Regeneration method of supported metal catalyst

Abstract

The invention discloses a regeneration method of a supported metal catalyst, which utilizes a UV-O3 coupling technology to convert carbon deposit on the surface of the supported metal catalyst into carbon dioxide under mild conditions, effectively solves the problem of carbon deposit, recovers the activity and selectivity of the catalyst, and avoids many defects brought by a traditional regeneration method.

Description

Technical Field

[0001] The invention relates to a method for regenerating a supported metal catalyst. Background Art

[0002] Supported metal catalysts are widely used in various fields, including chemical engineering and energy, such as hydrogenation and oxidation reactions. However, during catalyst use, reactants and their intermediates undergo polymerization and cyclization reactions on the catalyst surface, forming carbon deposits. This carbon deposit covers the catalyst's active centers, hindering contact between reactants and the active centers. This leads to decreased catalyst activity and selectivity, significantly impacting the efficiency of the catalytic reaction and the catalyst's service life.

[0003] Currently, commonly used catalyst regeneration methods include thermal regeneration and chemical solvent cleaning. Thermal regeneration involves burning carbon deposits at high temperatures to convert them into carbon dioxide. However, high temperatures can easily cause agglomeration and sintering of the catalyst's active components, as well as changes in the support structure, reducing catalyst performance. While chemical solvent cleaning can remove carbon deposits to a certain extent, the cleaning process is complex, and the chemical solvents can damage the catalyst's active components and support. Furthermore, there are issues with solvent recovery and environmental pollution. Therefore, there is a need for an efficient, gentle, and environmentally friendly method for regenerating supported metal catalysts. Summary of the Invention

[0004] The purpose of the present invention is to provide a method for regenerating a supported metal catalyst. By using UV-O3 combined technology, the carbon deposits on the surface of the supported metal catalyst are converted into carbon dioxide under mild conditions, effectively solving the carbon deposition problem, restoring the activity and selectivity of the catalyst, and avoiding the many disadvantages of traditional regeneration methods.

[0005] The technical solution adopted by the present invention is described in detail below.

[0006] The present invention provides a method for regenerating a supported metal catalyst, which comprises the following steps:

[0007] 1) Catalyst pretreatment: The supported metal catalyst to be regenerated is washed with water to remove impurities (such as dust) attached to its surface, and then placed in a reaction vessel after drying;

[0008] 2) UV-O3 treatment: ozone (O3) is introduced into the reaction vessel, and an ultraviolet (UV) irradiation device is turned on to irradiate the supported metal catalyst to be regenerated, and the UV-O3 combined treatment is carried out at room temperature and pressure;

[0009] 3) washing the catalyst treated in step 2) again to remove residual ozone and reaction by-products on the surface;

[0010] 4) The catalyst obtained in step 3) is dried in an oven to obtain a regenerated supported metal catalyst.

[0011] Furthermore, the drying temperature in step 1) is 60-120° C. and the drying time is 3-10 hours.

[0012] Furthermore, in step 2), ozone (O3) is introduced into the reaction vessel at a flow rate of 5 to 8 L / min to make the ozone concentration in the reaction vessel reach 100 to 120 mg / m 3 Then, the ultraviolet (UV) irradiation device is turned on to irradiate the supported metal catalyst to be regenerated. The ultraviolet wavelength is 100-280nm and the irradiation intensity is 100-200w / m 2 , the irradiation time is 1-5 hours.

[0013] Furthermore, in step 4), the drying temperature is 60-100° C. and the drying time is 5-8 hours.

[0014] The supported metal catalyst of the present invention comprises a support and a metal active center, wherein the metal active center can be at least one of palladium, platinum, ruthenium, rhodium, and copper, and the support can be at least one of aluminum oxide, aluminum nitride, silicon nitride, silicon oxide, activated carbon, titanium dioxide, and titanium nitride. The metal loading (based on the support) of the supported metal catalyst is generally 0.01 wt% to 10 wt%.

[0015] The supported metal catalyst of the present invention can be a commercially available product, or can be prepared according to methods reported in the literature, such as by an impregnation method. As an implementation method, the specific preparation steps of the supported metal catalyst are as follows:

[0016] 1) preparing a metal salt solution of a certain concentration according to the active component content of the desired catalyst, and immersing the selected support in the solution to obtain a mixture;

[0017] 2) keeping the mixture in step 1) at room temperature for 10 to 12 hours to allow the metal salt to be fully adsorbed on the surface of the support;

[0018] 3) drying the impregnated support in step 2) in an oven at 80°C to 200°C for 8 to 12 hours;

[0019] 4) calcining the dried sample in step 3) in a muffle furnace at 300-900° C. for 1-5 hours;

[0020] 5) Finally, reduction is carried out at 200-400° C. for 1-4 h under a hydrogen atmosphere to obtain a supported metal catalyst.

[0021] The supported metal catalyst of the present invention can be applied to reactions such as the selective hydrogenation of acetylenic compounds (such as acetylene, propyne, etc.) and the hydrogenation of olefinic compounds (such as ethylene, vinyl chloride, etc.).

[0022] Compared with the prior art, the beneficial effects of the present invention are:

[0023] 1. Efficient removal of carbon deposits: The present invention adopts UV-O3 combined technology, using the strong oxidizing active species generated by ozone under ultraviolet irradiation to quickly and effectively oxidize the carbon deposits on the catalyst surface into carbon dioxide. The carbon deposit removal rate is high, which can significantly restore the active center of the catalyst and improve the activity and selectivity of the catalyst.

[0024] 2. Mild operation: The entire regeneration process is carried out at room temperature and pressure, avoiding the damage of high temperature to the active components of the catalyst and the carrier structure, preventing problems such as agglomeration and sintering of the active components and deformation of the carrier, which is conducive to maintaining the original performance and structural stability of the catalyst.

[0025] 3. Green and environmentally friendly: This regeneration method does not use chemical solvents, reducing the consumption of chemical reagents and pollution to the environment. At the same time, ozone will decompose into oxygen after the reaction, without secondary pollution, which meets the development requirements of green chemistry.

[0026] 4. Wide range of applications: It is suitable for the regeneration of supported metal catalysts whose active centers are palladium, platinum, ruthenium, rhodium, copper, and whose carriers are various combinations of alumina, aluminum nitride, silicon nitride, silicon oxide, activated carbon, titanium dioxide, titanium nitride, etc. It has broad application prospects. DETAILED DESCRIPTION

[0027] The present invention is illustrated below using specific examples. It should be noted that the examples are intended only to further illustrate the present invention and are not to be construed as limiting the scope of the present invention. The present invention is not limited thereto in any way. Those skilled in the art may make non-essential improvements and adjustments based on the above-described invention.

[0028] In the examples of the present invention, if the specific conditions are not specified, the experiments were carried out according to conventional conditions or the conditions recommended by the manufacturer. The reagents or instruments used, if the manufacturer is not specified, are conventional products that can be obtained by conventional techniques or purchased commercially.

[0029] Example 1

[0030] 1) 0.0083 g of palladium chloride was dissolved in 5 ml of 6 mol / L dilute hydrochloric acid, and 50 ml of water was added. 10 g of γ-alumina with an average particle size of 100 μm was immersed in the solution.

[0031] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0032] 3) The carrier impregnated in step 2) was placed in an oven and dried at 120° C. for 10 h.

[0033] 4) The dried sample from step 3) was placed in an air atmosphere muffle furnace at 400° C. and calcined for 2 h.

[0034] 5) Finally, reduction was carried out at 300° C. for 1 h under a hydrogen atmosphere to obtain a catalyst with a metal loading of 0.05 wt%.

[0035] 6) Evaluation of acetylene hydrogenation reaction in a fixed bed reactor: Acetylene hydrogenation reaction at 80°C, acetylene space velocity 1000h -1 The reaction was carried out under the conditions of a hydrogen: acetylene volume ratio of 2:1, with a conversion rate of 75% and a selectivity of 80%. After carbon deposition, the conversion rate was 37% and the selectivity was 39%.

[0036] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100°C for 4 hours, and then place it in a reaction vessel;

[0037] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 5 L / min to make the ozone concentration in the vessel reach 100 mg / m 3 Then turn on the ultraviolet irradiation device, the ultraviolet wavelength is 254nm, and the light intensity is 110W / m 2 , the catalyst after carbon deposition was treated with UV-O3 combination at room temperature and pressure for 3 hours;

[0038] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0039] 10) Place in an oven and dry at 80° C. for 6 h to obtain a regenerated catalyst;

[0040] 11) The catalyst was weighed before and after regeneration, and the surface carbon removal rate was calculated to be 87%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 62% and its selectivity was 70%, and the performance was restored to 82% of the fresh catalyst (calculated as the conversion recovery rate, the same below).

[0041] Example 2

[0042] 1) 0.627 g of platinum chloride was dissolved in 30 ml of water, and 0.36 g of rhodium chloride was dissolved in 10 ml of 6 mol / L dilute hydrochloric acid, and then 30 ml of water was added. The two metal salt solutions were mixed together, and 10 g of α-silicon nitride with an average particle size of 5000 nm was immersed in the mixed solution.

[0043] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0044] 3) The carrier impregnated in step 2) was placed in an oven and dried at 150° C. for 12 hours.

[0045] 4) The dried sample from step 3) was placed in a muffle furnace at 500° C. and calcined for 2 h.

[0046] 5) Finally, reduction was carried out at 300°C for 2 h under a hydrogen atmosphere to obtain a catalyst.

[0047] 6) Evaluation of propyne hydrogenation reaction in a fixed bed reactor: Propylene hydrogenation reaction at 150 ° C, propyne space velocity 6000h -1 Under the condition of hydrogen: propyne volume ratio of 20:1, the conversion rate of the reaction is 95% and the selectivity is 89%. After carbon deposition, the conversion rate is 55% and the selectivity is 51%.

[0048] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0049] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 8 L / min to make the ozone concentration in the vessel reach 120 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 234nm, and the light intensity is 100W / m 2 , the catalyst after carbon deposition was treated with UV-O3 combination at room temperature and pressure for 3 hours;

[0050] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0051] 10) Place in an oven and dry at 90° C. for 5 h to obtain a regenerated catalyst;

[0052] 11) The weights before and after regeneration were measured, and the surface carbon removal rate was calculated to be 93%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6), and the results showed that its conversion rate was 84% ​​and its selectivity was 71%, and the performance was restored to 88% of the fresh catalyst.

[0053] Example 3

[0054] 1) Dissolve 0.415 g of copper nitrate in 30 ml of water, and immerse 5 g of powdered activated carbon with an average particle size of 20 μm in the solution.

[0055] 2) The mixture in step 1) was kept at room temperature for 11 h.

[0056] 3) The carrier impregnated in step 2) was placed in an oven and dried at 110° C. for 10 h.

[0057] 4) The dried sample from step 3) was placed in a muffle furnace at 600° C. and calcined for 2 h.

[0058] 5) Finally, reduction was carried out at 400°C for 1 h under a hydrogen atmosphere to obtain the catalyst.

[0059] 6) Evaluation of acetylene hydrogenation reaction in a fixed bed reactor: Acetylene hydrogenation reaction at 100°C, acetylene space velocity 3000h -1 The reaction was carried out under the conditions of a hydrogen: acetylene volume ratio of 20:1, with a conversion rate of 85% and a selectivity of 89%. After carbon deposition, the conversion rate was 45% and the selectivity was 47%.

[0060] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0061] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 6 L / min to make the ozone concentration in the vessel reach 110 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 200nm, and the light intensity is 130W / m 2 , the catalyst after carbon deposition was treated with UV-O3 at room temperature and pressure for 2 hours;

[0062] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0063] 10) Place in an oven and dry at 60° C. for 8 h to obtain a regenerated catalyst;

[0064] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to be 89%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 72% and its selectivity was 81%, and the performance was restored to 85% of the fresh catalyst.

[0065] Example 4

[0066] 1) 0.474 g of ruthenium chloride was dissolved in 30 ml of water, and 5 g of anatase titanium dioxide with an average particle size of 10 nm was immersed in the solution.

[0067] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0068] 3) The carrier impregnated in step 2) was placed in an oven and dried at 120° C. for 12 hours.

[0069] 4) The dried sample from step 3) was placed in a muffle furnace at 400° C. and calcined for 2 h.

[0070] 5) Finally, reduction was carried out at 300°C for 1 h under a hydrogen atmosphere to obtain a catalyst.

[0071] 6) Evaluation of acetylene hydrogenation reaction in a fixed bed reactor: Acetylene hydrogenation reaction at 130°C and acetylene space velocity 6000h -1 The reaction was carried out under the conditions of a hydrogen: acetylene volume ratio of 2:1, with an active conversion rate of 90% and a selectivity of 92%. After carbon deposition, the conversion rate was 50% and the selectivity was 51%.

[0072] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0073] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 7 L / min to make the ozone concentration in the vessel reach 115 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 190nm, and the light intensity is 150W / m 2 , the catalyst after carbon deposition was treated with UV-O3 combination at room temperature and pressure for 4 hours;

[0074] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0075] 10) Place in an oven and dry at 75° C. for 7 h to obtain a regenerated catalyst;

[0076] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to reach 92%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 77% and its selectivity was 75%, and its performance was restored to 86% of the fresh catalyst.

[0077] Example 5

[0078] 1) 0.21 g of palladium chloride was dissolved in 10 ml of 6 mol / L dilute hydrochloric acid and then 20 ml of water was added. 0.159 g of copper chloride was dissolved in 30 ml of water. The two metal salt solutions were mixed together, and 10 g of titanium nitride with an average particle size of 100 nm was immersed in the mixed solution.

[0079] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0080] 3) The carrier after impregnation in step 2) was placed in an oven and dried at 130° C. for 12 hours.

[0081] 4) The dried sample from step 3) was placed in a muffle furnace at 400° C. and calcined for 2 h.

[0082] 5) Finally, reduction was carried out at 400°C for 1 h under a hydrogen atmosphere to obtain the catalyst.

[0083] 6) Evaluation of propyne hydrogenation reaction in a fixed bed reactor: Propylene hydrogenation reaction at 100°C and propyne space velocity 4000h -1 Under the condition of hydrogen: propyne volume ratio of 2:1, the reaction conversion rate is 83% and the selectivity is 90%. The conversion rate after carbon deposition is 43% and the selectivity is 45%.

[0084] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0085] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 6.5 L / min to make the ozone concentration in the vessel reach 112 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 272nm, and the light intensity is 100W / m 2 , the catalyst after carbon deposition was treated with UV-O3 at room temperature and pressure for 2 hours;

[0086] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0087] 10) Place in an oven and dry at 75° C. for 7 h to obtain a regenerated catalyst;

[0088] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to be 89%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 70% and its selectivity was 71%, and its performance was restored to 84% of the fresh catalyst.

[0089] Example 6

[0090] 1) 0.307 g of rhodium chloride was dissolved in 10 ml of 6 mol / L dilute hydrochloric acid and then 30 ml of water was added. 10 g of mesoporous silica with an average particle size of 20 nm was immersed in the mixed solution.

[0091] 2) The mixture in step 1) was kept at room temperature for 10 h.

[0092] 3) The carrier impregnated in step 2) was placed in an oven and dried at 120° C. for 12 hours.

[0093] 4) The dried sample from step 3) was placed in a muffle furnace at 400° C. and calcined for 2 h.

[0094] 5) Finally, reduction was carried out at 300°C for 2 h under a hydrogen atmosphere to obtain a catalyst.

[0095] 6) Evaluation of vinyl chloride hydrogenation reaction in a fixed bed reactor: The vinyl chloride hydrogenation reaction was carried out at 110°C and a vinyl chloride space velocity of 3000 h -1 Under the condition of hydrogen: vinyl chloride volume ratio of 2:1, the reaction conversion rate is 87% and the selectivity is 80%. After carbon deposition, the conversion rate is 48% and the selectivity is 41%.

[0096] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0097] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 7 L / min to make the ozone concentration in the vessel reach 110 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 200nm, and the light intensity is 130W / m 2 , the catalyst after carbon deposition was treated with UV-O3 combination at room temperature and pressure for 3 hours;

[0098] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0099] 10) Place in an oven and dry at 85° C. for 5 h to obtain a regenerated catalyst;

[0100] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to be 91%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 75% and its selectivity was 63%, and its performance was restored to 86% of the fresh catalyst.

[0101] Example 7

[0102] 1) 0.147 g of ruthenium chloride and 0.082 g of copper chloride were dissolved in 20 ml of water, and 10 g of aluminum nitride with an average particle size of 100 nm was immersed in the mixed solution.

[0103] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0104] 3) The carrier impregnated in step 2) was placed in an oven and dried at 120° C. for 12 hours.

[0105] 4) The dried sample from step 3) was calcined in a muffle furnace at 300°C for 2 h.

[0106] 5) Finally, reduction was carried out at 300°C for 1 h under a hydrogen atmosphere to obtain a catalyst.

[0107] 6) Evaluation of vinyl chloride hydrogenation reaction in a fixed bed reactor: The vinyl chloride hydrogenation reaction was carried out at 90°C and a vinyl chloride space velocity of 5000 h -1Under the condition that the volume ratio of hydrogen to vinyl chloride is 20:1, the conversion rate of the reaction is 80% and the selectivity is 70%. After carbon deposition, the conversion rate is 40% and the selectivity is 35%.

[0108] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0109] 8) UV-O3 treatment: ozone was introduced into the reaction vessel, and the ozone flow rate was controlled at 6 L / min to make the ozone concentration in the vessel reach 105 mg / m 3 Turn on the ultraviolet irradiation device, the ultraviolet wavelength is 157nm, and the light intensity is 150W / m 2 , the catalyst after carbon deposition was treated with UV-O3 at room temperature and pressure for 2 hours;

[0110] 9) Take out the catalyst and rinse it with deionized water 5 times;

[0111] 10) Place in an oven and dry at 70° C. for 7 h to obtain a regenerated catalyst;

[0112] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to be 88%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 66% and its selectivity was 61%, and the performance was restored to 83% of the fresh catalyst.

[0113] Comparative Example 1 (thermal regeneration method): compared with Example 1

[0114] 1) 0.0083 g of palladium chloride was dissolved in 5 ml of 6 mol / L dilute hydrochloric acid, and 50 ml of water was added. 10 g of γ-alumina with an average particle size of 100 μm was immersed in the solution.

[0115] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0116] 3) The carrier impregnated in step 2) was placed in an oven and dried at 120° C. for 10 h.

[0117] 4) The dried sample from step 3) was placed in a muffle furnace at 400° C. and calcined for 2 h.

[0118] 5) Finally, reduction was carried out at 300°C for 1 h under a hydrogen atmosphere to obtain a catalyst.

[0119] 6) Evaluation of acetylene hydrogenation reaction in a fixed bed reactor: Acetylene hydrogenation reaction at 80°C, acetylene space velocity 1000h -1, the volume ratio of hydrogen to acetylene was 2:1; the reaction conversion rate was 75%, the selectivity was 80%, and the conversion rate after carbon deposition was 37%, and the selectivity was 39%.

[0120] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0121] 8) Thermal regeneration treatment: Place the catalyst in a high-temperature furnace and heat it at 500°C for 3 hours to burn the carbon deposits and convert them into carbon dioxide;

[0122] 9) After cooling, the catalyst was removed and subjected to the same catalytic reaction test; the surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to reach 70%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6), and the results showed that its conversion rate was 45% and its selectivity was 51%, and the performance was restored to 60% of the fresh catalyst.

[0123] Comparative Example 2 (Chemical Solvent Cleaning Method): Compare with Example 2

[0124] 1) 0.627 g of platinum chloride was dissolved in 30 ml of water, and 0.36 g of rhodium chloride was dissolved in 10 ml of 6 mol / L dilute hydrochloric acid, and then 30 ml of water was added. The two metal salt solutions were mixed together, and 10 g of α-silicon nitride with an average particle size of 5000 nm was immersed in the mixed solution.

[0125] 2) The mixture in step 1) was kept at room temperature for 12 h.

[0126] 3) The carrier impregnated in step 2) was placed in an oven and dried at 150° C. for 12 hours.

[0127] 4) The dried sample from step 3) was placed in a muffle furnace at 500° C. and calcined for 2 h.

[0128] 5) Finally, reduction was carried out at 300°C for 2 h under a hydrogen atmosphere to obtain a catalyst.

[0129] 6) Evaluation of propyne hydrogenation reaction in a fixed bed reactor: Propylene hydrogenation reaction at 150 ° C, propyne space velocity 6000h -1 Under the condition of hydrogen: propyne volume ratio of 20:1, the conversion rate of the reaction is 95% and the selectivity is 89%. After carbon deposition, the conversion rate is 55% and the selectivity is 51%.

[0130] 7) Wash the carbon-deposited catalyst with deionized water, dry it at 100° C. for 4 hours, and then place the carbon-deposited catalyst into a reaction vessel;

[0131] 8) Chemical solvent cleaning: Soak the catalyst in organic solvent N-methylpyrrolidone for 4 hours with constant stirring to remove carbon deposits;

[0132] 9) Rinse with deionized water 5 times;

[0133] 10) Dry in an oven at 90°C for 5 hours;

[0134] 11) The surface carbon removal rate was calculated by weighing the catalyst before and after regeneration to reach 75%. The performance of the regenerated catalyst was evaluated under the same catalytic reaction conditions as in step 6). The results showed that its conversion rate was 66% and its selectivity was 56%, and the performance was restored to 70% of the fresh catalyst.

Claims

1. A method for regenerating a supported metal catalyst, characterized in that: The specific steps of the regeneration method are as follows: 1) Catalyst pretreatment: The supported metal catalyst to be regenerated is washed with water to remove impurities attached to its surface, dried and placed in a reaction vessel; 2) UV-O3 treatment: ozone is introduced into the reaction vessel, and the ultraviolet irradiation device is turned on to irradiate the supported metal catalyst to be regenerated, and the UV-O3 combined treatment is carried out at room temperature and pressure; 3) washing the catalyst treated in step 2) again to remove residual ozone and reaction by-products on the surface; 4) The catalyst obtained in step 3) is dried in an oven to obtain a regenerated supported metal catalyst.

2. The regeneration method according to claim 1, wherein: The drying temperature in step 1) is 60-120° C. and the drying time is 3-10 hours.

3. The regeneration method according to claim 1, wherein: In step 2), ozone is introduced into the reaction vessel at a flow rate of 5 to 8 L / min to make the ozone concentration in the reaction vessel reach 100 to 120 mg / m 3 Then, the ultraviolet irradiation device is turned on to irradiate the supported metal catalyst to be regenerated. The ultraviolet wavelength is 100-280nm and the irradiation intensity is 100-200w / m 2 , the irradiation time is 1-5 hours.

4. The regeneration method according to claim 1, wherein: Step 4) The drying temperature is 60-100° C. and the drying time is 5-8 hours.

5. The regeneration method according to claim 1, wherein: The supported metal catalyst includes a carrier and a metal active center, wherein the metal active center is at least one of palladium, platinum, ruthenium, rhodium, and copper, and the carrier is at least one of aluminum oxide, aluminum nitride, silicon nitride, silicon oxide, activated carbon, titanium dioxide, and titanium nitride; and the metal loading amount based on the carrier in the supported metal catalyst is 0.01 wt% to 10 wt%.

6. The regeneration method according to claim 5, wherein: The supported metal catalyst is a catalyst used for the selective hydrogenation of acetylenic compounds or the hydrogenation reaction of olefinic compounds.