JP2016198691A - Regeneration catalyst for treating heavy oil and manufacturing method therefor and method for using regeneration catalyst for treating heavy oil - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a regeneration catalyst for treating heavy oil or the like capable of preventing reduction of economical efficiency by catalyst performance reduction or device utilization reduction due to abnormal heat generation in a reactor which becomes problem in a heavy oil hydrodesulfurization device or metal unloading device and achieving catalyst cost reduction or waste amount reduction.SOLUTION: There is provided a regeneration catalyst for treating heavy oil or the like for treating heavy oil with combing unused catalyst for treating heavy oil, which is (A) a used catalyst where the unused catalyst for treating heavy oil and (B) a regeneration catalyst for treating heavy oil or the like having (a) deposition amount of vanadium and nickel of 1 to 45 mass%, (b) carbon coating weight of 1 to 26 mass% and (c) at least one of desulfurization activity and desulfurization activity of 50 to 70%.SELECTED DRAWING: None

Description

  The present invention relates to a regenerated catalyst for treating heavy oil, a method for producing the same, and a method for using the regenerated catalyst for treating heavy oil.

  The regeneration of the catalyst, not limited to the heavy oil hydrorefining field, aims to restore the catalyst activity to the unused catalyst level as much as possible and reuse it. Therefore, the regeneration so far has mainly been a catalyst for kerosene and light oil, and mainly a method for producing and using a regenerated catalyst having higher catalytic activity (see, for example, Patent Documents 1 to 3).

JP 2012-86198 A JP 2011-200787 A JP 2011-143389 A

However, for example, in the case of a desulfurization catalyst, if the entire amount is started with an unused catalyst or an ordinary regenerated catalyst, the activity is too high and the catalyst performance cannot be controlled even if the temperature condition of the catalyst layer is set to the lower limit. As a result of abnormal heat generation, a coke precursor is generated, which causes clogging of the subsequent reactor, piping, and heat exchanger. In addition, the abnormal heat generation causes the catalysts to be fixed and solidified to cause an extreme deterioration in performance and a decrease in catalyst performance due to drift.
Here, an abnormal heat generation is defined as a temperature difference of 30 ° C. or more between the inlet and the outlet of the reactor filled with the catalyst. Detection of such abnormal heat generation can be calculated by measuring the temperatures at the inlet and outlet of the reaction tower.

  Therefore, in the present invention, it is possible to prevent a decrease in catalyst performance due to abnormal heat generation in a reaction tower, which is a problem in a heavy oil hydrodesulfurization apparatus, a demetallizer, etc., and a decrease in economy due to a decrease in apparatus operation, and to reduce catalyst costs. It is an object of the present invention to provide a heavy oil treatment regenerated catalyst that can achieve a reduction in the amount of waste, a method for producing the same, and a method for using the heavy oil treatment regenerated catalyst.

  As a result of intensive studies to solve the above problems, the present inventors have regenerated (deoiled) the spent catalyst extracted from the apparatus to a state of moderately lower activity than the unused catalyst. The present inventors have found that problems such as abnormal heat generation in the apparatus can be solved by filling the hydrodesulfurization apparatus or demetallization apparatus in combination with the catalyst used. That is, the present invention is as follows.

[1] A heavy oil treatment regenerated catalyst for treating heavy oil in combination with an unused heavy oil treatment catalyst,
The recycled catalyst for heavy oil treatment
(A) It is a used catalyst used for treating heavy oil, the unused heavy oil treatment catalyst,
(B) With respect to the unused heavy oil treatment catalyst, (a) the amount of vanadium and nickel deposited is 1 to 45% by mass, (b) the amount of carbon adhesion is 1 to 26% by mass, (c ) A regenerated catalyst for heavy oil treatment in which at least one of desulfurization activity and demetalization activity is 50 to 70%.
[2] The regenerated catalyst for heavy oil treatment according to [1], wherein the average particle size is 2 to 5 mm.
[3] The regenerated catalyst for heavy oil treatment according to [1] or [2], wherein the specific surface area is 50 to 300 m ² / g.

[4] A method for producing a recycled catalyst for treating heavy oil according to any one of [1] to [3], comprising the following steps (1) to (3) in sequence, and treating unused heavy oil A method for producing a regenerated catalyst for heavy oil treatment, which obtains a regenerated catalyst for heavy oil treatment in which at least one of desulfurization activity and demetalization activity for the catalyst for use is 50 to 70%.
Step (1): Step of measuring the content of vanadium and nickel with respect to an unused heavy oil treatment catalyst before being used for treatment of heavy oil Step (2): Treatment of the unused heavy oil The catalyst for heavy oil is used for heavy oil treatment, and the used catalyst after the treatment is selected to have a vanadium and nickel deposition amount of 1 to 45% by mass with respect to the measured vanadium and nickel content. Step (3) to perform: A step of subjecting the selected spent catalyst to a drying treatment or a solvent washing treatment to adjust the carbon adhesion amount to 1 to 26 mass%.

[5] Heavy oil treatment for treating heavy oil by combining the heavy oil treatment regenerated catalyst according to any one of [1] to [3] and an unused heavy oil treatment catalyst. To use regenerated catalyst.
[6] To [5], 10 to 50% by mass of the regenerated catalyst for heavy oil treatment is charged separately from the unused heavy oil treatment catalyst in the upstream portion of the reactor with respect to the total catalyst charge. Use of the regenerated catalyst for heavy oil treatment as described.

  According to the present invention, it is possible to prevent a decrease in catalyst performance due to abnormal heat generation in a reaction tower, which is a problem in a heavy oil hydrodesulfurization apparatus, a demetalization apparatus, etc., or an economic decrease due to a decrease in apparatus operation, and to reduce catalyst costs. It is possible to provide a recycled catalyst for heavy oil treatment that can achieve a reduction in the amount of waste, a method for producing the same, and a method for using the recycled catalyst for heavy oil treatment.

[1. Regenerated catalyst for heavy oil treatment and method for producing the same]
The regenerated catalyst for heavy oil treatment according to the present invention is a catalyst obtained by regenerating a catalyst used for hydrodesulfurization or demetalization of heavy oil or the like, and originally has a hydrotreating ability and a demetalization ability. There is a need. Since the regenerated catalyst is used in this way, catalyst cost reduction and waste amount reduction can be achieved.

As a basic catalyst structure of an unused catalyst, an oxide of molybdenum and cobalt and / or nickel is supported on an inorganic oxide carrier such as alumina, alumina-phosphorus carrier, alumina-boron carrier, alumina-silicon carrier, etc. What was used is used suitably.
Among these, an alumina carrier / nickel-molybdenum supported catalyst, an alumina-phosphorus carrier / nickel-molybdenum supported catalyst, an alumina-boron carrier / nickel-molybdenum supported catalyst, and an alumina-silicon carrier / nickel-molybdenum supported catalyst are preferable.

When phosphorus, silicon, or boron is contained in alumina as a support, the content of at least one of phosphorus, silicon, and boron oxide is preferably 30% by mass or less, and 0.1 to 10% by mass More preferably, it is 0.2-5 mass%.
The content of phosphorus or the like in the catalyst is expressed as mass% of the mass of phosphorus or the like with the reference mass being the one that has not been reduced by oxidation treatment at 400 ° C. or higher.

Furthermore, since it is heavy oil processing, it is preferable to contain 0.1-25 mass% of molybdenum as a support metal, and it is more preferable to contain 0.2-8 mass%. Moreover, it is preferable to contain 0.1-10 mass% of cobalt or nickel as a carrying | support metal, and it is more preferable to contain 0.2-8 mass%.
In addition, the metal content in the catalyst is expressed by mass% as the mass of the oxide of the metal to be measured, based on the mass that is not reduced by oxidation treatment at 400 ° C. or higher. The same applies to the following metal contents.

Moreover, it is preferable that the average particle diameter of an unused catalyst is 2-5 mm, and it is more preferable that it is 2.8-4.5 mm. When the average particle size exceeds 5 mm, the amount of packing per unit volume decreases, and therefore the amount of catalyst (the amount of supported metal) charged in the reactor may decrease. Moreover, when it is less than 2 mm, the gap diameter becomes small, and the differential pressure in the reaction tower rises, which may hinder the operation.
The average particle size is obtained by directly measuring with a caliper or the like and statistically processing 100 points.

The unused catalyst having the above configuration can be produced by a usual method.
Then, using this unused catalyst, hydrodesulfurization treatment of heavy oil such as atmospheric residual oil is carried out for one year. Thereafter, the spent catalyst is withdrawn from the reactor and regenerated by the following regenerating method to produce the regenerated catalyst for heavy oil processing of the present invention.
In the case of an upflow type reactor, the catalyst at the uppermost part of the reaction or the uppermost part of the reactor can be used as long as it meets the requirements of the present invention, but these usually have a large scale and metal content. It may be adhering and is preferably removed by sorting.

  In the following, the hydrodesulfurization treatment using a fixed bed reactor often used in the hydrotreatment process will be mainly described, but the present invention is not limited to this.

First, “heavy oil” according to the present invention refers to those containing residues such as atmospheric residual oil and vacuum residual oil, and does not include oils consisting only of distillate oil such as kerosene, light oil and vacuum gas oil. Usually, in heavy oil, sulfur content is 1 mass% or more, nitrogen content is 200 massppm or more, residual carbon content is 3 mass% or more, vanadium is 5 massppm or more, nickel is 30 massppm or more, asphaltene content is 0.5 mass% or more. It is included.
Examples of heavy oil include atmospheric residual oil, crude oil, asphalt oil, pyrolysis oil, tar sand oil, and mixed oils containing these. Any heavy oil can be used as long as it is as described above, but normal pressure residual oil, vacuum residual oil, vacuum residual oil, mixed oil of asphalt oil and cracked gas oil, etc. are preferably used. The

As the heavy oil treatment, a demetallation treatment is preferably mentioned in addition to the hydrodesulfurization treatment. As processing temperature in these processes, it is preferable that it is 280-430 degreeC, and it is more preferable that it is 300-423 degreeC. Moreover, it is preferable that it is 3-18 Mpa as a pressure, and it is more preferable that it is 4-17 Mpa. Preferably the liquid hourly space velocity is from 0.1 to 6.5 (time ^-1), and more preferably 0.2 to 6.0 (time ^-1). The treatment time is preferably 7680 to 30720 hours, and more preferably 7680 to 7920 hours.

  After the heavy oil treatment as described above is performed, the used catalyst is extracted from the apparatus, and through the following steps (1) to (3), the desulfurization activity and desulfurization activity on the unused heavy oil treatment catalyst are sequentially performed. A regenerated catalyst for heavy oil treatment in which at least one of the metal activities is 50 to 70% is obtained.

Step (1):
Step (1) is a step of measuring the contents of vanadium and nickel with respect to an unused heavy oil processing catalyst before being used for processing heavy oil. The contents of vanadium and nickel can be determined by plasma (ICP) emission spectrometry.

Step (2):
In step (2), an unused heavy oil treatment catalyst is used for heavy oil treatment, and the amount of vanadium and nickel deposited on the used catalyst after treatment is determined by the amount of vanadium and nickel measured in step (1). A used catalyst that is 1 to 45% by mass (preferably 5 to 35% by mass) based on the content is selected.
What is necessary is just to measure the content of vanadium and nickel in a used catalyst with the measuring method of process (1).
If the deposition amount is less than 1% by mass, the desulfurization activity is too high and the calorific value is increased, which is not preferable. If it exceeds 45% by mass, metal may adhere to the catalyst pores and desulfurization activity may be reduced.

Step (3):
In the step (3), the used catalyst selected in the step (2) is subjected to the following drying treatment or solvent washing treatment so that the carbon adhesion amount is 1 to 26 mass%.

i) Drying treatment The drying method according to the drying treatment is not particularly limited. For example, the catalyst is transferred using a belt conveyor, and the moisture and oil adhering to the surface of the catalyst are removed by drying at a high temperature during the transfer. Is mentioned. A fixed drying furnace can also be used.

  The drying temperature is preferably 100 to 500 ° C, more preferably 180 to 450 ° C. The drying time is preferably 3 to 24 hours, more preferably 5 to 10 hours. The oxygen concentration during drying is preferably 1% by volume or less, and more preferably 0.8% by volume or less.

ii) Solvent cleaning treatment The method related to the solvent cleaning treatment is not particularly limited, but as an example, a used catalyst is placed in a container, and liquid circulation cleaning is performed using a cleaning liquid to dissolve and remove oil adhering to the surface of the catalyst. Then, the oil that could not be removed by solvent washing is removed by a drying process. Cleaning can also be performed by a batch cleaning method.

As the cleaning liquid, solvents such as naphtha, kerosene, light oil, toluene, and acetone can be used, and kerosene is particularly preferable. Moreover, it is preferable to carry out liquid circulation washing | cleaning using these. The washing time is preferably 1 to 10 hours, and more preferably 3 to 6 hours.
In the case of liquid circulation cleaning, the circulation rate is preferably 50 to 300 L / min, and more preferably 120 to 200 L / min.

  After the solvent washing treatment, drying at a drying temperature of 50 to 250 ° C is preferable, and drying at 150 to 200 ° C is more preferable. The drying time is preferably 3 to 24 hours, more preferably 5 to 10 hours.

The above-mentioned drying treatment or solvent washing treatment is performed to obtain a used catalyst having a carbon adhesion amount of 1 to 26% by mass (preferably 5 to 24% by mass). If the carbon adhesion amount is less than 1% by mass, the active metals on the catalyst may cause sintering, resulting in a decrease in activity. If it exceeds 26% by mass, coke remains on the catalyst pores, which may reduce the desulfurization activity.
The carbon adhesion amount can be measured by a high frequency induction heating combustion-infrared absorption method.

The spent catalyst obtained as described above has a desulfurization activity and / or a demetallization activity of 50 to 70%, preferably 55 to 60% with respect to an unused heavy oil treatment catalyst. . And this used catalyst is used as a recycled catalyst for heavy oil treatment.
If at least one of the desulfurization activity and the demetalization activity for the unused heavy oil treatment catalyst is less than 50%, the catalyst activity when used again for the heavy oil treatment becomes insufficient. If it exceeds 70%, the activity is too high, and the problem of abnormal heat generation occurs.

The hydrodesulfurization activity of the used catalyst can be determined by the formula “(sulfur content in raw material oil−sulfur content in product oil) / sulfur content in raw material oil”. Further, the demetalization activity can be determined by the formula “(metal content in raw material oil−metal content in product oil) / metal content in raw material oil”.
Moreover, it can be confirmed by a pilot test whether the used catalyst satisfies that at least one of the desulfurization activity and the demetalization activity with respect to the unused heavy oil treatment catalyst is 50 to 70%. .

The regenerated catalyst for heavy oil treatment has an average particle diameter of preferably 2.0 to 5.0 mm, and more preferably 2.8 to 4.5 mm, like the unused catalyst. Preferably the specific surface area is 50 to 300 m ² / g, more preferably 70~200m ² / g. The specific surface area can be measured by the BET method.
The crushing strength is preferably 0.6 to 2.0 kg / mm, and more preferably 1.0 to 1.5 kg / mm. Furthermore, the abrasion strength (10 mesh sieve or less) is preferably 0.1 to 3.0% by mass, and more preferably 0.1 to 2.0% by mass. The crushing strength can be measured by using a crushing strength measuring device.

[2. Usage of regenerated catalyst for heavy oil treatment]
The method of using the regenerated catalyst for heavy oil treatment of the present invention is a treatment of heavy oil by combining the regenerated catalyst for heavy oil treatment of the present invention and an unused heavy oil treatment catalyst. . The types and conditions of heavy oil treatment are as described above.

At this time, 10-50 mass% (preferably 10-30 mass%) of the heavy oil processing regenerated catalyst is separated from the unused heavy oil processing catalyst upstream in the reactor with respect to the total catalyst charge. Filling is preferred. That is, the ratio of the heavy oil processing regenerated catalyst to the total catalyst amount is set to 10 to 50% by mass, and the heavy oil processing regenerated catalyst and the unused heavy oil processing catalyst are charged separately. . Then, an unused heavy oil processing catalyst is charged in the upstream portion of the reactor, and the unused heavy oil processing catalyst is charged in the downstream portion of the reactor rather than the filled heavy oil processing regenerated catalyst.
By such a filling method, since a mild reaction first proceeds with a regenerated catalyst for treating heavy oil with relatively low activity, it is considered that abnormal heat generation can be suppressed.

  In general, the hydrotreating process uses a fixed bed reactor, but there is no problem even if it is a reaction type such as a moving bed or a boiling bed. Further, the flow of the reactant may be an upward flow or a downward flow. As described above, desulfurization treatment and demetallation treatment of heavy oil can be cited as preferable hydrogenation treatment.

  In addition, when using the regeneration catalyst for heavy oil processing as a support catalyst, the regenerated catalyst for heavy oil processing of a moderately low activity is filled into the bottom part of a reactor instead of an unused catalyst as a support. Here, a support catalyst is a role which prevents the catalyst filled using the ceramic ball etc. as an example from flowing out downstream from a reactor.

  EXAMPLES Hereinafter, although this invention is demonstrated in detail with reference to an Example, this invention is not limited by these Examples.

(Preparation of unused catalyst)
An unused catalyst was prepared by the following procedure.
70 g of sodium hydroxide was dissolved in 2 liters of pure water, and 200 g of sodium aluminate was further added to obtain a uniform alumina solution (1). In addition, 1,000 g of aluminum nitrate was dissolved in 2 liters of pure water to obtain an alumina solution (2). First, 4 liters of pure water was heated to 70 ° C., and the alumina solution (2) was added to pH 3.6 while stirring. Next, the alumina solution (1) was added until pH 9.0 and aged with stirring for 5 minutes. Subsequently, the alumina solution (2) was added again to adjust the pH to 3.6 and aged for 5 minutes with stirring. Thus, the operation of changing the pH between 3.6 and 9.0 was repeated 9 times in total to obtain a boehmite gel aqueous solution.
The boehmite gel was filtered, washed with deionized water, dried, and extruded into a circle having a diameter of 1.5 mm. The extruded boehmite gel was dried at 120 ° C. for 160 hours and then calcined at 550 ° C. for 2 hours to obtain an alumina carrier. Next, 69.5 g of nickel carbonate (39.7 g as NiO), 220 g of molybdenum trioxide, and 31.5 g of orthophosphoric acid (purity 85 mass%, 19.5 g as P ₂ O ₅ ) were added to 250 cm ³ of pure water. The mixture was dissolved at 80 ° C. with stirring, cooled to room temperature, pure water was added again, and the volume was adjusted to 250 cm ³ to prepare an impregnation solution. Take 50 cm ^{3 of the} impregnating solution, add 6 g of polyethylene glycol (molecular weight 400), dilute and constant volume with pure water to match the water absorption of 100 g of carrier, impregnate at normal pressure, and at 70 ° C. for 1 hour. After vacuum drying, heat treatment was performed at 450 ° C. for 16 hours to prepare a catalyst. The physical properties of the catalyst are shown below. The unused catalyst thus obtained contains 3.0% by mass as NiO and 13.2% by mass as MoO ₃ , has a pore volume of 0.83 ml / g and a specific surface area of 100 m ² / g. there were.

(Preparation of spent catalyst A)
First, hydrodesulfurization treatment was performed by reacting the unused catalyst under the following conditions.
Reaction conditions (1) Raw material properties:
Normal pressure residual oil containing 4.5% by mass of sulfur, 240% by mass of nitrogen, 10.2% by mass of residual carbon, 85% by mass of vanadium and nickel, 0.5% by mass of asphaltene (2) Working temperature (reaction Temperature): 360-410 ° C
(3) Pressure: 15 MPa
(4) Liquid space velocity: 0.22 (time- ¹ )
(5) Use time (reaction time): 7680 hours

After performing the hydrodesulfurization reaction as described above, the catalyst was extracted from the reaction apparatus to obtain a used catalyst A. The obtained spent catalyst A contained 8% by mass as NiO and 45% by mass as V ₂ O ₅ and contained carbon.

Example 1
The spent catalyst A was subjected to the drying treatment described in Table 1 below to prepare a heavy oil treatment regenerated catalyst.
The specific surface area of the recycled catalyst for heavy oil treatment was measured. The results are shown in Table 1 below.
In addition, the average particle diameter was measured with calipers, and the measured values at 100 points were averaged. The specific surface area was measured by the BET method using nitrogen gas as an adsorption species.

  Further, (a) the amount of vanadium and nickel deposited, (b) the amount of carbon adhesion, and (c) the desulfurization activity ratio (activity degree) of the regenerated catalyst for heavy oil treatment to the desulfurization activity of the unused catalyst is as follows: I asked for it. The results are shown in Table 1 below.

(A) Amount of vanadium and nickel deposited After ashing the recycled catalyst for heavy oil treatment, the ash is melted with an alkaline flux, dissolved with an acid, and then inductively coupled plasma (ICP) emission spectrometry (Agilent Technology Co., Ltd.) Manufactured by agilent 720), the vanadium content and the nickel content of the regenerated catalyst for heavy oil treatment were analyzed.

(B) Carbon adhesion amount The carbon content of the regenerated catalyst for heavy oil treatment was measured with a carbon analyzer (EMIA-920V2 manufactured by Horiba, Ltd.) using a high-frequency induction heating combustion-infrared absorption method.

(C) Degree of activity An unused catalyst and a recycled catalyst for treating heavy oil were charged in the same amount (by volume) in a pilot plant, and heavy oil was hydrodesulfurized under the above reaction conditions. The degree of activity was confirmed by calculation from the amount of sulfur in each inlet and outlet oil and the amount of vanadium and nickel.

The recycled catalyst for heavy oil treatment and the unused catalyst were separately charged into the hydrodesulfurization reactor at a mass ratio of 20:80. The recycled catalyst for heavy oil treatment was packed in the upstream portion of the reactor with respect to the unused catalyst. After filling, hydrodesulfurization reaction was performed, the reactor inlet and outlet temperatures were confirmed, and the presence or absence of abnormal heat generation was examined. The results are shown in Table 1 below.
The fluid passing through the reactor was the above-described normal pressure residual oil, and the reactor inlet temperature was substantially constant.

(Example 2)
Except for the drying treatment described in Table 1 below, a regenerated catalyst for heavy oil treatment was prepared in the same manner as in Example 1, and hydrodesulfurization reaction was carried out in the same manner as in Example 1, and the reactor inlet and outlet temperatures Was checked for the presence or absence of abnormal fever. The results are shown in Table 1 below.

Example 3
A regenerated catalyst for heavy oil treatment was prepared in the same manner as in Example 1 except that the drying treatment was changed to the washing treatment described in Table 1 below (liquid circulation washing using kerosene and drying at about 150 ° C.), The hydrodesulfurization reaction was performed in the same manner as in Example 1, the reactor inlet and outlet temperatures were confirmed, and the presence or absence of abnormal heat generation was examined. The results are shown in Table 1 below.

(Comparative Example 1)
Only the unused catalyst was charged into the reactor, and hydrodesulfurization reaction was performed in the same manner as in Example 1. The reactor inlet and outlet temperatures were confirmed, and the presence or absence of abnormal heat generation was examined. The results are shown in Table 1 below.
The total catalyst amount in Examples 1 to 3 and Comparative Example 1 is the same.

  It has been found that abnormal heat generation in the reactor can be suppressed by filling a hydrodesulfurization apparatus with a regenerated catalyst for treating heavy oil, which has a moderately low activity, in combination with an unused catalyst.

Claims (6)

A heavy oil processing regenerated catalyst that processes heavy oil in combination with an unused heavy oil processing catalyst,
The recycled catalyst for heavy oil treatment
(A) It is a used catalyst used for treating heavy oil, the unused heavy oil treatment catalyst,
(B) With respect to the unused heavy oil treatment catalyst, (a) the amount of vanadium and nickel deposited is 1 to 45% by mass, (b) the amount of carbon adhesion is 1 to 26% by mass, (c ) A regenerated catalyst for heavy oil treatment in which at least one of desulfurization activity and demetalization activity is 50 to 70%.   The regenerated catalyst for heavy oil treatment according to claim 1, wherein the average particle size is 2 to 5 mm. The regenerated catalyst for heavy oil treatment according to claim 1, wherein the specific surface area is 50 to 300 m ² / g. It is a manufacturing method of the regenerated catalyst for heavy oil processing of any one of Claims 1-3, Comprising: The following process (1)-(3) is included in order, It is with respect to the catalyst for unused heavy oil processing. A method for producing a regenerated catalyst for treating heavy oil, wherein a regenerated catalyst for treating heavy oil having at least one of desulfurization activity and demetalization activity of 50 to 70% is obtained.
Step (1): Step of measuring the content of vanadium and nickel with respect to an unused heavy oil treatment catalyst before being used for treatment of heavy oil Step (2): Treatment of the unused heavy oil The catalyst for heavy oil is used for heavy oil treatment, and the used catalyst after the treatment is selected to have a vanadium and nickel deposition amount of 1 to 45% by mass with respect to the measured vanadium and nickel content. Step (3) to perform: A step of subjecting the selected spent catalyst to a drying treatment or a solvent washing treatment to adjust the carbon adhesion amount to 1 to 26 mass%.   The regenerated catalyst for heavy oil processing which processes heavy oil combining the regenerated catalyst for heavy oil processing of any one of Claims 1-3, and the catalyst for unused heavy oil processing. How to use.   The heavy catalyst according to claim 5, wherein 10 to 50 mass% of the recycled catalyst for processing heavy oil is packed separately from the unused heavy oil processing catalyst in the upstream portion of the reactor with respect to the total amount of catalyst charged. How to use regenerated catalyst for treating oil.