Photo-thermal multi-field coupling catalyst of metal phthalocyanine intercalation two-dimensional metal boride, preparation method of photo-thermal multi-field coupling catalyst and photo-thermal catalytic synthesis ammonia application

Abstract

The invention belongs to the technical field of two-dimensional metal boride catalytic materials, and particularly relates to a photo-thermal multi-field coupling catalyst of a metal phthalocyanine intercalation two-dimensional metal boride, a preparation method of the photo-thermal multi-field coupling catalyst and photo-thermal catalytic ammonia synthesis application of the photo-thermal multi-field coupling catalyst. The photo-thermal multi-field coupling catalyst of the metal phthalocyanine intercalated two-dimensional metal boride is a catalytic material in which a metal phthalocyanine photo-assisted N2 activation functional layer grows between hexagonal boride layers, and the introduction of the metal phthalocyanine functional layer significantly enhances the adsorption capacity of a RuMoBx / MPc composite material to N2 and H2, enriches the active sites of nitrogen reduction reaction, and enhances the adsorption capacity of the RuMoBx / MPc composite material to N2 and H2. And electron transfer in the photo-thermal catalysis process and interlayer transmission of reaction intermediates are promoted. In a photo-thermal synergistic catalysis mechanism, interlayer metal phthalocyanine molecules preferentially activate N2 molecules and generate a nitrogen intermediate under an illumination condition, and then overflow of nitrogen species to the surface of the RuMoBx two-dimensional material is realized through a thermocatalysis auxiliary effect, so that an ammonia synthesis reaction is efficiently completed.

Description

Technical Field

[0001] This invention belongs to the field of two-dimensional metal boride catalytic materials technology, specifically relating to photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides, their preparation methods, and their application in photothermal catalytic ammonia synthesis. Background Technology

[0002] Ammonia is not only an important agricultural fertilizer, industrial raw material, and refrigerant, but also considered a highly promising clean energy carrier and hydrogen storage medium due to its high energy density, easy liquefaction and storage, and zero-carbon characteristics. my country, as the world's largest producer of synthetic ammonia, has an annual output of 65 million tons, providing a solid foundation for the development of ammonia energy. However, the current mainstream industrial ammonia synthesis technology still uses the traditional Haber-Bosch process, which requires harsh conditions of high temperature (400℃~500℃) and high pressure (15MPa~25MPa), resulting in extremely high energy consumption and serious carbon emissions. Therefore, developing green catalytic technologies that can achieve efficient ammonia synthesis under mild conditions has become an urgent need to overcome industry bottlenecks and promote the transformation and upgrading of the synthetic ammonia industry.

[0003] From the perspective of the catalytic reaction itself, the ammonia synthesis process faces an inherent scientific challenge: the extremely high bond energy (941 kJ / mol) of the nitrogen-nitrogen triple bond necessitates a high activation energy for the dissociation of the N2 molecule, requiring a high temperature from a kinetic perspective. However, the ammonia synthesis reaction is exothermic, and from a thermodynamic equilibrium perspective, it is more suitable to proceed at low temperatures. This inherent contradiction in temperature requirements makes it difficult for the traditional single-temperature-field Haber-Bosch process to simultaneously achieve reaction efficiency and energy consumption control. In recent years, photothermal multi-field coupling technology has provided a new approach to resolving this contradiction. By constructing a catalytic system with spatial partitioning, the two elementary reactions of N2 activation and NH3 formation are carried out in different active regions of the catalyst. The photothermal field is used to achieve efficient N2 activation at low temperatures, and the thermal field promotes the subsequent hydrogenation step, thus overcoming the limitations of traditional thermodynamic equilibrium under mild conditions. The key to realizing this technological path lies in developing support materials capable of precisely constructing such partitioned catalytic systems.

[0004] Two-dimensional layered materials, due to their tunable interlayer microenvironment and unique electronic structure, provide an ideal platform for constructing partitioned catalytic systems. Among them, two-dimensional transition metal borosilicates (MBenes), as an emerging family of two-dimensional materials, not only possess a layered structure similar to MXenes and excellent ion transport performance, but their rich surface chemistry and tunable interlayer spacing also create conditions for precise interlayer engineering. However, MBenes materials face challenges in practical catalytic applications, such as easy layer stacking, active site embedding, and limited mass transfer, which restricts their efficiency in multi-step synergistic catalytic reactions. Summary of the Invention

[0005] In existing technologies, the high N≡N bond dissociation energy in the ammonia synthesis system and the difficulty in high-temperature hydrogenation of intermediates lead to the difficulty in N₂ cleavage and activation, and the challenges in NH₃ synthesis. x To address the problem of low hydrogenation efficiency of intermediates, this invention provides a photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal borides, its preparation method, and its application in photothermal catalytic ammonia synthesis. This invention first prepares RuMoB... x Two-dimensional material, then RuMoB x A photothermal multi-field coupled catalyst is prepared by solvothermal reaction of two-dimensional materials and metal phthalocyanines to intercalate two-dimensional metal borides with metal phthalocyanines. A catalytic material with a metal phthalocyanine photo-assisted N2 activation functional layer grown between hexagonal boride layers is constructed. This catalytic material not only effectively solves the aforementioned technical problems but also overcomes the technical defects of MBENS materials. Furthermore, the method of this invention is simple and operates under mild conditions, and the resulting product possesses a unique organic-inorganic heterostructure, which can significantly enhance the photothermal catalytic activity of MBENS materials, thereby achieving efficient ammonia synthesis under low temperature and low pressure.

[0006] Based on the above technical objectives, the present invention adopts the following technical solution: This invention protects a method for preparing a photothermal multi-field coupled catalyst of a metal phthalocyanine intercalated two-dimensional metal boride, comprising the following steps: Soluble ruthenium salt and MoB x Two-dimensional materials are co-dispersed in a solvent, and MoB is impregnated with soluble ruthenium salt. x Two-dimensional material, solvent evaporates during impregnation, then undergoes reduction reaction to obtain RuMoB. x Two-dimensional materials.

[0007] RuMoB x Two-dimensional materials and metal phthalocyanines were separately dispersed in DMF, then mixed, and subsequently subjected to a solvothermal reaction under ultravacuum conditions. The metal phthalocyanines then self-assembled with RuMoB in situ. x Two-dimensional material composites were synthesized, and a "freezing-vacuuming" operation was repeated five or more times under ultra-vacuum conditions. Liquid nitrogen was used for freezing during the freezing process to obtain a photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride. The crude product of the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride was filtered and washed with deionized water, ethanol, and tetrahydrofuran. Each of the three reagents was used for washing three times or more, followed by vacuum drying at 80°C for at least 24 hours.

[0008] Preferably, soluble ruthenium salts and MoB x The mass ratio of two-dimensional materials is 1~5:100; if the ruthenium loading is too low, the effective activity will be insufficient, and if it is too high, the atom utilization rate will decrease.

[0009] Preferably, the conditions for the reduction reaction are: heating at 400℃~500℃ for 2h~4h at a heating rate of 5℃ / min in a hydrogen or hydrogen-argon mixed atmosphere; in the hydrogen-argon mixed atmosphere, hydrogen accounts for 10%.

[0010] Preferably, the metal center of the metal phthalocyanine is selected from one or more of nickel, copper, and cobalt.

[0011] Preferably, in the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride, the metal phthalocyanine is intercalated in RuMoB x The loading amount on the two-dimensional material is 5wt%~30wt%. If the loading amount of metal phthalocyanine is too low, the number of active sites will be insufficient. If it is too high, the metal phthalocyanine will easily agglomerate, which will reduce the number of active sites. The loading amount refers to the mass percentage of metal phthalocyanine in the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride.

[0012] Preferably, the solvothermal reaction conditions are: in a flame-sealed ultra-vacuum reaction tube, the temperature is maintained at 150℃~200℃ for 12h~36h.

[0013] Preferred, MoB x Two-dimensional materials are prepared according to the following steps: Will (Mo 2 / 3 Y 1 / 3 AlB2 precursor powder was placed in a polytetrafluoroethylene reactor containing hydrofluoric acid and hydrochloric acid for etching to obtain MoB2 precursor powder. x Two-dimensional materials, the obtained MoB x Two-dimensional materials are washed with water until pH > 6, then freeze-dried for at least 24 hours. The hydrofluoric acid has a mass percentage concentration of 45%, and the hydrochloric acid has a mass percentage concentration of 20%. The etching conditions are: stirring at 40℃~60℃ for 30h~36h.

[0014] This invention also protects a photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride, prepared using the above-described method, MoB x Two-dimensional materials are rich in defect sites, which are metal vacancies used to anchor Ru metal. The transition metal of the metal phthalocyanine is anchored to RuMoB in one or more forms, such as single atoms or nanoparticles. x Vacancies or surfaces of two-dimensional materials, photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides exhibit highly efficient visible light response.

[0015] This invention also protects the application of photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides in the preparation of photothermal catalytic ammonia synthesis catalysts.

[0016] Preferably, the application method is as follows: the hydrogen / nitrogen volume ratio is 3:1 and the mass hourly space velocity is 24000 h⁻¹. -1 ~48000h -1 Under conditions of 320℃~420℃, 0.1MPa~5MPa, and 300W illumination, a photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride is used for photothermal catalytic synthesis of ammonia, exhibiting excellent ammonia synthesis performance.

[0017] Compared with the prior art, the beneficial effects of the present invention are as follows: 1. This invention provides a photothermal multi-field coupled catalyst of a metal phthalocyanine intercalated two-dimensional metal boride, which is prepared by the following technical solution: First, MoB with a two-dimensional layered structure is prepared by acid-assisted selective etching. x Two-dimensional materials; subsequently, an impregnation method combined with reduction calcination was used to prepare MoB. x Surface defect sites of two-dimensional materials were used to anchor ruthenium clusters to construct inorganic composite supports, and RuMoB was obtained. x Two-dimensional materials; furthermore, under strictly controlled conditions, RuMoB was synthesized using an ultravacuum-assisted solvothermal method. x In-situ interlayer growth of metal phthalocyanine molecules in two-dimensional materials ultimately constructs a composite material with photothermal synergistic catalytic function. This invention, through rational interlayer design and precise structural control, constructs active unit metal phthalocyanine with photo-assisted N2 activation function within the interlayer of MBENS materials, while maintaining its surface thermocatalytic hydrogenation performance, achieving true "dual-domain confinement" catalysis. This provides a novel material platform and solution for developing highly efficient photothermal synergistic ammonia synthesis catalysts.

[0018] 2. Compared with the prior art, the essential features of this invention are as follows: the van der Waals forces between adjacent layers of the stripped MBENS material are weakened, making it easier to regulate the interlayer catalytic environment using ions, atoms, and molecules, which is beneficial for charge transfer and intermediate mass transfer in the nitrogen reduction process. The defects exposed on its surface introduce the noble metal ruthenium, which has a strong affinity for nitrogen and can effectively activate it. Furthermore, the transition metal molybdenum present on the surface can serve as an active site for the reaction, exhibiting high activity and high atomic utilization. The stripped RuMoB... x Metal phthalocyanine, a sandwich material possessing both excellent N2 adsorption performance and strong light absorption capacity, was grown in situ between two-dimensional material layers. Light energy was used to assist in the activation of N2 formation. * N intermediate, then * N overflows onto the MBenes surface, aided by an external low-temperature heat source. * Nitrogen (N) is hydrogenated to produce ammonia. This synergistic effect overcomes the shortcomings of traditional single photocatalytic and thermocatalytic ammonia synthesis systems, enabling ammonia production through low-temperature and low-pressure hydrogenation.

[0019] 3. Compared with the prior art, the technical effects and advantages of the present invention are as follows: (1) In this invention, metal phthalocyanine, denoted as RuMoB, is grown between two-dimensional boride layers. x / MPc composite material. First, etch with hydrofluoric acid / hydrochloric acid (Mo). 2 / 3 Y 1 / 3 Preparation of MoB from AlB2 x Two-dimensional materials were then used to prepare Ru-loaded MoB by an impregnation method. x Two-dimensional materials (RuMoB) x (Two-dimensional material), and then in situ grow metal phthalocyanine on RuMoB under inert ultravacuum conditions. x In the interlayer of two-dimensional materials, the orderly growth of metal phthalocyanine molecules on RuMoB was finally achieved. x RuMoB between two-dimensional material layers x / MPc composite materials provide theoretical guidance for the design and synthesis of highly efficient two-dimensional metal boride catalysts.

[0020] (2) This invention investigated the effects of metal phthalocyanine loading, metal phthalocyanine type, light wavelength, and temperature and pressure conditions of the ammonia synthesis system on RuMoB x The study investigated the influence of / MPc composite materials on ammonia synthesis performance, using metal phthalocyanine as a photo-assisted N2 activation functional layer, providing a new approach for designing two-dimensional metal boride materials for low-temperature, low-pressure photothermal coupled ammonia synthesis.

[0021] 4. This invention provides a photothermal multi-field coupled catalyst for two-dimensional metal borides intercalated with metal phthalocyanines. This catalyst employs ultra-vacuum in-situ growth technology to precisely embed MPc molecules into RuMoB. x Two-dimensional material interlayer sites to achieve RuMoB x Effective regulation of the interlayer catalytic microenvironment in two-dimensional materials. X-ray diffraction results show that RuMoB x / MPc composite material fully retains RuMoB x The presence of a bulk crystalline structure in the two-dimensional material without impurity phase formation confirms that this strategy achieves effective intercalation while maintaining the structural integrity of the substrate material. Characterization analysis shows that the introduction of the MPc functional layer significantly enhances RuMoB. xThe adsorption capacity of the / MPc composite material for N2 and H2 enriches the active sites for nitrogen reduction reactions and promotes electron transfer and interlayer transport of reaction intermediates during photothermal catalysis. In the photothermal synergistic catalytic mechanism, interlayer metal phthalocyanine molecules preferentially activate N2 molecules and generate nitrogen intermediates under light irradiation. Subsequently, through thermocatalytic assistance, nitrogen species overflow to the surface of the two-dimensional metal boride, thereby efficiently completing the ammonia synthesis reaction. This process organically integrates the advantages of photocatalysis in nitrogen activation and the efficiency of thermocatalysis in hydrogenation synthesis. Under atmospheric pressure and 420℃ reaction conditions, the MPc-intercalated RuMoB x The ammonia synthesis activity of the / MPc composite material is increased to that of the original material MoB. x The two-dimensional material exhibits 6.0 times the strength, demonstrating significantly enhanced catalytic performance. Attached Figure Description

[0022] Figure 1 In Figure (a), MoB from Example 1 is shown. x SEM images of two-dimensional materials, (b) showing RuMoB from Example 1. x SEM image of a two-dimensional material.

[0023] Figure 2 In Figure (a), MoB from Example 1 is shown. x XRD patterns of two-dimensional materials, (b) shows MoB from Example 1. x Two-dimensional materials, NiPc, CuPc, RuMoB from Example 4 x / NiPc-20 and RuMoB of Example 6 x DRS diagram of / CuPc-20, (c) Figure is RuMoB of Example 4 x TEM image of / NiPc-20, (d) is RuMoB of Example 4. x Energy dispersive X-ray elemental distribution map of / NiPc-20.

[0024] Figure 3 Figure (a) shows RuMoB from Example 1. x Two-dimensional material, RuMoB of Example 4 x / NiPc-20 and RuMoB of Example 6 x Figure (b) shows the N2 temperature-programmed desorption process of / CuPc-20. x Two-dimensional material, RuMoB of Example 4 x / NiPc-20 and RuMoB of Example 6 x H2 programmed temperature desorption of / CuPc-20 (see attached diagram).

[0025] Figure 4In the figures, (a) shows the photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides from Examples 1-5 under no-light conditions for photothermal ammonia synthesis; (b) shows the photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides from Examples 1-5 under light conditions for photothermal ammonia synthesis; and (c) shows the RuMoB catalyst from Example 4. x / NiPc-20 and RuMoB of Example 6 x Photothermal catalytic ammonia synthesis activity of / CuPc-20 under no light and at different temperatures. Figure (d) shows the RuMoB activity of Example 4. x / NiPc-20 and RuMoB of Example 6 x Photothermal catalytic activity of / CuPc-20 for ammonia synthesis under illumination and at different temperatures.

[0026] Figure 5 In Figure (a), RuMoB of Example 4 is shown. x Photothermal coupling activity diagram of / NiPc-20 at different wavelengths for ammonia synthesis; (b) Figure shows RuMoB from Example 6. x Photothermal coupling ammonia synthesis activity diagram of / CuPc-20 at different wavelengths, (c) Figure shows RuMoB in Example 4. x Photothermal coupling activity diagrams of / NiPc-20 for ammonia synthesis under different pressures and in both light and dark environments, (d) shows the RuMoB of Example 6. x / CuPc-20 photothermal coupling ammonia synthesis activity diagram under different pressures in light and dark environments. Detailed Implementation

[0027] The present invention will be further described below with reference to embodiments and accompanying drawings, but the embodiments of the present invention are not limited thereto. Unless otherwise specified, the technical means used in the embodiments are conventional means well known to those skilled in the art.

[0028] Unless otherwise stated, the raw materials and reagents used in the following examples are commercially available products or can be prepared by known methods.

[0029] The preparation method of this invention features abundant raw materials and simple process. It effectively alleviates the problems of active site shielding and mass transfer resistance caused by interlayer stacking of two-dimensional metal borides through ultra-low vacuum technology. It provides a new technical path for precise control of the interlayer catalytic environment of two-dimensional materials, effectively overcomes the defects of existing MBenes materials, and shows important application prospects in the field of low-temperature and low-pressure ammonia synthesis.

[0030] The technical solution of the present invention will be further studied using the following embodiments, as detailed below: Example 1 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst includes the following steps: S1, Synthesis of MoB x Two-dimensional material: Mo powder (3.255g), Y powder (1.5084g), Al powder (0.6864g), and B powder (0.5502g) were first mixed and ground, then shaken in a centrifuge tube for 30 minutes to obtain a uniformly mixed sample. This sample was divided into three portions of 2g each and compressed into tablets using a tablet press. The three samples were then placed in corundum boats, which were placed in a tube furnace and reacted at 1500℃ for 200 minutes in an Ar atmosphere to obtain sintered samples. The sintered samples were thoroughly ground, and Mo powder with a pore size less than 38μm was sieved through a 200-mesh sieve. 2 / 3 Y 1 / 3 )2AlB2.

[0031] Weigh 1g of (Mo) with a particle size less than 38μm. 2 / 3 Y 1 / 3 2AlB2 was placed in a reaction vessel, and 8 mL of concentrated hydrochloric acid and 12 mL of HF were slowly added to the reaction vessel in a fume hood. The etching reaction was carried out at 50 °C for 35 h. After the etching reaction was completed, solid-liquid separation was performed in a high-speed centrifuge. The mixture was centrifuged at 7000 rpm for 5 min, washed with deionized water, and then centrifuged at 7000 rpm for 3 min and washed again. This step was repeated until the pH of the supernatant was >6, and the etched ultrathin two-dimensional MoB2 was obtained. x Materials; The precipitate was collected and placed in a vacuum freeze-drying oven, frozen at -40°C for 2 hours, and then freeze-dried under vacuum for 24 hours until the sample was powdery. The resulting black solid product was MoB. x Two-dimensional materials.

[0032] S2, Synthesis of RuMoB x Two-dimensional materials: MoB was prepared using an impregnation method. x The two-dimensional material was used to load the co-catalyst Ru. The specific procedure was as follows: Ru3(CO) was added to a 50 mL beaker. 12 (26.0mg), MoB x Two-dimensional material (500.0 mg) and tetrahydrofuran (30.0 mL) were mixed. The beaker was covered with aluminum foil, and the mixture was stirred at a constant speed with a magnetic stirrer for 4 hours until the tetrahydrofuran was completely volatilized, resulting in Ru3(CO). 12 In MoB x The powder is uniformly dispersed in the two-dimensional material; the powder in the beaker is collected and placed in a glass boat, which is then placed in a reduction furnace. A H2 / Ar mixed gas is introduced, and the reduction reaction is carried out at 420℃ for 3 hours to ensure the Ru3(CO) content is maintained. 12 In MoB xAfter complete decomposition on a two-dimensional material and cooling to room temperature, RuMoB was obtained. x Two-dimensional materials.

[0033] S3, RuMoB x Synthesis of NiPc-5 catalyst: Inert ultravacuum technology was used to synthesize the catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (475.0 mg) and nickel phthalocyanine (25.0 mg) were co-dispersed in 2 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed, followed by incubation at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, and then centrifuged and dried to obtain a composite material with a nickel phthalocyanine loading of 5 wt% (abbreviated as RuMoB). x / NiPc-5), namely, metal phthalocyanine (MPc) intercalated two-dimensional metal boride (RuMoB). x Photothermal multi-field coupling catalyst.

[0034] The MoB prepared in step S1 of this embodiment x SEM images of two-dimensional materials as shown Figure 1 As shown in Figure (a), after etching with concentrated hydrochloric acid and hydrofluoric acid, the bulk (Mo) 2 / 3 Y 1 / 3 The transformation of AlB2 into a layered structure indicates successful etching of the A-layer elements (Al and Y) in the original structure, resulting in a thinner layered MoB2. x Two-dimensional materials are advantageous for providing abundant sites for subsequent loading of Ru and metal phthalocyanines.

[0035] The RuMoB prepared in step S2 of this embodiment x SEM images of two-dimensional materials as shown Figure 1 As shown in Figure (b), after etching, MoB x After loading Ru onto the two-dimensional material, no obvious Ru nanoparticles were observed, indicating that Ru was dispersed in small amounts and uniformly in MoB. x The intralayer and interlayer structures of the two-dimensional material. Meanwhile, the metal borides still exhibit a layered structure, indicating that the impregnation method for loading Ru does not disrupt the lamellar microstructure and crystal phase type of the two-dimensional transition metal borides.

[0036] The MoB prepared in step S1 of this embodiment x XRD patterns of two-dimensional materials are shown below. Figure 2 Figure (a) shows the theoretically calculated (Mo) 2 / 3 Y1 / 3 )2AlB2, laboratory-prepared (Mo 2 / 3 Y 1 / 3 )2AlB2, MoB obtained after etching x The XRD results for the two-dimensional material show that etching reduces the atomic occupancy of the unit cell and significantly decreases the diffraction peak intensity. It should be noted that (Mo...) 2 / 3 Y 1 / 3 The primitive unit cell of 2AlB2 has a high atomic density, resulting in significant extinction of the (0001) low-plane lattice. Therefore, the diffraction peak of the (0001) plane is located at (Mo). 2 / 3 Y 1 / 3 It is difficult to observe in 2AlB2. The (0003) diffraction peak disappears, and the (0001) peak appears at 2θ=6.8º. (Mo) 2 / 3 Y 1 / 3 The interlayer spacing of 2AlB2 is 7.6 Å, and after etching, MoB x The interplanar spacing of the two-dimensional material is increased to 13.0 Å.

[0037] Example 2 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst is the same as that in Example 1, except that the nickel phthalocyanine loading is replaced from 5 wt% to 10 wt%, and includes the following steps: RuMoB x Synthesis of NiPc-10 catalyst: Inert ultravacuum technology was used to synthesize the catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (450.0 mg) and nickel phthalocyanine (50.0 mg) were co-dispersed in 3 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed, followed by incubation at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, centrifuged, and dried to obtain a composite material with a nickel phthalocyanine loading of 10 wt% (abbreviated as RuMoB). x / NiPc-10), namely, a two-dimensional metal boride (RuMoB) intercalated with metal phthalocyanine (MPc). x Photothermal multi-field coupling catalyst.

[0038] Example 3 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) xThe preparation method of the photothermal multi-field coupled catalyst is the same as that in Example 1, except that the nickel phthalocyanine loading is replaced from 5 wt% to 15 wt%, and includes the following steps: RuMoB x Synthesis of NiPc-15 catalyst: Inert ultravacuum technology was used in the synthesis of NiPc-15 catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (425.0 mg) and nickel phthalocyanine (75.0 mg) were co-dispersed in 4 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed. The mixture was incubated at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, centrifuged, and dried to obtain a composite material with a nickel phthalocyanine loading of 15 wt% (abbreviated as RuMoB). x / NiPc-15), namely, a two-dimensional metal boride (RuMoB) intercalated with metal phthalocyanine (MPc). x Photothermal multi-field coupling catalyst.

[0039] Example 4 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst is the same as that in Example 1, except that the nickel phthalocyanine loading is replaced from 5 wt% to 20 wt%, and includes the following steps: RuMoB x Synthesis of NiPc-20 catalyst: Inert ultravacuum technology was used to synthesize the catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (400.0 mg) and nickel phthalocyanine (100.0 mg) were co-dispersed in 5 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed. The mixture was incubated at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, centrifuged, and dried to obtain a composite material with a nickel phthalocyanine loading of 20 wt% (abbreviated as RuMoB). x / NiPc-20), namely, a two-dimensional metal boride (RuMoB) intercalated with metal phthalocyanine (MPc). x Photothermal multi-field coupling catalyst.

[0040] Example 5 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst is the same as that in Example 1, except that the nickel phthalocyanine loading is replaced from 5 wt% to 30 wt%, and includes the following steps: RuMoB x Synthesis of NiPc-30 catalyst: Inert ultravacuum technology was used in the synthesis of NiPc-30 catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (350.0 mg) and nickel phthalocyanine (150.0 mg) were co-dispersed in 7 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed, followed by incubation at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, centrifuged, and dried to obtain a composite material with a nickel phthalocyanine loading of 30 wt% (abbreviated as RuMoB). x / NiPc-30), namely, metal phthalocyanine (MPc) intercalated two-dimensional metal boride (RuMoB). x Photothermal multi-field coupling catalyst.

[0041] Example 6 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst is the same as that in Example 4, except that nickel phthalocyanine is replaced with an equal amount of copper phthalocyanine, and includes the following steps: RuMoB x Synthesis of CuPc-20 catalyst: An inert ultravacuum technique was used to synthesize the catalyst in RuMoB2. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (400.0 mg) and copper phthalocyanine (100.0 mg) were co-dispersed in 75 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed, followed by incubation at 160 °C for 24 h in a flame-sealed ultra-vacuum reaction tube. The mixture was repeatedly washed with deionized water, ethanol, and tetrahydrofuran, centrifuged, and dried to obtain a composite material with a copper phthalocyanine loading of 20 wt% (abbreviated as RuMoB).x / CuPc-20), namely, metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB). x Photothermal multi-field coupling catalyst.

[0042] Example 7 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst includes the following steps: S1, Synthesis of MoB x Two-dimensional material: Mo powder (3.255g), Y powder (1.5084g), Al powder (0.6864g), and B powder (0.5502g) were first mixed and ground, then shaken in a centrifuge tube for 30 minutes to obtain a uniformly mixed sample. This sample was divided into three portions of 2g each and compressed into tablets using a tablet press. The three samples were then placed in corundum boats, which were placed in a tube furnace and reacted at 1500℃ for 200 minutes in an Ar atmosphere to obtain sintered samples. The sintered samples were thoroughly ground, and Mo powder with a pore size less than 38μm was sieved through a 200-mesh sieve. 2 / 3 Y 1 / 3 )2AlB2.

[0043] Weigh 1g of (Mo) with a particle size less than 38μm. 2 / 3 Y 1 / 3 2AlB2 was placed in a reaction vessel, and 8 mL of concentrated hydrochloric acid and 12 mL of HF were slowly added to the reaction vessel in a fume hood. The etching reaction was carried out at 40 °C for 36 h. After the etching reaction was completed, solid-liquid separation was performed in a high-speed centrifuge. The mixture was centrifuged at 7000 rpm for 5 min, washed with deionized water, and then centrifuged at 7000 rpm for 3 min and washed again. This step was repeated until the pH of the supernatant was >6, and the etched ultrathin two-dimensional MoB2 was obtained. x Materials; The precipitate was collected and placed in a vacuum freeze-drying oven, frozen at -40°C for 2 hours, and then freeze-dried under vacuum for 24 hours until the sample was powdery. The resulting black solid product was MoB. x Two-dimensional materials.

[0044] S2, Synthesis of RuMoB x Two-dimensional materials: MoB was prepared using an impregnation method. x The two-dimensional material was used to load the co-catalyst Ru. The specific procedure was as follows: Ru3(CO) was added to a 50 mL beaker. 12 (15.0mg), MoB x Two-dimensional material (500.0 mg) and tetrahydrofuran (30.0 mL) were mixed. The beaker was covered with aluminum foil, and the mixture was stirred at a constant speed with a magnetic stirrer for 4 hours until the tetrahydrofuran was completely volatilized, resulting in Ru3(CO). 12 In MoBx The powder is uniformly dispersed in the two-dimensional material; the powder in the beaker is collected and placed in a glass boat, which is then placed in a reduction furnace. A H2 / Ar mixed gas is introduced, and the reduction reaction is carried out at 400℃ for 4 hours to ensure the Ru3(CO) content is maintained. 12 In MoB x After complete decomposition on a two-dimensional material and cooling to room temperature, RuMoB was obtained. x Two-dimensional materials.

[0045] S3, RuMoB x Synthesis of / CoPc-5 catalyst: Inert ultravacuum technology was used in the synthesis of RuMoB catalyst. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (450.0 mg) and cobalt phthalocyanine (50.0 mg) were co-dispersed in 2 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Five "freeze-vacuum" cycles were then performed. The mixture was incubated at 150 °C for 36 h in a flame-sealed ultra-vacuum reaction tube. After repeated washing with deionized water, ethanol, and tetrahydrofuran, and centrifugation and drying, a two-dimensional metal boride (RuMoB) intercalated with metal phthalocyanine (MPc) was obtained. x Photothermal multi-field coupling catalyst.

[0046] Example 8 Metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) x The preparation method of the photothermal multi-field coupled catalyst includes the following steps: S1, Synthesis of MoB x Two-dimensional material: Mo powder (3.255g), Y powder (1.5084g), Al powder (0.6864g), and B powder (0.5502g) were first mixed and ground, then shaken in a centrifuge tube for 30 minutes to obtain a uniformly mixed sample. This sample was divided into three portions of 2g each and compressed into tablets using a tablet press. The three samples were then placed in corundum boats, which were placed in a tube furnace and reacted at 1500℃ for 200 minutes in an Ar atmosphere to obtain sintered samples. The sintered samples were thoroughly ground, and Mo powder with a pore size less than 38μm was sieved through a 200-mesh sieve. 2 / 3 Y 1 / 3 )2AlB2.

[0047] Weigh 1g of (Mo) with a particle size less than 38μm. 2 / 3 Y 1 / 32AlB2 was placed in a reaction vessel, and 8 mL of concentrated hydrochloric acid and 12 mL of HF were slowly added to the reaction vessel in a fume hood. The etching reaction was carried out at 60 °C for 30 h. After the etching reaction was completed, solid-liquid separation was performed in a high-speed centrifuge. The mixture was centrifuged at 7000 rpm for 5 min, washed with deionized water, and then centrifuged at 7000 rpm for 3 min and washed. This step was repeated until the pH of the supernatant was >6, and the etched ultrathin two-dimensional MoB2 was obtained. x Materials; The precipitate was collected and placed in a vacuum freeze-drying oven, frozen at -40°C for 2 hours, and then freeze-dried under vacuum for 24 hours until the sample was powdery. The resulting black solid product was MoB. x Two-dimensional materials.

[0048] S2, Synthesis of RuMoB x Two-dimensional materials: MoB was prepared using an impregnation method. x The two-dimensional material was used to load the co-catalyst Ru. The specific procedure was as follows: Ru3(CO) was added to a 50 mL beaker. 12 (5.0mg), MoB x Two-dimensional material (500.0 mg) and tetrahydrofuran (30.0 mL) were mixed. The beaker was covered with aluminum foil, and the mixture was stirred at a constant speed with a magnetic stirrer for 4 hours until the tetrahydrofuran was completely volatilized, resulting in Ru3(CO). 12 In MoB x The powder is uniformly dispersed in the two-dimensional material; the powder in the beaker is collected and placed in a glass boat, which is then placed in a reduction furnace. A H2 / Ar mixed gas is introduced, and the reduction reaction is carried out at 500℃ for 2 hours to ensure that Ru3(CO) is uniformly dispersed. 12 In MoB x After complete decomposition on a two-dimensional material and cooling to room temperature, RuMoB was obtained. x Two-dimensional materials.

[0049] S3, RuMoB x Synthesis of / CoPc-5 catalyst: Inert ultravacuum technology was used in the synthesis of RuMoB catalyst. x In-situ growth of metal phthalocyanine photo-assisted N2 activation functional layers between two-dimensional material layers to activate RuMoB x The interlayer catalytic environment of two-dimensional materials can be controlled by: [the method described is missing from the original text]. x Two-dimensional material (450.0 mg) and cobalt phthalocyanine (50.0 mg) were co-dispersed in 2 mL of DMF and stirred with a magnetic stirrer for 30 min, followed by sonication for 30 min. Then, five "freeze-vacuum" cycles were performed. The mixture was kept at 200 °C for 12 h in a flame-sealed ultra-vacuum reaction tube. After repeated washing with deionized water, ethanol, and tetrahydrofuran, the mixture was centrifuged and dried to obtain a photothermal multi-field coupled catalyst of metal phthalocyanine (MPc) intercalated two-dimensional metal boride (RuMoBx).

[0050] Examples 1-8 of this invention all yielded photothermal multi-field coupled catalysts with excellent ammonia synthesis catalytic performance using metal phthalocyanine intercalated two-dimensional metal borides. The following studies use the photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides from Examples 1-6 as examples. Specific research methods and results are shown below: Figure 2 Figure (b) in the diagram is MoB x Two-dimensional materials, NiPc, CuPc, RuMoB x / NiPc-20 and RuMoB x The diffuse reflectance absorption spectrum (DRS) of / CuPc-20. The figure shows that MoB... x Two-dimensional materials do not exhibit obvious light absorption peaks, while NiPc and CuPc show distinct absorption peaks in the visible light range (B band, 400 nm~450 nm; Q band, 660 nm~700 nm), indicating that metal phthalocyanines possess excellent light absorption capabilities. RuMoB x After loading metal phthalocyanines onto two-dimensional materials, RuMoB x / NiPc-20 and RuMoB x / CuPc-20 exhibits broad absorption peaks in both the 450 nm–500 nm and 640 nm–680 nm ranges. These results indicate that RuMoB x / NiPc-20 and RuMoB x / CuPc-20 possesses the visible light absorption properties of metal phthalocyanines, which can enhance RuMoB x Photocatalytic ammonia synthesis performance of two-dimensional materials.

[0051] Figure 2 Figures (c) and (d) in the figure represent RuMoB. x High-resolution transmission electron microscopy (TEM) images and energy-dispersive X-ray elemental mapping of / NiPc-20. NiPc was grown in situ in a vacuum-sealed quartz tube using an impregnation method with Ru-loaded material and an oxyhydrogen flame. RuMoB x / NiPc-20 exhibits an ultrathin, sheet-like structure without obvious accumulation of nanoparticles, consistent with SEM analysis results. Its energy-dispersive X-ray elemental distribution map shows that Mo, B, Ru, and Ni are uniformly distributed in the RuMoB matrix. x Two-dimensional material surfaces. These results demonstrate that Ru and NiPc on MoB x Successful in-situ growth of uniformly distributed Ru and Ni sites on two-dimensional materials is beneficial to improving the catalytic performance of composite materials.

[0052] Figure 3 It is RuMoB x Two-dimensional materials, RuMoB x / NiPc-20 and RuMoB x The N2 and H2 temperature program for removing / CuPc-20 is shown in the attached figure. From the figure, it can be seen that RuMoB x Two-dimensional materials exhibit N2 desorption peaks at 530℃, 650℃, and 750℃, and H2 desorption peaks at 590℃, 700℃, and 800℃; RuMoB x / NiPc-20 exhibits N2 desorption peaks at 500℃, 640℃, and 850℃, and H2 desorption peaks at 600℃, 690℃, and 750℃; RuMoB x / CuPc-20 exhibits N2 desorption peaks at 520℃, 620℃, and 780℃, and H2 desorption peaks at 580℃, 690℃, and 800℃. The reasons for the appearance of the three peaks in the N2 and H2 temperature-programmed desorption images can be attributed, in order: desorption following physical adsorption of N2 / H2, desorption following chemical adsorption of N2 / H2, and desorption following intra-lattice storage of N2 / H2. Comparison of peak area and full width at half maximum (FWHM) reveals that metal phthalocyanines in RuMoB... x After interlayer growth of two-dimensional materials, RuMoB x The N2 and H2 adsorption properties of the two-dimensional material RuMoB are significantly altered. x / NiPc-20 and RuMoB x / CuPc-20 has excellent intra-lattice adsorption capacity for N2 / H2, which will be beneficial to improving the ammonia synthesis performance of composite materials.

[0053] The metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) prepared in various embodiments of the present invention x The photothermal multi-field coupled catalyst was used in a photothermal catalytic synthesis experiment to detect its photothermal catalytic activity. The relevant results are as follows: Figure 4 and Figure 5 As shown. The specific steps are as follows:

[0054] The metal phthalocyanine (MPc) intercalated two-dimensional metal borides (RuMoB) prepared in each embodiment were used. x The photothermal multi-field coupled catalyst was tested under the following conditions: darkness or xenon lamp irradiation, at a temperature of 320℃~420℃, a pressure of 0.1MPa~1.5MPa, a hydrogen / nitrogen volume ratio of 3:1, and a mass hourly space velocity of 36000h⁻¹. -1 Under certain conditions, the performance of photothermal catalytic ammonia synthesis was tested, and the results were used for photothermal catalytic ammonia production.

[0055] Take the metal phthalocyanine (MPc) intercalated two-dimensional metal boride (RuMoB) from each embodiment x 100 mg of each of the photothermal multi-field coupling catalyst were used to determine the ammonia synthesis rate in a fixed reaction bed. The outlet tail gas was passed into a dilute sulfuric acid absorption solution, and the change in the concentration of ammonium ions in the solution was determined by ion chromatography.

[0056] Figure 4 Figures (a) and (b) show the photothermal catalytic ammonia synthesis activity tests for different metal phthalocyanine loadings. The results show that the catalytic activity first increases and then decreases with the increase of metal phthalocyanine loading, which may be related to the occupation of active sites. The ammonia synthesis activity of the composite material will be further improved after the introduction of a light source. Figure 4 Figures (c) and (d) show that RuMoB x / NiPc-20 and RuMoB x The catalytic activity of both CuPc-20 and RuMoB catalysts increased with increasing temperature, and the activity of both was further enhanced upon the addition of light. x / CuPc-20 is significantly superior to RuMoB x Catalytic activity of NiPc-20; RuMoB at 420℃ x The catalytic activity of CuPc-20 is 335.0 μmol g. -1 h -1 After the addition of light irradiation, the catalytic activity increased to 358.0 μmolg. -1 h -1 Under the same conditions, RuMoB x The thermal catalytic activity of NiPc-20 is 289.6 μmol g. -1 h -1 The photothermal catalytic activity is 316.5 μmol g. -1 h -1 These results indicate that copper phthalocyanine loading is better than nickel phthalocyanine loading of RuMoB. x Two-dimensional materials exhibit superior photothermal coupling catalytic effects, which may be related to the different d-orbital electron arrangements of Cu and Ni. The catalytic activity of the composite material is further enhanced upon illumination, demonstrating excellent photothermal coupling performance for ammonia synthesis.

[0057] Figure 5 Figures (a) and (b) show RuMoB under different wavelengths of irradiation. x / NiPc-20 and RuMoB x The activity diagram of ammonia synthesis using CuPc-20 shows that RuMoB... as light intensity gradually decreases... x / NiPc-20 and RuMoB x The ammonia synthesis activity of / CuPc-20 gradually decreased, eventually exhibiting only thermal catalytic activity, further demonstrating that photocatalysis is enhanced by loading metal phthalocyanines onto RuMoB. x Ammonia synthesis activity of two-dimensional materials. Figure 5 Figures (c) and (d) show the RuMoB at 420℃ and different pressures, respectively. x / NiPc-20 and RuMoBx The photothermal coupling ammonia synthesis activity diagram of / CuPc-20 shows that the catalytic activity of both composite materials initially increases and then decreases with increasing pressure, and is significantly improved compared to the catalytic activity under normal pressure. Under 1.5 MPa and 300W xenon lamp irradiation conditions, both exhibit the highest ammonia synthesis activity. RuMoB x / CuPc-20 exhibited the best ammonia synthesis activity, at 543.8 μmol g. -1 h -1 It has excellent potential for industrial applications.

[0058] The above description is only used to illustrate the technical solution of the present invention and is not intended to limit it. Although the present invention has been described in detail through the above embodiments, those skilled in the art should understand that various changes in form and detail can be made without departing from the scope defined by the claims of the present invention.

Claims

1. A method for preparing a photothermal multi-field coupled catalyst of a metal phthalocyanine intercalated two-dimensional metal boride, characterized in that, Includes the following steps: Soluble ruthenium salt and MoB x Two-dimensional materials are co-dispersed in a solvent, and MoB is impregnated with soluble ruthenium salt. x After the two-dimensional material is processed, a reduction reaction is carried out to obtain RuMoB. x Two-dimensional materials; RuMoB x Two-dimensional material solutions and metal phthalocyanine solutions were mixed and dispersed, and then subjected to a solvothermal reaction under ultravacuum conditions in RuMoB. x In situ interlayer growth of metal phthalocyanine molecules in two-dimensional materials yields photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides.

2. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, Soluble ruthenium salts and MoB x The mass ratio of the two-dimensional materials is 1~5:

100.

3. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, The conditions for the reduction reaction are: heating at 400℃~500℃ for 2h~4h in a hydrogen or hydrogen-argon mixed atmosphere.

4. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, The metal center of a metal phthalocyanine is selected from one or more of nickel, copper, and cobalt.

5. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, In photothermal multi-field coupled catalysts of metal phthalocyanine intercalated two-dimensional metal borides, metal phthalocyanines in RuMoB x The loading on the two-dimensional material is 5wt%~30wt%.

6. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, The conditions for the solvothermal reaction are: in a flame-sealed ultra-vacuum reaction tube, the temperature is maintained at 150℃~200℃ for 12h~36h.

7. The method for preparing the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 1, characterized in that, MoB x Two-dimensional materials are prepared according to the following steps: Will (Mo 2 / 3 Y 1 / 3 The AlB2 precursor powder was etched with hydrofluoric acid and hydrochloric acid to obtain MoB2. x Two-dimensional materials; The hydrofluoric acid has a mass percentage concentration of 45%, and the hydrochloric acid has a mass percentage concentration of 20%. The etching conditions are: stirring at 40℃~60℃ for 30h~36h.

8. A photothermal multi-field coupled catalyst of a metal phthalocyanine intercalated two-dimensional metal boride, characterized in that, MoB was prepared by the preparation method according to any one of claims 1 to 7. x Two-dimensional materials are rich in defect sites, which are metal vacancies used to anchor Ru metal. The transition metal of the metal phthalocyanine is anchored to RuMoB in one or more forms, such as single atoms or nanoparticles. x Vacancies or surfaces of two-dimensional materials.

9. The application of the photothermal multi-field coupled catalyst of the metal phthalocyanine intercalated two-dimensional metal boride as described in claim 8 in the preparation of a photothermal catalytic ammonia synthesis catalyst.

10. The application of the photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride according to claim 9 in the preparation of a photothermal catalytic ammonia synthesis catalyst, characterized in that, The application method is as follows: with a hydrogen / nitrogen volume ratio of 3:1 and a mass hourly space velocity of 24000 h⁻¹. -1 ~48000h -1 Ammonia was synthesized by photothermal catalysis using a photothermal multi-field coupled catalyst of metal phthalocyanine intercalated two-dimensional metal boride under the conditions of 320℃~420℃, 0.1MPa~5MPa, and 300W illumination.

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