Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

Ayagoz Bakkara; Bakhtiyar Sadykov; Anar Zhapekova; Timur Oserov; Aisulu Batkal; Ainur Khairullina; Nina Mofa

doi:10.3390/chemengineering6060090

Bakkara, Ayagoz;Sadykov, Bakhtiyar;Zhapekova, Anar;Oserov, Timur;Batkal, Aisulu;Khairullina, Ainur;Mofa, Nina

2022-11-15 00:00:00

chemengineering Review Efﬁciency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems 1 , 2 1 , 2 , 1 , 2 1 1 Ayagoz Bakkara , Bakhtiyar Sadykov *, Anar Zhapekova , Timur Oserov , Aisulu Batkal , 1 1 Ainur Khairullina and Nina Mofa Institute of Combustion Problems, 172, Bogenbay Batyr St., Almaty 050012, Kazakhstan Faculty of Chemistry and Chemical Technology, Al-Farabi Kazakh National University, 71, Al-Farabi Ave., Almaty 050000, Kazakhstan * Correspondence: sadykoff_baha@mail.ru Abstract: This review is devoted to the possibilities of using mechanochemical processing and to achievements in this ﬁeld for obtaining materials for a wide range of purposes. The mechanochemical processing of various materials and compositions in energy-intensive grinding devices allows the production of innovative systems, ensuring the necessary complex structure and properties. A detailed analysis of the processes of mechanochemical processing in the production of designs for various purposes is given, and the latest practical results in this area are highlighted. A detailed analysis of the processes of mechanochemical processing in the production of structures for various purposes is given, as well as recent practical results in this area, such as the use of mechanochemical processing to increase the performance of aluminum and other metals used as a combustible substance in energy-intensive systems. This review also presents the prospects for the use of mechanochemical processing to obtain physiologically active drugs from plant materials, which is an effective method for creating new materials in the ﬁeld of pharmaceuticals, animal husbandry, veterinary medicine, Citation: Bakkara, A.; Sadykov, B.; crop production, etc. Zhapekova, A.; Oserov, T.; Batkal, A.; Khairullina, A.; Mofa, N. Efﬁciency Keywords: mechanochemical treatment; grinding; modiﬁcation; composite materials and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems. ChemEngineering 2022, 6, 90. 1. Introduction https://doi.org/10.3390/ chemengineering6060090 Mechanochemical processing of organic and inorganic materials using energy-intensive grinding devices is currently one of the innovative methods for obtaining new materials, Academic Editor: Alírio E. Rodrigues with desirable properties for various functional purposes (energy-intensive systems, cata- Received: 15 September 2022 lysts, sorbents, building materials, etc.) [1,2]. During mechanochemical treatment (MCT), Accepted: 31 October 2022 in addition to the dispersion of particles, the following occurs: deformation of crystals, Published: 15 November 2022 formation of a large number of defects, changes in the size of micro blocks forming a crystal, shear stresses, aggregation of crystallites, heat release, a local rise in temperature Publisher’s Note: MDPI stays neutral and pressure, emission of light and electrons, phase transformations, amorphization and with regard to jurisdictional claims in breaking of chemical bonds, acceleration of diffusion processes, and formation of centers published maps and institutional afﬁl- with increased activity on newly formed surfaces [3,4]. All these processes provide an iations. increase in the activity of processed solids as a result of the occurrence of vibrationally and electronically excited states of interatomic bonds, as well as mechanically stressed and broken bonds, including the presence of free radicals, coordinatively unsaturated Copyright: © 2022 by the authors. atoms, various structural defects, the ionization of particles of matter, and stabilization Licensee MDPI, Basel, Switzerland. of electrically charged centers [5–7]. All structural changes result from the absorption This article is an open access article of mechanical energy by the substance during automated processing, which leads to its distributed under the terms and activation [8]. Such a system with a developed defect structure and accumulated excess conditions of the Creative Commons free energy is not in thermodynamic equilibrium, providing it with an increased reactivity. Attribution (CC BY) license (https:// Identifying speciﬁc factors responsible for the increase in reactivity is one of the creativecommons.org/licenses/by/ most critical tasks in studying the physicochemical properties of mechanically activated 4.0/). ChemEngineering 2022, 6, 90. https://doi.org/10.3390/chemengineering6060090 https://www.mdpi.com/journal/chemengineering ChemEngineering 2022, 6, x FOR PEER REV IEW 2 o f 17 ChemEngineering 2022, 6, 90 2 of 17 Ident ify ing specific fact or s r esponsib le for t he incr ease in r eact iv it y is one of t he m ost cr it ical t asks in st udy ing t he phy sicochemical pr oper t ies of mechanically act ivat ed sub- substances. The increased activity (reactivity) of various materials after MCT is used in st ances. The incr ea sed act iv it y (r ea ct iv it y) of v ar ious m at er ia ls aft er MCT is used in sub- subsequent processes for the practical application of treated systems (sintering, synthesis, sequent pr ocesses for the pr actical application of tr eated systems (sinter ing, synthesis, combustion, catalysis, sorption processes, dissolution, etc.). MCT is used to accelerate combustion, catalysis, sorption processes, dissolution, etc.). MCT is used to accelerate technological processes or as a way to change the technical parameters of the processing t echnological pr ocesses or as a w ay t o change t he t echnical par amet er s of t he pr ocessing mode of various mineral raw materials. During mechanochemical treatment of metal m ode of v a r ious m iner al r a w m at er ials. Dur ing m echa nochem ical t r eat m ent of m et al par- particles, the concentration of dislocations increases. As a result, the thermokinetic charac- t icles, t he concent r at ion of dislocat ions incr ea ses. As a r esult , t he t her m okinet ic char acter- teristics of the combustion process are also intensiﬁed. From the obtained thermograms, it ist ics of t he comb ust ion pr ocess ar e also int ensified. Fr om t he ob t ained t her mogr ams, it follows that after the MCT of the mixture, the induction period of ignition decreases and follow s t hat aft er t he MCT of t he mixt ur e, t he induct ion per iod of ignit ion decr eases and the combustion temperature of the thermite mixture increases [9]. A general scheme for the t he comb ust ion t emper at ur e of the t her mit e mixt ur e incr eases [9]. A general scheme for use of mechanochemical processing in modern technological processes, according to the t he use of mechanochemical pr ocessing in moder n t echnological pr ocesses, accor ding t o results of work in [10], is shown in Figure 1. t he r esult s of w or k in [10], is show n in Figur e 1. Figure 1. Applic a tion of me c ha noc hemic al te chnology in mode rn ma terials s cience [10]. Figure 1. Application of mechanochemical technology in modern materials science [10]. At the same time, the ener gy costs for activation ar e paid off b y saving time and en- At the same time, the energy costs for activation are paid off by saving time and ergy costs in the subsequent technological processes, particularly in self-pr opagating energy costs in the subsequent technological processes, particularly in self-propagating high- t em per at ur e sy nt hesis (SHS) [11]. high-temperature synthesis (SHS) [11]. The importance of using MCT in the pr ocessing of v ar ious solid m a t er ials lies in t he The importance of using MCT in the processing of various solid materials lies in the ab ilit y t o cont r ol t he for mat ion of the st r uct ur e (nanoar chitect ure), t he cr eat ion of act ive ability to control the formation of the structure (nanoarchitecture), the creation of active centers, and control of the chemistry of the surface layer of particles, det er mining t heir centers, and control of the chemistry of the surface layer of particles, determining their r eactiv ity a nd the funct iona l dir ect ion of t heir sub sequent use. To contr ol such t asks dur - reactivity and the functional direction of their subsequent use. To control such tasks during ing MCT, in m ost cases, pr ocessing of t he m ixt ur e, i.e., pr ocessing of inor ganic and or ga nic MCT, in most cases, processing of the mixture, i.e., processing of inorganic and organic sub st ances, is car r ied out sim ult aneously [ 2], t hus ensur ing t he m odificat ion of t he sur fa ce substances, is carried out simultaneously [2], thus ensuring the modiﬁcation of the surface the cr ushed mat er ials [12,13]. Acceler a t ion of chem ica l r ea ct ions b et w een or ga nic a nd in- the crushed materials [12,13]. Acceleration of chemical reactions between organic and organic substances during MCT is mainly due to electrificat ion of t he char act er in t he inorganic substances during MCT is mainly due to electriﬁcation of the character in the places of w her e split t ing and cr a cks of the solid pa r t icles occur s, w hich ar e a kind of m icro places of where splitting and cracks of the solid particles occurs, which are a kind of −1 1 capacitor , w it h high elect r ic fields r eaching 10 7 V cm . Elect r ons in such ar eas ar e accel- micro capacitor, with high electric ﬁelds reaching 107 V cm . Electrons in such areas are erated to high speeds, causing polymerization of the organic compounds in the treated accelerated to high speeds, causing polymerization of the organic compounds in the treated m ixt ur e and t heir gr aft ing t o t he new ly for m ed sur face of the solid inor ganic pa r t icles, i.e., mixture and their grafting to the newly formed surface of the solid inorganic particles, i.e., t heir m odificat ion [ 14,15]. their modiﬁcation [14,15]. When processing metal plastic powders under the conditions of mechanochemical action (i.e., the simultaneous mechanical action of the tool and a chemically active medium), facilitation of the initiation and development of microcracks in the oxidized metal layer takes place. In this case, with the simultaneous modiﬁcation of the surface with organic ChemEngineering 2022, 6, 90 3 of 17 compounds, it is possible to signiﬁcantly accelerate the chemical reactions of the treated metal particles with other substances; for example, when creating various metal–ceramic compositions [16]. To increase the efﬁciency of grinding viscoelastic plastic bodies and metals, various surface-active substances (surfactants) are used. The use of liquid surfactants does not entirely eliminate the oxidation of the material being ground, due to the heating of the mixture to 60–80 C and higher during MCT and the presence of water and oxygen dissolved in the surfactant, as well as the air present in the working space of the grinding equipment. As mechanically destructible organic substances that facilitate metal dispersion, in most cases, solid-phase high-molecular compounds are used, which undergo mechanical destruction under the mechanical action [17]. The products of the mechanical destruction of a high-molecular compound penetrate the surface microcracks, and polymerization processes begin to occur on their faces, with the formation of a high-molecular product, thus leading to a sharp increase in stresses in the dead-end region of the microcracks and advancement of the crack front into the depths of the metal. The kinetics of crack development is determined by the rate of mechanochemical processes and the concentration of mechano- and thermal destruction products. Polymethyl methacrylate, characterized by a deﬁciency of bound oxygen, is used as a high molecular medium capable of undergoing mechanical destruction and generating low molecularly active components. The products of polymethyl methacrylate mechanocracking penetrate into the surface cracks, forming thin ﬁlms on the faces and preventing their closing [17]. Thus, when processing a mixture of magnesium with ﬂuorine-chloropolymers (ﬂuoroplast), a ﬁlm is formed on the surface of metal particles, due to an increased concentration of active particles of ﬂuoroplast macroradicals during MCT [18,19]. In this case, two types of radicals are possible: macroradicals formed upon rupture of polymer molecules, and peroxide macroradicals, which are adsorbed on the surface of metal particles. When a polymer ﬁlm is formed on the surface of the particles, the composition is a mixture, with a high contact surface of the reagents. All this ensures the high reactivity of the mix of metal and ﬂuoroplastics. Consequently, a high rate of transformation over a wide concentration range can contribute to a change in the explosive properties of such composites consisting of a metal and ﬂuoroplast [20]. 2. Features of the Structure and Properties of Energy-Intensive Metal Compositions Obtained by Mechanochemical Processing If the last century was the time of the formation of mechanochemistry as an indepen- dent scientiﬁc ﬁeld of controlling the structure and properties of solid-phase systems, a method of accelerating chemical and physicochemical transformations, the 21st century has been the time of expanding the practical implementation of theoretical developments on the reactivity of matter after MCT. At ﬁrst, attention was paid to the MCT of non-metallic systems for obtaining various ceramic compositions [3,21,22]. Currently, more and more attention is being paid to using MCT to obtain energy-intensive combustible pieces for multiple purposes, especially for rocket engines. In such systems, a signiﬁcant role is assigned to metallic fuels. These include aluminum, magnesium, zinc, zirconium, boron, beryllium, lithium, and their hydrates and alloys. As a rule, these are used in mixed solid fuels (MSF). The metal in the fuel composition is an energy additive that increases the heat output, speciﬁc impulse, and fuel combustion rate [23]. Each of the metal additives has its speciﬁc manner of changing the quality of fuel mixtures. Adding zirconium leads to a high fuel density but reduces the speciﬁc thrust. From a safety point of view, boron does not cause any difﬁculties, while aluminum and magnesium have a low ﬂammability, and lithium and zirconium are the most explosive; when working with beryllium, special measures must be taken due to its toxicity. In addition, metal additives increase the speciﬁc gravity of the fuel, which improves the characteristics of the engine and the rocket as a whole [24]. It should be taken into account ChemEngineering 2022, 6, x FOR PEER REV IEW 4 o f 17 magnesium have a low flammability, and lit hium and zir conium ar e t he most explosive; w hen w or king w it h b er y llium , special m easur es m ust b e t aken due t o it s t oxicit y . In addit ion, m et al addit iv es incr ease t he specific gr av it y of t he fuel, w hich im pr ov es the characteristics of the engine and the rocket as a w hole [24]. It should be taken into account t hat t he higher t he cont ent of met al-cont aining fuel, t he higher t he t emper at ure of t heir com b ust ion pr oduct s. Alm ost all m oder n com posit e fuels cont a in m et als as com - ponents. The most w idely used and cheapest met al fuel is aluminum. Due t o t he high heat of ChemEngineering 2022, 6, 90 4 of 17 combustion (∆H = −837.5 kJ/mol), powdered metallic aluminum is commonly used in high- ener gy sy st em s: in t her m it e com posit ions, m ixed fuels, and explosiv es, as w ell as in designs for the self-propagating high-temper atur e synthesis of r efr actor y compounds. that the higher the content of metal-containing fuel, the higher the temperature of their The reactivity of aluminum pow ders largely depends on the particle size and increases combustion products. Almost all modern composite fuels contain metals as components. significant ly w hen moving t o par t icles smaller t han 1 μm [ 25]. The use of finely ground The most widely used and cheapest metal fuel is aluminum. Due to the high heat of a lum inum pow der in mixed fuels incr eases t he specific t hr ust of engines, impr oves t heir combustion (DH = 837.5 kJ/mol), powdered metallic aluminum is commonly used in star t- up r elia b ilit y, and incr eases t he st ab ilit y of fuel com b ust ion [26,27]. high-energy systems: in thermite compositions, mixed fuels, and explosives, as well as Micr on-sized aluminum par t icles only burn due to diffusion of the oxidizing agent in designs for the self-propagating high-temperature synthesis of refractory compounds. t hr ough t he oxide film on t he sur face of t he par t icles. The b ur ning r at e depends on t he The reactivity of aluminum powders largely depends on the particle size and increases diffusion r at e. W hen aluminum melt s inside a par t icle, the volumet r ic expansion and in- signiﬁcantly when moving to particles smaller than 1 m [25]. The use of ﬁnely ground cr eased int er nal pr essur e r esult in t he peeling of t he oxide shell and splashing of molt en aluminum powder in mixed fuels increases the speciﬁc thrust of engines, improves their aluminum, w it h oxidat ion in t he gas phase [28–30 ] . The com b ust ion schem e of a n alum i- start-up reliability, and increases the stability of fuel combustion [26,27]. num pa r t icle is show n in Figur e 2. Figur e 2 show s t he com b ust ion m odel of an alum inum Micron-sized aluminum particles only burn due to diffusion of the oxidizing agent particle. This model was developed to describe the combustion of aluminum in rocket through the oxide ﬁlm on the surface of the particles. The burning rate depends on engines. In r ocket engines, t he aluminum par t icle t y pically ignit es near t he sur face of t he the diffusion rate. When aluminum melts inside a particle, the volumetric expansion pr opellant . Hence in t his model, ignit ion is initially assumed to have occurred, and the and increased internal pressure result in the peeling of the oxide shell and splashing of m odel concent r at es on t he com b ust ion aft er t he ignit ion. molten aluminum, with oxidation in the gas phase [28–30]. The combustion scheme of Accor ding t o t his comb ust ion m echanism , w e can assum e t he follow ing: (1) The par - an aluminum particle is shown in Figure 2. Figure 2 shows the combustion model of an t icle is spher ical; (2) The flow ar ound t he par t icle is laminar . The flow ar ound an alumi- aluminum particle. This model was developed to describe the combustion of aluminum in num pa r t icle under r ocket engine condit ions is usually la m inar , due t o t he small par t icle rocket engines. In rocket engines, the aluminum particle typically ignites near the surface size (t y pically less t han 200 mm in diameter); (3) The local homogeneous flow model is of the propellant. Hence in this model, ignition is initially assumed to have occurred, and a pplicab le t o liquid alum inum [30]. the model concentrates on the combustion after the ignition. Figure 2. Combustion of an aluminum particle [30]. Figure 2. Combus tion of a n a luminum pa rtic le [30]. According to this combustion mechanism, we can assume the following: (1) The The traditional methods of activating aluminum and magnesium metals use the particle is spherical; (2) The ﬂow around the particle is laminar. The ﬂow around an pr epar at ion of alloy s. For aluminum, t hese ar e alloy s b ased on mer cur y or gallium, w ith aluminum particle under rocket engine conditions is usually laminar, due to the small additions of indium, tin, thallium, and some other metals; for magnesium, alloys w ith particle size (typically less than 200 mm in diameter); (3) The local homogeneous ﬂow nickel ar e used. The alum inum act iv at ion m et hod uses t he immer sion of aluminum into model is applicable to liquid aluminum [30]. gallama, in t he r ange of melt ing t emper at ur es of gallama and/or aluminum, in t he pr es- The traditional methods of activating aluminum and magnesium metals use the ence of ult r asonic vib r at ions. Ob t ained using alkox technology, aluminum oxide differs preparation of alloys. For aluminum, these are alloys based on mercury or gallium, with in its st r uct ur al and t ext ur al character ist ics. The main disadvant ages of t his method are additions of indium, tin, thallium, and some other metals; for magnesium, alloys with nickel are used. The aluminum activation method uses the immersion of aluminum into gallama, in the range of melting temperatures of gallama and/or aluminum, in the presence of ultrasonic vibrations. Obtained using alkox technology, aluminum oxide differs in its structural and textural characteristics. The main disadvantages of this method are the following: ﬁrst, the need to introduce metals in the form of chips. As is known from practice, the grinding stage is very laborious and is accompanied by an inevitable loss of metal. In addition, this method does not provide for the possibility of the regeneration of gallium, for its reuse [31]. To increase the activity of aluminum and other metals used as fuel in energy-intensive systems for various purposes, it is necessary, not only to increase the dispersion of powders, ChemEngineering 2022, 6, x FOR PEER REV IEW 5 o f 17 t he follow ing: fir st , t he need t o int r oduce met als in t he for m of chips. As is know n fr om pr act ice, t he gr inding st age is ver y lab or ious and is accompanied b y an inev it ab le loss of met al. In addit ion, t his met hod does not pr ovide for t he possib ilit y of the r egener at ion of ChemEngineering 2022, 6, 90 5 of 17 gallium, for it s r euse [ 31 ] . To incr ease t he act ivit y of aluminum and ot her met als used as fuel in ener gy-inten- sive sy st ems for var ious pur poses, it is necessar y, not only t o incr ease t he disper sion of but also to change the structural characteristics both in the volume and on the surface of pow der s, b ut also t o change t he st r uct ur al char acter istics b ot h in t he volume and on t he the particles. The processing of metal powders in dynamic mills changes the surface energy surface of the particles. The processing of metal pow ders in dynamic mills changes the and the internal energy of the residual stress zones in the ground particle presented as sur face ener gy and t he int er nal ener gy of t he r esidual st r ess zones in t he gr ound par t icle a “frozen” metastable state [32]. In this case, the change in the structure and form of the pr esent ed as a “ fr ozen” m et ast ab le st at e [32 ] . In t his case, t he change in t he st r uct ur e and surface oxide layer of particles due to using various organic additives during the MCT of for m of t he sur face oxide lay er of par t icles due t o using var ious or ganic addit ives dur ing aluminum is of great importance [33,34]. t he MCT of aluminum is of gr eat impor t ance [33,34]. The stage-by-stage transformation of the surface layer and the subgrain structure of The stage-by- stage t r ansfor m at ion of t he sur face lay er and t he sub gr ain st r uct ur e of aluminum particles during the MCT process is presented in the model (Figure 3), which aluminum par t icles dur ing t he MCT pr ocess is pr esent ed in t he model (Figur e 3), which reﬂects the concept of the modiﬁcation process of metal particles [34]. During the MCT, the reflects the concept of the modification process of metal particles [34]. During the MCT, following stages occur: destruction of the oxide layer on the surface of aluminum particles; t he follow ing st ages occur : dest r uct ion of t he oxide la y er on t he sur face of a lum inum par- a change in the subgrain structure, as a result of accumulation and redistribution of defects t icles; a change in t he sub gr ain st r uct ur e, as a r esult of accum ulat ion and r edist r ib ution of in the bulk of the particle; and the formation of an encapsulating layer of modifying organic defect s in t he b ulk of t he par t icle; and t he for m at ion of an encapsulat ing lay er of m odify - additives on the surface of the particles. ing or ganic addit ives on t he sur face of t he par t icles. Figure 3. Mode l of the tra ns formation of the s urfa ce la yer a nd the s ubgrain s truc ture of a luminum Figure 3. Model of the transformation of the surface layer and the subgrain structure of aluminum pa rtic le s during MCT [34]. particles during MCT [34]. The dest r uct ion pr oduct s of or ganic com pounds dur ing MCT, penet r at ing t he near - The destruction products of organic compounds during MCT, penetrating the near- sur face lay er along the sub gr ain b oundar ies, cont r ib ut e t o an incr ease in t he act ivit y of surface layer along the subgrain boundaries, contribute to an increase in the activity of aluminum particles. Thus, a defective structure is formed and, consequently, the “exces- aluminum particles. Thus, a defective structure is formed and, consequently, the “excessive” siv e” ener gy of t he sy st em , ensur ing it s st ab le act iv e st a t e. energy of the system, ensuring its stable active state. A change in t he fr ee ener gy of a sub st a nce under m echanica l a ct ion is associated with A change in the free energy of a substance under mechanical action is associated dist or t ions of t he cr y st al lat tice, an incr ease in it s defect iv eness, i.e., t he for m at ion of point with distortions of the crystal lattice, an increase in its defectiveness, i.e., the formation defect s in t he cr y st al lat t ice or dislocat ions, or the destr uction w ith the tr ansition of a cr y s- of point defects in the crystal lattice or dislocations, or the destruction with the transition talline sub stance to an amor phous state. Accor ding to the dislocation theor y, the activa- of a crystalline substance to an amorphous state. According to the dislocation theory, the tion of substances under mechanical action occurs due to dislocations emerging on the activation of substances under mechanical action occurs due to dislocations emerging on sur face, due t o t he defor m a t ion of solids [35 ] , leading t o an incr ease in t he chem ical act iv- the surface, due to the deformation of solids [35], leading to an increase in the chemical ity at t he place w her e the disloca t ions occur . Num er ous exper im ent s hav e show n t hat the activity at the place where the dislocations occur. Numerous experiments have shown exit point s of dislocat ions ar e indeed char act er ized b y an increased chemical activity. that the exit points of dislocations are indeed characterized by an increased chemical High-fr equency phonons accompany t he mot ion of dislocat ions in a solid, due to the in- activity. High-frequency phonons accompany the motion of dislocations in a solid, due to t er act ion of the developing dislocat ions w it h ot her dislocat ions, defect s, impur it y ele- the interaction of the developing dislocations with other dislocations, defects, impurity ment s, or int er faces. In t ur n, high- fr equency phonons can init iat e chem ical r ea ct ions. elements, or interfaces. In turn, high-frequency phonons can initiate chemical reactions. As shown in [7], mechanochemical reactions are associated with the presence of short- lived active centers (SLCs). The death of the SLCs is the relaxation of excess energy. The end of SLCs is usually an exothermic process, accompanied by luminescence or other phenomena, due to the emission of energy observed during MCT. The degree of grinding and activation of metal powders, particularly aluminum, depends on the processing conditions (time, medium, and speed), the energy intensity of the mechanical reactor, and the choice of the additives that contribute to the grinding of metal particles. The use ChemEngineering 2022, 6, x FOR PEER REV IEW 6 o f 17 As show n in [7], mechanochemical reactions are associated with the presence of shor t-lived act ive cent er s (SLCs). The deat h of t he SLCs is t he r elaxat ion of excess ener gy . The end of SLCs is usua lly an exot her m ic pr ocess, accom pa nied b y lum inescence or ot her phenomena, due t o t he em ission of ener gy ob ser v ed during MCT. The degree of grinding a nd a ct iv a t ion of m et al pow der s, par t icular ly alum inum , depends on t he pr ocessing con- dit ions (t im e, m edium , and speed), t he ener gy int ensit y of t he m echanica l r ea ct or , and t he ChemEngineering 2022, 6, 90 6 of 17 choice of the a dditiv es that contr ibute to the gr inding of m et al par t icles. The use of or ganic ca r b on sub st a nces has pr oven t o b e t he m ost effect iv e. Thus, due t o pr ocessing alum inum w it h gr a phit e, it is st at ed t hat alum inum is char act er ized b y an anom alously high r eact iv- of organic carbon substances has proven to be the most effective. Thus, due to processing ity [36,37] , w hich is associa t ed w it h a n incr ea se in t he specific sur face a r ea of pa r t icles and aluminum with graphite, it is stated that aluminum is characterized by an anomalously a change in t he st at e of t heir cr y st al st ructur e (changes in t he size of the coher ent scat t ering high reactivity [36,37], which is associated with an increase in the speciﬁc surface area r egions and r elat ive lat t ice defor mat ion). Mechanically , it is possib le t o ob t ain nanopow- of particles and a change in the state of their crystal structure (changes in the size of the der s w it h a pa r t icle siz e fr om 5–10 t o 200 nm . coherent scattering regions and relative lattice deformation). Mechanically, it is possible to The presence of aluminum nanoparticles in fuel systems significantly changes the obtain nanopowders with a particle size from 5–10 to 200 nm. ignit ion and t he ent ir e com b ust ion pr ocess [38,39 ] . The int r oduct ion of ev en a t iny am ount The presence of aluminum nanoparticles in fuel systems significantly changes the igni- of alum inum nanopar t icles int o hy dr ocar b on fuel sy st em s int ensifies t he oxidat ion of hy - tion and the entire combustion process [38,39]. The introduction of even a tiny amount of dr ocar bons. This leads t o t he development of a chain mechanism in t he com b ust ion pr o- aluminum nanoparticles into hydrocarbon fuel systems intensifies the oxidation of hydrocar- cess. Using t he example of a mixt ur e of nano- alum inum w it h et hanol, t he r esult of a chain bons. This leads to the development of a chain mechanism in the combustion process. Using com b ust ion m echanism is show n [40], w hich ensur es a high flame pr opagat ion r at e, due the example of a mixture of nano-aluminum with ethanol, the result of a chain combustion t o an incr ease in t he diffusion r at e of t he act ive component s of t he chain pr ocess (Figur e mechanism is shown [40], which ensures a high flame propagation rate, due to an increase in 4). the diffusion rate of the active components of the chain process (Figure 4). Figure 4. Hydrocarbon fuels containing aluminum particles will also have a higher ﬂame propagation Figure 4. Hydroc a rbon fue ls c ontaining a luminum pa rtic le s will a ls o ha ve a highe r fla me propaga- velocity. The acceleration is conditioned by an increase in the rate of diffusion of active radicals, from tion ve loc ity. The a c celeration is c onditione d by a n inc rease in the ra te of diffus ion of a c tive radicals, the hot to the cold zone of the ﬂame. from the hot to the c old zone of the fla me . As a result of such a chain reaction, and as shown in [40], hydrocarbon fuels containing As a r esult of such a chain r eact ion, and as show n in [40 ] , hy dr ocar b on fuels cont ain- aluminum particles will also have a higher ﬂame propagation velocity. The acceleration is ing a lum inum par t icles w ill also hav e a higher flam e pr opagat ion v elocit y . The acceler a- conditioned by an increase in the rate of diffusion of active radicals from the hot to the cold t ion is condit ioned b y an incr ease in t he r at e of diffusion of act iv e r adicals fr om t he hot t o zone of the ﬂame. t he cold zone of t he flame. An increase in the activity of metal powders also occurs due to their mechanochemical An incr ease in t he act ivit y of met al pow der s also occur s due t o t heir mechanochem- treatment with various oxides, the presence of which ensures the minimum size of metal ical treatment w ith various oxides, the presence of w hich ensures the minimum size of particles and their maximum defectiveness [41,42]. An increase in the activity of the m et al par t icles a nd t heir m axim um defect iv eness [41,42] . An incr ease in t he act iv it y of t he obtained composite systems is then realized in the combustion processes, particularly in the SHS, increasing the combustion rate up to the detonation reaction mode. An increase in the reactivity of aluminum particles due to mechanochemical treatment is of particular interest in the manufacturing of metalized solid propellants (SRPs). Most of the currently known solid rocket fuels contain up to 15–20% aluminum powder as a metal fuel, thus making it possible to signiﬁcantly increase the combustion temperature, the product outﬂow rate, and, consequently, the efﬁciency of rocket fuel, providing an increase in ﬂight range and the possibility of delivering a larger mass. Activation of aluminum ChemEngineering 2022, 6, x FOR PEER REV IEW 7 o f 17 ob t ained composit e sy st ems is t hen r ealized in the com b ust ion pr ocesses, par t icular ly in the SHS, incr easing t he com b ust ion r at e up t o t he det onat ion r eact ion m ode. An incr ease in t he r eact ivit y of aluminum par t icles due t o mechanochemical t r eat- ment is of par t icular int er est in t he manufact ur ing of met alized solid pr opellant s (SRPs). Most of t he cur r ent ly know n solid r ocket fuels cont ain up t o 15–20% aluminum pow der as a m et al fuel, t hus m aking it possib le t o significant ly incr ease t he com b ust ion t em per a- t ur e, t he pr oduct out flow r at e, and, consequent ly , t he efficiency of r ocket fuel, pr oviding ChemEngineering 2022, 6, 90 7 of 17 an increase in flight range and the possibility of delivering a larger mass. Activation of alum inum pow der s a llow s for an incr ease in t he b allist ic char act eristics of pr opulsion sys- t ems in a w ide r ange of values. powders allows for an increase in the ballistic characteristics of propulsion systems in a Modern mixed solid rocket fuels (SRT) usually consist of ammonium perchlorate, wide range of values. w hich act s as an oxidizing agent , aluminum in a finely disper sed spher ical pow der , and Modern mixed solid rocket fuels (SRT) usually consist of ammonium perchlorate, an or ganic poly m er , as a b inder . The met al and poly mer play t he r ole of fuel. Met al is t he which acts as an oxidizing agent, aluminum in a ﬁnely dispersed spherical powder, and pr imar y ener gy sour ce, and t he b inder is t he pr imar y sour ce of gaseous pr oduct s. Due t o an organic polymer, as a binder. The metal and polymer play the role of fuel. Metal is the t he high b oiling point , alum inum oxide cannot b e in gas for m in a r ocket engine. It ca nnot primary energy source, and the binder is the primary source of gaseous products. Due do w or k w hen expanding in a nozzle. The combustion process of such systems largely to the high boiling point, aluminum oxide cannot be in gas form in a rocket engine. It depends on t he disper sit y , t he shape of aluminum par t icles, and t he densit y of t he com- cannot do work when expanding in a nozzle. The combustion process of such systems b ust ib le m ixt ur e [43,44]. largely depends on the dispersity, the shape of aluminum particles, and the density of the Studies of the effect of MCT on ballistic properties when using a mixture of combustible mixture [43,44]. PA/Al/HTPB (68%/18%/14%), and w her e the PA w as ammonium per chlor at e and HTPB Studies of the effect of MCT on ballistic properties when using a mixture of PA/Al/HTPB w as poly b ut adiene w it h t er minal hy dr oxy l gr oups of gr ade R-45, w hich w as used as a (68%/18%/14%), and where the PA was ammonium perchlorate and HTPB was polybuta- binder betw een the fuel and an oxidizing agent, show ed a significant effect of the pre- diene with terminal hydroxyl groups of grade R-45, which was used as a binder between tr eatm ent of aluminum w it h modify ing or ganic addit ives (in t he pr esence of SiO2) on t he the fuel and an oxidizing agent, showed a significant effect of the pretreatment of aluminum com b ustion r ate of the SRF m ixtur e [45]. with modifying organic additives (in the presence of SiO ) on the combustion rate of the SRF mixture [45]. r b = aP (1) r = aP (1) w her e r b is SRF b ur ning r ate; a is the constant of pr opor tionality; P is t he pr essur e inside where r is SRF burning rate; a is the constant of proportionality; P is the pressure inside t he com b ust ion cb ham b er ; n is t he pr essur e exponent . the combustion chamber; n is the pressure exponent. The b allist ic char acter istics of solid pr opellant s ar e pr esent ed in Figur e 5a. The use of The ballistic characteristics of solid propellants are presented in Figure 5a. The act ivat ed aluminum cont r ib uted t o an overall increase in the burning rate of the SRF. It use of activated aluminum contributed to an overall increase in the burning rate of follows from the figure that the combustion rate of the composition with (Al + 20% the SRF. It follows from the ﬁgure that the combustion rate of the composition with (C2H3OH)n + 20% SiO2) increases by 25%, and the pressure exponent decreases from (Al + 20% (C H OH)n + 20% SiO ) increases by 25%, and the pressure exponent decreases 2 3 2 0 .5 57 2 t o 0.492 7. from 0.5572 to 0.4927. (a) (b) Figure 5. Cha nge in the burning ra te for PA/HTPB/Alx fue ls with non-a c tiva ted a luminum (1), after Figure 5. Change in the burning rate for PA/HTPB/Alx fuels with non-activated aluminum (1), after MCT with a compos ite (a)—[Al+20%(C 2H3OH)n +5%SiO 2] (2) a nd [Al+20%(C 2H3OH)n +20%SiO 2] MCT with a composite (a)—[Al+20%(C H OH)n +5%SiO ] (2) and [Al+20%(C H OH)n +20%SiO ] (3) 2 3 2 2 3 2 (3) a nd with compos ite (b)—Al+3% C 17H35COO H +5%S iO 2 (2) a nd Al+3%C 17H35COO H +20%S iO 2 (3) and with composite (b)—Al+3% C H COOH +5%SiO (2) and Al+3%C H COOH +20%SiO (3) [45]. 17 35 2 17 35 2 [45]. The best result in terms of burning rate and pressure exponent was demonstrated The b est r esult in t er m s of b ur ning r a t e and pr essur e exponent w a s dem onst r at ed by by compositions based on PA/HTPB/(Al+C H COOH+SiO ) (Figure 5b). At present, 17 35 2 com posit ions b ased on PA/HTPB/(Al+ C17H35COOH+SiO2) (Figur e 5b ). At pr esent , st earic stearic acid is used in the industrial scale passivation of aluminum powders. First, stearic a cid is used in t he indust r ia l scale passiv at ion of alum inum pow der s. Fir st , st ear ic acid is acid is hydrophobic, second, during MCT, it ﬁlls cracks in the oxide ﬁlm on the surface of aluminum particles, and third, it increases the chemical resistance of aluminum with respect to other fuel components, thereby increasing the shelf life of SRF. Aluminum particles in the composition of solid rocket propellants are initially localized between large oxidizer particles. Upon reaching the melting point of 660 C, aluminum particles pass into a liquid state, but at the same time they are still within the volume of the oxide ﬁlm, i.e., in an isolated state. The melting point of alumina is three times that of aluminum. In our case, liquid aluminum can ﬂow out due to cracks in the oxide shell formed during the MCT and ﬁlled with stearic acid, which can facilitate ignition of the particles. The subsequent agglomeration of particles can occur in the heating zone adjacent to the burning surface layer. ChemEngineering 2022, 6, 90 8 of 17 After the introduction of a mechanically activated composite (Al + 3% C17H35COOH + 5% SiO ) into the composition of the SRF, a good increase in the combustion rate was observed, from 13.5% at 5 atm to 15.9% at 40 atm. The use of powder (Al + 3%C17H35COOH + 20%SiO ) caused only minor changes in the combustion rate compared to (Al + 3% C17H35COOH + 5% SiO ), within Drb = 17.6% in the considered pressure range. At the same time, the content of active aluminum, which was determined by the volumetric method, in the system was no more than ~85.1%. A possible factor in this result is that the active combustible system is a completely composite [Al + 3% C17H35COOH + 20% SiO ] [45]. An advantage of using aluminum powders as an ingredient in solid fuels is the high heat generated during combustion. Due to this, the heat released during t oxidation of the metal increases the ﬂame’s temperature. For this reason, the value of the speciﬁc impulse in the aluminized fuel is increased by 10%. In addition, there is another important characteristic: the unstable combustion of aluminum and systems based on it, which is essential when using aluminum in condensed systems. An analysis of the effect of additives of powdered aluminum, including nanosized particles, on the propelling ability of explosive compositions is described in [46]. The addition of highly dispersed aluminum can increase the propelling power of pieces of pure combustible substances (ES). The addition of nanosized aluminum also makes it possible to increase the propelling ability of explosives. However, the observed increase is somewhat lower than micron-sized aluminum, due to the high content of oxide on the surface of the nanoparticles. On the other hand, the addition of aluminum powders to the composition of rocket fuel also has a negative impact: a two-phase ﬂow, which provides additional losses in speciﬁc impulse, luminescent (luminous) exhaust trails, slag accumulation, nozzle erosion, and a high temperature of the combustion products. Since most of these problems are associated with the formation of condensed combustion products, many investigations have focused on the need to understand the mechanisms of combustion and the accumulation of aluminum particles. Many works have aimed to ﬁnd a solid fuel that produces as few condensed combustion products as possible, with a minor proportion of unburned aluminum. According to the results of the studies in [47], concentrated combustion products (CCPs) can be divided into two types: agglomerates, and ﬁne oxide particles (FOPs). The agglomerates are typically 100 m or more signiﬁcant in size and are formed by the adhesion of aluminum particles. Agglomerates may contain alumina and other condensed products, and they can reduce ﬂuctuations up to 500 Hz. The particle size of FOPs is about 1 m, and they are formed as a result of the combustion of one particle, as well as due to the explosion of the non-agglomerated fraction of the metal; the frequency they can lower to is about 4000 Hz. These agglomerates interfere with the uniformity of fuel combustion, leading to a decrease in gas generation, a reduction in the fuel burning rate and the amount of heat released during the reaction, and a decrease in the speciﬁc impulse of the rocket. When the metal concentration in the fuel exceeds the set threshold, the agglomeration process becomes dominant and increases with the increase in the metal particle size in the fuel mixture. The increase in volumetric and gravimetric speciﬁc impulses, which determine the spacecraft’s performance, is signiﬁcant for the actual volume of the propulsion system and the amount of fuel needed for a particular mission. Solid propellants must meet speciﬁc compactness requirements and have a high density, but have limited gravimetric speciﬁc impulse values compared to other fuel systems (hybrid and liquid) [48,49]. 3. Prospects for the Use of Mechanochemical Processing for the Production of Physiologically Active Drugs from Plant Materials One of the most effective areas of the application of mechanochemical processing has been the processing of plant materials. Impressive results have already been achieved in this direction. The central concept of mechano-chemical technologies is that carrying out reactions in the solid phase shortens the technological chain [50]. Plant material is ChemEngineering 2022, 6, 90 9 of 17 a composite material: it is complex structured and contains many different components. Cells of higher vascular plants (for example, cereals) can be non-ligniﬁed and ligniﬁed. In the ﬁrst case, cell membranes contain only structural carbohydrates (cellulose and hemicellulose), so they are easily crushed during mechanical processing. Ligniﬁed cells also have lignins, which are complex, chemically stable polymer formations that give the cell membrane strength. Using the mechanochemical processing of various plants, products for pharmaceuti- cals, animal husbandry, veterinary medicine, plant growing, etc., can be obtained [4,51]. The efﬁciency of mechanochemical processing of plant raw materials can be increased by carrying out a preliminary chemical or biochemical treatment, in such a way as to break the bonds between the main macrostructural elements; for example, between lignin and hemicellulose. With the help of the mechanochemical approach, many useful preparations were obtained at the ICTTM SB RAS. For example, environmentally friendly substitutes for feed antibiotics. Substitutes for antibiotics are mannan-oligosaccharide preparations obtained from the cell walls of microorganisms (yeast and fungi). Preparations containing triterpene acids are obtained from coniferous trees, which can be used instead of very ex- pensive plant growth regulators [52]. Millet husk contains a large number of phytosterols. However, it is not possible to use the husk as a feed additive; phytosterols are not absorbed in the animal’s digestive tract. In a mechanochemical product, they change into a soluble complex. However, the main mechanochemical “topic” in bio-additives is the development of technology for antioxidant preparations containing soluble chelated forms of silicon. This drug is obtained from rice husks, and the silicon dioxide located there is converted into a soluble form with the help of green tea gallocatechin [53,54]. In recent decades, special attention has been paid to the mechanochemical processing of material from plant materials, with their subsequent use in the production of medicines, i.e., in pharmaceutical technology [4,55]. Thus, the effect of the mechanochemical process- ing of potato and corn starches on their physicochemical and technological characteristics in pharmaceutical preparations was considered [56]. Starch is used as a binding, loosening, and antifriction agent, as well as to provide the necessary technological properties for granules and tablets, and also reduces the concentration of starches in prolonged dosage forms, while maintaining the high viscosity of the dispersion medium. Mechanochemical treatment of medicinal substances (MS) in the presence of various auxiliary additives (for example, acetylsalicylic acid with plant ﬂavonoids) contributes to an increase in solubility; i.e., their effectiveness [57]. This is due to a decrease in particle size, modiﬁcation of the crystal structure, and the formation of solid dispersions in which medicinal substances are dispersed in molecular form or in an amorphous state, with the construction of water-soluble complexes, etc. (Figure 6). Mechanochemical treatment of substances leads to an increase in the area of grain boundaries and the formation of new surfaces [58]. A technique has been developed for the mechanochemical preparation of supramicrostructured forms for the prolongation of different chemical natures (Na-CMC—sodium carboxymethylcellulose, PVA—polyvinyl alcohol, a combined prolongation of Na-CMC and PVA in various ratios), and it has been shown that, as a result of such processing, a change in the shape and size of the particles occurs, as well as the accumulation of microparticles [59]. As a result of the solid-phase mechanochemical treatment of prolongation, the rheological parameters of aqueous solutions change; in particular, the viscosity increases. With an increase in the duration of the mechanochemical treatment of the prolongation of different chemical natures, an increase in the kinematic viscosity of the aqueous solutions is noted. The use of an effect discovered for increasing the density in the development of formulations and the technology of prolonged liquid dosage forms, in particular ophthalmological ones, will make it possible to reduce the concentration of the prolongation, while maintaining the high viscosity of the dispersion medium. Presumably, eventually, the use of such prolongation in the composition of drugs will contribute to their bioavailability and therapeutic efﬁcacy. ChemEngineering 2022, 6, x FOR PEER REV IEW 10 o f 17 ChemEngineering 2022, 6, 90 10 of 17 Figure 6. Scheme of mechanochemical transformations in mixtures of solids (drugs + excipients) Figure 6. Sche me of me chanochemical tra ns formations in mixture s of s olids (drugs + e xcipie nts) during mechanochemical processing [57]. during me cha nochemic al proc essing [57]. Mechanochemical treatment isolates biologically active substances from plant ma- Mechanochemical treatment of substances leads to an increase in the area of grain terials, particularly water-soluble salt forms of triterpene acids and dichloroisocyanuric b oundar ies and t he for mat ion of new sur faces [58]. A technique has been developed for acid [60]. The practical signiﬁcance of the studies carried out lies in using these drugs as t he m echanochem ica l pr epa r a t ion of supr a m icr ost ruct ured for ms for t he pr olongat ion of regulators of the growth and development of plants and animals in agriculture. Using differ ent chemical nat ur es (Na-CMC—sodium car b oxy m et hylcellulose, PV A—polyvinyl the example of triterpene acids, phytoecdysteroids, and phytosterols, it has been shown alcohol, a comb ined pr olongat ion of Na- CMC and PV A in v ar ious r at ios), and it has b een that the solubilization of sparingly soluble organic compounds can be based on known show n that, as a r esult of such pr ocessing, a change in t he shape and size of t he par t icles physicochemical effects that can be carried out mechanochemically in situ, i.e., in the matrix occurs, as w ell as the accumulat ion of micr opar t icles [59]. As a r esult of t he solid-phase of raw materials that are usually used for extraction. m echanochem ical t r eat m ent of pr olongat ion, t he r heological pa r a m et er s of a queous solu- In [61], a comparative analysis of various methods for the extraction of plant raw t ions change; in par t icular , t he v iscosit y incr eases. W it h an incr ease in t he dur at ion of t he materials is given. Figure 7 shows a scheme of the most common extractions and uses of m echanochem ical t r eat m ent of the pr olongat ion of differ ent chem ical nat ur es, an incr ease ChemEngineering 2022, 6, x FOR PEER REV IEW 11 o f 17 mechanochemical processing. in t he kinem a t ic v iscosit y of t he aqueous solut ions is not ed. The use of an effect discover ed for incr easing t he densit y in t he development of for mulat ions and the t echnology of pr o- longed liquid dosa ge for m s, in par t icular opht halm ologica l ones, w ill m ake it possib le t o r educe t he concent r at ion of t he pr olongat ion, w hile m aint aining t he high v iscosit y of t he disper sion medium. Pr esumably, eventually , t he use of such pr olongat ion in t he com po- sit ion of dr ugs w ill cont r ib ut e t o t heir b ioav ailab ility and t her apeut ic effica cy . Mecha nochem ica l t r eat m ent isola t es b iologica lly act iv e sub st ances fr om plant m at e- r ials, pa r t icularly water -solub le salt for m s of t r it er pene acids and dichlor oisocyanuric acid [60]. The pr act ical significance of t he st udies car r ied out lies in using t hese dr ugs as r egu- lat or s of t he gr ow t h and development of plant s and animals in agr icult ur e. Using t he ex- a m ple of tr iter pene acids, phytoecdyster oids, and phytosterols, it has b een show n that the solub ilizat ion of spar ingly solub le or ganic compounds can b e based on know n physico- chemical effects that can be carried out mechanochemically in situ, i.e., in the matrix of r a w m at er ia ls t ha t ar e usually used for ext r act ion. In [61], a compar at ive analy sis of var ious met hods for t he ext r act ion of plant raw m at er ials is given. Figur e 7 show s a scheme of the most common extractions and uses of m echa nochem ical pr ocessing. Figure 7. Compa ris on of the best-known me thods for the sepa ration of biologic ally ac tive substances Figure 7. Comparison of the best-known methods for the separation of biologically active substances a nd me c ha nochemic al e xtraction from pla nt ma terials [61]. and mechanochemical extraction from plant materials [61]. Accor ding t o t he gener ally accept ed ext r act ion scheme, veget ab le r aw mat er ials are cr ushed and ext r act ed in var ious or ganic solv ent s w it h differ ent polar it ies. The final st age of t hese t echnologies is separ at ing t he ext r a ct b y ev a por at ion of t he solv ent . Dur ing m ech- anochemical ext r act ion, a mixt ur e of plant mat er ials and a solid r eagent is pr ocessed in m echanochem ica l r eact or s; as a r esult of this pr ocessing, t he t ar get sub st ance is conv er ted int o a chemical for m w it h t he highest solub ilit y in w ater . The ext r act , in t his case, is iso- lat ed w it h w at er . The pr oduct can b e ob t ained in a higher yield and higher purity than ext r act s isolat ed using or ganic solv ent s. The pr oduct ob t ained b y m echanochem ica l t r eat- ment has t he same pr oper t ies as t he pr oduct s of t r adit ional ext r action t echnologies. The undoub t ed advant age of t he mechanochemical met hod is the r educt ion in t he numb er of st ages r equir ed t o give t he pr oduct t he desir ed pr oper t ies and t he ease of or ganizing pr o- duction. Pr oduct ion of phenolic com pounds of plant or igin dur ing t he m echanochem ica l pr o- cessing of a str uctur ed m ulticom ponent system using v eget a b le r a w m at er ia ls (gr een t ea Camellia Sinensis L., St . Jon’s w or t Hypericum perforatum L.) for pr epa r a t ions of phenol com - pounds, cat echins and gallocat echin of t ea and diant hr one com pounds of St . Jon’s w or t in a solub le b iologically accessib le for m, w as consider ed in [62] . Cha nges in t he st r uct ur e of the veget ab le r aw mat er ials at t he macr o and micr o levels dur ing mechanical pr ocessing under var ious condit ions w er e studied. The threshold nature of the dependence of the degr adat ion r at e of ant ioxidant compounds in plant r aw mat er ials on t he int ensit y and the t im e of m echanica l t r ea t m ent w a s found; and t he condit ions for pr ocessing gr een t ea and St . John’s w ort w er e det er m ined, as a r esult of w hich a pow der ed pr oduct w as for med w ithout degradation of the target compounds. Based on these studies, methods for ob- t a ining pow der ed pr oducts w er e developed [63]. The catechin- cont aining pr oduct s w ere char act er ized b y a 40% incr eased w at er -soluble gr een t ea cat echins y ield and a tw ofold increase in shelf life. The hyper icin-cont aining pr oduct s w er e char acter ized b y a 12-fold incr ease in t he cont ent of solub le hy per icin. These pr oduct s can b e used as a food addit ive in medicine and animal husb andr y, as pr epar at ions w it h an ant ioxidant effect . The use of the m echanochem ica l pr ocessing of plant m at er ials t oget her w it h var ious reagents makes it possible to obtain reactive mechanocomposites. As show n in [64,65], chemical r eact ions involving such mechanocomposit es pr oceed mor e efficient ly, due t o a ChemEngineering 2022, 6, 90 11 of 17 According to the generally accepted extraction scheme, vegetable raw materials are crushed and extracted in various organic solvents with different polarities. The ﬁnal stage of these technologies is separating the extract by evaporation of the solvent. During mechanochemical extraction, a mixture of plant materials and a solid reagent is processed in mechanochemical reactors; as a result of this processing, the target substance is converted into a chemical form with the highest solubility in water. The extract, in this case, is isolated with water. The product can be obtained in a higher yield and higher purity than extracts isolated using organic solvents. The product obtained by mechanochemical treatment has the same properties as the products of traditional extraction technologies. The undoubted advantage of the mechanochemical method is the reduction in the number of stages re- quired to give the product the desired properties and the ease of organizing production. Production of phenolic compounds of plant origin during the mechanochemical processing of a structured multicomponent system using vegetable raw materials (green tea Camellia Sinensis L., St. Jon’s wort Hypericum perforatum L.) for preparations of phenol compounds, catechins and gallocatechin of tea and dianthrone compounds of St. Jon’s wort in a soluble biologically accessible form, was considered in [62]. Changes in the structure of the vegetable raw materials at the macro and micro levels during mechanical processing under various conditions were studied. The threshold nature of the dependence of the degradation rate of antioxidant compounds in plant raw materials on the intensity and the time of mechanical treatment was found; and the conditions for processing green tea and St. John’s wort were determined, as a result of which a powdered product was formed without degradation of the target compounds. Based on these studies, methods for obtaining powdered products were developed [63]. The catechin-containing products were characterized by a 40% increased water-soluble green tea catechins yield and a twofold increase in shelf life. The hypericin-containing products were characterized by a 12-fold increase in the content of soluble hypericin. These products can be used as a food additive in medicine and animal husbandry, as preparations with an antioxidant effect. The use of the mechanochemical processing of plant materials together with various reagents makes it possible to obtain reactive mechanocomposites. As shown in [64,65], chemical reactions involving such mechanocomposites proceed more efﬁciently, due to a decrease in diffusion paths and an increase in the stability of the target substances or enzymes (in the case of enzymatic processes), as a result of mechanochemical processing, the reactivity of the substances that make up the plant material increases due to the increase in the speciﬁc surface area, a decrease in the crystallinity of cellulose, and a general disordering of the supramolecular structure of the cell walls. The efﬁciency of mechanochemical processing of plant raw materials largely depends on the choice of process parameters that ensure the destruction of cells and the isolation of the necessary compounds. These parameters include material, size and density of grinding balls, chamber ﬁlling and mixing speed, grinding time, suspension composition, etc. (Figure 8). The optimal selection of parameters provides the advantage of a mechanochemical process with a high degree of destruction of various plants and microalgae, increases the yield of bioactive products during extraction, and allows solubilization of substances in water at room temperature instead of using organic solvents, reducing the extraction time and simplifying the puriﬁcation steps [66]. ChemEngineering 2022, 6, x FOR PEER REV IEW 12 o f 17 decr ease in diffusion pat hs and an incr ease in t he st ab ilit y of the tar get sub st ances or en- zymes (in the case of enzymatic processes), as a result of mechanochemical processing, t he r eact ivit y of t he sub st ances t hat make up t he plant mat er ial incr eases due t o t he in- cr ease in t he specific sur face ar ea, a decr ease in t he cr y st allinity of cellulose, a nd a gener al disor dering of t he supr a m olecular st ruct ure of the cell w alls. The efficiency of mechanochemical processing of plant raw materials largely de- pends on the choice of process parameters that ensure the destruction of cells and the isolat ion of t he necessar y compounds. These par amet er s include mat er ial, size and den- ChemEngineering 2022, 6, 90 12 of 17 sit y of gr inding b alls, chamb er filling and mixing speed, gr inding t ime, suspension com- posit ion, et c. (Figur e 8). Figure 8. Pa ra me ters of the me chanochemic al proc essing of ve getable ra w ma terials [66]. Figure 8. Parameters of the mechanochemical processing of vegetable raw materials [66]. The opt imal select ion of par amet er s pr ovides t he advant age of a mechanochemical Much attention has been paid to the mechanochemical processing of wood, which pr ocess w ith a high degr ee of dest r uct ion of v a r ious pla nt s a nd m icr oa lga e, incr eases t he is a raw material for producing various products. The most modern and most promising technological y ield of b ioact pr iv ocess e pr ois du the cts d mechanochemic ur ing extr actioal n, modiﬁcation and allow s soof lub wood. ilizat ioThis n of stechnology ub st ances in consists w at er a of t rthe oom impr t em egnation per a t ur e i of nthe st ea wood d of us substance ing or ganwith ic solan v en aqueous t s, r educsolution ing t he eas xt r a amodiﬁer ct ion t im ,e which a nd sim enters plifyinto ing t h aechemical pur ifica t io reaction n st eps [ with 66]. the natural components of the tree during thermal Mu and ch a mechanical ttention ha activation. s b een paid The t o tmodiﬁer he mecha , in no the chepr moposed ical pr otechnology cessing of w , is oo carbamide; d, w hich is a asubstance raw matethat rial f not or p only roducan cingr eact vario with us pthe rodu elementary cts. The mo components st modern an of d m wood, ost pbut romalso ising dramatically enhances the effect of the functional additives added to the modiﬁer, to give t echnological pr ocess is t he m echa nochem ica l m odifica t ion of w ood. This t echnology con- the siswood t s of t he pr ioduct m pr eg the na tspeciﬁed ion of t he physical, w ood submechanical, st ance w it h a and n aq operational ueous soluti pr on operties. as a mod The ifier, modiﬁer, penetrating with the help of water to the cellular level of the wood substance w hich ent er s int o a chem ical r eact ion w it h t he nat ur al com ponent s of t he t r ee dur ing t her- and reacting with it, changes the structure of the wood in the manner desired by the m al and m echa nical a ct iv at ion. The m odifier , in t he pr oposed t echnology , is car b amide; a manufacturer of products from mechanochemically modiﬁed wood (MCMW). An MCMW sub stance that not only can r eact w ith the elem entar y com ponent s of w ood, b ut also dr a- product may be hydrophobic or non-combustible. It is possible to change the color and m at ically enhances t he effect of the funct ional a ddit iv es added t o t he m odifier , to giv e the texture of the original wood, the density and strength of MCMW, as well as the hardness, w ood product the specified physical, mechanical, a nd oper a t iona l pr oper t ies. The m odi- abrasion, and technological properties. fier , penet r at ing w it h t he help of w at er t o the cellular level of the w ood substance and The combination of the developed technologies for mechanochemical modiﬁcation r eacting w ith it, changes the str uctur e of the w ood in t he m anner desir ed b y t he m a nufa c- of wood makes it possible to create a multidisciplinary production unit and easily switch t ur er of pr oduct s fr om mechanochemically modified w ood (MCMW ). An MCMW pr od- from the production of non-pressed moldings, for example, to the production of parquet uct m ay b e hy dr ophob ic or non-combustible. It is possib le t o change t he color and t ext ur e boards from solid wood, facing products or doors, furniture elements or ﬁnishes, according of t he or iginal w ood, t he densit y and st r engt h of MCMW , as w ell as t he har dness, ab ra- to orders, which dramatically expands the scope and opportunities of the sales market. sion, and t echnological pr oper t ies. Some of these technologies are exclusive. Mechanochemically modiﬁed wood is at the stage of being introduced to the market, and the technology is at the stage of implemen- tation and optimization; that is, from both an economic and technical point of view, we are talking about innovative technologies that allow creating a new material with the desired properties. Mechanochemical processing is also used in the pulp and paper industry to prepare cellulose-containing ﬁbers in the presence of, for example, alkali to reduce the content of extractive substances in cellulose: resins, and fats. Under mechanical action, the destruction of cellulose occurs, namely, the rupture of glycosidic and carbon-carbon bonds, i.e., a decrease in the degree of polymerization of cellulose and a change in the reactivity of cellulose under the action of mechanical forces. The possibility of breaking chemical bonds ChemEngineering 2022, 6, 90 13 of 17 in macromolecular compounds under mechanical impacts (grinding, crushing), leading to the destruction of macromolecules, was reported for various classes of polymers; in particular, starch and cellulose methylcellulose polystyrene. Systematized data on the processes of mechanochemical degradation of polymers are given in the monograph by Baramboim. For cellulose and its derivatives, it has been reported that, under the action of a mechanical force, both the initiation of the actual destruction (breaking of the central valence bonds) and the activated mechanochemical destruction associated with hydrolysis alcoholysis, aminolysis, etc. are possible. Technological processes for alkaline extraction and pulp bleaching with hydrogen peroxide were developed on specially designed apparatus for the mechanical processing of high-concentration pulp [67]. It has been stated that in the process of mechanochemical treatment, degumming takes place and an increase in the reactivity of cellulose to viscose formation [68]. The development of technical solutions that signiﬁcantly reduce the mass fraction of resins and fats in unbleached viscose cellulose before bleaching will ensure a high quality of viscose pulp, in terms of resins and lard and, at the same time, increase the product yield, and save chemicals and energy. The stated changes in cellulose structure as a result of mechanochemical processing are a new stage in the evolution of the technology in the pulp and paper industry. The high value of the reactivity index after MCT does not allow the possibility of using cellulose for paper in the production of chemical ﬁbers. Nevertheless, this only indicates a signiﬁcant effect of reagents on cellulose macromolecules in cell walls. Both the technical cellulose and waste ﬁbers of medium and high concentration are subjected to mechanochemical processing. 4. Conclusions 1. An analysis was made of examples of mechanochemical treatment (MCT) of various materials, of both mineral and vegetable origin, and both metal and polymer systems, as well as the use of various methods of mechanical action in the systems under study (treat- ment in activator mills or ultrasonic treatment), demonstrating the signiﬁcant possibilities of MCT for obtaining materials for a wide range of purposes. 2. The effect of mechanochemical treatment and the nature of the modiﬁer on the microstructure and reactivity of activated and modiﬁed aluminum was studied. A change in the state and composition of the surface oxide layer of aluminum particles after MCT, its saturation with an organic modiﬁer, and the stabilization of structural changes were shown. The high activity of metal particles in Al/modiﬁer and Al/modiﬁer/SiO composites is due to the transformation of the structure of the surface layer and the minimum size of crystallites (i.e., high defectiveness of particles), which together determine a high level of reactivity when they are used as part of combustible condensed systems. 3. The optimal conditions for carrying out the MCT process of aluminum with various modiﬁers (stearic acid, polyvinyl alcohol), and which ensure the formation of an organic surface layer protective against oxidation during storage in air and the activation of chemi- cal reactions in combustion processes, were determined. A maximum increase in activity after MCT of aluminum by 20 and 25% was established as a result of the MCT of the Al/modiﬁer/SiO composite with 20% polyvinyl alcohol and 3% stearic acid, respectively, at a SiO content of 20 and 5%. Silicon dioxide in an aluminum-based composite plays the role of a promoter of the combustion of condensed systems. 4. The prospects for the use of MCT for the production of physiologically active preparations from plant materials were presented, which is an effective way to create new materials in the ﬁeld of pharmaceuticals, animal husbandry, veterinary medicine, plant growth, etc. After MCT, substances can be obtained with a higher yield and higher purity, compared with extracts isolated using organic solvents. The advantage of this method is the reduction in the number of stages and equipment required to give the product the desired properties, as well as the ease of production. Author Contributions: A.B. (Ayagoz Bakkara): Data curation, writing, original draft preparation. B.S.: Writing draft version of paper. A.Z.: Visualization, investigation. T.O.: Conceptualization, ChemEngineering 2022, 6, 90 14 of 17 methodology, software. A.B. (Aisulu Batkal): Conceptualization, methodology, software. A.K.: Visualization, Investigation. N.M.: Writing-reviewing and editing. All authors have read and agreed to the published version of the manuscript. Funding: This research has is funded by the Science Committee of the Ministry of Education and Science of the Republic of Kazakhstan (Grant No. OR11465430-OT-21). Conﬂicts of Interest: The authors declare no conﬂict of interest. References 1. Avvakumo, E.G. (Ed.) Fundamental Foundations of Mechanical Activation, Mechanosynthesis and Mechanochemical Technolo- gies. In Integration Projects of the Siberian Branch of the Russian Academy of Sciences Issue 19; Publishing House of the Siberian Branch of the Russian Academy of Sciences: Novosibirsk, Russia, 2009; 343p. Available online: http://www.prometeus.nsc.ru/contents/ integrpr/019.ssi (accessed on 8 October 2021). (In Russian) 2. Mansurov, Z.A.; Mofa, N.N. Mechanochemical synthesis of composite materials. In Mekhanohimicheskij Sintez Kompozicionnyh Materialov; Almaty Kazakh University: Almaty, Kazakhstan, 2016; 376p, ISBN 978-601-04-1688-8. 3. 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Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

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ISSN: 2305-7084
DOI: 10.3390/chemengineering6060090
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Abstract

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ChemEngineering – Multidisciplinary Digital Publishing Institute

Published: Nov 15, 2022

Keywords: mechanochemical treatment; grinding; modification; composite materials

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Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

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Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

Efficiency and Prospects of the Use of Mechanochemical Treatment to Obtain Innovative Composite Systems

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