Copper monatomic catalyst for removing organic pollutants in direct oxidation transfer process as well as preparation method and application of copper monatomic catalyst

By preparing the Cu-N4 coordination structure with pyrrole nitrogen-rich graphite-phase carbon nitride as the support, the problems of low efficiency of traditional H2O2 activation technology and insufficient stability of heterogeneous catalysts are solved, and the effect of efficient and selective removal of organic pollutants is achieved.

CN120550841APending Publication Date: 2025-08-29NANCHANG HANGKONG UNIVERSITY +2
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Patent Information

Application Number
CN202510547903.X
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-04-28
Publication Date
2025-08-29

AI Technical Summary

Technical Problem

In the prior art, traditional H2O2 activation technology has low efficiency, non-selective free radical paths and is susceptible to complex ions of water bodies, resulting in insufficient oxidant utilization and intermediate toxic by-product generation, while heterogeneous catalysts have problems of metal leaching and insufficient stability.

Method used

The copper single-atom catalyst is used to prepare a Cu-N4 coordinated structure of Cu-N4 through supramolecular self-assembly and pyrolytic, using pyrrole nitrogen-rich graphite phase carbon nitride as a support, and activate H2O2 to remove organic pollutants in the direct oxidation transfer process to avoid free radical pathways.

Benefits of technology

It achieves efficient and selective removal of organic pollutants. The copper single-atom catalyst exhibits strong anti-interference ability and efficient pollutant removal performance under low H2O2 dosage, avoiding the ineffective consumption of free radicals and the generation of intermediate toxic by-products.

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Abstract

The invention discloses a copper monatomic catalyst for removing organic pollutants in a direct oxidation transfer process (DOTP) as well as a preparation method and application of the copper monatomic catalyst. The monatomic catalyst comprises a graphite phase carbon nitride carrier rich in pyrrole nitrogen and copper monatomic loaded on the carrier, the carrier is graphite phase carbon nitride rich in pyrrole nitrogen; the single atom is a Cu single atom and is combined on the carrier in a stable Cu-N4 coordination structure (the mass fraction of copper is 2-12%). Compared with a traditional free radical path, the method has the advantages that the graphite phase carbon nitride rich in pyrrole nitrogen is used as a carrier, copper single atoms are uniformly dispersed, hydrogen peroxide is activated to remove pollutants through DOTP, and the DOTP avoids invalid consumption of free radicals such as. OH and the like and generation of toxic byproducts; therefore, the copper monatomic catalyst provided by the invention can efficiently and selectively remove organic pollutants at a low H2O2 addition amount, and has strong anti-interference capability on complex water quality.
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Description

Technical Field

[0001] The present invention relates to the field of single-atom catalysts for removing refractory organic pollutants, and in particular to a copper single-atom catalyst for removing organic pollutants through a direct oxidation transfer process, and a preparation method and application thereof. Background Art

[0002] Hydrogen peroxide (H2O2), a green oxidant, has attracted considerable attention in the treatment of refractory organic pollutants due to its unique nature as a water-only reaction product and its lack of secondary pollution. Traditional H2O2 activation techniques (such as the Fenton reaction) rely on free radical pathways (e.g., ·OH) to degrade pollutants. However, these free radical chain reactions require the addition of excessive amounts of H2O2 and are easily quenched by complex ions and dissolved organic matter in the water, resulting in oxidant utilization rates of less than 30%. Furthermore, the non-selective attack of ·OH can easily trigger partial mineralization of pollutants, generating more toxic intermediates (e.g., halogenated quinones and polycyclic aromatic hydrocarbons), exacerbating environmental risks. Traditional homogeneous Fenton systems are limited by a narrow pH range and the accumulation of iron sludge byproducts, making them difficult to adapt to complex water conditions. However, while heterogeneous catalysts have improved pH adaptability (3-9) and recyclability through immobilization, they are still limited by leaching of metal active sites (>1.5 mg / L), low H2O2 activation efficiency (utilization <30%), and insufficient long-term stability. Single-atom catalysts (SACs), with their atomically dispersed active sites and tunable coordination microenvironment, offer a new avenue for breaking through the bottlenecks of traditional catalytic systems. Existing technologies, while doping and modifying SACs improve the efficiency of H2O2 activation, still rely heavily on free radical pathways for pollutant degradation. Therefore, developing a novel single-atom catalyst system that combines efficient H2O2 activation with high selectivity and robust anti-interference capabilities is crucial for advancing green water treatment technologies. Summary of the Invention

[0003] The purpose of the present invention is to solve the technical problems existing in the prior art and to provide a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process, as well as a preparation method and application thereof.

[0004] To achieve the above objectives, the present invention provides a technical solution: a method for preparing a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process, wherein the method comprises the following steps:

[0005] Step 1: Melamine, cyanuric acid, guanine and copper acetylacetonate are added to an agate ball mill and ball milled in a planetary ball mill to obtain a precursor through supramolecular self-assembly;

[0006] Step 2: Pyrolyze the precursor obtained in step 1 under a protective atmosphere to obtain a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process.

[0007] Preferably, in step 1, the sum of the amount of melamine and the amount of guanine in the mixture is equal to the amount of cyanuric acid.

[0008] Preferably, the ball milling speed in the planetary ball mill in step 1 is 200-500 rpm, and the ball milling time is 2-5 h.

[0009] Preferably, in step 2, the precursor is pyrolyzed under a protective atmosphere at a temperature of 500-600° C. and a pyrolysis time of 2-6 h.

[0010] Preferably, the carrier of the copper single-atom catalyst for removing organic pollutants in the direct oxidation transfer process obtained in step 2 is pyrrole-nitrogen-rich graphitic carbon nitride, and the copper single atoms are bound to the carrier in a Cu-N4 coordination structure; the copper single atoms account for 2%-12% of the mass fraction of the copper single-atom catalyst.

[0011] The present invention also provides a copper single-atom catalyst prepared by the above-mentioned method for preparing a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process. The copper single-atom catalyst uses pyrrolic nitrogen-rich graphite phase carbon nitride as a carrier; the copper single atoms are bound to the pyrrolic nitrogen-rich graphite phase carbon nitride carrier in a Cu-N4 coordination structure; the molar ratio of guanine, cyanuric acid and melamine is: 0.04-0.5:0.5-1.0:1; and the mass fraction of the copper single atoms in the copper single-atom catalyst is 2%-12%.

[0012] Preferably, the molar ratio of guanine, cyanuric acid and melamine is 0.04-0.4:0.6-1.0:1.

[0013] The present invention also discloses an application of a copper single-atom catalyst for removing organic pollutants through a direct oxidation transfer process in the catalytic removal of organic pollutants. The copper single-atom catalyst, hydrogen peroxide, and the organic pollutants to be treated are mixed, and H2O2 is activated to remove the pollutants through a DOTP non-radical pathway to remove the organic pollutants. The reaction mechanism of the direct oxidation transfer process for removing organic pollutants avoids the ineffective consumption of H2O2 by free radicals such as ·OH and the generation of intermediate toxic byproducts.

[0014] Beneficial effects of the present invention:

[0015] 1. The present invention discloses a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process and a preparation method thereof, which can successfully prepare a copper single-atom catalyst. The preparation method is simple to operate, has a wide source of raw materials, low production cost, and controllable copper atom content.

[0016] 2. The copper single-atom catalyst prepared by the preparation method of the present invention uses pyrrole nitrogen-rich graphitic carbon nitride as a carrier, wherein the pyrrole nitrogen-rich graphitic carbon nitride has abundant nitrogen atoms, so that the copper atoms are evenly dispersed, thereby making the single-atom catalyst provided by the present invention have strong robustness in activating hydrogen peroxide to remove pollutants.

[0017] 3. The single-atom catalyst provided by the present invention has high efficiency when used to activate hydrogen peroxide to remove organic pollutants, requires a small amount of oxidant, removes pollutants through a direct oxidation transfer process, and has strong anti-interference ability. BRIEF DESCRIPTION OF THE DRAWINGS

[0018] The drawings described herein are used to provide further understanding of the present invention and constitute a part of the present invention. The exemplary embodiments of the present invention and their descriptions are used to explain the present invention and do not constitute improper limitations on the present invention.

[0019] Figure 1 X-ray diffraction (XRD) patterns of Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3;

[0020] Figure 2 The following are Fourier transform infrared spectra (FT-IR) of Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3;

[0021] Figure 3 X-ray photoelectron spectroscopy (XPS) graphs of Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3;

[0022] Figure 4 Transmission electron microscopy (TEM) images of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1;

[0023] Figure 5 Element distribution diagram of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1;

[0024] Figure 6 spherical aberration corrected high-angle annular dark field scanning transmission electron microscopy (AC-HAADF-STEM) images of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1;

[0025] Figure 7 X-ray absorption near-edge structure (XANES) images of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1;

[0026] Figure 8The extended X-ray absorption fine structure (EXAFS) images of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1 are shown;

[0027] Figure 9 This is the rate diagram of removing guaiacol (2-MeOP) by activating H2O2 with Cu / CN-G obtained in Example 1;

[0028] Figure 10 5,5-Dimethyl-1-pyrroline-N-oxide (DMPO) was used as ·OH and ·O2 - As a probe, 2,2,6,6-tetramethylpiperidine (TEMP) 1 O2 probe, EPR graph of the activation solution obtained by activating H2O2 with Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1;

[0029] Figure 11 This is a comparison chart of the thermogravimetric analysis (TGA) of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1 before and after the activation of H2O2 reaction;

[0030] Figure 12 The COD remaining on the catalyst after the Cu / CN-G obtained in Example 1 activated H2O2 to remove 2-MeOP was washed with different solvents; DETAILED DESCRIPTION

[0031] This section will describe in detail the specific embodiments of the present invention. The preferred embodiments of the present invention are shown in the accompanying drawings. The purpose of the accompanying drawings is to supplement the description of the text part of the specification with graphics, so that people can intuitively and vividly understand each technical feature and the overall technical solution of the present invention, but it should not be understood as a limitation on the scope of protection of the present invention.

[0032] In the description of the present invention, it should be understood that descriptions involving orientations, such as up, down, front, back, left, right, etc., indicating orientations or positional relationships, are based on the orientations or positional relationships shown in the accompanying drawings. They are only for the convenience of describing the present invention and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, be constructed and operated in a specific orientation. Therefore, they cannot be understood as limitations on the present invention.

[0033] In the description of the present invention, "several" means one or more, "many" means more than two, "greater than," "less than," and "exceed" are understood to exclude the number itself, while "above," "below," and "within" are understood to include the number itself. The use of "first" and "second" in the description is solely for the purpose of distinguishing technical features and should not be construed as indicating or implying relative importance, implicitly specifying the number of the indicated technical features, or implicitly specifying the order of the indicated technical features.

[0034] In the description of the present invention, unless otherwise clearly defined, terms such as setting, installing, and connecting should be understood in a broad sense, and technicians in the relevant technical field can reasonably determine the specific meanings of the above terms in the present invention based on the specific content of the technical solution.

[0035] Reference Figures 1-12 A preferred embodiment of the present invention provides a method for preparing a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process, the method comprising the following steps:

[0036] Step 1: Melamine, cyanuric acid, guanine and copper acetylacetonate are added to an agate ball mill and ball milled in a planetary ball mill to obtain a precursor through supramolecular self-assembly;

[0037] Step 2: Pyrolyze the precursor obtained in step 1 under a protective atmosphere to obtain a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process.

[0038] Furthermore, in step 1, the sum of the amount of melamine and the amount of guanine in the mixture is equal to the amount of cyanuric acid.

[0039] Furthermore, in step 1, the ball milling speed in the planetary ball mill is 200-500 rpm, and the ball milling time is 2-5 h.

[0040] Furthermore, in step 2, the precursor is pyrolyzed under a protective atmosphere at a temperature of 500-600° C. and a pyrolysis time of 2-6 h.

[0041] Furthermore, the carrier of the copper single-atom catalyst for removing organic pollutants in the direct oxidation transfer process obtained in step 2 is pyrrolic nitrogen-rich graphitic carbon nitride, and the copper single atoms are bound to the carrier in a Cu-N4 coordination structure; the copper single atoms account for 2%-12% of the mass fraction of the copper single-atom catalyst.

[0042] The present invention also provides a copper single-atom catalyst prepared by the above-mentioned method for preparing a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process. The copper single-atom catalyst uses pyrrolic nitrogen-rich graphite phase carbon nitride as a carrier; the copper single atoms are bound to the pyrrolic nitrogen-rich graphite phase carbon nitride carrier in a Cu-N4 coordination structure; the molar ratio of guanine, cyanuric acid and melamine is: 0.04-0.5:0.5-1.0:1; and the mass fraction of the copper single atoms in the copper single-atom catalyst is 2%-12%.

[0043] Furthermore, the molar ratio of guanine, cyanuric acid and melamine is 0.04-0.4:0.6-1.0:1.

[0044] The present invention also discloses the use of the above-mentioned copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process (DOTP) in the catalytic removal of organic pollutants. The copper single-atom catalyst, hydrogen peroxide and the organic pollutants to be treated are mixed, and H2O2 is activated to remove the pollutants via a DOTP non-radical pathway to remove the organic pollutants. The reaction mechanism of the direct oxidation transfer process for removing organic pollutants avoids the ineffective consumption of H2O2 by free radicals such as ·OH and the generation of intermediate toxic byproducts.

[0045] Example 1

[0046] (1) Weigh 1.0 g of cyanuric acid, 0.7 g of melamine, 0.3 g of guanine, and 0.1 g of copper acetylacetonate in an agate ball mill. Add a certain amount of ball milling beads to the ball mill and add 4 mL of ethanol as solvent. Mill the mixture at 400 rpm for 4 h.

[0047] (2) After ball milling, the precursor was dried at 60°C for 24 h to obtain the precursor;

[0048] (3) The precursor was placed in a tube furnace, heated to 600°C at a rate of 5°C / min under an argon atmosphere and kept at this temperature for 4 h to obtain a copper single-atom catalyst, which was recorded as Cu / CN-G. The copper atom content was determined to be 5.0% by ICP-MS.

[0049] Comparative Example 1

[0050] (1) Weigh 1.0 g of cyanuric acid, 1.0 g of melamine, and 0.1 g of copper acetylacetonate into an agate ball mill. Add a certain amount of ball milling beads to the ball mill and add 4 mL of ethanol as solvent. Mill the mixture at 400 rpm for 4 h.

[0051] (2) After ball milling, the precursor was dried at 60°C for 24 h to obtain the precursor;

[0052] (3) The precursor was placed in a tube furnace, heated to 600°C at 5°C / min under an argon atmosphere and kept warm for 4 h to obtain a copper single-atom catalyst denoted as Cu / CN. The copper atom content was determined to be 5.2% by ICP-MS.

[0053] Comparative Example 2

[0054] (1) Weigh 1.0 g of cyanuric acid, 0.7 g of melamine, and 0.3 g of guanine into an agate ball mill. Add a certain amount of ball milling beads to the ball mill and add 4 mL of ethanol as solvent. Mill the mixture at 400 rpm for 4 h.

[0055] (2) After ball milling, the precursor was dried at 60°C for 24 h to obtain the precursor;

[0056] (3) The precursor was placed in a tube furnace, heated to 600 °C at 5 °C / min under an argon atmosphere and kept at this temperature for 4 h to obtain a CN-G catalyst.

[0057] Comparative Example 3

[0058] (1) Weigh 1.0 g of cyanuric acid and 1.0 g of melamine into an agate ball mill. Add a certain amount of ball milling beads to the ball mill and add 4 mL of ethanol as solvent. Mill at a speed of 400 rpm for 4 h.

[0059] (2) After ball milling, the precursor was dried at 60°C for 24 h to obtain the precursor;

[0060] (3) The precursor was placed in a tube furnace, heated to 600 °C at 5 °C / min under an argon atmosphere and kept at this temperature for 4 h to obtain a CN catalyst.

[0061] Figure 1 and Figure 2 The XRD patterns and FT-IR patterns of Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3 are shown respectively. Figure 1 It can be seen that the Cu / CN-G catalyst prepared in Example 1 has diffraction peaks at 13.1° and 27.8°, which correspond to the (100) and (002) crystal plane diffraction peaks of graphitic carbon nitride, respectively. No diffraction peaks of copper and its compounds appear;

[0062] from Figure 2 See, 807cm -1 The peaks corresponding to the stretching vibration of the heptazine ring and 1700-1200 cm -1 Characteristic absorption peaks corresponding to the CN heterocyclic stretching vibration and aromatic stretching vibration modes appeared. Figure 1 and 2 As shown, the characteristic peaks of Cu / CN-G obtained in Example 1 are similar to those of CN-G obtained in Comparative Example 2, while the Cu / CN obtained in Comparative Example 1 is similar to the CN obtained in Comparative Example 3. The above results indicate that the support of Cu / CN-G is CN-G, and the support of Cu / CN is CN.

[0063] Figure 3 The N1s XPS spectra of Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3 are shown. As can be seen from the figure, the content of pyrrole nitrogen in Cu / CN-G obtained in Example 1 and CN-G obtained in Comparative Example 2 is significantly increased compared to Cu / CN obtained in Comparative Example 1 and CN obtained in Comparative Example 3. In addition, the position of pyrrole nitrogen also shifts significantly, indicating that the carrier bound to the single atom may have undergone certain changes.

[0064] Figure 4 and Figure 5 TEM images and elemental distribution maps of the Cu / CN-G obtained in Example 1 and the Cu / CN obtained in Comparative Example 1, respectively. (a) Cu / CN-G, b Cu / CN. As can be seen from the figures, no metallic copper clusters or nanoparticles are observed, and all elements are uniformly dispersed.

[0065] Figure 6 AC-HAADF-STEM images of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1, where a is Cu / CN-G and b is Cu / CN. It can be seen that Cu is evenly distributed on CN-G and CN, respectively.

[0066] Figure 7 The XANES of Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1 are shown. As shown in the figure, the near edge of Cu in Cu / CN-G and Cu / CN is located between the Cu2O and CuO benchmarks, indicating that the valence state of Cu is between +1 and +2. In order to accurately obtain the coordination environment of Cu atoms, the EXAFS of Cu / CN-G and Cu / CN were fitted and analyzed ( Figure 8 ), the average coordination numbers of Cu / CN-G and Cu / CN were 4 and 3, respectively, confirming that the coordination structures of Cu / CN-G and Cu / CN were Cu-N4 and Cu-N3, respectively.

[0067] Figure 9 This is a diagram showing the effects of H2O2 activation on 2-MeOP removal by Cu / CN-G obtained in Example 1, Cu / CN obtained in Comparative Example 1, CN-G obtained in Comparative Example 2, and CN obtained in Comparative Example 3 (reaction conditions: 50 mL, 0.3 g / L catalyst, [H2O2]:[2-MeOP]=5:1). As shown in the figure, Cu / CN-G can quickly remove 2-MeOP at a removal rate 7 times that of Cu / CN, indicating that Cu / CN-G is highly efficient in removing organic pollutants at a low H2O2 dosage.

[0068] 5,5-Dimethyl-1-pyrroline-N-oxide (DMPO) was used as ·OH and ·O2 - As a probe, 2,2,6,6-tetramethylpiperidine (TEMP) 1 The activation solution obtained by activating H2O2 with Cu / CN-G obtained in Example 1 and Cu / CN obtained in Comparative Example 1 was subjected to EPR test. The results are as follows: Figure 10 As shown. The activation solution obtained by Cu / CN activation of H2O2 detected ·OH and ·O2 - The characteristic peaks of ·OH and ·O2 are shown in Figure 2. -However, no ·OH and ·O2 were detected in the activation solution obtained by Cu / CN-G activation of H2O2. - This also indicates that there are no free radicals in H2O2 activated by Cu / CN-G. 2,2,6,6-Tetramethylpiperidine (TEMP) was used as 1 When the probe of O2 was used, no detection was found in the activation solution obtained by activating H2O2 with Cu / CN-G obtained in Example 1 and the activation solution obtained by activating H2O2 with Cu / CN obtained in Comparative Example 1. 1 O2 characteristic peaks indicate that there is no 1 The above results show that Cu / CN activates H2O2 to produce ·OH and ·O2 - , while there are no free radicals in the activation of H2O2 by Cu / CN.

[0069] The TG curves of the Cu / CN-G catalyst obtained in Example 1 and the Cu / CN catalyst obtained in Comparative Example 1 before and after the reaction were analyzed. Figure 11 As shown in the figure, the mass loss of the Cu / CN-G catalyst after the reaction was as high as 5.3%, while the mass of Cu / CN was almost unchanged. These results indicate that in the Cu / CN-G activated H2O2 system, most of the 2-MeOP in the aqueous solution was transferred and accumulated on the Cu / CN-G catalyst surface during the oxidation process, removing the pollutant through a direct oxidation transfer process.

[0070] Figure 12 The Cu / CN-G obtained in Example 1 after the reaction was eluted with different solvents. Figure 12 As shown, water or acid cannot remove contaminants accumulated on the Cu / CN-G surface, while ethanol and toluene can effectively elute the catalyst. Ethanol can remove products of 2-MeOP in the aqueous phase that accumulate on the catalyst surface in the form of C-C coupling, while toluene can remove products that accumulate on the catalyst surface in the form of CO polymerization. This directly demonstrates that H2O2 activated by Cu / CN-G removes contaminants via a direct oxidative transfer process, a non-radical pathway.

[0071] The advantages of the Cu / CN-G catalyst of the present invention are: 1. Cu atoms are uniformly distributed on the support; 2. At low H₂O₂ dosages, Cu / CN-G efficiently removes pollutants via a direct oxidative transfer process, a non-radical pathway; 3. It exhibits high pollutant removal efficiency, strong anti-interference capabilities, and excellent practical applicability. In particular, the Cu / CN-G catalyst prepared in Example 1 exhibits exceptional removal performance at low H₂O₂ dosages. This work demonstrates the green and efficient treatment of organic pollutant wastewater.

[0072] Under the premise that no conflict occurs, those skilled in the art may freely combine and superimpose the above-mentioned additional technical features.

[0073] The above descriptions are only preferred embodiments of the present invention. Any technical solution that achieves the purpose of the present invention by substantially the same means shall fall within the scope of protection of the present invention.

Claims

1. A method for preparing a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process, characterized in that: The method for preparing the copper single-atom catalyst specifically comprises the following steps: Step 1: Melamine, cyanuric acid, guanine and copper acetylacetonate are added to an agate ball mill and ball milled in a planetary ball mill to obtain a precursor through supramolecular self-assembly; Step 2: Pyrolyze the precursor obtained in step 1 under a protective atmosphere to obtain a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process.

2. The method for preparing a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process according to claim 1, characterized in that: The sum of the amount of substance of melamine and the amount of substance of guanine in the mixture in step 1 is equal to the amount of substance of cyanuric acid.

3. The method for preparing a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process according to claim 1, characterized in that: In step 1, the ball milling speed in the planetary ball mill is 200-500 rpm, and the ball milling time is 2-5 h.

4. The method for preparing a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process according to claim 1, characterized in that: In step 2, the precursor is pyrolyzed under a protective atmosphere at a temperature of 500-600° C. and a pyrolysis time of 2-6 hours.

5. The method for preparing a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process according to claim 1, characterized in that: The carrier of the copper single-atom catalyst for removing organic pollutants in the direct oxidation transfer process obtained in step 2 is pyrrole-nitrogen-rich graphitic carbon nitride, and the copper single atoms are bound to the carrier in a Cu-N4 coordination structure; the copper single atoms account for 2%-12% of the mass fraction of the copper single-atom catalyst.

6. The copper single-atom catalyst prepared by the method for preparing a copper single-atom catalyst for removing organic pollutants in a direct oxidation transfer process according to any one of claims 1 to 5, characterized in that: The copper single-atom catalyst uses pyrrolic nitrogen-rich graphitic carbon nitride as a carrier; the copper single atoms are bound to the pyrrolic nitrogen-rich graphitic carbon nitride carrier via a Cu-N4 coordination structure; the molar ratio of guanine, cyanuric acid, and melamine is 0.04-0.5:0.5-1.0:1; and the mass fraction of the copper single atoms in the copper single-atom catalyst is 2%-12%.

7. The copper single-atom catalyst for removing organic pollutants by direct oxidation transfer process according to claim 6, characterized in that: The molar ratio of guanine, cyanuric acid and melamine is 0.04-0.4:0.6-1.0:

1.

8. Use of a copper single-atom catalyst for removing organic pollutants by a direct oxidation transfer process according to any one of claims 6 to 7 in catalytic removal of organic pollutants, characterized in that: Copper single-atom catalyst, hydrogen peroxide and the organic pollutants to be treated are mixed to activate H2O2 to remove pollutants through the DOTP non-radical pathway to remove organic pollutants; the reaction mechanism of removing organic pollutants through the direct oxidation transfer process avoids the ineffective consumption of H2O2 by free radicals such as OH and the generation of intermediate toxic byproducts.