Carbon-based desulfurization and denitrification catalyst capable of being cyclically regenerated at low temperature as well as preparation method and application thereof

Abstract

The invention provides a carbon-based desulfurization and denitrification catalyst capable of being cyclically regenerated at low temperature as well as a preparation method and application thereof. The carbon-based desulfurization and denitrification catalyst capable of being cyclically regenerated at low temperature comprises a carrier and an active component, wherein the active component is highly dispersed on the surface of the carbon material carrier; wherein the carrier is a carbon material with a graded pore structure, and the surface and / or pores of the carbon material are rich in oxygen-containing functional groups with negative charges; the active component is a transition metal oxide, and the transition metal oxide is highly dispersed on the surface and / or in pores of the carbon material carrier; the carbon material carrier and the transition metal oxide active component form an oxygen-containing functional group-carbon-transition metal oxide coordination structure. According to the carbon-based desulfurization and denitrification catalyst capable of being cyclically regenerated at low temperature, decomposition of sulfate formed on the surface of the catalyst can be accelerated, low-temperature regeneration of the carbon-based desulfurization and denitrification catalyst is achieved, and material consumption and energy consumption in the flue gas pollutant removal process are effectively reduced.

Description

Technical Field

[0001] The present invention relates to the field of air pollution control technology, in particular to low-temperature flue gas desulfurization and denitrification technology, and specifically proposes a carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration, and a preparation method and use thereof. Technical Background

[0002] Nitrogen oxides (NO x ) and sulfur dioxide (SO2) emissions have seriously exceeded the carrying limit of the atmospheric environment, seriously affecting the balance and stability of the ecosystem and human health. Activated carbon flue gas multi-pollutant synergistic removal technology has the ability to synergistically remove NO in flue gas at low temperature (120-150℃) x The advantages of no wastewater and no secondary pollutants in the process of SO2 and pollutant treatment are particularly suitable for the treatment of flue gas pollutants in non-power industries. However, since ordinary activated carbon materials lack active sites for desulfurization and denitrification, it is difficult to achieve efficient SO2 catalytic oxidation and NH3-SCR reaction at low temperatures, resulting in low pollutant removal efficiency, large regeneration cycle volume, and high regeneration energy consumption during the operation of traditional activated carbon technology.

[0003] In view of the poor desulfurization and denitration performance of ordinary activated carbon materials, a large amount of research work has focused on introducing various transition metal oxides to prepare carbon-based catalysts. Transition metal oxides can serve as active sites in SO2 catalytic oxidation and NH3-SCR reactions to enhance the desulfurization and denitration performance of carbon-based catalysts. However, as Chinese patents CN201510439617.8 and CN201210306545.6 respectively disclose methods for increasing the sulfur adsorption capacity of carbon-based catalysts by loading a manganese-iron bimetallic oxide active component and increasing the denitration activity of carbon-based catalysts by loading cerium and manganese oxides. However, during the desulfurization and denitration process, the surface of such catalysts is easily sulfated to form metal sulfates, thereby losing activity. Although existing reports show that thermal regeneration at 500-900°C can decompose metal sulfates and restore them to transition metal oxides, high-temperature regeneration has high energy consumption and large carbon material consumption, resulting in the inability to recycle carbon-based catalysts. Therefore, enhancing the low-temperature regeneration performance of carbon-based desulfurization and denitration catalysts is a key problem to be solved by the present invention.

[0004] In addition, no relevant research on carbon-based desulfurization and denitration catalysts that can be recycled at low temperature and their preparation methods and uses has been reported. In order to effectively reduce the regeneration temperature of carbon-based desulfurization and denitration catalysts, it has become a technical problem to be solved to develop and design new and efficient carbon-based desulfurization and denitration catalysts that can be recycled at low temperature. Summary of the invention

[0005] Problem that the invention aims to solve

[0006] In view of the deficiencies in the prior art, the present invention aims to provide a carbon-based desulfurization and denitrification catalyst that can be regenerated at low temperature, so as to reduce the regeneration temperature and energy consumption, improve the regeneration performance and recycling stability of the catalyst, and achieve the coordinated control goals of pollution reduction and carbon reduction.

[0007] Furthermore, the present invention also provides a method for preparing a carbon-based desulfurization and denitrification catalyst that can be recycled and regenerated at low temperature. The preparation method is simple and easy, the raw materials are easy to obtain, and it is suitable for mass production.

[0008] Solutions for solving problems

[0009] [1] A method for preparing a carbon-based desulfurization and denitrification catalyst that can be regenerated at low temperature, wherein the catalyst has a carrier and an active component, and the active component is highly dispersed on the surface of the carbon material carrier; wherein the carrier comprises a carbon material with a multi-level pore structure, and the surface and / or pores of the carbon material are rich in negatively charged oxygen-containing functional groups; and the active component comprises a transition metal oxide; and a transition metal-carbon coordination structure is formed between the active component and the carrier.

[0010] [2] A low-temperature regenerable carbon-based desulfurization and denitrification catalyst according to [1] above, wherein the mass ratio of transition metal oxide to carbon material in the catalyst is 1:9-2:8; and the transition metal oxide comprises a combination of one or more oxides of iron oxide, cobalt oxide, copper oxide, manganese oxide and nickel oxide.

[0011] [3] The low-temperature recyclable carbon-based desulfurization and denitrification catalyst according to claim [1] is characterized in that the carbon material carrier in the catalyst has micropores and / or mesopores, and the BET specific surface area of ​​the carbon material is 750 m 2 / g or above.

[0012] [4] The low-temperature regenerable carbon-based desulfurization and denitrification catalyst according to any one of claims [1] to [3], characterized in that the transition metal oxide is in-situ grown and highly dispersed on the surface and / or pores of the carbon material.

[0013] [5] A method for preparing a low-temperature regenerable carbon-based desulfurization and denitrification catalyst according to any one of [1] to [4] above, comprising the step of highly dispersing the catalyst active components on the surface of the carbon material carrier.

[0014] [6] The preparation method according to the above [5], wherein the preparation method comprises the following steps: using coal-based materials to prepare a carbon material carrier having a multi-level pore structure and rich in negatively charged oxygen-containing functional groups; immersing the carbon material carrier in a solution containing a transition metal oxide precursor to obtain a catalyst precursor; and calcining the catalyst precursor to obtain the carbon-based desulfurization and denitrification catalyst that can be regenerated at low temperature.

[0015] [7] The preparation method according to [6] above, wherein the coal-based material includes but is not limited to a combination of one or more of lignite, bituminous coal, and anthracite; the coal-based material is subjected to a solvent thermal reaction to obtain a carbon material carrier; the temperature of the solvent thermal reaction is 180-260°C; and the solvent reaction time is 3-5 hours.

[0016] [8] The preparation method according to claim 6 or 7 is characterized in that, in the process of preparing a carbon material carrier using a coal-based material, the preparation method also includes a step of making the carbon material carrier have a multi-level pore structure and rich in negatively charged oxygen-containing functional groups; the step of making the carbon material carrier have a multi-level pore structure and rich in negatively charged oxygen-containing functional groups includes placing the coal-based material in an ammonium persulfate solution for a solvothermal reaction; the concentration of the ammonium persulfate solution is 1.5-2.5 mol / L.

[0017] [9] The preparation method according to [6] above, wherein the precursor solution of the transition metal oxide comprises a metal nitrate and / or chloride solution.

[0018]

[10] The preparation method according to [6] above, wherein the calcination temperature is 300-500°C and the calcination time is 4-6 hours.

[0019]

[11] Use of a low-temperature cyclically regenerable carbon-based desulfurization and denitrification catalyst according to any one of claims 1 to 5 in the field of flue gas desulfurization and denitrification.

[0020] Effects of the Invention

[0021] Compared with the existing technology, the carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration of the present invention has at least one of the following technical effects.

[0022] (1) The low-temperature cyclically regenerated carbon-based desulfurization and denitrification catalyst of the present invention can achieve high dispersion of the transition metal oxide active components on the surface and / or in the pores of the carbon material carrier, and has higher desulfurization and denitrification reaction activity than ordinary supported catalytic regeneration materials.

[0023] (2) The carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration of the present invention has an active component and a carrier forming a transition metal-carbon coordination structure, and has higher cyclic desulfurization and denitrification reaction stability than ordinary supported catalytic regeneration materials.

[0024] (3) In the low-temperature regenerative carbon-based desulfurization and denitrification catalyst of the present invention, the oxygen-containing functional groups in the coordination environment of the transition metal oxide can serve as auxiliary sites to accelerate the decomposition of sulfates formed on the catalyst surface, thereby achieving low-temperature regeneration of the carbon-based desulfurization and denitrification catalyst at 350°C.

[0025] (4) The carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration of the present invention has a microporous and / or mesoporous multi-level pore structure and a high specific surface area, which is helpful for gas diffusion, adsorption and desorption processes in the cyclic regeneration reaction.

[0026] (5) The carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration of the present invention can achieve SO2 and NO x Efficient synergistic removal, and recycling through 350℃ low-temperature regeneration, effectively reducing material and energy consumption in the process of flue gas pollutant removal.

[0027] Furthermore, the method for preparing the carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration of the present invention has cheap and readily available raw materials, a simple preparation method, and no by-products in the preparation process. It can exhibit high desulfurization and denitrification performance and excellent regeneration stability, and can be widely used in the field of flue gas desulfurization and denitrification in key industries in my country. BRIEF DESCRIPTION OF THE DRAWINGS

[0028] Figure 1 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MC and FeO x / Denitrification (NO conversion rate) diagram of AC during 5 desulfurization and denitrification cycle regeneration process.

[0029] Figure 2 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MC and FeO x / Desulfurization (sulfur capacity) performance diagram of AC during 5 desulfurization and denitrification cycle regeneration process.

[0030] Figure 3 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MC and FeO x / EDS surface scan elemental analysis image of AC.

[0031] Figure 4 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MC and FeO x / AC SO2 analysis curve during N2 thermal regeneration process after 5 cycles of desulfurization and denitrification reaction. DETAILED DESCRIPTION

[0032] In order to better understand the technical solution of the present invention, the present invention is described below with specific examples. It is necessary to point out that the embodiments are only further explanations of the present invention, and the applicable situations are not limited to the scope of the embodiments, and the present invention is not limited thereto in any way. Those skilled in the art in this field can make some non-essential improvements and adjustments based on the content of the above invention.

[0033] Unless otherwise stated, the units used in this specification are all international standard units, and the numerical values ​​and numerical ranges appearing in the present invention should be understood to include the inevitable systematic errors in industrial production.

[0034] In this specification, the references to "some specific / preferred embodiments", "other specific / preferred embodiments", "embodiments", etc., mean that the specific elements (e.g., features, structures, properties and / or characteristics) described in connection with the embodiments are included in at least one embodiment described herein, and may or may not exist in other embodiments. In addition, it should be understood that the elements may be combined in various embodiments in any suitable manner.

[0035] Embodiment 1:

[0036] An iron oxide (FeO x ) as an active component of a carbon-based desulfurization and denitrification catalyst that can be recycled and regenerated at low temperature, and its preparation method and use.

[0037] (1) Step 1: The anthracite is crushed into particles, and then ground and sieved to 40-60 mesh, and then washed with ultrapure water and fully dried to obtain a coal-based material. The coal-based material and a 2.0 mol / L ammonium persulfate solution are placed in a solvent thermal reactor at a liquid-solid ratio of 1 g:10 mL, and then subjected to a solvent thermal reaction at 200° C. for 3 hours to obtain a carbon material carrier, which is recorded as MDC.

[0038] (2) Step 2: Use the equal volume impregnation method to immerse 10 g of MDC in the ferric nitrate solution, and ultrasonicate for 1 hour, let it stand for 12 hours, and put it in a drying oven at 105°C to dry to constant weight. The content of the active components is calculated according to the corresponding oxides, and the amount of ferric nitrate nonahydrate required is converted, as shown in Table 1:

[0039] Table 1 Preparation of FeO x / MDC required raw materials list

[0040]

[0041] The X represents that the metal oxide may be in multiple valence states simultaneously.

[0042] (3) Step 3: The impregnated catalyst precursor was calcined at 400°C for 4 hours under nitrogen conditions to obtain iron oxide (FeO x ) as the active component of a carbon-based desulfurization and denitrification catalyst that can be recycled at low temperature, denoted as FeO x / MDC.

[0043] (4) Step 4: Desulfurization / denitrification performance test: 1.0 g of FeO x / MDC is the experimental object. The specific test conditions for denitrification performance are: simulated flue gas atmosphere includes 500ppm NO, 500ppm NH3, 10% O2 and balance gas N2, reaction space velocity is 12000m 3 ·h -1 , the temperature is 120℃. Under this condition, the test results show that the denitrification activity reaches 99.49% at . The specific test conditions for desulfurization performance are to simulate the flue gas atmosphere including 1000ppm SO2, 10% O2, 10% H2O and balance gas N2, and the reaction space velocity is 12000m 3 ·h -1 , the temperature is 120°C. Under this condition, the test results show that the sulfur capacity is 61.17 mg / g.

[0044] (5) Step 5: Cyclic regeneration performance test: In this example, 1.0 g of FeO x / MDC was used as the experimental object. After the denitration and desulfurization reactions were completed at 120°C, it was thermally regenerated at 350°C under N2 protection. The test results showed that the catalyst FeO obtained in Example 1 x / MDC has no desulfurization and denitrification performance decline after 5 regenerations. x / MDC's denitrification activity reaches 99.23% at 120°C, and its sulfur capacity is 61.65mg / g. For specific test results, see the attached manual Figure 1 and Figure 2 .

[0045] Embodiment 2:

[0046] A copper oxide (CuO x ) as an active component of a carbon-based desulfurization and denitrification catalyst that can be recycled and regenerated at low temperature, and its preparation method and use.

[0047] (1) In this embodiment, a CuO xPreparation method of carbon-based desulfurization and denitrification catalyst with low temperature cyclic regeneration as active component. This embodiment is basically the same as the first embodiment, except that: without changing the carbon material carrier MDC, another active component (CuO x ) to prepare a carbon-based desulfurization and denitrification catalyst that can be recycled and regenerated at low temperature, that is, replacing the precursor solution with a copper nitrate trihydrate solution during the impregnation process, and converting the required mass of copper nitrate trihydrate. And the CuO x CuO x The mass percentage of / MDC is 10wt.%.

[0048] (2) Desulfurization / denitrification performance test: 1.0 g of CuO in the present invention x / MDC is the experimental object, and the specific test conditions for denitrification performance are: the simulated flue gas atmosphere includes 500ppm NO, 500ppm NH3, 10% O2 and balance gas N2, and the reaction space velocity is 12000m 3 ·h -1 , the temperature is 120℃. Under this condition, the test results show that the denitrification activity reaches 92.10% at . The specific test conditions for desulfurization performance are to simulate the flue gas atmosphere including 1000ppm SO2, 10% O2, 10% H2O and balance gas N2, and the reaction space velocity is 12,000m 3 ·h -1 , the temperature is 120°C. Under this condition, the test results show that the sulfur capacity is 48.17 mg / g.

[0049] (3) Cyclic regeneration performance test: In this example, 1.0 g of CuO x / MDC was used as the experimental object. After the denitration and desulfurization reactions were completed at 120°C, it was thermally regenerated at 350°C under N2 protection. The test results showed that the catalyst CuO obtained in Example 1 x / MDC has no desulfurization and denitrification performance decline after 5 regenerations. x The denitrification activity of / MDC reaches 93.23% at 120℃, and the sulfur capacity is 47.83mg / g.

[0050] Embodiment three:

[0051] A manganese oxide (MnO x Preparation method of carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration using ) as active component

[0052] (1) In this embodiment, a MnO xPreparation method of carbon-based desulfurization and denitrification catalyst with low temperature cyclic regeneration as active component. This embodiment is basically the same as the first embodiment, except that: without changing the carbon material carrier MDC, another active component (MnO x ) to prepare a carbon-based desulfurization and denitrification catalyst that can be recycled and regenerated at low temperature, that is, replacing the precursor solution with a manganese nitrate solution during the impregnation process, and converting the required mass of manganese nitrate. And the metal oxide accounts for 1% of the catalyst MnO x The mass percentage of / MDC is 10wt.%.

[0053] (2) Desulfurization / denitrification performance test: 1.0 g of MnO x / MDC is the experimental object, and the specific test conditions for denitrification performance are: the simulated flue gas atmosphere includes 500ppm NO, 500ppm NH3, 10% O2 and balance gas N2, and the reaction space velocity is 12000m 3 ·h -1 , the temperature is 120℃. Under this condition, the test results show that the denitrification activity reaches 87.82% at . The specific test conditions for desulfurization performance are to simulate the flue gas atmosphere including 1000ppm SO2, 10% O2, 10% H2O and balance gas N2, and the reaction space velocity is 12000m 3 ·h -1 , the temperature is 120°C. Under this condition, the test results show that the sulfur capacity is 98.02 mg / g.

[0054] (3) Cyclic regeneration performance test: In this example, 1.0 g of MnO x / MDC was used as the experimental object. After the denitration and desulfurization reactions were completed at 120°C, it was thermally regenerated at 350°C under N2 protection. The test results showed that the catalyst MnO obtained in Example 1 x / MDC has no desulfurization and denitrification performance decline after 5 regenerations. x The denitrification activity of / MDC reaches 89.57% at 120℃, and the sulfur capacity is 100.75mg / g.

[0055] Comparative Example 1:

[0056] An iron oxide (FeO x ) as a common desulfurization and denitrification catalyst with active components, and its preparation method and use.

[0057] (1) This comparative example is basically the same as Example 1: anthracite is crushed into particles, then ground and sieved to 40-60 mesh, and then washed with ultrapure water and fully dried to obtain a coal-based material. The coal-based material and ultrapure water are placed in a solvent thermal reactor at a liquid-solid ratio of 1g:10mL and mixed, and no ammonium persulfate solution is added. Subsequently, a solvent thermal reaction is carried out at 200°C for 3 hours to obtain a carbon material carrier, and the carbon material carrier is recorded as AC. According to the required amount of raw materials in Table 1, 10g of AC is immersed in a nonahydrate ferric nitrate solution by an equal volume impregnation method, and ultrasonicated for 1 hour, allowed to stand for 12 hours, and placed in a 110°C drying oven to dry to constant weight. Finally, it is calcined at 400°C for 4 hours in a tubular furnace under N2 protection to obtain a loaded transition metal oxide FeO x A common desulfurization and denitration catalyst, the catalyst is denoted as FeO x / AC.

[0058] (1) Desulfurization / denitrification performance test: x / AC was taken as the experimental object. In the temperature range of 100-250°C, the simulated flue gas atmosphere included 500ppm NO, 500ppm NH3, 10% O2 and the balance gas N2 (purity of 99.99%). The test results showed that the denitrification activity reached 65.21% at 120°C. The desulfurization activity test was carried out at 120°C, and the simulated flue gas atmosphere included 1000ppm SO2, 10% O2, 10% H2O and the balance gas N2 (purity of 99.99%). The test results showed that the sulfur capacity was 60.87mg / g.

[0059] (2) Cyclic regeneration performance test: 1.0 g of FeO x / MDC and FeO x / AC was the experimental object. After the denitration and desulfurization reactions were completed at 120°C, it was thermally regenerated at 350°C under N2 protection. The test results showed that the catalyst FeO obtained in Comparative Example 1 x / AC showed a significant decrease in desulfurization and denitrification activity after 5 regenerations. At 120°C, the denitrification activity dropped to 39.01% and the sulfur capacity dropped to 53.08 mg / g. For specific test results, see the attached manual Figure 1 and Figure 2 .

[0060] Figure 1 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MDC and FeO x / AC denitrification performance diagram (NO conversion rate) during the 5-cycle desulfurization and denitrification regeneration process. As can be seen from the figure, during the 5-cycle desulfurization and denitrification regeneration process, the catalyst sample FeO obtained in Example 1 x / MDC can be recycled and reused, and the denitrification performance during the cyclic reaction is higher than that of the catalyst sample FeO obtained in the comparative example 1 x / AC.

[0061] Figure 2 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MDC and FeO x / AC desulfurization (sulfur capacity) performance diagram during the 5-cycle desulfurization and denitrification regeneration process. As can be seen from the figure, during the 5-cycle desulfurization and denitrification regeneration process, the catalyst sample FeO obtained in Example 1 x / MDC can be recycled and reused, and the denitrification performance during the cyclic reaction is higher than that of the catalyst sample FeO obtained in the comparative example 1 x / AC.

[0062] Figure 3 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MDC and FeO x / EDS surface scan elemental analysis image of AC. Figure 3 a shows that the catalyst sample FeO obtained in Example 1 x / MDC active component FeO x The nanoparticles are evenly dispersed on the surface of the carrier MDC. Figure 3 b shows that the FeO x FeO on the surface of AC catalyst x Agglomeration phenomenon occurs. It is further confirmed that the preparation method described in Example 1 makes the active components uniformly dispersed on the surface of the carrier, which is beneficial to improving the desulfurization and denitrification reaction activity and cyclic regeneration stability of the catalyst.

[0063] Figure 4 The catalyst sample FeO was prepared by the method described in Example 1 and Comparative Example 1 of the present invention. x / MDC and FeO x / AC SO2 analysis curve during N2 thermal regeneration process after 5 cycles of desulfurization and denitrification reaction. Figure 4 It shows that compared with the catalyst sample FeO obtained in comparative example 1 x / AC, catalyst sample FeO obtained in Example 1 x / The sulfate species formed on the surface of MDC can be decomposed at a lower temperature, and the amount of SO2 released during the regeneration process is greater. Figure 1 , Example 1 Catalyst sample FeO x / MDC has high desulfurization and denitrification activity, excellent renewability and is expected to achieve efficient recycling of SO2 resources during its application in the field of desulfurization and denitrification.

[0064] The present invention uses the above-mentioned embodiments to illustrate in detail the detailed composition and preparation method of the materials described in the present invention, but the present invention is not limited to the above-mentioned embodiments, and various changes can be made according to the purpose of the invention of the present invention. Any changes, modifications, substitutions, combinations or simplifications made according to the spirit and principle of the technical scheme of the present invention should be equivalent replacement methods. As long as they meet the purpose of the invention of the present invention and do not deviate from the technical principles and inventive concepts of the method for preparing a carbon-based desulfurization and denitrification catalyst that can be regenerated at low temperature, they belong to the protection scope of the present invention.

Claims

1. A carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration and its preparation method and use, characterized in that: The catalyst has a carrier and an active component, and the active component is highly dispersed on the surface of the carbon material carrier; The carrier is a carbon material with a hierarchical pore structure, and the surface and / or pores of the carbon material are rich in negatively charged oxygen-containing functional groups; The active component is a transition metal oxide, and the transition metal oxide is highly dispersed on the surface and / or pores of the carbon material carrier; The carbon material carrier and the transition metal oxide active component form an oxygen-containing functional group-carbon-transition metal oxide coordination structure, and the transition metal oxide in the coordination structure is rich in coupled oxygen vacancy defects.

2. The low-temperature cyclically regenerable carbon-based desulfurization and denitrification catalyst according to claim 1, characterized in that: The mass ratio of the transition metal oxide active component to the carbon material carrier in the catalyst is 1:9 to 2:8, and the transition metal oxide includes a combination of one or more oxides of iron oxide, cobalt oxide, copper oxide, manganese oxide and nickel oxide.

3. The low-temperature cyclically regenerable carbon-based desulfurization and denitrification catalyst according to claim 1 or 2, characterized in that: The carbon material carrier in the catalyst has micropores and mesopores, and the BET specific surface area of ​​the carbon material is 750 m 2 / g or above.

4. The low-temperature cyclically regenerable carbon-based desulfurization and denitration catalyst according to any one of claims 1 to 3, characterized in that: The transition metal oxide active component of the catalyst is highly dispersed on the surface and / or in the pores of the carbon material carrier in a manner of directional anchoring of oxygen-containing functional groups.

5. The method for preparing a carbon-based desulfurization and denitrification catalyst capable of low-temperature cyclic regeneration according to claim 4, characterized in that: The preparation method comprises the following steps: (1) A carbon material carrier having a multi-level pore structure and rich in negatively charged oxygen-containing functional groups is prepared using coal-based materials; (2) The carbon material carrier is impregnated with a solution of a transition metal oxide precursor and then calcined in a nitrogen atmosphere to obtain the carbon-based desulfurization and denitrification catalyst that can be cyclically regenerated at low temperature.

6. The preparation method according to claim 5, characterized in that: The coal-based material includes but is not limited to a combination of one or more of lignite, bituminous coal, and anthracite; The coal-based material is subjected to a solvent thermal reaction to obtain a carbon material carrier; the temperature of the solvent thermal reaction is 180 to 260° C.; and the solvent thermal reaction time is 3 to 5 hours.

7. The preparation method according to claim 5 or 6, characterized in that: In the process of preparing a carbon material carrier using a coal-based material, the preparation method further comprises the steps of making the carbon material carrier have a hierarchical pore structure and rich in negatively charged oxygen-containing functional groups; The step of making the carbon material carrier have a multi-level pore structure and rich in negatively charged oxygen-containing functional groups comprises adding the coal-based material to an ammonium persulfate solution and then performing a solvothermal reaction, wherein the volume ratio of the coal-based material to the ammonium persulfate solution is 1:10 to 1:5, and the concentration of the ammonium persulfate solution is 1.5 to 2.5 mol / L.

8. The preparation method according to claim 5, characterized in that: The precursor solution of the transition metal oxide includes a metal nitrate and / or chloride solution.

9. The preparation method according to claim 5, characterized in that: The calcination temperature is 300 to 500° C., and the heat treatment time is 4 to 6 hours.

10. Use of the low-temperature cyclically regenerable carbon-based desulfurization and denitrification catalyst according to any one of claims 1 to 4 in the field of industrial flue gas desulfurization and denitrification.

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