CN110981651B - graphene-Schiff base nickel compound for solid propellant and preparation method thereof - Google Patents
graphene-Schiff base nickel compound for solid propellant and preparation method thereof Download PDFInfo
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- CN110981651B CN110981651B CN201911215553.8A CN201911215553A CN110981651B CN 110981651 B CN110981651 B CN 110981651B CN 201911215553 A CN201911215553 A CN 201911215553A CN 110981651 B CN110981651 B CN 110981651B
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- C—CHEMISTRY; METALLURGY
- C06—EXPLOSIVES; MATCHES
- C06B—EXPLOSIVES OR THERMIC COMPOSITIONS; MANUFACTURE THEREOF; USE OF SINGLE SUBSTANCES AS EXPLOSIVES
- C06B23/00—Compositions characterised by non-explosive or non-thermic constituents
- C06B23/007—Ballistic modifiers, burning rate catalysts, burning rate depressing agents, e.g. for gas generating
Abstract
The invention discloses a preparation method of a graphene-Schiff base nickel compound, and the structural formula of the compound is shown as I or II. The synthesis process comprisesThe method comprises the following steps: (1) modifying graphene oxide by using a coupling agent to obtain aminated graphene; (2) reacting aminated graphene with salicylaldehyde to synthesize a graphene-Schiff base ligand; (3) and reacting the graphene-Schiff base ligand with nickel nitrate to prepare the graphene-Schiff base nickel compound. The graphene-Schiff base nickel compound synthesized by the method can obviously improve the burning rate of the modified double-base propellant containing HMX, and is an efficient combustion catalyst of a solid propellant.
Description
Technical Field
The invention relates to a graphene-Schiff base nickel compound and a preparation method thereof, wherein the graphene-Schiff base nickel can effectively improve the burning rate of a modified double-base solid propellant containing HMX and can be used as a burning rate catalyst of the modified double-base propellant.
Background
The solid propellant has wide application in tactical missiles and rockets, and the comprehensive performance of the solid propellant is directly related to the accurate striking, high-energy damage and survival capability of modern weapon equipment systems. By adding HMX, RDX and CL-20, the energy characteristic of the propellant can be effectively improved, and the requirements of modern tactical missile and rocket weapon on long range and rapid penetration are met.
The increase of the solid content can cause the reduction of the burning rate of the modified biradical propellant, the burning rate of the modified biradical propellant can be increased within a certain range by using a lead-copper-carbon compound catalytic system, and the pressure index is reduced, but the requirement of a modern weaponry system on the high burning rate of the modified biradical propellant is still difficult to meet. The combustion speed of the solid propellant can be effectively improved by adding the Schiff base nickel complex on the basis of a lead-copper-carbon compound catalytic system, but the pressure index of the solid propellant is improved, so that the application requirements of a modern weapons and equipment system on high combustion speed, low pressure index and wide platform of the modified biradical propellant are difficult to meet. The carbon materials such as graphene and the like are used as effective combustion catalysts in the modified double formula, and the carbon materials are combined with the effective combustion catalysts, so that the dispersity of catalytic active nickel and nickel oxide can be improved, more catalytic active sites can be obtained, and more efficacy and performance can be given to the propellant.
In view of the above, the graphene-schiff base nickel complex is designed and synthesized, and combines the excellent performances of schiff base nickel and a graphene carrier, so that the dispersion of catalytic active metal nickel and nickel oxide is effectively promoted, and more catalytic active sites are provided to meet the development requirement of a modified double-base propellant.
Disclosure of Invention
In order to solve the defects of the existing catalytic system, the invention provides a graphene-Schiff base nickel compound and a synthesis method thereof.
The structural formula of the graphene-Schiff base nickel compound is shown as I or II:
the synthesis route of the graphene-Schiff base nickel compound comprises the following steps:
in order to achieve the above purpose, the synthesis method of the graphene-schiff base nickel compound provided by the invention comprises the following steps:
(1) synthesis of aminated graphene:
placing the graphene oxide ethanol dispersion liquid subjected to ultrasonic dispersion in a three-neck flask, dropwise adding a proper amount of gamma-aminopropyltriethoxysilane KH550 or N-beta- (aminoethyl) -gamma-aminopropyltrimethoxysilane KH792 ethanol solution, reacting for 1-6 h under a reflux condition, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the aminated graphene. Wherein the mass ratio of KH550 or KH-792 to graphene oxide is 5-15: 1;
(2) synthesizing a graphene-Schiff base ligand:
placing the aminated graphene ethanol dispersion liquid synthesized in the step (1) into a three-neck flask, dropwise adding a proper amount of salicylaldehyde ethanol solution, reacting for 2-6 hours under a reflux condition, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the graphene-Schiff base ligand. Wherein the ratio of salicylaldehyde to aminated graphene is 5-15: 1;
(3) synthesis of graphene-Schiff base nickel compound
And (3) dispersing the graphene-Schiff base ligand synthesized in the step (2) in ethanol, mixing with the prepared nickel nitrate aqueous solution, reacting at 50-70 ℃ for 4-12 h, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the graphene-Schiff base nickel compound. Wherein the mass ratio of the graphene-Schiff base ligand to the nickel nitrate is 0.2-1: 1, and the volume ratio of the ethanol to the water is 2-5: 1.
The invention has the advantages and positive effects that:
the graphene-Schiff base nickel compound realizes the assembly of catalytic active substances Schiff base, active metal nickel and a two-dimensional graphene material on a molecular level, when the synthesized graphene-Schiff base nickel compound is used as a combustion catalyst, uniform and nascent nickel oxide is generated by decomposition and is used as a main catalytic active component, and a large amount of carbon substances are generated and are used as auxiliary catalytic components, so that the catalytic combustion effect can be further improved.
Drawings
Figure 1 SEM and EDS spectra of graphene-schiff base nickel complexes.
Fig. 2 FTIR spectrum of graphene-schiff base nickel complex.
Fig. 3 is a burning rate-pressure curve of the modified bistatic propellant with the addition of graphene-schiff base nickel according to the present invention.
Detailed Description
The morphology was characterized by a Quanta600 scanning electron microscope from Quantachrome, USA, and by an IR Fourier transform IR spectrometer from Tensor27, Bruker, Germany.
Synthesis of graphene-Schiff base nickel compound
(1) Synthesis of aminated graphene:
placing the graphene oxide ethanol dispersion liquid subjected to ultrasonic dispersion in a three-neck flask, dropwise adding a proper amount of gamma-aminopropyltriethoxysilane KH550 or N-beta- (aminoethyl) -gamma-aminopropyltrimethoxysilane KH792 ethanol solution, reacting for 2 hours under a reflux condition, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the aminated graphene. Wherein, KH550
Or the mass ratio of KH-792 to graphene oxide is 15;
(2) synthesizing a graphene-Schiff base ligand:
and (2) placing the aminated graphene ethanol dispersion liquid synthesized in the step (1) into a three-neck flask, dropwise adding a proper amount of salicylaldehyde ethanol solution, reacting for 3 hours under a reflux condition, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the graphene-Schiff base ligand. Wherein the mass ratio of the salicylaldehyde to the aminated graphene is 15;
(3) synthesis of graphene-Schiff base nickel compound
And (3) dispersing the graphene-Schiff base ligand synthesized in the step (2) in ethanol, mixing with a prepared nickel nitrate aqueous solution, reacting at 60 ℃ for 6 hours, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain the graphene-Schiff base nickel compound. Wherein the mass ratio of the graphene-Schiff base ligand to the nickel nitrate is 0.2, and the volume ratio of the ethanol to the water is 5.
Characterization of graphene-schiff base nickel complexes
(1) Scanning electron microscope:
scanning electron micrographs of graphene-schiff base nickel complexes prepared by using KH792 or KH550 are shown in fig. 1(a) and (b), the graphene-schiff base nickel complexes retain a better few-layer structure of graphene, schiff base ligands are combined on the surfaces of the graphene-schiff base nickel complexes, and the coordinated metal nickel has better dispersibility as an active site. EDS results confirmed successful binding of Ni to the graphene surface.
(2) Infrared spectrum:
IR (ATR, cm) as shown in FIG. 2(a)-1):3258,1604,1309,1061,903,759,612.
IR (ATR, cm) as shown in FIG. 2(b)-1):3182,1725,1607,1056,981.
Application of graphene-Schiff base nickel compound
The basic formulation of the modified biradical propellant sample used in the experiment was: 63.4% of double-base adhesive (NC + NG), 26% of HMX and 10.6% of functional auxiliary agent. The medicine materials are prepared according to 500 g. The catalyst is added, the Pb-Cu-C compound catalyst is 3.9 percent, the graphene-Schiff base nickel compound is 0.5 percent, and the contrast group contains 3.9 percent of the Pb-Cu-C catalyst.
The solid propellant sample is prepared by adopting a conventional solvent-free extrusion molding process of absorbing, driving water, cooking and cutting into medicine strips. The burning rate of the sample was measured by the target line method. Coating the side surface of the treated small grain of phi 5mm multiplied by 150mm with polyvinyl alcohol solution for 6 times, drying, and then carrying out burning rate test in a nitrogen-filled slow-acting burning rate instrument. The experimental temperature is 20 ℃, and the pressure intensity is 2-20 MPa.
In fig. 3, u is the burning rate, p is the pressure, a is the modified bis-based control formulation, b and c are the modified bis-based propellant formulations containing KH-550 and KH-792, respectively, of graphene-schiff base nickel prepared as coupling agents. As can be seen from FIG. 3, the graphene-Schiff base nickel compound prepared by the invention can effectively improve the burning rate of the propellant, wherein the graphene-Schiff base nickel compound prepared by using KH-792 as a coupling agent has a better improvement effect on the burning rate of the modified biradical propellant and also has a better reduction effect on the pressure index.
Claims (2)
1. A graphene-Schiff base nickel complex for a solid propellant is characterized in that the structural formula is shown as I:
2. the method for synthesizing the graphene-schiff base nickel composite for the solid propellant according to claim 1, wherein the method comprises the following steps:
(1) synthesis of aminated graphene:
placing the graphene oxide ethanol dispersion liquid subjected to ultrasonic dispersion in a three-neck flask, dropwise adding a proper amount of gamma-aminopropyltriethoxysilane KH550 ethanol solution, reacting for 1-6 hours under a reflux condition, cooling to room temperature after the reaction is finished, centrifuging, collecting, and washing with ethanol to obtain aminated graphene; wherein the mass ratio of the KH550 to the graphene oxide is 5-15: 1;
(2) synthesizing a graphene-Schiff base ligand:
placing the aminated graphene ethanol dispersion liquid synthesized in the step (1) into a three-neck flask, dropwise adding a proper amount of salicylaldehyde ethanol solution, reacting for 2-6 hours under a reflux condition, cooling to room temperature after the reaction is finished, centrifugally collecting, and washing with ethanol to obtain a graphene-Schiff base ligand; wherein the ratio of salicylaldehyde to aminated graphene is 5-15: 1;
(3) synthesis of graphene-Schiff base nickel compound
Dispersing the graphene-Schiff base ligand synthesized in the step (2) in ethanol, mixing with a prepared nickel nitrate aqueous solution, reacting at 50-70 ℃ for 4-12 h, cooling to room temperature after the reaction is finished, centrifugally collecting, and washing with ethanol to obtain a graphene-Schiff base nickel compound; wherein the mass ratio of the graphene-Schiff base ligand to the nickel nitrate is 0.2-1: 1, and the volume ratio of the ethanol to the water is 2-5: 1.
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| CN104993160A (en) * | 2015-08-04 | 2015-10-21 | 重庆大学 | Preparing method for non-precious metal ion complexation Schiff base graphene catalyst |
| CN108586623A (en) * | 2018-03-23 | 2018-09-28 | 昆明理工大学 | A kind of cellulose base Schiff base catalyst and its preparation method and application |
| CN110330394A (en) * | 2019-08-07 | 2019-10-15 | 西安近代化学研究所 | A kind of graphene-schiff bases lead compound and preparation method thereof |
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| CN104993160A (en) * | 2015-08-04 | 2015-10-21 | 重庆大学 | Preparing method for non-precious metal ion complexation Schiff base graphene catalyst |
| CN108586623A (en) * | 2018-03-23 | 2018-09-28 | 昆明理工大学 | A kind of cellulose base Schiff base catalyst and its preparation method and application |
| CN110330394A (en) * | 2019-08-07 | 2019-10-15 | 西安近代化学研究所 | A kind of graphene-schiff bases lead compound and preparation method thereof |
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