Electrode material of carbon nanotube confined one-dimensional ptte atomic chain, preparation method and application thereof

Abstract

The application discloses an electrode material of carbon nanotube limited one-dimensional PtTe atomic chain, a preparation method and application thereof, and the preparation method comprises the following steps: opening a carbon nanotube to obtain an open carbon nanotube; placing a tellurium source precursor in a reaction space communicated with the open carbon nanotube, and performing a gas phase transmission reaction under a negative pressure condition to obtain an intermediate material; and then placing a platinum source precursor in a reaction space communicated with the intermediate material, and performing a gas phase transmission reaction under a negative pressure condition to obtain the electrode material of carbon nanotube limited one-dimensional PtTe atomic chain. By constructing a one-dimensional PtTe atomic chain structure in a carbon nanotube limited channel, stable exposure of an atomic level active site is realized, the electrode material can continuously participate in charge release in a high potential area of a selected working voltage window, and therefore the discharge capacity of the electrode material in the high working potential area is improved.

Description

Technical Field

[0001] This invention belongs to the technical field of nano-carbon materials and electrochemical electrode materials, specifically relating to an electrode material with one-dimensional PtTe atomic chains confined in carbon nanotubes, its preparation method and application. Background Technology

[0002] Electrode materials are key components in electrochemical charge storage systems, and their structural characteristics and electrochemical performance directly affect the system's operating potential range and charge release behavior. Carbon nanotubes, due to their excellent conductivity and structural stability, have been widely studied and applied in the field of electrode materials. However, traditional carbon nanotube electrodes mainly rely on the electric double-layer charge storage mechanism, and their ability to participate in charge exchange is limited in the higher potential region, making it difficult to achieve continuous and reversible charge release near the upper potential limit.

[0003] To improve the charge storage performance of carbon-based electrode materials, existing technologies typically introduce metal compounds or other active components to increase electrochemical reaction sites. However, these active components often exist in particulate or disordered structures, making them prone to aggregation or structural degradation during charge and discharge. This results in insufficient stability and sustained discharge capability of the electrode material in the high-potential region. Furthermore, there is a lack of electrode material design schemes that can stably construct active structures at the atomic scale and continuously participate in charge release in the high-potential region.

[0004] One-dimensional heterogeneous atomic chains, due to their continuous atomic arrangement and fully exposed atomic-level active sites, possess the potential to continuously participate in charge exchange under high operating potentials. However, in existing technologies, such structures are difficult to stably construct and effectively incorporate into electrode materials, and problems such as structural instability and easy aggregation still exist.

[0005] Therefore, there is an urgent need for a new electrode material and its preparation method that can stably construct a one-dimensional heterogeneous atomic chain structure within the confined channels of carbon nanotubes, so as to improve the continuous discharge capability and charge storage performance of the electrode material in the high working potential region. Summary of the Invention

[0006] The purpose of this invention is to provide an electrode material with a one-dimensional PtTe atomic chain confined within a carbon nanotube, its preparation method, and its application. This invention constructs a one-dimensional PtTe atomic chain structure within a confined channel of a carbon nanotube, thereby achieving stable exposure of atomic-level active sites. This electrode material can continuously participate in charge release in the high potential region of a selected working voltage window, thereby improving the discharge capability of the electrode material in the high working potential region.

[0007] To achieve the above objectives, a specific embodiment of the present invention provides the following technical solution:

[0008] A method for preparing an electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes, the method comprising the following steps:

[0009] Open the carbon nanotubes to obtain open carbon nanotubes;

[0010] The tellurium source precursor is placed in a reaction space connected to an open carbon nanotube, and a gas-phase transport reaction is carried out under negative pressure to obtain an intermediate material.

[0011] The platinum source precursor is then placed in a reaction space connected to the intermediate material, and a gas-phase transport reaction is carried out under negative pressure to obtain an electrode material with a one-dimensional PtTe atomic chain confined by carbon nanotubes.

[0012] In one or more embodiments of the present invention, the platinum source precursor is at least one selected from chloroplatinic acid, platinum acetylacetonate, and platinum tetrachloride; and / or,

[0013] The tellurium source precursor is at least one of tellurium powder, dimethyl tellurium, and diethyl tellurium.

[0014] In one or more embodiments of the present invention, the platinum source precursor and the tellurium source precursor are in a molar ratio of platinum atoms to tellurium atoms of 1:0.8-1.5; and / or,

[0015] The mass ratio of the platinum source precursor to carbon nanotubes is 1:4-1:5.

[0016] In one or more embodiments of the present invention, the tellurium source precursor and the open carbon nanotubes undergo a gas-phase transport reaction at 500°C-800°C for 3-5 days; and / or,

[0017] The platinum source precursor and intermediate material undergo a gas-phase transport reaction at 200℃-300℃ for 2h-10h.

[0018] In one or more embodiments of the present invention, the negative pressure in the reaction space is 10. -1 Pa-10 -3 Pa.

[0019] In one or more embodiments of the present invention, carbon nanotubes are taken and subjected to acid treatment, plasma treatment, or heat treatment to obtain open carbon nanotubes; wherein, acid treatment is performed by acid washing with a hydrochloric acid aqueous solution with a concentration of 5M-7M; plasma treatment is performed using oxygen plasma at a power of 90W-110W for 160s-200s; heat treatment is performed at 400℃-600℃ for 0.5h-2h; and / or,

[0020] The inner diameter of the carbon nanotubes is 0.8 nm-3 nm; and / or,

[0021] The carbon nanotubes are single-walled carbon nanotubes or few-walled carbon nanotubes.

[0022] In one or more embodiments of the present invention, after the gas-phase transport reaction is completed, the obtained product is acid-washed with a 0.5 mol / L-2 mol / L hydrochloric acid aqueous solution for 1 h-3 h. After acid washing, it is washed with deionized water until the washing solution is neutral, and then vacuum dried at 70℃-100℃ for 10 h-24 h to obtain an electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains.

[0023] Another specific embodiment of the present invention provides the following technical solution:

[0024] An electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes was prepared by the above-described method.

[0025] Another specific embodiment of the present invention provides the following technical solution:

[0026] Application of an electrode material with one-dimensional PtTe atomic chains confined in carbon nanotubes in electrodes.

[0027] In one or more embodiments of the present invention, the electrode material of the carbon nanotube confined one-dimensional PtTe atomic chain and the binder are mixed in a mass ratio of 8:1-8:3 to obtain a slurry; the slurry is coated on the current collector with a coating mass of 50mg-100mg, and then dried at 100℃-150℃ for 12h-24h to obtain the electrode.

[0028] Compared with existing technologies, the carbon nanotube-confined one-dimensional heterogeneous atomic chain electrode material of this invention achieves continuous and reversible charge storage by constructing continuous one-dimensional PtTe atomic chains within carbon nanotubes. This allows the atomic orbitals of different elements within the chains to couple and form localized energy levels capable of participating in electron transfer at higher operating potentials. The carbon nanotube framework provides a highly efficient conductive network, ensuring rapid electron transport to the active sites, while the confined structure stabilizes the arrangement of the PtTe atomic chains, preventing aggregation or shedding, and ensuring full exposure of the active sites while maintaining structural integrity. In a three-electrode system, cyclic voltammetry and galvanostatic charge-discharge tests demonstrate that this material exhibits a sustained charge release capability in the high-potential region, significantly enhancing charge storage performance. This provides reliable experimental evidence for the study of the relationship between material structure and electrochemical performance, as well as fundamental research on rapid charge storage in the high-potential region. Attached Figure Description

[0029] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments recorded in the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0030] Figure 1 This is a flowchart of a method for preparing an electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in one embodiment of the present invention;

[0031] Figure 2 This is a transmission electron microscope image of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in Embodiment 1 of the present invention;

[0032] Figure 3 This is a selected area elemental distribution diagram of the electrode material with a one-dimensional PtTe atomic chain confined in carbon nanotubes in Embodiment 1 of the present invention;

[0033] Figure 4 The image shows the X-ray photoelectron spectroscopy (XPS) spectrum of the electrode material with one-dimensional PtTe atomic chains confined by carbon nanotubes in Embodiment 1 of the present invention.

[0034] Figure 5 This is a cyclic voltammetry curve of the electrode material with one-dimensional PtTe atomic chains confined by carbon nanotubes in Embodiment 1 of the present invention under different scan rate conditions.

[0035] Figure 6 This is a comparison of the linear relationship between the scan rate and peak current obtained from the cyclic voltammetry test of carbon nanotubes in Example 1 of the present invention and Comparative Example 1, which is a carbon nanotube-confined one-dimensional PtTe atomic chain electrode material and a carbon nanotube cyclic voltammetry test obtained from Comparative Example 1.

[0036] Figure 7 The graph shows the calculated pseudocapacitance of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in Embodiment 1 of the present invention under different scan rate conditions.

[0037] Figure 8 This is a constant current discharge curve of a one-dimensional PtTe atomic chain confined in a carbon nanotube under different current density conditions in Embodiment 1 of the present invention. Detailed Implementation

[0038] To enable those skilled in the art to better understand the technical solutions in this disclosure, the technical solutions in the embodiments of this disclosure are described clearly and completely below. Obviously, the described embodiments are only some embodiments of this disclosure, and not all embodiments. Based on the embodiments in this disclosure, all other embodiments obtained by those skilled in the art without creative effort should fall within the scope of protection of this disclosure.

[0039] One specific embodiment of the present invention provides a method for preparing an electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes, such as... Figure 1 As shown, the specific steps include the following:

[0040] Step 1: Pretreatment and opening of carbon nanotubes.

[0041] Specifically, the carbon nanotubes are single-walled or few-walled carbon nanotubes. The carbon nanotubes undergo end-opening treatment via acid treatment, plasma treatment, or air / inert atmosphere heat treatment. Specifically, acid treatment involves washing with a 5M-7M hydrochloric acid aqueous solution, followed by drying in a 100℃ vacuum oven for 12 hours. Plasma treatment uses oxygen plasma at a power of 90W-110W for 160-200 seconds. Heat treatment is performed in air or an inert atmosphere, with an opening temperature of 400℃-600℃ and an opening time of 0.5-2 hours. This step yields carbon nanotube precursors with an inner diameter distribution of 0.8nm-3nm and open ends, providing a uniform and stable support surface and confined channels for subsequent atomic deposition.

[0042] Step 2, the first step of gas-phase transport reaction.

[0043] Specifically, a platinum source precursor and a tellurium source precursor are provided. The platinum source precursor is selected from at least one of chloroplatinic acid, platinum acetylacetonate, and platinum tetrachloride. The tellurium source precursor is selected from at least one of tellurium powder, dimethyl tellurium, diethyl tellurium, sodium tellurate, and sodium tellurite. The platinum source precursor and the tellurium source precursor exist in the form of a solid inorganic metal salt or a liquid organometallic compound. The molar ratio of platinum atoms to tellurium atoms is 1:0.8-1.5, and the mass ratio of platinum source precursor to carbon nanotubes is 1:4-1:5. The tellurium source precursor is placed in the reaction region connected to the carbon nanotubes, that is, the carbon nanotubes and the tellurium source precursor are placed together in the same region of the reaction vessel.

[0044] The reaction vessel was evacuated to bring the pressure to 10. -1 Pa-10 -3A negative pressure range of Pa is used to remove oxygen and moisture from the reaction environment, creating a controlled reaction environment to prevent oxidation or aggregation of the precursor during the reaction and ensure the directional deposition of the precursor within the carbon nanotubes. The reaction vessel is then sealed and reacted at 500℃-800℃ for 3-5 days to obtain the intermediate material.

[0045] In this step, the tellurium source precursor is introduced into the confined channel of carbon nanotubes in gas phase form to form a continuous one-dimensional Te atomic chain structure.

[0046] Step 3, the second gas-phase transport reaction.

[0047] Specifically, remove the intermediate material from the reaction vessel in step 2, place the platinum source precursor and the intermediate material together in the same area of ​​the reaction vessel, and evacuate the reaction vessel to adjust the pressure to 10. -1 Pa-10 -3 The reaction vessel is then sealed and reacted at 200℃-300℃ for 2-10 hours under negative pressure.

[0048] In this step, the platinum source precursor diffuses into the interior of the carbon nanotube under the combined action of the gas phase environment and the unique confined space of the carbon nanotube. The Pt element undergoes in-situ transformation on the basis of the already formed one-dimensional Te atomic chain and is atomically assembled along the carbon nanotube axis to form a one-dimensional PtTe atomic chain.

[0049] In this step, the total gas-phase reaction time is controlled to be 2-10 hours. By regulating the reaction time, the deposition behavior in the unconfined region is suppressed, thereby improving the construction selectivity of the one-dimensional PtTe atomic chain.

[0050] In steps 2 and 3, by controlling the order of introduction of platinum source precursor and tellurium source precursor, reaction temperature and holding time, the one-dimensional atomic structure is gradually evolved in the confined channel of carbon nanotubes, realizing the orderly construction of heterogeneous atomic chains, while suppressing the deposition behavior in the unconfined region.

[0051] Step 4, post-processing of the product.

[0052] Specifically, after the reaction, the system is cooled to room temperature or below 50°C in the furnace. The obtained product is then removed and acid-washed with a 0.5 mol / L-2 mol / L hydrochloric acid aqueous solution at room temperature for 1-3 hours to remove residual precursors or byproducts on the outer surface of the carbon nanotubes. After acid washing, the product is repeatedly washed with deionized water until the washing solution is neutral. Finally, it is vacuum-dried at 70°C-100°C for 10-24 hours to collect the electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes.

[0053] Another specific embodiment of the present invention provides an electrode material with a one-dimensional PtTe atomic chain confined by carbon nanotubes, which is prepared by the above preparation method.

[0054] Specifically, this invention constructs a one-dimensional PtTe atomic chain structure within confined channels of carbon nanotubes, achieving stable exposure of atomic-level active sites. Through the composite of Pt and Te, a synergistic effect is achieved, enabling the prepared electrode material to exhibit charge storage performance dominated by pseudocapacitance in electrochemical testing, and continuous and reversible charge release capability in the high-potential region of the operating voltage window. If only a Pt source precursor is used, defects such as agglomeration and low specific surface area are easily observed, and the contribution of pseudocapacitance is limited; if only a Te source precursor is used, conductivity is poor, reaction kinetics are slow, and both capacity and rate capability are inferior.

[0055] Another specific embodiment of the present invention provides an application of an electrode material with a carbon nanotube-confined one-dimensional PtTe atomic chain in an electrode.

[0056] Specifically, an electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes and a binder such as polyvinylidene fluoride (PVDF) are mixed at a mass ratio of 8:1 to 8:3 to obtain a slurry. The slurry is coated onto a current collector and dried. The coated sample mass is 50 mg to 100 mg, and the drying temperature and time are 100℃ to 150℃ and 12 h to 24 h, respectively, to prepare the working electrode of the electrochemical charge storage device. This working electrode can be directly used for electrochemical testing, ensuring good conductivity and structural integrity. The working electrode maintains sustainable charge release capability and excellent structural stability in the high potential region.

[0057] The obtained working electrode can be subjected to electrochemical performance testing using a three-electrode system, where the working electrode is PtTe@SWCNT, the counter electrode is Ag / AgCl, and the reference electrode is a graphite rod. Electrochemical tests include cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) to systematically evaluate the electrode's charge storage capacity, discharge reversibility, and sustained charge release performance in different operating potential regions, providing experimental evidence for the structure-property relationship of the material.

[0058] The present invention will be further described in detail below with reference to specific embodiments.

[0059] Example 1

[0060] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is as follows:

[0061] (1) Openings of carbon nanotubes

[0062] 30 mg of single-walled carbon nanotubes (OCSiAl, Tuball 99%) were placed in a muffle furnace and annealed at 500 °C for 0.5 hours in air atmosphere to remove amorphous carbon and residual metal catalyst, while simultaneously opening the ends of the carbon nanotubes. After annealing, the mixture was allowed to cool naturally to room temperature.

[0063] (2) Confined synthesis of Te nanowire framework

[0064] The pretreated carbon nanotubes and 70 mg of accurately weighed sodium tellurate powder were placed together in the same area of ​​a quartz reaction tube to ensure full contact during the reaction. The quartz tube was then evacuated to reduce the internal pressure to 1 × 10⁻⁶. -2 The tube was subjected to a high vacuum state (Pa). Finally, the tube opening was melted at high temperature using a hydrogen flame gun in a vacuum environment to achieve a complete seal of the quartz tube. The reaction was carried out at 600°C for 4 days.

[0065] (3) In-situ construction of PtTe heteroatomic chains within carbon nanotubes

[0066] After completing the first step of gas-phase packing, the sample was removed and placed in a quartz tube along with 150 mg of platinum acetylacetone. The system was then evacuated again to a pressure of 1 × 10⁻⁶. -2 Pa was applied and sealed. Subsequently, the sealed quartz tube was transferred into a tube furnace and reacted at a constant temperature of 200°C for 3 hours. During this process, the platinum source precursor diffused into the interior of the carbon nanotube under the combined action of the gaseous environment and the unique confined space of the carbon nanotube, and underwent in-situ transformation based on the structure formed in the first step, ultimately forming a one-dimensional heterogeneous atomic chain structure arranged along the axis of the carbon nanotube.

[0067] (4) Acid washing, purification and drying

[0068] After the reaction was completed, the furnace was cooled to room temperature. The resulting sample was then removed and added to a 1 mol / L hydrochloric acid aqueous solution. The sample was stirred and washed at room temperature for 2 hours to remove any residual precursors or byproducts on the outer surface of the carbon nanotubes. After washing, the sample was repeatedly washed with deionized water until the washing solution was neutral. The sample was then dried under vacuum at 80°C for 10 hours to obtain a carbon nanotube-confined one-dimensional heterogeneous atomic chain electrode material.

[0069] Example 2

[0070] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is as follows:

[0071] (1) Pretreatment of openings in carbon nanotubes

[0072] 40 mg of single-walled carbon nanotubes (OCSiAl, Tuball 99%) were placed in a muffle furnace and annealed at 550 °C for 2 hours in air atmosphere to remove amorphous carbon and residual metal catalyst, while simultaneously achieving controllable opening at the ends of the carbon nanotubes. After annealing, the nanotubes were allowed to cool naturally to room temperature inside the furnace.

[0073] (2) Confined synthesis of Te nanowires from carbon nanotubes

[0074] The pretreated carbon nanotubes were thoroughly mixed with 80 mg of accurately weighed sodium tellurate powder and placed in the same reaction zone of a quartz reaction tube, ensuring full contact between the two. The quartz tube was then evacuated to a pressure of 5 × 10⁻⁶. -3 Under a high vacuum of Pa, the nozzle was melted and sealed using a hydrogen flame gun in a vacuum environment, and then placed in a tube furnace and reacted at 500°C for 5 days.

[0075] (3) In-situ construction of PtTe heteroatomic chains within carbon nanotubes

[0076] The sample from the first step of the reaction was removed and placed in a quartz tube along with 160 mg of platinum acetylacetone. The tube was then re-evacuated to a pressure of 5 × 10⁻⁶. -3 Pa and seal. Place the sealed quartz tube into a tube furnace and react at 300°C for 2 hours. Under the influence of the gas phase environment and the confined space of the carbon nanotube, the platinum precursor enters the interior of the carbon nanotube and undergoes in-situ transformation on the surface of the existing Te nanowires, ultimately forming a one-dimensional heterogeneous atomic chain structure of PtTe arranged along the axial direction of the carbon nanotube.

[0077] (4) Acid washing, purification and drying

[0078] After the reaction was completed, the furnace was cooled to room temperature. The sample was then removed and added to a 0.6 mol / L hydrochloric acid aqueous solution. The mixture was stirred and washed at room temperature for 2 hours to remove residual precursors and byproducts from the surface. Subsequently, the sample was repeatedly washed with deionized water until the washing solution was neutral. The product was then dried in a vacuum oven at 100°C for 12 hours to obtain a carbon nanotube-confined one-dimensional PtTe heteroatomic chain electrode material.

[0079] Example 3

[0080] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is as follows:

[0081] (1) Controllable opening treatment of carbon nanotubes

[0082] 50 mg of single-walled carbon nanotubes (OCSiAl, Tuball 99%) were placed in a muffle furnace and annealed at 600 °C for 45 minutes in air atmosphere to remove amorphous carbon impurities and catalyst residues from the surface, while simultaneously achieving controllable opening at the ends of the carbon nanotubes. After the annealing process, the nanotubes were allowed to cool naturally to room temperature inside the furnace.

[0083] (2) Confined synthesis of tellurium nanowire framework using carbon nanotubes

[0084] The pretreated carbon nanotubes were uniformly mixed with 100 mg of precisely weighed sodium tellurite powder and then placed into the same reaction zone of a quartz reaction tube. The quartz tube was then evacuated to a pressure of 3 × 10⁻⁶. -3 Under a high vacuum of Pa, the neck of the tube was melt-sealed using a hydrogen flame gun while maintaining the vacuum. The sealed quartz tube was then placed in a single-zone tube furnace and reacted continuously at 620°C for 3 days.

[0085] (3) In-situ synthesis of PtTe heteroatom chains in carbon nanotubes

[0086] The sample obtained after the first step of the reaction was removed and placed together with 200 mg of acetylacetone platinum precursor in a clean quartz tube. The reaction system was then evacuated again to a pressure of 3 × 10⁻⁶. -3 After Pa, the tube was sealed. The sealed quartz tube was then placed in a tube furnace and reacted at a constant temperature of 220°C for 5 hours. Under the synergistic effect of gas-phase transport and the confinement effect of carbon nanotubes, the platinum precursor diffused into the tube and reacted in situ with the already formed selenium nanowire structure, ultimately forming a one-dimensional heterogeneous chain of PtTe atoms aligned along the axial direction of the carbon nanotubes.

[0087] (4) Acid washing, purification and drying treatment

[0088] After the reaction was completed, the sample was cooled to below 50°C in the furnace and then dispersed in a 0.8 mol / L hydrochloric acid solution. It was then stirred in a 35°C constant temperature water bath for 2.5 hours to remove surface impurities. Subsequently, it was washed with deionized water by centrifugation until neutral, and finally dried in a 70°C vacuum drying oven for 15 hours to obtain carbon nanotube-confined PtTe heteroatomic chain functional materials.

[0089] Example 4

[0090] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is as follows:

[0091] (1) Controllable opening treatment of carbon nanotubes

[0092] 50 mg of single-walled carbon nanotubes (OCSiAl, Tuball 99%) were placed in a muffle furnace and annealed at 500 °C for 1 h under a nitrogen atmosphere to remove amorphous carbon impurities and catalyst residues from the surface, while simultaneously achieving controllable opening at the ends of the carbon nanotubes. After the annealing process, the nanotubes were allowed to cool naturally to room temperature inside the furnace.

[0093] (2) Confined synthesis of tellurium nanowire framework using carbon nanotubes

[0094] The pretreated carbon nanotubes were uniformly mixed with 100 mg of precisely weighed sodium tellurite powder and then placed into the same reaction zone of a quartz reaction tube. The quartz tube was then evacuated to a pressure of 1 × 10⁻⁶. -3 Under a high vacuum of Pa, the neck of the tube was melt-sealed using a hydrogen flame gun while maintaining the vacuum. The sealed quartz tube was then placed in a single-zone tube furnace and reacted continuously at 800°C for 4 days.

[0095] (3) In-situ synthesis of PtTe heteroatom chains in carbon nanotubes

[0096] The sample obtained after the first step of the reaction was removed and placed together with 210 mg of acetylacetone platinum precursor in a clean quartz tube. The reaction system was then evacuated again to a pressure of 3 × 10⁻⁶. -3 After Pa, the tube was sealed. The sealed quartz tube was then placed in a tube furnace and reacted at a constant temperature of 300°C for 2 hours. Under the synergistic effect of gas-phase transport and the confinement effect of carbon nanotubes, the platinum precursor diffused into the tube and reacted in situ with the already formed selenium nanowire structure, ultimately forming a one-dimensional heterogeneous chain of PtTe atoms aligned along the axial direction of the carbon nanotubes.

[0097] (4) Acid washing, purification and drying treatment

[0098] After the reaction, the sample was cooled to below 50°C in the furnace and then dispersed in a 2 mol / L hydrochloric acid solution. It was then stirred in a 50°C constant temperature water bath for 2.5 hours to remove surface impurities. Subsequently, it was washed with deionized water by centrifugation until neutral, and finally dried in a 70°C vacuum drying oven for 24 hours to obtain carbon nanotube-confined PtTe heteroatomic chain functional materials.

[0099] Example 5

[0100] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is basically the same as that in Example 1. The difference is that the amount of sodium tellurate is changed, and the mass ratio of carbon nanotubes to sodium tellurate is 3:7.

[0101] Example 6

[0102] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is basically the same as that in Example 1. The difference is that the amount of sodium tellurate is changed, and the mass ratio of carbon nanotubes to sodium tellurate is 1:9.

[0103] Example 7

[0104] The preparation method of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains in this embodiment is basically the same as that in Example 1. The difference is that the amount of sodium tellurate is changed, and the mass ratio of carbon nanotubes to sodium tellurate is 5:5.

[0105] Comparative Example 1

[0106] 30 mg of single-walled carbon nanotubes (OCSiAl, Tuball 99%) were placed in a muffle furnace and annealed at 500 °C for 0.5 hours in air atmosphere to remove amorphous carbon and residual metal catalyst, while simultaneously opening the ends of the carbon nanotubes. After annealing, the mixture was allowed to cool naturally to room temperature.

[0107] The pretreated carbon nanotubes were placed in a quartz reaction tube, and then the quartz tube was evacuated to reduce the internal pressure to 1×10⁻⁶. −2 The tube was subjected to a high vacuum state (Pa). Finally, the tube opening was melted at high temperature using a hydrogen flame gun in a vacuum environment to achieve a complete seal of the quartz tube, and then treated at 600°C for 4 days.

[0108] The processed carbon nanotubes were removed and placed back into a quartz tube. The quartz tube was then subjected to a vacuum treatment again until the pressure reached 1 × 10⁻⁶. -2 Pa, and then sealed. Subsequently, the sealed quartz tube was transferred into a tube furnace and kept at a constant temperature of 200°C for 3 hours.

[0109] After treatment, the sample was cooled to room temperature in the furnace. The sample was then removed and added to a 1 mol / L hydrochloric acid aqueous solution. The solution was stirred and washed for 2 hours at room temperature. After washing, the sample was repeatedly washed with deionized water until the washing solution was neutral. The sample was then dried under vacuum at 80°C for 10 hours to obtain carbon nanotubes.

[0110] Samples from Example 1 and Comparative Example 1 were taken respectively, and mixed with polyvinylidene fluoride (PVDF) at a mass ratio of 8:2 to obtain a slurry. The slurry was coated onto a 2cm×2cm carbon cloth and dried. The mass of the coated sample was 100mg, and the drying temperature and time were 120℃ and 12h, respectively, to prepare the working electrode.

[0111] Electrochemical performance was tested using a three-electrode system under consistent electrolyte conditions, voltage window, and testing conditions. The counter electrode was Ag / AgCl, and the reference electrode was a graphite rod. Electrochemical tests included cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD).

[0112] Depend on Figures 2-4 As can be seen, in Example 1, the one-dimensional PtTe atomic chains were successfully assembled in carbon nanotubes and were well dispersed without obvious aggregation.

[0113] The purpose of Comparative Example 1 was to compare the electrochemical performance differences between the bulk carbon nanotubes and those with embedded active species. Carbon nanotubes from the same source and pretreatment method as in Example 1 were selected as the comparative material. Under conditions where no metal or non-metal gaseous precursors were introduced, heat treatment was performed in a vacuum environment and temperature program completely consistent with Example 1, ensuring that the internal channels of the carbon nanotubes remained empty. Figure 6 It can be seen that the electrode of Comparative Example 1, which is composed of only carbon nanotubes, mainly exhibits double-layer capacitance behavior and no obvious reversible pseudocapacitance characteristics were observed. Its specific capacitance and discharge persistence in the high potential region are lower than those of the carbon nanotube electrode with embedded heteroatoms.

[0114] In addition, combined Figure 5 , Figures 7-8 It can be seen that the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains prepared in this invention has a continuous one-dimensional atomic arrangement. Its atomic-level structural units are fully exposed in the carbon nanotube confinement environment, and can undergo a continuous and reversible surface-controlled charge exchange process in the high potential region. As a result, the electrode material still exhibits a long discharge behavior in the high potential region of its working voltage window, and shows charge storage performance dominated by pseudocapacitance in electrochemical tests, and has a continuous charge release capability in the high potential region.

[0115] It will be apparent to those skilled in the art that this disclosure is not limited to the details of the exemplary embodiments described above, and that this disclosure can be implemented in other specific forms without departing from the spirit or essential characteristics of this disclosure. Therefore, the embodiments should be considered in all respects as exemplary and non-limiting, and the scope of this disclosure is defined by the appended claims rather than the foregoing description. Thus, it is intended that all variations falling within the meaning and scope of equivalents of the claims be included within this disclosure.

[0116] Furthermore, it should be understood that although this specification describes embodiments, not every embodiment contains only one independent technical solution. This narrative style is merely for clarity. Those skilled in the art should consider the specification as a whole, and the technical solutions in each embodiment can also be appropriately combined to form other embodiments that can be understood by those skilled in the art.

Claims

1. A method for preparing an electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes, characterized in that, The preparation method includes the following steps: Open the carbon nanotubes to obtain open carbon nanotubes; The tellurium source precursor is placed in a reaction space connected to an open carbon nanotube, and a gas-phase transport reaction is carried out under negative pressure to obtain an intermediate material. The platinum source precursor is then placed in a reaction space connected to the intermediate material, and a gas-phase transport reaction is carried out under negative pressure to obtain an electrode material with a one-dimensional PtTe atomic chain confined by carbon nanotubes.

2. The method for preparing the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains according to claim 1, characterized in that, The platinum source precursor is at least one of chloroplatinic acid, platinum acetylacetonate, and platinum tetrachloride; and / or... The tellurium source precursor is at least one of tellurium powder, dimethyl tellurium, and diethyl tellurium.

3. The method for preparing the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains according to claim 1, characterized in that, The platinum source precursor and tellurium source precursor have a molar ratio of platinum atoms to tellurium atoms of 1:0.8-1.5; and / or, The mass ratio of the platinum source precursor to carbon nanotubes is 1:4-1:

5.

4. The method for preparing the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains according to claim 1, characterized in that, The tellurium source precursor and open carbon nanotubes undergo a gas-phase transport reaction at 500℃-800℃ for 3-5 days; and / or, The platinum source precursor and intermediate material undergo a gas-phase transport reaction at 200℃-300℃ for 2h-10h.

5. The method for preparing the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains according to claim 1, characterized in that, The negative pressure within the reaction space is 10. -1 Pa-10 -3 Pa.

6. The method for preparing the electrode material with one-dimensional PtTe atomic chains confined by carbon nanotubes according to claim 1, characterized in that, Carbon nanotubes are obtained by acid treatment, plasma treatment, or heat treatment; wherein, acid treatment involves acid washing with a 5M-7M hydrochloric acid aqueous solution; plasma treatment involves using oxygen plasma at a power of 90W-110W for 160s-200s; heat treatment involves treating at 400℃-600℃ for 0.5h-2h; and / or, The inner diameter of the carbon nanotubes is 0.8 nm-3 nm; and / or, The carbon nanotubes are single-walled carbon nanotubes or few-walled carbon nanotubes.

7. The method for preparing the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains according to claim 1, characterized in that, After the gas-phase transport reaction is completed, the obtained product is acid-washed with 0.5 mol / L-2 mol / L hydrochloric acid aqueous solution for 1 h-3 h. After acid washing, it is washed with deionized water until the washing solution is neutral. Then, it is vacuum dried at 70℃-100℃ for 10 h-24 h to obtain an electrode material with carbon nanotube confined one-dimensional PtTe atomic chains.

8. An electrode material with one-dimensional PtTe atomic chains confined within carbon nanotubes, characterized in that, It is prepared by the preparation method according to any one of claims 1-7.

9. The application of the electrode material with carbon nanotube-confined one-dimensional PtTe atomic chains as described in claim 8 in an electrode.

10. The application according to claim 9, characterized in that, The electrode material with one-dimensional PtTe atomic chains confined by carbon nanotubes and the binder are mixed at a mass ratio of 8:1-8:3 to obtain a slurry; the slurry is coated on the current collector with a coating mass of 50mg-100mg, and then dried at 100℃-150℃ for 12h-24h to obtain the electrode.

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