
  9. A synthesis method of sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) or sodium(diaminetetrakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), characterized in that it comprises process steps of;
    • Dissolving cobalt(II)nitrate (Co(NO3)2.6H2O), cobalt(III)nitrate (Co(NO3)3.6H2O), iron(II)nitrate (Fe(NO3)2.6H2O) or iron(III)nitrate (Fe(NO3)3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4]2CO3) solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the solution at60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting ammonium(diaminedicarbonateo)cobaltate(II) ((NH4)2[Co(NH3)2(CO3)2]), ammonium(diaminedicarbonateo)cobaltate(III) (NH4)[Co(NH3)2(CO3)2], ammonium(diaminedicarbonateo)ferrate(II) (NH4)2[Fe(NH3)2(CO3)2] or ammonium(diaminedicarbonateo)ferrate(III) (NH4)[Fe(NH3)2(CO3)2] complex so obtained with perchloric acid solution at room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the 4-nitro-5(dinitromethyl)imidazole solution prepared in 4 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the diaminetetraaquacobalt(II)perchlorate ([Co(NH3)2(H2O)4](ClO4)2), diaminetetraaquacobalt(III)perchlorate ([Co(NH3)2(H2O)4](ClO4)3), diaminetetraaquairon(II)perchlorate ([Fe(NH3)2(H2O)4](ClO4)2) or diaminetetraaquairon(III)perchlorate ([Fe(NH3)2(H2O)4](ClO4)3) solution so obtained,
    • Addition of sodium chloride (Nacl) to the mixture at an equivalent mole amount at minimum, and then agitation,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  10. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 9, characterized in that, when cobalt(II)nitrate (Co(NO3)2.6H2O) or iron(II)nitrate (Fe(NO3)2.6H2O) is used; the process step of oxidizing the product obtained after the process step of dropwise addition of ammonium carbonate solution prepared in 2 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by mixing with 1-3 mL 3% hydrogen peroxide (H2O2) solution can be applied.
  11. A synthesis method of ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(II) or ammonium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), characterized in that it comprises process steps of;
    • Dissolving cobalt(II)chloride (CoCl2.6H2O), cobalt(III)chloride (CoCl3.6H2O), iron(II)chloride (FeCl2.6H2O) or iron(III)chloride (FeCl3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of the 4-nitro-5(dinitromethyl)imidazole solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution,
    • Refluxing the mixture for 2-3 hours at 50-90°C
    • Addition of equivalent mole amount of ammonium chloride (NH4Cl) to the mixture,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  12. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 11, characterized in that, when cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) is used; the process step of oxidizing the product by mixing the solution with 1-3 ml 3% hydrogen peroxide (H2O2) solution can be applied after the process step of dissolving cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide.
  13. A synthesis method of sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(II), sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)cobaltate(III), sodium(hexakis (4-nitro-5(dinitromethyl)imidazole)ferrate(II) or sodium(hexakis(4-nitro-5(dinitromethyl)imidazole)ferrate(III), characterized in that it comprises process steps of;
    • Dissolving cobalt(II)chloride (CoCl2.6H2O), cobalt(III)chloride (CoCl3.6H2O), iron(II)chloride (FeCl2.6H2O) or iron(III)chloride (FeCl3.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of the 4-nitro-5(dinitromethyl)imidazole solution prepared in 6 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution,
    • Refluxing the mixture for 2-3 hours at 50-90°C,
    • Addition of equivalent mole amount of sodium chloride (NaCI) to the mixture,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
  14. A synthesis method of the compounds that can be used as primary explosive as mentioned in claim 13, characterized in that, when cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) is used; the process step of oxidizing the product by mixing the solution with 1-3 ml 3% hydrogen peroxide (H2O2) solution can be applied after the process step of dissolving cobalt(II)chloride (CoCl2.6H2O) or iron(II)chloride (FeCl2.6H2O) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide.
  15. A synthesis method of triamine(4-nitro-5(dinitromethyl)imidazole copper(ll)hexafluorophosphate, triamine(4-nitro-5(dinitromethyl)imidazole copper(ll)carbonate, triamine(4-nitro-5(dinitromethyl)imidazole zinc(ll)hexafluorophosphate or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II)carbonate, characterized in that it comprises process steps of;
    • Dissolving Copper(ll)nitrate (Cu(NO3)2.5H2O) or zinc(II)nitrate (Zn(NO3)2) in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of ammonium carbonate ((NH4)2CO3) solution prepared within water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution at equal amount by agitation,
    • Refluxing the solution at60-80°C for 1-3 hours as accompanied by surplus NH3 solution available in the medium,
    • Reacting the triaminecarbonateocopper(ll) ([Cu(NH3)3.(NH4)2CO3]NO3) or triaminecarbonateozinc(II) ([Zn(NH3)3.(NH4)2CO3]NO3) complexes with perchloric acid (HClO4) solution at the room temperature,
    • Refluxing the mixture for 2-3 hours at 75-90°C,
    • Dropwise addition of the 4-nitro-5(dinitromethyl)imidazole solution prepared in equivalent amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the aquatriaminecopper(ll)perchlorate/nitrate ([Cu(NH3)3(H2O)](ClO4)2 or [Cu(NH3)3(H2O)](NO3)2) or aquatriaminezinc(ll)perchlorate/nitrate ([Zn(NH3)3(H2O)](ClO4)2 or [Zn(NH3)3(H2O)](NO3)2) solution so obtained,
    • Separating, by filtering, triamine(4-nitro-5(dinitromethyl)imidazole copper(II) perchlorate/nitrate ([Cu(NH4)3(L)]ClO4 or [Cu(NH4)3(L)]NO3) or triamine(4-nitro-5(dinitromethyl)imidazole zinc(II) perchlorate/nitrate ([Zn(NH4)3(L)]ClO4 or [Zn(NH4)3(L)]NO3) so obtained,
    • Dropwise addition of tetrabutylammoniumhexafluorophosphate ([(C4H9)4N]PF6) or ammonium carbonate ((NH4)2CO3) solution prepared in equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide at minimum to [Cu(NH4)3(L)]ClO4, [Cu(NH4)3(L)]NO3, [Zn(NH4)3(L)]ClO4 or [Zn(NH4)3(L)]NO3 solution prepared in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Drying the product so obtained.
  16. A synthesis method of ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(ll), sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)cuprate(II), ammonium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II) or sodium(tetrakis(4-nitro-5(dinitromethyl)imidazole)zincate(II), characterized in that it comprises process steps of;
    • Dissolving 4 moles of 4-nitro-5(dinitromethyl)imidazole solution in water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide,
    • Dropwise addition of copper chloride (CuCl2) or zinc chloride (ZnCl2) prepared in 1 equivalent mole amount of water, acetonitrile, alcohol, acetone, dichloromethane, dimethylformamide, hexane, pentane, toluene or dimethyl sulfoxide to the solution by agitation,
    • Refluxing the mixture for 2-3 hours at 50-85°C,
    • Addition of ammonium chloride (NH4Cl) or sodium chloride (NaCI) at an equivalent mole amount at minimum to the solution at room temperature,
    • Separating, by filtering, the product so formed, and
    • Drying the product so obtained.
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