Systems and methods for low-temperature hydrocarbon cracking via atomically-dispersed titanium-aluminum-boron nanocatalysts

Abstract

A catalytic system comprising a vessel configured with a controllable heating environment; and a catalyst composition disposed in the vessel, the catalyst composition comprising at least one transition metal atomically dispersed in a matrix of at least one main group element, wherein the catalyst composition is an amorphous solid configured to promote carbon-hydrogen bond activation and carbon-carbon bond transformation of an organic material under thermal conditions, and wherein the catalytic system is operated in an inert atmosphere.

Description

Attorney Docket No. : 3229-7 PCTSYSTEMS AND METHODS FOR LOW-TEMPERATURE HYDROCARBON CRACKING VIA ATOMICALLY-DISPERSED TITANIUM-ALUMINUM-BORON NANOCATALYSTSCROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims the benefit of and priority to U. S. Provisional Patent Application No. 63 / 688,071 filed on August 28, 2024, the entire contents of which are incorporated by reference herein.TECHNICAL FIELD

[0002] The subject matter of the present disclosure relates generally to systems and methods for catalytic activation of carbon-hydrogen and carbon-carbon bonds via atomically-dispersed titanium-aluminum-boron nanocatalysts and, in particular, to systems and methods for promoting hydrocarbon cracking, dehydrogenation, reforming, and related transformations across diverse organic substrates including fuels, polymers, feedstocks, and other carbon-containing materials.BACKGROUND

[0003] Current catalytic materials intended for the activation of carbon-hydrogen and carbon-carbon bonds in hydrocarbons and other organic substrates are frequently inadequate in their performance, accessibility, and scalability. Conventional heterogeneous catalysts such as platinum, palladium, and related noble metals exhibit high activity, but their prohibitive cost, limited natural abundance, and susceptibility to deactivation through coke formation or poisoning restrict their practical deployment. Acidic supports such as zeolites are widely used in catalytic cracking, yet they offer limited selectivity, require elevated reaction temperatures, and often generate undesired byproducts. Homogeneous catalysts,Attorney Docket No. : 3229-7 PCT including organometallic complexes, can achieve high specificity for certain bond activations but suffer from poor thermal stability, limited recyclability, and incompatibility with industrial process conditions. These shortcomings collectively impose constraints on catalytic efficiency, operational lifetime, and cost-effectiveness across applications ranging from fuel processing and chemical manufacturing to polymer degradation and waste-to- energy conversion. As a result, the routine use of robust, low-cost, and selective catalysts for general C-H bond activation and C-C bond transformation in diverse organic systems remains an unmet technological challenge.

[0004] Accordingly, there remains a need for systems and methods that employ atomically-dispersed titanium-aluminum-boron nanocatalysts capable of promoting C-H and C-C bond activation under milder conditions than conventional catalysts, while maintaining structural integrity and chemical selectivity. In particular, there is a need for catalytic materials and systems that can be applied universally across a wide spectrum of organic substrates, including saturated and unsaturated hydrocarbons, fuels, polymers, biomass- derived compounds, and mixed feedstocks, without reliance on expensive noble metals or fragile organometallic complexes.SUMMARY

[0005] In accordance with aspects of the disclosure, a catalytic system includes a vessel configured with a controllable heating environment; and a catalyst composition disposed in the vessel, the catalyst composition including at least one transition metal atomically dispersed in a matrix of at least one main group element. The catalyst composition may be a an amorphous solid configured to promote carbon-hydrogen bond activation and carbon-Attorney Docket No. : 3229-7 PCT carbon bond transformation of an organic material under thermal conditions. The system may be operated in an inert atmosphere.

[0006] In an aspect of the present disclosure, the vessel may be a resistively heated tube.

[0007] In an aspect of the present disclosure, the transition metal may include titanium.

[0008] In an aspect of the present disclosure, the main group element may include aluminum and / or boron.

[0009] In an aspect of the present disclosure, the catalyst composition may be synthesized by a sonochemically mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride.

[0010] In an aspect of the present disclosure, the catalyst composition may be amorphous with atomically dispersed metals having mutual interatomic linkages.

[0011] In an aspect of the present disclosure, the organic material may include a hydrocarbon fuel selected from JP-10 and F-24, a polymer selected from polyethylene or polypropylene, and / or a biomass-derived compound.

[0012] In an aspect of the present disclosure, the catalytic system may be configured to initiate decomposition of hydrocarbons at a temperature ranging from about room temperature to about 750 K.

[0013] In an aspect of the present disclosure, the catalytic system may further include a product analysis interface 150 configured to detect volatile products formed during catalytic transformation of the organic material.

[0014] In an aspect of the present disclosure, the catalyst composition may include a titanium-aluminum-boron nanopowder.Attorney Docket No. : 3229-7 PCT

[0015] In accordance with aspects of the disclosure, a method for catalytic transformation of an organic material includes: adding a catalyst composition comprising at least one transition metal atomically dispersed in a matrix of at least one main group element to a vessel; adding an organic material having carbon-hydrogen bonds to the vessel; and heating the organic material in the presence of the catalyst composition in an inert atmosphere to induce catalytic decomposition, cracking, dehydrogenation, reforming, or related transformations of the organic material.

[0016] In an aspect of the present disclosure, the transition metal may include titanium.

[0017] In an aspect of the present disclosure, the main group element may include aluminum and / or boron.

[0018] In an aspect of the present disclosure, the method may further include synthesizing the catalyst composition by a sonochemically-mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride.

[0019] In an aspect of the present disclosure, the method may further include adding the catalyst composition in the form of an amorphous nanopowder with atomically-dispersed metals.

[0020] In an aspect of the present disclosure, the organic material may include a hydrocarbon fuel selected from JP-10 and F-24, a polymer selected from polyethylene or polypropylene, and / or a biomass-derived compound.

[0021] In an aspect of the present disclosure, the method may further include heating the organic material in the presence of the catalyst composition to initiate decomposition at a temperature ranging from about room temperature to at about 750 K.Attorney Docket No. : 3229-7 PCT

[0022] In an aspect of the present disclosure, the method may further include detecting products of the catalytic decomposition including at least one of 1,3-cyclopentadiene, cyclopentene, pentadiene, or molecular hydrogen.

[0023] In an aspect of the present disclosure, the catalyst composition may include a titanium-aluminum-boron nanopowder.

[0024] In accordance with aspects of the disclosure, a catalytic system for hydrocarbon decomposition includes a titanium-aluminum-boron nanopowder synthesized by a sonochemically-mediated reaction of titanium chloride with lithium borohydride and lithium aluminum hydride in an inert atmosphere. The titanium-aluminum-boron nanopowder may be amorphous with atomically dispersed titanium, aluminum, and boron, and may be configured to initiate catalytic decomposition of a hydrocarbon fuel at an onset temperature of about 750 K to produce products including 1,3-cyclopentadiene, cyclopentene, pentadiene, and molecular hydrogen.

[0025] Further details and aspects of exemplary embodiments of the present disclosure are described in more detail below with reference to the appended figures.BRIEF DESCRIPTION OF THE DRAWINGS

[0026] A better understanding of the features and advantages of the present disclosure will be obtained by reference to the following detailed description that sets forth illustrative embodiments, in which the principles of the present disclosure are utilized, and the accompanying drawings of which:

[0027] FIG. 1 is an illustration of an exemplary system for catalytic transformation of organic materials, in accordance with aspects of the present disclosure;Attorney Docket No. : 3229-7 PCT

[0028] FIG. 2A is an illustration of a27Al magic angle spinning NMR spectrum showing structural characterization of a titanium-aluminum-boron hydride-bearing nanopowder, in accordance with aspects of the present disclosure;

[0029] FIG. 2B is an illustration of annB magic angle spinning NMR spectrum showing structural characterization of a titanium-aluminum-boron hydride-bearing nanopowder, in accordance with aspects of the present disclosure;

[0030] FIG. 2C is an illustration of a deconvoluted Raman spectrum showing structural characterization of a titanium-aluminum-boron hydride-bearing nanopowder, in accordance with aspects of the present disclosure;

[0031] FIG. 3A is an illustration of mass spectra recorded during catalytic decomposition of exo-CioHie over a titanium-aluminum-boron nanopowder, in accordance with aspects of the present disclosure;

[0032] FIG. 3B is an illustration of photoionization efficiency curves confirming isomer- selective identification of initial catalytic decomposition products, in accordance with aspects of the present disclosure;

[0033] FIG. 4 is an illustration of decomposition ratio curves showing catalytic effects of a titanium-aluminum-boron nanopowder compared to uncatalyzed decomposition, in accordance with aspects of the present disclosure;

[0034] FIG. 5A is an illustration of computational TiAhBe cluster isomers showing representative low-energy motifs with calculated relative energies and populations, in accordance with aspects of the present disclosure;Attorney Docket No. : 3229-7 PCT

[0035] FIG. 5B is an illustration of binding complexes of exo-CioHis with the most stable TiALBe cluster showing multiple docking geometries, in accordance with aspects of the present disclosure;

[0036] FIG. 6A is an illustration of a natural population analysis charge distribution for exo-CioHi6, in accordance with aspects of the present disclosure;

[0037] FIG. 6B is an illustration of a natural population analysis charge distribution for a TiALBe cluster, in accordance with aspects of the present disclosure;

[0038] FIG. 6C is an illustration of a natural population analysis charge distribution for a bound complex of exo-CioHi6 with a TiALBe cluster, in accordance with aspects of the present disclosure;

[0039] FIG. 7A is an illustration of an entropy-corrected free energy surface showing C- H and C-C activation steps of exo-CioHi6 on a TiAhBe cluster at 750 K, in accordance with aspects of the present disclosure;

[0040] FIG. 7B is an illustration of an entropy-corrected free energy surface showing desorption of products from a TiALBe cluster at 750 K, in accordance with aspects of the present disclosure;

[0041] FIG. 8A is an illustration of an ab initio molecular dynamics trajectory showing the first hydrogen transfer along a distal pathway on a TiALBe cluster, in accordance with aspects of the present disclosure;

[0042] FIG. 8B is an illustration of an ab initio molecular dynamics trajectory showing the first hydrogen transfer along a proximal pathway on a TiALBe cluster, in accordance with aspects of the present disclosure;Attorney Docket No. : 3229-7 PCT

[0043] FIG. 8C is an illustration of an entropy-corrected free energy profile for the first hydrogen transfer step comparing distal and proximal pathways, in accordance with aspects of the present disclosure;

[0044] FIG. 8D is an illustration of an entropy-corrected free energy profile for the second hydrogen transfer step comparing distal and proximal pathways, in accordance with aspects of the present disclosure;

[0045] FIG. 9 is an illustration of an exemplary flowchart of a method for catalytic transformation of an organic material, in accordance with aspects of the present disclosure; and

[0046] FIG. 10 is a block diagram of a controller configured for use with the system of FIG. 1, in accordance with aspects of the present disclosure.DETAILED DESCRIPTION

[0047] The present disclosure relates generally to systems and methods for catalytic activation of carbon-hydrogen and carbon-carbon bonds via atomically-dispersed titanium- aluminum-boron nanocatalysts, and, in particular, to systems and methods for performing selective cracking, dehydrogenation, reforming, and related transformations of a wide range of organic substrates including fuels, polymers, biomass-derived compounds, and mixed feedstocks using accessible reactor platforms, minimal technical requirements, and cost- effective materials.

[0048] Although the present disclosure will be described in terms of specific examples, it will be readily apparent to those skilled in this art that various modifications,Attorney Docket No. : 3229-7 PCT rearrangements, and substitutions may be made without departing from the spirit of the present disclosure.

[0049] For the purpose of promoting an understanding of the principles of the present disclosure, reference will now be made to exemplary embodiments illustrated in the drawings, and specific language will be used to describe the same. It will nevertheless be understood that no limitation of the scope of the present disclosure is thereby intended. Any alterations and further modifications of the novel features illustrated herein, and any additional applications of the principles of the present disclosure as illustrated herein, which would occur to one skilled in the relevant art and having possession of this disclosure, are to be considered within the scope of the present disclosure.

[0050] Referring to FIG. 1, a catalytic system 100 for catalytic transformation of organic materials is shown. The catalytic system 100 includes a vessel 110 configured with a controllable heating environment 140. The controllable heating environment 140 may include one or more heaters, power supplies, and feedback control elements configured to regulate the temperature profile within vessel 110 with high precision. In certain embodiments, the controllable heating environment 140 may further include thermal insulation, distributed heating zones, or active cooling features. In other embodiments, the controllable heating environment 140 may interface with a controller 1000 (FIG. 10) to permit automated programming of heating cycles, ramp rates, or steady-state conditions for repeatable catalytic performance. The vessel 110 may take multiple forms depending on application. In some embodiments, the vessel 110 may be constructed as a chemical microreactor, such as a resistively heated tube designed for precise thermal control and short residence times that capture surface-catalyzed chemistry. In other embodiments, the vesselAttorney Docket No. : 3229-7 PCT110 may be a larger fixed-bed tubular reactor, a stirred tank reactor, a flow channel reactor, or even a microfluidic cartridge for low- volume or portable uses. These formats allow the catalytic system 100 to be scaled from laboratory characterization to industrial operation or field deployment.

[0051] In certain embodiments, the vessel 110 may be fabricated from materials selected to tolerate elevated temperatures and reactive organic environments while maintaining dimensional stability and low background reactivity. For example, the vessel 110 may include silicon carbide to provide high thermal conductivity and mechanical robustness at operating temperatures. In embodiments, alternative refractory constructions for the vessel 110 may include quartz, alumina, or stainless steel, selected according to thermal ramp-rate needs, compatibility with a catalyst composition 114 (e.g., a nanopowder, a coating, or immobilized on a substrate), and the desired interaction with a reactant stream 112. Internal surfaces of the vessel 110 may be smooth-bore to minimize stagnant zones and secondary gas-phase chemistry, or may include light texturing or inert liners where mechanical retention of a packed catalyst bed is beneficial. The vessel 110 may include a resistively heated silicon carbide tube having a length of about 20 millimeters and an inner diameter of about 1 millimeter, with a packed section of about 10 millimeters to establish a well-defined residence time across the catalyst composition 114.

[0052] In embodiments, the vessel 110 may be heated in several ways to deliver a controllable thermal profile. In some embodiments, resistive heating of a conductive tube or heater cartridge surrounding the tube may be used to achieve rapid, stable temperature control over a range from about 300 Kelvin to about 1600 Kelvin. Inductive or radiative heating may be used where electrical isolation or optical access is desired, while stillAttorney Docket No. : 3229-7 PCT meeting the same temperature and stability targets. Tn some embodiments, the vessel 1 10 may include thermal insulation to limit heat loss and axial gradients, including external insulating jackets and internal heat- spreading features appropriate to the tube geometry. The vessel 110 may further include ports positioned upstream, within, or downstream of the packed section for insertion of a thermocouple 105, for connection of the reactant stream 112, and for transition to a nozzle 116. In some embodiments, a temperature monitor, such as a type C thermocouple 105, may be inserted directly into or adjacent to the catalyst bed within the vessel 110 to monitor the local temperature that governs catalytic onset and product formation.

[0053] The vessel 110 may be operated under an inert atmosphere to suppress combustion chemistry and to isolate catalytic transformations occurring on the catalyst composition 11 . In some cases, helium may be selected as the inert carrier because of its high thermal conductivity, chemical inertness, and compatibility with downstream molecular beam sampling. A representative operating pressure may be about 500 Torr, which establishes short residence times that emphasize surface-catalyzed pathways rather than bulk pyrolysis. Other inert gases such as neon, argon, or nitrogen may also be used individually or in mixtures to tune heat transfer characteristics and to modulate quenching rates of reactive intermediates. The inert environment ensures that catalytic decomposition, dehydrogenation, and reforming proceed without unwanted ignition or flame chemistry, thereby preserving clear temperature-programmed catalytic signatures.

[0054] The reactant stream 112 is introduced into the vessel 110 under these controlled inert conditions. The reactant stream 112 generally includes an organic material carried in a selected inert gas, with the carrier acting both as a diluent and as a heat transfer medium.Attorney Docket No. : 3229-7 PCTThe organic component may include hydrocarbons, polymers, biomass-derived compounds, or other organics as described herein, depending on the application. In certain configurations, minor additions of gases such as hydrogen, carbon dioxide, or methane may be blended into the reactant stream 112 in low concentrations to adjust thermal conductivity, simulate realistic combustion environments, or probe the influence of co-reactants. Flow rates can vary widely depending on reactor design. For example, microreactor systems may operate at a few standard cubic centimeters per minute with residence times on the order of 100 microseconds to 1 millisecond, conditions that allow nascent volatile products to be sampled directly at the nozzle 116. Larger-scale tubular or fixed-bed systems may accommodate higher flow rates, up to several liters per minute, with residence times extending into the seconds, permitting evaluation of secondary catalytic processes or product stabilization pathways.

[0055] The inert operating envelope and the defined flow regime allow repeated heating and cooling cycles to be performed without significant memory effects, ensuring reproducibility in the onset temperature of decomposition. The combination of vessel 110 geometry, reactant stream 112 composition, and inert carrier selection also minimizes condensable transfer artifacts prior to analysis, thereby providing product distributions that reflect authentic catalytic behavior of the catalyst composition 114.

[0056] Contained within the vessel 110 is catalyst composition 114 that is arranged as a catalyst bed. The catalyst composition 1 14 includes at least one transition metal atomically dispersed in a matrix of at least one main group element. This structure provides a network of interatomic linkages within the constituents of the catalyst composition 114 that is designed to promote carbon-hydrogen bond activation and carbon-carbon bondAttorney Docket No. : 3229-7 PCT transformation of organic materials under controlled thermal conditions. The catalytic effect arises from the intimate distribution of metallic species at the atomic scale, which provides high surface accessibility and avoids bulk phase segregation that typically limits catalytic activity.

[0057] The transition metal component of the catalyst composition 114 may be selected from a wide range of elements in the transition series. In some embodiments, the transition metal may include titanium, which has been shown to act as a docking and activation site for organic molecules. In other embodiments, the transition metal may include zirconium or hafnium, which share similar electronic structure to titanium and can provide altered binding energies or thermal stabilities. Transition metals from groups 5 through 12 are also contemplated, including vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, iron, cobalt, nickel, copper, palladium, platinum, and mixtures thereof. These elements may be included individually or in combination to tune hydrogen abstraction energies, hydrocarbon adsorption strengths, and product branching behavior. In some cases, noble metals such as palladium or platinum may be atomically dispersed within the hydridic matrix to couple hydrogenation and dehydrogenation cycles with high efficiency.

[0058] The main group element component of the catalyst composition 114 provides structural support and a hydrogen reservoir that works in concert with the transition metal. In certain embodiments, the main group element may include aluminum or boron. Aluminum contributes electronic stabilization and provides space for transient hydrogen storage, while boron serves as a highly effective site for hydride binding and transfer. In other embodiments, the main group element may include carbon, silicon, gallium, germanium, indium, tin, antimony, thallium, lead, or bismuth, either individually or asAttorney Docket No. : 3229-7 PCT mixtures. Each of these elements may adjust the electronic structure, hydride capacity, or conductivity of the matrix. For example, silicon or germanium incorporation may increase thermal stability, while gallium or indium substitution may adjust the fluxionality of the network and support cooperative hydrogen transfer. Certain main group element(s) have the potential to enhance the catalytic potential of d-block elements.

[0059] The structural state of the catalyst composition 114 may vary depending on synthesis. In some embodiments, the catalyst composition 114 is amorphous with atomically dispersed metals forming a metallic glass-like structure. This amorphous state provides uniform catalytic motifs without long-range crystalline order, which has been shown to improve both activity and resistance to coking. In other embodiments, the catalyst composition 114 may include partially ordered or nanocrystalline domains embedded within an amorphous matrix, which can introduce additional sites for bond activation. These mixed states may be advantageous for maintaining hydride storage while providing localized crystalline motifs that stabilize reactive intermediates.

[0060] The catalyst composition 114 may be synthesized through several possible approaches. In one representative method, the catalyst composition 114 may be prepared by a sonochemically mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride. This process involves dissolution of the transition metal chloride in a solvent such as diethyl ether, followed by reaction under ultrasonic agitation in the presence of the hydride salts. The sonochemical treatment promotes dispersion, nucleation, and hydride incorporation into the forming solid. The resulting material may then be washed with tetrahydrofuran or related solvents to remove salts and dried under vacuum.Attorney Docket No. : 3229-7 PCT

[0061] Other preparation routes are also possible. Tn some embodiments, mechanochemical milling of transition metal salts with borohydrides or aluminum hydrides may be used to produce reactive powders. In other embodiments, plasma reduction may be employed, where metal precursors are reduced in the presence of hydrogen-rich plasmas. Solvothermal processing in ethers, glymes, or other polar solvents can also yield mixed- metal hydride solids with adjustable stoichiometry. Aerosol-assisted or spray-drying methods may produce nanopowders with uniform particle sizes and large surface areas. These alternative methods provide flexibility to control atomic dispersion, hydride content, and residual anion levels.

[0062] In some embodiments, catalyst composition 114 includes a titanium-aluminum- boron nanopowder synthesized in an inert atmosphere. This material is amorphous with titanium, aluminum, and boron distributed at the atomic scale within a hydridic matrix. In this configuration, titanium acts as an active docking site where organic substrates bind and undergo bond activation. Boron serves as a hydrogen storage and transfer element, allowing hydrogen atoms abstracted from the organic substrate to be temporarily stored as hydrides before recombination into molecular hydrogen. Aluminum stabilizes the framework, provides additional sites for hydrogen accommodation, and maintains overall structural integrity of the matrix under repeated thermal cycling. Spectroscopic analysis, including solid-state NMR, XPS, and Raman spectroscopy, confirms that titanium is atomically dispersed and that Ti-Al-B linkages persist throughout the structure, while microscopy indicates minimal segregation into separate phases.

[0063] Together, these features of the catalyst composition 114 support its use as a highly reactive and durable catalytic bed material within the vessel 110. The amorphousAttorney Docket No. : 3229-7 PCT hydridic state with atomically dispersed metals promotes early catalytic onset, typically around 750 Kelvin, while the specific combination of titanium, aluminum, and boron provides stable cycling, low coking, and reproducible product distributions across a range of organic materials.

[0064] The catalytic system 100 may be configured to initiate decomposition of hydrocarbons at a temperature ranging from about room temperature to about 750 Kelvin. This early onset reflects the hydride-bearing and atomically dispersed nature of the catalyst composition 114, which lowers the thermal barrier for bond activation relative to purely thermal pyrolysis. In certain embodiments, the onset of catalytic decomposition may be detected when the catalyst composition 114 promotes the release of molecular hydrogen or the formation of defined unsaturated fragments such as alkenes or conjugated dienes. These products provide a direct signature of carbon-hydrogen bond activation and subsequent hydrogen transfer onto boron or other matrix sites.

[0065] In embodiments, the temperature of the vessel 110 may be monitored by thermocouple 105 positioned directly in or adjacent to the catalyst bed, and may be controlled to span from about 300 Kelvin up to about 1600 Kelvin. This broad thermal window allows the catalytic system 100 to be operated under laboratory characterization conditions as well as under industrially relevant or propulsion-relevant conditions. In certain cases, the most efficient catalytic decomposition and reforming may be optimized between about 750 Kelvin and about 1050 Kelvin, where low-temperature carbon-hydrogen activation and controlled carbon-carbon reorganization are emphasized.

[0066] The catalytic processes supported by the catalytic system 100 can be applied broadly to virtually any organic material that contains carbon-hydrogen bonds. This includesAttorney Docket No. : 3229-7 PCT small alkanes such as propane, where catalytic dehydrogenation to propene and hydrogen provides a valuable chemical transformation. In this case, the titanium centers of the catalyst composition 114 act as docking sites for multiple C-H bonds of propane, while adjacent boron centers store the abstracted hydrogen. The resulting propene can desorb readily while hydrogen recombines on the surface to form H2, thereby providing a direct pathway for alkane dehydrogenation at reduced temperatures.

[0067] Beyond fuels and light alkanes, the catalyst composition 114 may serve as a scaffold for catalytic upgrading of polymers, waste plastics, or biomass-derived compounds. Polyethylene and polypropylene, for example, may be depolymerized into olefinic monomers or shorter-chain hydrocarbons under catalytic conditions that minimize coking and secondary polymerization. Solid fuels such as composite propellants or polymer-bound energetic materials may incorporate the catalyst composition 114 directly into their matrices, where it functions as both a structural scaffold and an active catalytic phase. In this role, the catalyst composition 114 facilitates binder decomposition, gas generation, or tailored release of unsaturated fragments under the thermal environments encountered during combustion or propulsion.

[0068] The same principles apply across oxygenated, nitrogen-containing, and sulfur- containing organics, where the catalyst composition 114 mediates early carbon-hydrogen activation, dehydrogenation, and selective carbon-carbon transformations. Because the active state of the material resides in atomically dispersed metals within a hydridic matrix, the catalytic system 100 can be applied universally to rupture carbon-hydrogen bonds and to promote subsequent carbon-carbon bond rearrangement, scission, or formation. This universality allows the catalytic system 100 to function not only as a decompositionAttorney Docket No. : 3229-7 PCT platform for specialized fuels, but also as a general-purpose catalytic framework for chemical processing, waste recycling, and advanced materials applications.

[0069] The catalytic system 100 further includes nozzle 116 through which volatile products exit the vessel 110 after contact with the catalyst composition 114. The gases form a stream 122 that reflects the immediate products of catalytic transformation. The capillary outlet (not shown) or the nozzle 116 provides a controlled expansion that directs the stream 122 into a low-pressure region without significant condensation or wall interaction. In some cases, the nozzle 116 may be a conical orifice with an aperture on the order of hundreds of micrometers that expands the stream 122 directly into vacuum. In other cases, the nozzle 116 may include multi-stage orifices, skimmers, or capillary extensions to maintain pressure differentials and focus the stream 122 while minimizing secondary collisions. The function of the nozzle 116 is to preserve the chemical identity of products formed on the surface of the catalyst composition 114 and transfer them directly to the analysis interface.

[0070] The stream 122 passes into a molecular beam sampling assembly 120. The molecular beam sampling assembly 120 collimates the stream 122 and removes background gases so that nascent products are isolated prior to further analysis. In some configurations, the molecular beam sampling assembly 120 may include aerodynamic skimmers, apertures, or ion guides positioned to refine the trajectory of the stream 122. The molecular beam sampling assembly 120 helps ensure that the detected composition reflects catalytic events occurring within the vessel 1 10 rather than downstream reactions. The use of a molecular beam sampling assembly 120 approach provides access to the primary decomposition products in real time and at relevant onset temperatures.Attorney Docket No. : 3229-7 PCT

[0071] Downstream of the molecular beam sampling assembly 120 is a mass spectrometer 130, or any other suitable analysis device, that interrogates the stream 122. The mass spectrometer 130 may be an isomer-selective single photon photoionization reflectron time-of-flight analyzer. In such cases, tunable vacuum ultraviolet light at controlled photon energies may be used to ionize specific products in the stream 122. Photon energies around 10.0 eV may distinguish primary hydrocarbon fragments along with the photon energy scan generating unique isomer-selective photoionization efficiency curves. The isomeric products such as cyclopentadiene, cyclopentene, and pentadiene can be identified; while higher photon energies such as 15.4 eV allow detection of hydrogen and methane. The vacuum ultraviolet-coupled reflectron configuration of the mass spectrometer 130 provides high mass resolution for ions and separates structural isomers based on their photoionization efficiency curves. The ability to collect spectra in fine increments, for example 0.05 eV steps, supports unambiguous assignment of radicals, isomers, and molecular fragments that emerge from the vessel 110.

[0072] In some embodiments, the product analysis interface 150 formed by the nozzle 116, stream 122, molecular beam sampling assembly 120, and mass spectrometer 130 may instead or additionally employ other detectors. Gas chromatography-mass spectrometry may be used to separate complex mixtures and quantify minor products. Fourier transform infrared spectroscopy may record vibrational signatures of species such as aromatics, dienes, or oxygenates in the stream 122. In some cases, multiple detectors may be used in combination to provide a more complete picture of the products exiting the vessel 110.

[0073] Together, the nozzle 116, stream 122, molecular beam sampling assembly 120, and mass spectrometer 130 define a product analysis interface 150 configured to detectAttorney Docket No. : 3229-7 PCT volatile products formed during catalytic transformation of the organic material. This interface may record mass spectra, generate photoionization efficiency curves, and quantify branching ratios of products such as cyclopentadiene, cyclopentene, pentadiene, benzene, and hydrogen. In some cases, the analysis interface may provide continuous real-time monitoring of product distributions as temperature in the vessel 110 is ramped.

[0074] In some embodiments, the catalytic system 100 introduces an organic feed in the reactant stream 112 into the vessel 110, where it contacts the catalyst composition 114 under an inert atmosphere. The inert environment suppresses unwanted combustion pathways, ensuring that catalytic transformations dominate. As the temperature of the vessel 110 is gradually raised, catalytic onset typically occurs near 750 Kelvin. At this threshold, the product analysis interface 150 registers the first appearance of unsaturated products such as 1,3-cyclopentadiene, cyclopentene, and pentadiene, together with molecular hydrogen.These early products reflect selective carbon-hydrogen activation and hydrogen transfer facilitated by the hydride-bearing structure of the catalyst composition 114.

[0075] When the vessel 110 is operated at higher temperatures, the product spectrum evolves to include additional transformation products. Aromatic species such as benzene and substituted benzenes become more abundant, alongside lighter alkenes and alkanes produced by carbon-carbon bond scission. The stream 122 analyzed by the product analysis interface 150 may reveal shifting branching ratios, with conjugated dienes and cyclic products giving way to aromatics and small fragments as temperature increases from the catalytic onset region into the 900-1050 Kelvin range. This progression highlights the versatility of the catalyst composition 114 in supporting carbon-hydrogen bond activation,Attorney Docket No. : 3229-7 PCT dehydrogenation, cracking, reforming, and ring-contraction pathways as the operating conditions are tuned.

[0076] The catalytic system 100 may also be operated dynamically to probe reproducibility and long-term stability. Repeated heating and cooling cycles can be applied to the vessel 110 while monitoring the stream 122. The product analysis interface 150 confirms that onset conditions remain consistent across cycles, with no significant drift in the temperature. These cycles further demonstrate that the catalyst composition 114 maintains its structural integrity, with spectroscopic fingerprints showing only minor changes even after repeated exposure to elevated temperatures.

[0077] An additional advantage of the catalytic system 100 is the absence of reactor memory effects. Because the stream 122 exits directly through the nozzle 116 into the molecular beam sampling assembly 120 without condensable transfer lines, the products detected represent the real-time outcome of surface-catalyzed chemistry. This configuration avoids buildup of residues or recirculation of prior products, allowing each heating cycle to be measured independently. In some cases, side-by-side comparisons of neat organic feeds and catalyst-contacted feeds can be run in the same vessel 110, with the product analysis interface 150 clearly resolving the catalytic lowering of onset temperature and suppression of soot precursors.

[0078] Through these operations, the catalytic system 100 demonstrates a reliable, repeatable platform for probing catalytic bond activation in a wide variety of organic materials. From saturated hydrocarbons and fuels to polymers and biomass-derived molecules, the combination of vessel 110, catalyst composition 114, and product analysis interface 150 provides direct insight into how reactive mixed metal nanopowders initiateAttorney Docket No. : 3229-7 PCT decomposition, promote unsaturation, and stabilize hydrogen release under thermal conditions.

[0079] Referring to FIGS. 2A-2C, a synthesis route and structural fingerprints of representative titanium-aluminum-boron nanopowder are shown. In a nitrogen or argon glovebox, titanium chloride dissolved in diethyl ether is prepared on a Schlenk line and cannula-transferred under continuous inert purge into a sonicating suspension containing lithium borohydride and lithium aluminum hydride. Immediate formation of a black solid occurs, with vigorous gas evolution and significant heat release. The mixture remains under sonication overnight, often reaching reflux temperature while continuously purged with inert gas to exclude moisture and oxygen. After cooling, the solid is separated by filtration through fine porosity frits. Post-treatment includes vacuum heating at about 100 Celsius to remove volatile species and washing with tetrahydrofuran to eliminate salts or unreacted precursors. The order of heating and washing may be reversed, with variations in sequence influencing residual chloride, hydride distribution, and catalytic activity.

[0080] Reaction parameters strongly influence the final structure and reactivity. The choice of inert atmosphere (nitrogen, argon, or helium), ultrasonication bath temperature (commonly 25-35 Celsius), and reagent stoichiometry each shape the product. By varying the lithium borohydride to lithium aluminum hydride ratio, fully reduced or partially reduced nanopowders are produced, with distinct catalytic onset temperatures. ICP-OES provides compositional control, while XPS reveals residual chloride, Raman and solid-state NMR identify bonding motifs, and DSC-TGA quantify hydride content and stability.

[0081] Thermogravimetric and differential scanning calorimetry demonstrate minimal mass loss below about 500 Celsius apart from controlled hydride release, with structuralAttorney Docket No. : 3229-7 PCT integrity maintained up to about 1000 Celsius. These results confirm robustness for repeated catalytic cycling, preconditioning, or integration into solid fuel matrices. Beyond titanium- aluminum-boron, similar sonochemical synthesis and analysis extend to reactive mixed metal nanopowders with zirconium, hafnium, gallium, silicon, or germanium, where hydride release, hydrogen buffering, and conductivity can be tuned for specialized catalytic or electrocatalytic functions.

[0082] FIG. 2A presents a27Al magic angle spinning NMR spectrum with a dominant resonance near 1642 ppm assigned to elemental aluminum and a secondary peak near 75 ppm corresponding to aluminate-type coordination. These signals show diverse aluminum environments, consistent with dual roles in structural stabilization and electronic mediation.

[0083] FIG. 2B shows annB magic angle spinning NMR spectrum with a broad peak centered near 65 ppm, characteristic of three-fold coordinated boron in a Be-type framework. This shift reflects covalency with adjacent titanium and aluminum atoms and confirms boron’s role in hydrogen storage.

[0084] FIG. 2C presents a deconvoluted Raman spectrum, with experimental data plotted as a dotted trace and individual fits resolved separately. Strong bands appear between 300 and 1000 cm '. corresponding to Ti-Al-B bending, Ti-Al stretching, Ti-B stretching, and Al- B stretching. Small features of TiB2 and TiO2 may be present, but the framework remains amorphous and predominantly mixed-metal. Together with electron microscopy, elemental mapping, and XPS, which detects elemental titanium with only trace oxidation, these data establish a uniform amorphous mixed-metal hydridic matrix with minimal segregation.

[0085] Raman analysis confirms structural stability. The Ti-Al-B vibrational bands persist even after repeated thermal cycling up to catalytic operating temperatures, while onlyAttorney Docket No. : 3229-7 PCT weak graphitic D and G bands near 1350-1600 cm1appear, confirming minimal carbon deposition. The resilience of these vibrational modes demonstrates that the nanopowder maintains its mixed-metal framework and hydridic state under catalytic turnover.

[0086] Taken together, microscopy, spectroscopy, and thermal analyses demonstrate that the amorphous material constitutes atomically dispersed titanium, aluminum, and boron having the interatomic Ti-B, Al-B, and Ti-Al linkages that support both stability and catalytic function. This structural state underlies observed catalytic behavior: early carbonhydrogen activation, hydrogen release at reduced temperatures, and hydrocarbon reforming. Light alkanes such as propane may undergo dehydrogenation to propene, polymers such as polyethylene may depolymerize to olefins, and biomass-derived compounds may transform to deoxygenated aromatics. The nanopowder also serves as a scaffold for other catalytic systems, supporting nanoparticles, tethered complexes, or adjuncts such as zeolites and reducible oxides.

[0087] Referring to FIG. 3A, mass spectra recorded during the decomposition of helium- seeded exo-CioHie (“JP-10”) over the catalyst composition 114 in the vessel 110 at photon energy of 10.0 electron volts show clear temperature dependence. At 300 Kelvin the spectrum is dominated by the parent ion (m / z = 136). At 750 Kelvin in the presence of the hydride-bearing nanopowder, new product peaks emerge at m / z = 66 and 68.

[0088] As depicted in FIG. 3B, isomer-selective photoionization efficiency curves confirm that m / z = 66 corresponds to 1 ,3-cyclopentadiene, while m / z = 68 is a combination of cyclopentene and 1,3 -pentadiene. Hydrogen is additionally detected when the photon energy is raised to 15.4 electron volts, consistent with catalytic dehydrogenation. The dataAttorney Docket No. : 3229-7 PCT establishes a catalytic onset near 750 Kelvin, several hundred Kelvin below the onset observed for uncatalyzed thermal decomposition.

[0089] As temperature is raised toward 900 Kelvin, signals for the Cs unsaturated products intensify, and by 1050 Kelvin the parent exo-CioHi6 ion is almost absent. The spectrum broadens to include benzene and smaller open-chain hydrocarbons. Importantly, no net mass growth beyond the parent peak is observed, showing that residence times are sufficiently short to suppress uncontrolled gas-phase polymerization. These results highlight that the catalyst composition 114 lowers activation barriers for C-H cleavage and guides intermediates into defined unsaturated fragments and hydrogen.

[0090] These signatures are general across organic feeds. Light alkanes such as propane undergo dehydrogenation to propene and hydrogen. Linear and branched alkanes yield defined unsaturates and shorter fragments. Cyclic and polycyclic hydrocarbons undergo controlled ring opening and contraction. Polymers such as polyethylene and polypropylene yield olefins and oligomers at lower thresholds than pyrolysis, while biomass-derived compounds undergo deoxygenation and aromatic formation. Oxygenates, nitrides, and sulfides follow analogous selective C-H activation, with coke suppression aided by hydrogen buffering on the hydridic matrix. Across these feed classes, the mechanistic motif involves docking at titanium, hydrogen abstraction at boron, stabilization by aluminum, and recombination to molecular hydrogen that clears the surface for repeated turnover.

[0091] These results confirm that catalyst composition 11 reduces the onset of C-H bond activation by several hundred Kelvin relative to uncatalyzed pyrolysis, steering the chemistry toward selective unsaturates at lower temperature. The isomer-selective capability of the analysis distinguishes overlapping products and supports mechanistic assignments ofAttorney Docket No. : 3229-7 PCT stepwise dehydrogenation and retro-Diels-Alder scission as the origin of the early fragments.

[0092] Alternative embodiments expand upon this baseline catalytic framework by functionalizing the nanopowder surface or integrating adjunct phases. For example, nitrogen incorporation during synthesis produces nitrogen-functionalized active sites detectable by XPS, which correlate with increased low-temperature reactivity toward hydrocarbon composites. Depositing reducible oxides such as iron oxides, titania, or ceria may promote hydrogen spillover or couple with water-gas shift chemistry. Incorporation of zeolite frameworks introduces microporous acid sites that combine with the hydridic solid to couple C-H activation with shape-selective transformations.

[0093] These hybrid systems illustrate expansion of the catalytic platform. The hydride- bearing Ti-Al-B nanopowder provides hydrogen buffering and early C-H activation, while adjunct phases offer redox or acidic pathways. Together, these combinations generate multifunctional catalysts that can achieve multistep upgrading, dehydrogenation, and reforming of diverse organic materials, including fuels, polymers, and biomass, under controlled thermal conditions.

[0094] Referring to FIG. 4, decomposition ratio curves illustrate the catalytic advantage of catalyst composition 114, in the form of Ti-Al-B nanopowder, in vessel 110. With the catalyst composition 114 in place, decomposition of exo-CioHie initiates near 750 Kelvin and reaches nearly complete conversion by 1050 Kelvin. In contrast, without the catalyst composition 114, decomposition does not begin until about 1200 Kelvin and requires heating to nearly 1600 Kelvin for complete conversion in the same reactor geometry.Attorney Docket No. : 3229-7 PCT

[0095] The plot also shows error bars for both axes, with y-axis uncertainties arising from experimental variation in parent mass intensities (m / z = 136) and x-axis uncertainties from temperature measurements. The circle at 300 Kelvin represents undecomposed hydrocarbon. This several-hundred-Kelvin reduction in onset temperature and faster rise in decomposition ratio demonstrate the strong catalytic effect of the Ti-Al-B nanopowder, lowering activation barriers for C-H and C-C bond transformations under thermal conditions.

[0096] Referring to FIG. 5A, computational models of TiAbBe clusters illustrate representative low-energy isomers that emulate local motifs of the catalyst composition 114 in the form of amorphous titanium-aluminum-boron nanopowder. Seven isomers are shown, each with calculated relative energies and Boltzmann populations at 750 Kelvin. Most preserve an asymmetric hexagonal bipyramidal topology, with aluminum and titanium atoms coordinated to a boron-rich Be framework. Natural population analysis indicates that titanium and aluminum carry fractional positive charges, while the boron framework bears anionic character, consistent with electron donation from metals to boron. This electronic structure supports the experimental observation of boron acting as a hydrogen acceptor and storage site, titanium serving as a docking center, and aluminum providing structural stabilization and fluxional flexibility.

[0097] Referring to FIG. 5B, calculated binding complexes of exo-CioHie with the most stable TiAbBe cluster show multiple low-energy docking configurations (labeled A-I). In the global minimum complex, the hydrocarbon is anchored to the titanium atom through several C-H- - Ti interactions, forming stabilizing quasi-cyclic motifs. Other binding modes involve cyclic or bridged contacts between the hydrocarbon and the cluster, reflecting the ability ofAttorney Docket No. : 3229-7 PCT the Ti center to simultaneously engage multiple C-H bonds. Adjacent boron centers function as hydrogen sinks during transfer, while aluminum atoms exhibit fluxional repositioning that accommodates hydrogen storage and stabilizes intermediates. These computed complexes rationalize the experimentally observed low-temperature onset for C-H activation, showing that docking at titanium, hydrogen abstraction to boron, and structural stabilization by aluminum are thermodynamically accessible at 750 Kelvin.

[0098] Taken together, FIGS. 5 A and 5B provide an atomistic picture of the Ti-Al-B catalytic motif. The boron-rich framework stores hydrogen, titanium serves as the singleatom active site for C-H docking, and aluminum adjusts dynamically to stabilize transition states. This synergy explains the robust hydrogen evolution, early C-H activation, and controlled C-C bond scission observed experimentally in the vessel 110 with catalyst composition 114.

[0099] Referring to FIGS. 6A-6C, natural population analysis (NPA) provides charge distributions for exo-CioHie, the TiALBe cluster, and the bound complex of exo-CioHie with TiABBe. In the isolated hydrocarbon, electron density is localized on the C-H bonds, consistent with saturated bonding. In the bare TiAhBe cluster, fractional positive charge resides on titanium and aluminum atoms, while the boron-rich Be framework bears negative charge, reflecting electron donation from the metals and establishing an anionic boron scaffold. Upon formation of the binding complex, electron density redistributes: the titanium center accepts electron density from multiple C-H bonds of the hydrocarbon, reducing its positive charge, while adjacent boron centers accumulate negative charge corresponding to hydrogen abstraction. Aluminum atoms adjust their partial charges during complexation, reflecting fluxional motion and stabilization of the binding geometry.Attorney Docket No. : 3229-7 PCT

[0100] These charge maps illustrate the synergistic roles of the three elements. Titanium acts as the docking and activation site, engaging directly with C-H bonds. Boron centers function as transient hydrogen sinks, storing electron density during transfer. Aluminum contributes to charge redistribution and stabilizes the dynamic framework. This electronic structure underpins the observed catalytic function: early C-H activation at reduced temperatures, reversible hydrogen storage, and controlled C-C transformations.

[0101] Referring to FIG. 7A, entropy-corrected free energy profiles at about 750 Kelvin show the activation steps of exo-CioHi6 on the global minimum TiALBe cluster. The sequence of intermediates and transition states demonstrates that C-H activation at the titanium center is thermally accessible, with hydrogen transferred sequentially to adjacent boron atoms. These steps proceed with barriers on the order of only tens of kilojoules per mole, which accounts for the experimentally observed catalytic onset several hundred Kelvin below uncatalyzed pyrolysis. After hydrogen abstraction, the hydrocarbon fragment bound to titanium undergoes C-C activation events including P-scission and ring opening, producing dehydrogenated intermediates that evolve toward Cs unsaturated species.

[0102] Referring to FIG. 7B, the subsequent desorption steps are illustrated. At catalytic temperatures, cyclopentene desorption is enthalpically favored, while desorption of 1,3- cyclopentadiene is driven largely by entropy. Recombination of stored hydrogen atoms produces molecular hydrogen, which clears the active sites and restores the TiAhBe motif for continued turnover. The dotted connections on the free energy diagram correspond to transitions that appear uphill on a purely enthalpic potential energy surface, but are stabilized by entropy at elevated temperature, resulting in overall downhill free energy trajectories.Attorney Docket No. : 3229-7 PCT

[0103] FIGS. 7A and 7B depict the catalytic cycle as a sequence of C-H and C-C activations followed by product desorption and hydrogen release. These energetics confirm that the titanium sites provide docking and activation, boron centers function as transient hydrogen sinks, and aluminum stabilizes the local framework, yielding a dynamic hydride- bearing matrix that supports repeated catalytic cycling under thermal conditions.

[0104] Referring to FIGS. 8A-8D, ab initio molecular dynamics simulations adopting a slow-growth approach illustrate sequential hydrogen transfer during the catalytic cycle on the TiALBs cluster.

[0105] FIG. 8A shows the first hydrogen transfer from exo-CioHie to a boron center distal to the exterior aluminum atom, proceeding through intermediates DAI to DA3. FIG. 8B depicts the alternate pathway where hydrogen transfer occurs to a boron center proximal to the exterior aluminum atom, described as DB1 to DB3. Both distal and proximal pathways are thermally accessible at 750 Kelvin and exhibit barriers on the order of several tens of kilojoules per mole.

[0106] FIG. 8C presents the entropy-corrected free energy profile for the first hydrogen transfer step relative to intermediates DA3 and DB3, which correspond to single hydrogen- transferred TiALBe clusters bound to CioHis. FIG. 8D presents the entropy-corrected free energy profile for the second hydrogen transfer step along both distal (DA3— >DA5) and proximal (DB3— >DB5) pathways. In both FIGS. 8C and 8D, the longer dashed trajectory (bottom curve in FIG. 8C and top curve in FIG. 8D) corresponds to the distal route and the shorter dashed trajectory (top curve in FIG. 8C and bottom curve in FIG. 8D) corresponds to the proximal route.Attorney Docket No. : 3229-7 PCT

[0107] Together, these results confirm that sequential hydrogen abstraction is accessible under catalytic conditions, with both distal and proximal pathways providing modest banders relative to gas-phase bond dissociation. The simulations further reveal fluxional motion of aluminum atoms relative to the boron framework. This motion transiently stabilizes transition configurations during hydrogen transfer while maintaining the structural integrity of the Ti-B-Al cluster. Collectively, the AIMD results validate a hydrogenshuttling mechanism in which titanium provides docking, boron stores hydrogen transiently, and aluminum dynamically stabilizes the process.

[0108] Referring to FIG. 9, a flowchart of a method 900 for catalytic transformation of an organic material under thermal conditions using an atomically dispersed reactive mixed metal nanopowder is shown.

[0109] The method 900 includes providing the vessel 110 with controllable heating environment 140. The vessel 110 may be a packed microreactor tube, a fixed-bed reactor, a stirred reactor, a flow channel, a microplate well, or a microfluidic cartridge suitable for laboratory, pilot, portable, or field deployment. The vessel 110 may further include optical windows, pressure control ports, or integrated heaters. The method 900 may further include operating the vessel 110 under an inert atmosphere selected from helium, neon, argon, nitrogen, or mixtures thereof to suppress combustion and confine surface-catalyzed transformations.

[0110] At block 902, the method 900 includes adding (e.g., by flowing, by entraining) the catalyst composition 114 to the vessel 110. The catalyst composition 114 includes at least one transition metal atomically dispersed in a matrix of at least one main group element and containing interatomic linkages between the constituents to promote carbon-Attorney Docket No. : 3229-7 PCT hydrogen activation and carbon-carbon transformation. In embodiments, the transition metal includes titanium and the main group elements include aluminum and boron. The catalyst composition 114 may be provided as an amorphous nanopowder with atomically dispersed metals, arranged as a packed catalyst bed within vessel 110. The method 900 may further include delivering the catalyst composition 114 as pelletized material, bound into a porous monolith, or co-formulated with adjuncts such as zeolites or iron oxides to extend catalytic function.

[0111] At block 904, the method 900 includes introducing the reactant stream 112 into the vessel 110. The reactant stream 112 may include an organic material having carbonhydrogen diluted in an inert carrier gas, where the organic material may be selected from aviation fuels such as JP-10 and F-24, light alkanes such as propane or hexane, cyclic and polycyclic hydrocarbons, aromatics, oxygenates, biomass-derived molecules such as furfural or guaiacol, or polymers including polyethylene and polypropylene. The reactant stream 112 may be introduced as a liquid, gas, aerosol, or solution, with flow rates and pressures adjusted to control residence time within vessel 110.

[0112] At block 906, the method 900 includes heating the reactant stream 112 in contact with the catalyst composition 114 within the vessel 110 under inert atmosphere to induce catalytic transformation. Thermal conditions may be selected to promote decomposition, cracking, dehydrogenation, reforming, or retro Diels- Alder cleavage depending on the feedstock. For saturated hydrocarbons, catalytic onset near 750 Kelvin produces hydrogen release and unsaturated fragments such as 1,3-cyclopentadiene, cyclopentene, and pentadiene. At elevated temperatures, further transformations may yield aromatics andAttorney Docket No. : 3229-7 PCT smaller open-chain fragments. Control of temperature, flow, and pressure within vessel 110 may be used to steer the product distribution and suppress soot formation.

[0113] The method 900 may further include synthesizing the catalyst composition 114 by a sonochemically mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride under inert gas, followed by washing and drying to set hydride content. Variants may include mechanochemical milling, plasma reduction, solvothermal processing, or aerosol-assisted routes.

[0114] The method 900 may further include detecting volatile products exiting the vessel 110 through nozzle 116 and stream 122. The stream 122 may be analyzed by mass spectrometer 130, which in embodiments includes an isomer-selective single-photon photoionization reflectron time-of-flight mass spectrometer. Alternative configurations of mass spectrometer 130 may include gas chromatography-mass spectrometry, Fourier transform infrared spectroscopy, or Raman spectroscopy.

[0115] The method 900 may further include regenerating active sites of catalyst composition 114 by desorption of products and recombination of stored hydrogen to release H2, supporting continuous catalytic turnover with reduced coke accumulation.

[0116] The method 900 may further include adapting to specific feedstocks. For example, light alkanes such as propane may undergo selective dehydrogenation to propene and hydrogen; polymers may be depolymerized to olefins or aromatic oils; biomass-derived compounds may be deoxygenated and converted to aromatic fuels; and mixed waste plastics may be cracked into defined hydrocarbon fractions with soot suppression.

[0117] Referring to FIG. 10, controller 1000 is configured to manage and coordinate operation of the catalytic system 100, including preparation and processing steps of methodAttorney Docket No. : 3229-7 PCT900 as well as subsystems such as the vessel 1 10, reactant stream 1 12, catalyst composition 114, nozzle 116, stream 122, and mass spectrometer 130. The controller 1000 includes a processor 1200 operatively connected to a memory 1300. The memory 1300 may be volatile, such as random access memory, or non-volatile, such as flash, disk, optical, or solid-state storage, and is configured to store computer-readable instructions and operating data. The processor 1200 may include a microprocessor, a digital signal processor, a graphics processing unit, a central processing unit, an application-specific integrated circuit, or a field-programmable gate array 1500. In some configurations, alternative computational platforms such as memristor-based logic or chemically encoded inference engines may be applied to manage catalytic processes.

[0118] The memory 1300 stores instructions that, when executed by the processor 1200, operate the controller 1000 to coordinate and control subsystems of the catalytic system 100. In some cases, the memory 1300 may be integrated within controller 1000, while in others it may be external and connected by high-speed buses or communication cabling. The controller 1000 may further include a network interface 1400 that allows the catalytic system 100 to communicate with external computers, distributed control modules, or remote servers for monitoring and data sharing. Storage 1100 associated with controller 1000 may retain calibration tables, branching ratio data, vibrational fingerprints, mass spectra, and historical operating records for reproducibility.

[0119] In representative operation, controller 1000 monitors operating conditions of catalytic system 100, including heating within vessel 110, composition and flow of reactant stream 112, status of catalyst composition 114, flow through nozzle 116, and detection parameters in mass spectrometer 130. The controller 1000 may adjust pumps, flowAttorney Docket No. : 3229-7 PCT controllers, heaters, and valves to regulate the introduction of reactant stream 1 12, the cycling of catalyst composition 114, and the channeling of stream 122 into the mass spectrometer 130.

[0120] The processor 1200 may execute algorithms from memory 1300 to conduct background subtraction, noise reduction, calibration curve application, branching ratio determination, and product identification. In certain embodiments, separate modules of catalytic system 100 may be networked through network interface 1400, with redundant communication paths for fail-safe operation.

[0121] The controller 1000 may further operate actuators, heaters, and detectors to selectively adjust (i) delivery of reactant stream 112 into vessel 110; (ii) heating profiles and residence time within vessel 110; and (iii) analytical conditions within mass spectrometer 130, such as photon energy scans, spectral resolution, or chromatographic separation conditions. Sensor inputs from thermocouples (e.g., thermocouple 105), flow meters, pressure gauges, and optical probes may be logged into memory 1300 and used by processor 1200 to dynamically modulate these operating parameters.

[0122] Additional functions of controller 1000 may include scheduling repeated catalytic cycles, executing regeneration protocols for catalyst composition 114, applying calibration profiles to identify products such as 1,3-cyclopentadiene, cyclopentene, pentadiene, and molecular hydrogen, and transmitting data via network interface 1400. Storage 1100 may further archive results for long-term performance tracking, quality assurance, and external reporting.

[0123] Certain embodiments of the present disclosure may include some, all, or none of the above advantages and / or one or more other advantages readily apparent to those skilledAttorney Docket No. : 3229-7 PCT in the art from the drawings, descriptions, and claims included herein. Moreover, while specific advantages have been enumerated above, the various embodiments of the present disclosure may include all, some, or none of the enumerated advantages and / or other advantages not specifically enumerated above.

[0124] The embodiments disclosed herein are examples of the disclosure and may be embodied in various forms. For instance, although certain embodiments herein are described as separate embodiments, each of the embodiments herein may be combined with one or more of the other embodiments herein. Specific structural and functional details disclosed herein are not to be interpreted as limiting, but as a basis for the claims and as a representative basis for teaching one skilled in the art to variously employ the present disclosure in virtually any appropriately detailed structure. Like reference numerals may refer to similar or identical elements throughout the description of the figures.

[0125] The phrases “in an embodiment,” “in embodiments,” “in various embodiments,” “in some embodiments,” or “in other embodiments” may each refer to one or more of the same or different example embodiments provided in the present disclosure. A phrase in the form “A or B” means “(A), (B), or (A and B).” A phrase in the form “at least one of A, B, or C” means “(A); (B); (C); (A and B); (A and C); (B and C); or (A, B, and .”

[0126] It should be understood that the foregoing description is only illustrative of the present disclosure. Various alternatives and modifications can be devised by those skilled in the art without departing from the disclosure. Accordingly, the present disclosure is intended to embrace all such alternatives, modifications, and variances. The embodiments described with reference to the attached drawing figures are presented only to demonstrate certain examples of the disclosure. Other elements, steps, methods, and techniques that areAttorney Docket No. : 3229-7 PCT insubstantially different from those described above and / or in the appended claims are also intended to be within the scope of the disclosure.

Claims

Attorney Docket No. : 3229-7 PCTWHAT IS CLAIMED IS:

1. A catalytic system comprising: a vessel configured with a controllable heating environment; and a catalyst composition disposed in the vessel, the catalyst composition comprising at least one transition metal atomically dispersed in a matrix of at least one main group element, wherein the catalyst composition is an amorphous solid configured to promote carbonhydrogen bond activation and carbon-carbon bond transformation of an organic material under thermal conditions, and wherein the catalytic system is operated in an inert atmosphere.

2. The catalytic system of claim 1, wherein the vessel comprises a resistively heated tube.

3. The catalytic system of claim 1, wherein the transition metal comprises titanium.

4. The catalytic system of claim 1, wherein the main group element comprises at least one of aluminum or boron.

5. The catalytic system of claim 1, wherein the catalyst composition is synthesized by a sonochemically mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride.Attorney Docket No. : 3229-7 PCT6. The catalytic system of claim 1 , wherein the catalyst composition is amorphous with atomically dispersed metals having mutual interatomic linkages.

7. The catalytic system of claim 1, wherein the organic material comprises at least one of a hydrocarbon fuel selected from JP-1O and F-24, a polymer selected from polyethylene or polypropylene, or a biomass-derived compound.

8. The catalytic system of claim 1, wherein the catalytic system is configured to initiate decomposition of hydrocarbons at a temperature ranging from about room temperature to about 750 K.

9. The catalytic system of claim 1, further comprising a product analysis interface configured to detect volatile products formed during catalytic transformation of the organic material.

10. The catalytic system of claim 1, wherein the catalyst composition comprises a titanium- aluminum-boron nanopowder.

11. A method for catalytic transformation of an organic material, comprising: adding a catalyst composition comprising at least one transition metal atomically dispersed in a matrix of at least one main group element to a vessel; adding an organic material having carbon-hydrogen bonds to the vessel; and heating the organic material in the presence of the catalyst composition in an inert atmosphere to induce catalytic decomposition, cracking, dehydrogenation, reforming, or relatedAttorney Docket No. : 3229-7 PCT transformations of the organic material.

12. The method of claim 11, wherein the transition metal comprises titanium.

13. The method of claim 11, wherein the main group element comprises at least one of aluminum or boron.

14. The method of claim 11, further comprising synthesizing the catalyst composition by a sonochemically-mediated reaction of a transition metal chloride with lithium borohydride and lithium aluminum hydride.

15. The method of claim 11, further comprising adding the catalyst composition in the form of an amorphous nanopowder with atomically-dispersed metals.

16. The method of claim 11, wherein the organic material comprises at least one of a hydrocarbon fuel selected from JP-10 and F-24, a polymer selected from polyethylene or polypropylene, or a biomass -derived compound.

17. The method of claim 11, further comprising heating the organic material in the presence of the catalyst composition to initiate decomposition at a temperature ranging from about room temperature to at about 750 K.Attorney Docket No. : 3229-7 PCT18. The method of claim 11 , further comprising detecting products of the catalytic decomposition including at least one of 1 ,3-cyclopentadiene, cyclopentene, pentadiene, or molecular hydrogen.

19. The method of claim 11, wherein the catalyst composition comprises a titanium-aluminum- boron nanopowder.

20. A catalytic system for hydrocarbon decomposition, comprising: a titanium-aluminum-boron nanopowder synthesized by a sonochemically-mediated reaction of titanium chloride with lithium borohydride and lithium aluminum hydride in an inert atmosphere, wherein the titanium- aluminum-boron nanopowder is amorphous with atomically-dispersed titanium, aluminum, and boron, and is configured to initiate catalytic decomposition of a hydrocarbon fuel at an onset temperature of about 750 K to produce products including 1,3-cyclopentadiene, cyclopentene, pentadiene, and molecular hydrogen.

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