Two-dimensional Ni1Ce1O3 solid solution catalysts, their preparation methods and applications

Abstract

This invention provides a two-dimensional Ni1Ce1O3 solid solution catalyst, its preparation method, and its application. This invention synthesizes a two-dimensional fluorite-type Ni1Ce1O3 solid solution for ultra-low temperature CO2 methanation reactions, achieving CH4 yields of 80.4 and 2138 mmol g at 200℃ and 300℃, respectively. ‑1 h ‑1 The CH4 selectivity was >99.5%, superior to all reported catalysts. Furthermore, the combination of 2D Ni1Ce1O3 with a thermal radiation isolation device demonstrated a standard sunlight-driven photothermal CO2 methanation rate of 2901 mmol g / L. ‑1 h ‑1 (This is 5 times the highest reported value), and in the dark, the CO2 methanation rate is ~910 mmol g. ‑1 h ‑1 The preparation method of this invention has the advantages of being environmentally friendly and having wide applicability, making it very suitable for industrial production and practical applications.

Description

Technical Field

[0001] This invention relates to the field of catalyst technology, specifically to a two-dimensional Ni1Ce1O3 solid solution catalyst, its preparation method, and its application. Background Technology

[0002] Methane (CH4) is one of the most important chemical substances for humankind. It is the compound with the highest hydrogen storage capacity (25 wt%) among carbon-based supports and is also the only synthetic fuel in space. CO2 methanation (CO2 + 4H2 → CH4 + 2H2O) has shown great potential for recovering large-scale CO2 emissions and providing fuel for long-term space exploration, along with the storage of green hydrogen. Although CO2 methanation is an exothermic reaction, high temperatures are still required to activate the thermodynamically stable CO2 molecules. In recent years, a series of high-performance ruthenium (Ru) and nickel (Ni)-based catalysts have been developed. Among them, nickel-cerium composites have seen rapid development as methanation catalysts. Currently, nickel-cerium composites are divided into two categories: one is a nickel oxide / cerium oxide heterogeneous structure, and the other is a perovskite-type solid solution structure. The low-temperature methanation performance of both types of nickel-cerium composites is weaker than that of ruthenium-based catalysts. Summary of the Invention

[0003] The purpose of this invention is to provide a two-dimensional Ni1Ce1O3 solid solution catalyst, its preparation method and application. This two-dimensional Ni1Ce1O3 solid solution catalyst has a novel crystal structure and exhibits ultra-high methanation activity at low temperatures, which is superior to any known catalyst.

[0004] This invention is implemented as follows:

[0005] A two-dimensional Ni1Ce1O3 solid solution catalyst, which has diffraction peaks of fluorite structure.

[0006] Preferably, the two-dimensional Ni1Ce1O3 solid solution catalyst is synthesized by an explosive method. Specifically, a gel is prepared using the citric acid sol-gel method, dried, and then annealed in a tube furnace at 400°C for 3 hours. Finally, it is calcined in a muffle furnace at 450°C for 5 hours to obtain a two-dimensional Ni1Ce1O3 solid solution catalyst with a large specific surface area and excellent CO2 hydrogenation catalytic performance.

[0007] The two-dimensional Ni1Ce1O3 solid solution catalyst provided by this invention is a nickel-cerium two-dimensional solid solution catalyst with a novel crystal structure. Using it, the catalytic temperature can be reduced to below 350°C while maintaining a CO2 methanation rate of ~1000 mmol g. -1 h -1 This leads to CO2 photothermal methanation to avoid secondary energy consumption.

[0008] The method for preparing the two-dimensional Ni1Ce1O3 solid solution catalyst provided by this invention specifically includes the following steps:

[0009] a. Add citric acid, cerium nitrate and nickel nitrate to a beaker, add nitric acid, and then titrate with ammonia until the solution pH = 6;

[0010] b. Place the solution from step a on a heated stirring table and stir at 80°C to form a gel;

[0011] c. Place the gel obtained in step b into an oven to dry;

[0012] d. Place the dried gel into a tube furnace at 400°C. The gel will explode rapidly after entering the tube furnace. Then, calcine the gel in the tube furnace for 3 hours to obtain the catalyst precursor.

[0013] e. After cooling the catalyst precursor to room temperature, place it in a muffle furnace and calcine it at 450°C for 5 hours to obtain a two-dimensional Ni1Ce1O3 solid solution catalyst.

[0014] Preferably, in step a, the molar ratio of cerium nitrate to nickel nitrate is 1:1.

[0015] Preferably, in step c, the gel obtained in step b is placed in an oven at 100°C and dried for 24 hours.

[0016] Preferably, in step d, calcination is carried out in an Ar environment in a tube furnace for 3 hours; in step e, calcination is carried out in an air environment in a muffle furnace for 5 hours.

[0017] This invention discloses a method for preparing two-dimensional nanosheet-like Ni1Ce1O3 solid solution catalysts. The prepared catalysts have the characteristics of high specific surface area, uniform element distribution, and nanosheet morphology.

[0018] This invention further discloses the application of a two-dimensional Ni1Ce1O3 solid solution catalyst to the carbon dioxide methanation reaction. Specifically, CO2 and H2 are introduced into the reactor, and the catalytic activity is tested by heating. The results show that Ni1Ce1O3 has good catalytic performance and selectivity for carbon dioxide methanation.

[0019] This invention discloses the synthesis of a two-dimensional Ni1Ce1O3 solid solution (NiO and CeO2 in a 1:1 ratio) with a two-dimensional fluorite crystal form, used for ultra-low temperature CO2 methanation reaction. The yields of CH4 at 200℃ and 300℃ were 80.4 and 2138 mmol g, respectively. -1 h -1The CH4 selectivity was >99.5%, superior to all reported catalysts. This is because 2D Ni1Ce1O3 enhanced CO2 adsorption, altering the CO2 methanation pathway. Furthermore, the combination of 2D Ni1Ce1O3 with a thermal radiation isolation device showed that the standard solar-driven photothermal CO2 methanation rate was 2901 mmol g / L. -1 h -1 (This is 5 times the highest reported value), and in the dark, the CO2 methanation rate is ~910 mmol g. -1 h -1 Therefore, magnification to 4.8m 2 A large-scale demonstration can continuously drive outdoor CO2 methanation for 5 days and nights, with a total CH4 yield of 898m³. 3 This invention enables the industrial-scale methanation of CO2 using only 10 tons of boiling water, requiring no energy input. The method described in this invention is environmentally friendly, widely applicable, and highly suitable for industrial production and practical applications. Attached Figure Description

[0020] Figure 1 This is a flowchart of the preparation method of the 2D Ni1Ce1O3 catalyst provided by the present invention.

[0021] Figure 2 The image shows the XRD pattern of Ni1Ce1O3 obtained in Example 1, indicating that Ni1Ce1O3 is in the fluorite crystal form.

[0022] Figure 3 This is a morphological characterization (shown as a two-dimensional morphology), elemental distribution map, and structural features of Ni1Ce1O3 obtained in Example 1.

[0023] Figure 4 The images show the XRD and electron microscopy results of Ni / CeO2 obtained in Comparative Example 1.

[0024] Figure 5 The image shows the nitrogen adsorption-desorption isotherm of Ni1Ce1O3 obtained in Example 1.

[0025] Figure 6 This study investigates the carbon dioxide methanation performance and mechanism of 2D Ni1Ce1O3 in Example 1 and Ni / CeO2 in Comparative Example 1.

[0026] Figure 7 It is the carbon dioxide conversion rate of Ni1Ce1O3 thermocatalytic carbon dioxide methanation obtained in Example 1.

[0027] Figure 8 After thermocatalytic carbon dioxide methanation, 2D Ni1Ce1O3 is produced at Ni 2p (corresponding to...) Figure 8 (a)), Ce 3d (corresponding to) Figure 8(b)) and O1s (corresponding to Figure 8 XPS spectra in (c)).

[0028] Figure 9 This is a graph showing the CH4 generation rate and temperature variation under light irradiation in a novel photothermal system with a two-dimensional Ni1Ce1O3 catalyst.

[0029] Figure 10 This is a graph showing the CO2 conversion rate of a novel solar thermal system as a function of light intensity under outdoor sunlight. Detailed Implementation

[0030] The present invention will be further described in detail below with reference to specific embodiments.

[0031] Example 1, Preparation method of two-dimensional Ni1Ce1O3 solid solution catalyst (in conjunction with...) Figure 1 ).

[0032] (1) Add 5g citric acid, 2g Ce(NO3)3·6H2O and 1.339g Ni(NO3)2·6H2O to a beaker, add 2.5mL nitric acid, and finally titrate with ammonia water until the solution pH=6, and stir well.

[0033] (2) Place the mixed solution from step a on a heated stirring table and stir at 80°C for 8 hours until the magnetic stir bar stops rotating, thus forming a gel.

[0034] (3) Place the gel obtained in step b into a 100°C oven and dry for 24 hours to remove additional moisture.

[0035] (4) The dried gel obtained in step c is placed in a tube furnace filled with Ar at 400°C. The sample is immediately heated from room temperature to 400°C. The rapid heating causes expansion, that is, the gel will explode rapidly after entering the tube furnace. After the explosion, the gel is calcined in the tube furnace for 3 hours to obtain the catalyst precursor.

[0036] (5) After cooling the catalyst precursor obtained in step d to room temperature, place it in a muffle furnace and anneal it by calcining at 450°C (heating rate 10°C / min) for 5 hours in air to obtain a two-dimensional (2D) Ni1Ce1O3 solid solution catalyst.

[0037] To achieve rapid and large-scale preparation of the catalyst, this invention employs an explosive method to synthesize 2D Ni1Ce1O3. For example... Figure 1As shown, in addition to nickel and cerium metal salts, citric acid (C6H8O7), nitric acid (HNO3), and ammonia were added to the solution to form a gel containing the explosive substance NH4NO3. The gel was then placed directly into a high-temperature furnace and detonated for a short time (approximately 1 minute) to obtain pure metal oxides. The X-ray diffraction (XRD) pattern of 2D Ni1Ce1O3 is shown below. Figure 2 As shown, the diffraction peaks reveal a fluorite structure. Therefore, the 2D Ni1Ce1O3 prepared in this invention is a previously unseen fluorite-structured solid solution. NiO and CeO2 exhibit a large lattice mismatch, making it impossible to prepare a solid solution structure with an equal ratio (i.e., a 1:1 ratio of NiO to CeO2) using conventional processes. In this invention, the inventors hypothesize that the ultrafast preparation time of the explosive method hinders the phase separation of NiO and CeO2, thereby forming a novel solid solution structure.

[0038] Electron microscopy and elemental analysis were performed on the 2D Ni1Ce1O3 prepared in this embodiment, and the results are as follows: Figure 3 As shown. Figure 3 (a) is a SEM image. Figure 3 (b) is a TEM image. Figure 3 (c) is the element mapping image corresponding to the three elements O, Ni, and Ce. Figure 3 (d) is a HAADF-STEM image. As can be seen from the SEM and TEM images, the 2D Ni1Ce1O3 catalyst exhibits a two-dimensional nanosheet morphology. Figure 3 (c) is a high-resolution elemental mapping image at the 5nm × 5nm scale. The image shows that O, Ni, and Ce are uniformly dispersed at the atomic scale on the 2D Ni1Ce1O3 catalyst. Meanwhile, from... Figure 3 The HAADF-STEM image of the 2D Ni1Ce1O3 catalyst in (d) confirms uniform atomic contrast, indicating zero segregation of nickel and cerium.

[0039] Comparative Example 1: Synthesis of Ni / CeO2.

[0040] First, 2g of Ce(NO3)3·6H2O and 1.339g of Ni(NO3)2·6H2O were dissolved in 10mL of deionized water to form a homogeneous solution. Second, 1mL of ammonia solution was gradually added dropwise to the solution with continuous stirring to form a precipitate, which was then separated from the solution by centrifugation. Third, the precipitate was annealed by calcination at 450℃ (heating rate 10℃ / min) for 5 hours in a muffle furnace. Fourth, the annealed sample was placed in a tube furnace, and H2 and Ar (volume ratio 1:9) were introduced into the tube furnace. The temperature was increased to 400℃ at a heating rate of 1℃ / min, and then reduced at 400℃ for 6 hours to obtain Ni / CeO2.

[0041] Comparative Example 1 shows the preparation of a Ni / CeO2 catalyst using a co-precipitation method. XRD and electron microscopy analyses were performed on this catalyst, and the results are as follows: Figure 4 As shown. Figure 4 (a) is the XRD pattern. Figure 4 (b) is the SEM image. Figure 4 (c) is a TEM image. Figure 4 (d) is a high-resolution TEM image. Figure 4 (a) It can be seen that there are obvious Ni diffraction peaks in the XRD pattern. Figure 4 (b) The SEM image shows that the catalyst has an irregular blocky morphology. Figure 4 (d) shows the Ni(200) crystal plane with a lattice spacing of 0.176 nm.

[0042] The 2D Ni1Ce1O3 catalyst prepared in Example 1 of this invention was subjected to nitrogen adsorption-desorption tests, and the results are as follows: Figure 5 As shown. According to Figure 5 The results show that the specific surface area of ​​the 2D Ni1Ce1O3 catalyst is 103.25 m². 2 g -1 .

[0043] Application of two-dimensional Ni1Ce1O3 solid solution catalysts in CO2 hydrogenation methanation:

[0044] 1 mg of the 2D Ni1Ce1O3 catalyst prepared in Example 1 was weighed and placed in a quartz tube. Catalytic testing was performed by introducing reaction gases CO2 and H2. The results are as follows: Figures 6-7 As shown in the figure, the CH4 yield of 2D Ni1Ce1O3 reaches 2138 mmol g at 300 °C. -1 h -1 The CO2 conversion efficiency was 87.3%, compared to 8.36 mmol / g for Ni / CeO2 at 300℃ in Comparative Example 1. -1 h -1 It is 255 times higher. In addition to the excellent CH4 formation rate, the CH4 selectivity of 2D Ni1Ce1O3 is above 99.5% in the temperature range of 150℃ to 300℃.

[0045] Table 1 compares the CO2 methanation rates of the 2D Ni1Ce1O3 of this invention with those of the best available catalysts. The CH4 yields of the 2D Ni1Ce1O3 of this invention at 300°C, 250°C, and 200°C are 2138, 1000, and 80.4 mmol g, respectively. -1 h -1 It is at least four times that of the optimal catalyst at the corresponding temperature.

[0046] Table 1. Comparison of CO2 methanation performance of 2D Ni1Ce1O3 with advanced CO2 methanation catalysts

[0047]

[0048] The carbon dioxide methanation performance and mechanism of 2D Ni1Ce1O3 prepared in Example 1 and Ni / CeO2 prepared in Comparative Example 1 were studied, and the results are as follows: Figure 6 As shown. Figure 6 In the figures, (a) shows the rate of thermocatalytic carbon dioxide methanation of methane on 2D Ni1Ce1O3 and Ni / CeO2. (b) shows the selectivity of thermocatalytic carbon dioxide methanation of 2D Ni1Ce1O3, where methane selectivity = CH4 / (CH4+CO), and methane and CO are the rates of carbon dioxide methanation to methane and CO, respectively. (c) shows the stability test of 2D Ni1Ce1O3 at 300℃ for 168 hours of carbon dioxide methanation. (d) shows the atomic structure of 2D Ni1Ce1O3 and Ni / CeO2. (e) shows the energy distribution of the hydrogenation reaction of carbon dioxide on the surfaces of 2D Ni1Ce1O3 and Ni / CeO2, and the atomic structure of the carbon-based intermediate. The y-axis represents the energy level of each stage. Catalyst dosage = 10 mg, carbon dioxide flow rate = 10 mL / min. -1 H2 flow rate = 40 mL / min -1 Pressure = 0.

[0049] The CO2 methanation mechanism on 2D Ni1Ce1O3 was studied using spin-polarized density functional theory (DFT). Ni atoms randomly replaced Ce atoms in CeO2, forming a 2D Ni1Ce1O3 model with a fluorite structure, as shown below. Figure 6 As shown in (d). According to Figure 8 XPS results show that Ni and Ce in 2D Ni1Ce1O3 maintain a stable oxidation state during CO2 methanation. For comparison, CeO2 (Ni / CeO2) loaded with Ni nanoparticles obtained in Comparative Example 1 was constructed (see...). Figure 6 (d)). The energy curve of CO2 methanation and the atomic structure of carbon-based intermediates are as follows: Figure 6As shown in (e), firstly, the CO2 adsorption energies of 2D Ni1Ce1O3 and Ni / CeO2 are 1.07 eV and 0.752 eV, respectively, demonstrating the strong adsorption of CO2 by 2D Ni1Ce1O3. Secondly, the rate-limiting steps for CO2 methanation on both 2D Ni1Ce1O3 and Ni / CeO2 are the hydrogenation of the CO intermediate, with activation energy barriers of 0.915 eV and 1.474 eV, respectively, indicating that CO2 is more readily methanated at the Ni site of 2D Ni1Ce1O3. The Bader charges of Ni in 2D Ni1Ce1O3 and Ni / CeO2 are +1.17 and +0.07|e|, respectively. This makes Ni in 2D Ni1Ce1O3 tend to adsorb electron-rich oxygen ions from CO2, and metallic nickel has a strong interaction with electron-deficient carbon ions in CO2. Figure 6 (e)).

[0050] like Figure 6 As shown in (e), the evolution of the carbon-based intermediate on Ni / CeO2 is *CO2-*COOH-*CO-*CHO-*COH-*CHOH-*CH-*CH2-*CH3-CH4, while the evolution of the carbon-based intermediate on 2D Ni1Ce1O3 is *OCO-*OCOH-*OC-*OCH-*OCH2-*OCH3-*OHCH3-*OH2CH3-*CH3-CH4. Previous studies have shown that CO2 methanation of metallic nickel involves the complete deoxygenation of CO2 and the hydrogenation of carbon atoms. Interestingly, CO2 methanation on 2D Ni1Ce1O3 involves the partial deoxygenation of CO2 and the hydrogenation of CO. Since CO is a highly reactive molecule, the hydrogenation of CO is easier than the hydrogenation of carbon atoms. Therefore, the change in intermediates is the reason for the high CO2 methanation performance of 2DNi1Ce1O3. Furthermore, the CO adsorption energy of 2D Ni1Ce1O3 (2.315 eV) is higher than that of Ni / CeO2 (1.133 eV). Strong CO adsorption can reduce CO production in 2D Ni1Ce1O3 during CO2 methanation and improve CH4 selectivity.

[0051] Weigh 5 mg of the 2D Ni1Ce1O3 catalyst prepared in Example 1 and place it in a quartz tube. Place the quartz tube in a photothermal device and pass in CO2 and H2 reaction gases for catalytic testing. The results are as follows: Figure 9-10 As shown in the figure. It can be seen from the figure that at 0.2kW m -2Under irradiation with solar intensity (0.2 times that of sunlight), the catalyst temperature reached 150℃, and the photothermal CO2 methanation reaction clearly began. With increasing solar intensity to 0.5 times and 1 times that of sunlight, the catalyst temperature rose to 243℃ and 352℃, respectively. Simultaneously, under irradiation with 0.5 times and 1 times that of sunlight, the photothermal CH4 yield surged to 773 mmol g. -1 h -1 and 2901 mmol g -1 h -1 The CH4 selectivity of this system remained above 99% throughout the entire process.

[0052] This invention successfully prepared a two-dimensional solid solution (2D Ni1Ce1O3) of equal amounts of NiO and CeO2, yielding 2138 mmol g at 300 °C. -1 h -1 The CO2 methanation rate was high, with a selectivity of up to 99.5% and a CO2 conversion rate of 87.3%. Theoretical calculations show that the CO2 methanation on 2D Ni1Ce1O3 is achieved by replacing the hydrogenation of carbon atoms with the hydrogenation of CO, resulting in an activation energy barrier of 0.915 eV. This photothermal device, covered with a Cu film of approximately 20 μm thickness and a TiC layer of 14 nm thickness, exhibits approximately 90% solar absorptivity and 5% infrared emissivity. Under 1 mmol / L sunlight irradiation, this photothermal device can heat 2D Ni1Ce1O3 to 352 °C, achieving a yield of 2901 mmol / L. -1 h -1 The CH4 production rate was then stabilized at approximately 910 mmol g for 84 hours without sunlight. -1 h -1 The operating temperature is approximately 340℃. During a five-day outdoor demonstration, the 2DNi1Ce1O3 and photothermal device were scaled up, achieving a CH4 production of 898 cubic meters and 10 tons of boiling water. This work reveals the design principles of a highly efficient low-temperature methanation catalyst and represents a photothermal CO2 methanation method that can operate stably around the clock without the need for heating support. By avoiding the costs of heating equipment and energy inputs, autonomous photothermal CO2 methanation offers significant advantages in converting large quantities of green hydrogen and CO2 into CH4 to facilitate long-distance transportation.

[0053] The references in Table 1 of the specific embodiments of this invention are as follows:

[0054] 1.Zhao,C.et al.Ordered mesoporous carbon-supported mono-dispersed Coand Ru–Co catalysts for low-temperature CO2 methanation.Functional MaterialsLetters 13,2051019,(2020).

[0055] 2.Khan,I.S.et al.An Efficient Metal–Organic Framework-Derived NickelCatalyst for the Light Driven Methanation of CO2.Angew.Chem.-Int.Edit.60,26476-26482,(2021).

[0056] 3.Sakpal,T.&Lefferts,L.Structure-dependent activity of CeO2 supportedRu catalysts for CO2methanation.Journal of Catalysis 367,171-180,(2018).

[0057] 4.Zhang,T.et al.Enhancing the low-temperature CO2 methanation overNi / La-CeO2 catal yst:The effects of surface oxygen vacancy and basic site onthe catalytic performance.App l.Catal.B-Environ.312,121385,(2022).

[0058] 5.Zhu,M.et al.Vacancy engineering of the nickel-based catalysts forenhanced CO2 met hanation.Appl.Catal.B-Environ.282,119561,(2021).

[0059] 6.Quindimil,A.,Bacariza,M.C.,González-Marcos,J.A.,Henriques,C.&González-Vela sco,J.R.Enhancing the CO2 methanation activity ofγ-Al2O3 supportedmono-and bi-metal lic catalysts prepared by glycerol assistedimpregnation.Appl.Catal.B-Environ.296,120322,(2021).

[0060] 7.Ye,R.-P.et al.High-performance of nanostructured Ni / CeO2 catalyston CO2 methanatio n.Appl.Catal.B-Environ.268,118474,(2020).

[0061] 8.Zhou,J.et al.Interfacial compatibility critically controls Ru / TiO2metal-support interacti on modes in CO2 hydrogenation.Nat.Commun.13,327,(2022).

[0062] 9.Ge,H.,Kuwahara,Y.,Kusu,K.,Bian,Z.&Yamashita,H.Ru / H x MoO 3-y withplasmoni c effect for boosting photothermal catalytic CO2methanation.Appl.Catal.B-Environ.317,121734,(2022).

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Claims

1. A two-dimensional Ni1Ce1O3 solid solution catalyst, characterized in that, The two-dimensional Ni1Ce1O3 solid solution catalyst exhibits diffraction peaks with a fluorite structure; the two-dimensional Ni1Ce1O3 solid solution catalyst is synthesized by an explosive method; The preparation method of the two-dimensional Ni1Ce1O3 solid solution catalyst includes the following steps: a. Add citric acid, cerium nitrate and nickel nitrate to a beaker, add nitric acid, and then titrate with ammonia until the solution pH=6; b. Place the solution from step a on a heated stirring table and stir at 80°C to form a gel; c. Place the gel obtained in step b into an oven to dry; d. Place the dried gel into a tube furnace at 400°C. The gel will explode rapidly after entering the tube furnace. Then, calcine the gel in the tube furnace for 3 hours to obtain the catalyst precursor. e. After cooling the catalyst precursor to room temperature, place it in a muffle furnace and calcine it at 450°C for 5 hours to obtain a two-dimensional Ni1Ce1O3 solid solution catalyst.

2. A method for preparing a two-dimensional Ni1Ce1O3 solid solution catalyst, characterized in that, Includes the following steps: a. Add citric acid, cerium nitrate and nickel nitrate to a beaker, add nitric acid, and then titrate with ammonia until the solution pH=6; b. Place the solution from step a on a heated stirring table and stir at 80°C to form a gel; c. Place the gel obtained in step b into an oven to dry; d. Place the dried gel into a tube furnace at 400°C. The gel will explode rapidly after entering the tube furnace. Then, calcine the gel in the tube furnace for 3 hours to obtain the catalyst precursor. e. After cooling the catalyst precursor to room temperature, place it in a muffle furnace and calcine it at 450°C for 5 hours to obtain a two-dimensional Ni1Ce1O3 solid solution catalyst.

3. The method for preparing the two-dimensional Ni1Ce1O3 solid solution catalyst according to claim 2, characterized in that, In step a, the molar ratio of cerium nitrate to nickel nitrate is 1:

1.

4. The method for preparing the two-dimensional Ni1Ce1O3 solid solution catalyst according to claim 2, characterized in that, In step c, the gel obtained in step b is placed in a 100°C oven and dried for 24 hours.

5. The method for preparing the two-dimensional Ni1Ce1O3 solid solution catalyst according to claim 2, characterized in that, In step d, calcination is carried out in an Ar environment in a tube furnace for 3 hours; in step e, calcination is carried out in an air environment in a muffle furnace for 5 hours.

6. The application of the two-dimensional Ni1Ce1O3 solid solution catalyst according to claim 1 or the two-dimensional Ni1Ce1O3 solid solution catalyst prepared according to any one of claims 2 to 5 in the carbon dioxide methanation reaction.

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