CN109225244A - Wide temperature range denitrating catalyst of a kind of cerium oxide ferrozirconium composite titanium vanadium system and preparation method thereof - Google Patents

Wide temperature range denitrating catalyst of a kind of cerium oxide ferrozirconium composite titanium vanadium system and preparation method thereof Download PDF

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CN109225244A
CN109225244A CN201811187778.2A CN201811187778A CN109225244A CN 109225244 A CN109225244 A CN 109225244A CN 201811187778 A CN201811187778 A CN 201811187778A CN 109225244 A CN109225244 A CN 109225244A
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denitrating catalyst
cerium
preparation
oxide
zirconium
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刘瑾
王新翠
李�真
夏莉
王卓
吴东兴
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Anhui Jianzhu University
Anhui University of Architecture
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Anhui University of Architecture
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/847—Vanadium, niobium or tantalum or polonium
    • B01J23/8472—Vanadium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8625—Nitrogen oxides
    • B01D53/8628—Processes characterised by a specific catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/002—Mixed oxides other than spinels, e.g. perovskite
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • B01J37/082—Decomposition and pyrolysis
    • B01J37/088—Decomposition of a metal salt
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
    • B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
    • B01J37/343—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of ultrasonic wave energy
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2523/00—Constitutive chemical elements of heterogeneous catalysts

Abstract

The invention belongs to industrial denitration technology fields, and in particular to a kind of wide temperature range denitrating catalyst of cerium oxide ferrozirconium composite titanium vanadium system, the denitrating catalyst include the metal oxide of cerium, zirconium and iron；The invention further relates to the preparation method of above-mentioned denitrating catalyst, the steps include: a) to prepare metal composite oxide；B) support body material is prepared；C) denitrating catalyst is prepared.Compared with prior art, denitrating catalyst of the invention can not only keep catalytic activity under the high temperature conditions, and also show stronger catalytic activity in low-temperature space；Denitrating catalyst preparation process is simple, raw material is easy to get, input cost is low, and gained denitrating catalyst Applicable temperature range obtains very big expansion, lower to temperature requirement is used, and can satisfy the needs of more catalytic environments.

Description

Wide temperature range denitrating catalyst of a kind of cerium oxide ferrozirconium composite titanium vanadium system and preparation method thereof
Technical field
The invention belongs to industrial denitration technology fields, and in particular to a kind of wide temperature range denitration of cerium oxide ferrozirconium composite titanium vanadium system Catalyst and preparation method thereof.
Background technique
With the development of industry, environmental problem brought by industrial gas emission is gradually valued by people, and removes work Nitrogen oxides in industry exhaust gas, just at research hotspot in recent years.Wherein, nitric oxide is since it is insoluble in water-soluble reagent Characteristic, solution absorption method cannot generally remove it, therefore, increasingly to the research of the nitric oxide production catalyst of efficient removal It is more.
Most widely used denitrating catalyst is titanium vanadium series catalyst, such as V currently on the market2O5-WO3(MoO3)-TiO2.Though The catalytic activity of right this kind of catalyst is higher, but since its catalytic activity temperature window is higher, causes in low-temperature catalyzed denitration Application in field is restricted.Therefore, on the basis of maintaining titanium vanadium series catalyst high-temperature catalytic performance, raising is explored The method of its low-temperature catalyzed performance is the development trend in titanium vanadium series catalyst field.
Summary of the invention
The object of the present invention is to provide it is a kind of it is safe and reliable, be able to maintain high-temperature catalytic denitration activity and low-temperature catalyzed de- The nitre activity also high wide temperature range denitrating catalyst of cerium oxide ferrozirconium composite titanium vanadium system.
To achieve the above object, a kind of the technical solution adopted by the present invention are as follows: the wide temperature range of cerium oxide ferrozirconium composite titanium vanadium system Denitrating catalyst, the denitrating catalyst include the metal oxide of cerium, zirconium and iron.
Compared with prior art, denitrating catalyst of the invention can not only keep catalytic activity under the high temperature conditions, and Stronger catalytic activity is also shown in low-temperature space, Applicable temperature range obtains very big expansion, and it is lower to reaction condition requirement, it can To meet the needs of different catalytic applications.
Another object of the present invention is to provide a kind of wide temperature range denitrating catalysts of above-mentioned cerium oxide ferrozirconium composite titanium vanadium system Preparation method, preparation method is simple, safe and reliable, be not only able to maintain gained catalyst high-temperature catalytic denitration activity, but also Low-temperature catalyzed denitration activity can be greatly improved.
To achieve the above object, the technical scheme adopted by the invention is as follows: a kind of cerium oxide ferrozirconium as described above is compound The preparation method of the wide temperature range denitrating catalyst of titanium vanadium system, the specific steps are as follows:
A) it prepares metal composite oxide: taking the soluble-salt of three kinds of cerium, zirconium and iron metals, add deionized water stirring molten Solution, is slow added into sodium hydroxide, persistently stirs 0.5~4h, calcines to obtain cerium zirconium iron metal composite oxide after dry；
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing；
C) prepare denitrating catalyst: by support body material, ultrasonic disperse is handled in dehydrated alcohol, obtains suspension, then by cerium Ferrozirconium metal composite oxide is added in suspension, is dried after ultrasonic disperse, obtains cerium zirconium iron metal composite oxide denitration Catalyst.
Compared with prior art, the preparation method of denitrating catalyst of the invention, simple process, raw material be easy to get, put at This is low, and gained denitrating catalyst Applicable temperature range obtains very big expansion, lower to temperature requirement is used, and can satisfy and more urges Change the needs of environment.
Preferably, the soluble-salt of three kinds of metals is six nitric hydrate ceriums, eight hydrations respectively in the step a) Basic zirconium chloride and ferric chloride hexahydrate, wherein the molar ratio of six nitric hydrate ceriums and chlorine hydrate zirconium oxide is 5~15:1.It is mixed It closes and starts to generate precipitating after sodium hydroxide is added in liquid, the precipitating generated in mixed liquor is handled after stirring 1~3h.
Specifically, mixed liquor stands and removes supernatant liquor, successively washs 2~3 times with deionized water and dehydrated alcohol, often Carry out suction filtration processing after secondary washing, products therefrom dry 8 at 100~130 DEG C~for 24 hours, then through calcining, cooling, milled processed Cerium zirconium iron metal composite oxide is obtained afterwards.The condition of calcining is: in air atmosphere, the product after drying being put into tube furnace In, after rising to 200~500 DEG C with the heating rate of 5~20 DEG C/min, calcine 2~5h.
Further preferably, in the step c), cerium zirconium iron metal composite oxide additional amount is support body material quality 0.5~5%；Drying process be dry 8 under the conditions of 100~130 DEG C~for 24 hours.
The denitrating catalyst prepared using method disclosed by the invention, simple process and environmental protection, time is short, process conditions are held Denitrating catalyst easy to control, being prepared, is able to maintain catalytic activity under the high temperature conditions, and low-temperature space also show compared with Strong catalytic activity, Applicable temperature range obtain very big expansion, lower to use condition requirement, can satisfy different catalytic applications Needs.Test result shows catalyst that the present invention synthesizes under low temperature window, and denitration efficiency reaches as high as 100%, shows Show the catalytic performance of good low-temperature denitration.
Detailed description of the invention
Fig. 1 is the X-ray diffractogram of metal composite oxide obtained by Examples 1 to 5；
Fig. 2 is catalysis effect of the catalyst and blank support body material obtained by Examples 1 to 5 under the conditions of 90~250 DEG C Rate curve；
Fig. 3 is catalytic efficiency curve of the catalyst obtained by Examples 1 to 5 under the conditions of 270~460 DEG C.
Specific embodiment
Technical solution of the present invention is described in further detail with reference to the accompanying drawing.
Embodiment 1: cerium oxide and zirconium oxide compound composite titanium vanadium system denitrating catalyst is prepared
A) it prepares metal composite oxide: weighing six nitric hydrate cerium of 3.8331g respectively and 0.3271g eight is hydrated oxychlorination Zirconium adds to stirring and dissolving in deionized water, is slowly added to NaOH to precipitating completely, is further continued for after stirring 2h, and mixed solution is quiet It sets half an hour, supernatant liquor is sucked out, is successively washed 2~3 times with deionized water and dehydrated alcohol, is carried out at suction filtration each time after washing Reason, at 110 DEG C after dry 12h, place the product in tube furnace, in air atmosphere with 500 DEG C of calcining 3h, heating rate is 4 DEG C/min, after being cooled to room temperature, grind into powder is to get cerium zirconium metal composite oxide.
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing.
C) it prepares catalyst: support body material being taken to be added to absolute ethanol, ultrasonic disperse 1h obtains suspension, then takes the quality to be The cerium zirconium metal composite oxide of support body material 2% adds in suspension, and mixed liquor is then placed in by ultrasonic disperse 30min Dry 12h is at 110 DEG C to get denitrating catalyst.
Embodiment 2: cerium oxide ferrozirconium composite titanium vanadium system denitrating catalyst is prepared
A) it prepares metal composite oxide: weighing six nitric hydrate cerium of 3.9130g respectively, 0.3223g eight is hydrated oxychlorination Zirconium and 0.1613g ferric chloride hexahydrate, add to stirring and dissolving in deionized water, are slowly added to NaOH extremely precipitating completely, followed by After continuous stirring 2h, mixed solution is stood into half an hour, supernatant liquor is removed, successively washs 2~3 with deionized water and dehydrated alcohol It is secondary, suction filtration processing is carried out each time after washing, at 110 DEG C after dry 12h, place the product in tube furnace, in air atmosphere With 500 DEG C of calcining 3h, heating rate is 4 DEG C/min, and after being cooled to room temperature, grind into powder is to get cerium zirconium iron composition metal oxygen Compound.
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing.
C) it prepares denitrating catalyst: support body material being taken to be added to absolute ethanol, ultrasonic disperse 1h obtains suspension, then takes matter Amount is that the cerium zirconium iron metal composite oxide of support body material 2% adds in suspension, and ultrasonic disperse 30min then will mixing Liquid is placed at 110 DEG C dry 12h to get denitrating catalyst.
Embodiment 3: cerium oxide ferrozirconium composite titanium vanadium system denitrating catalyst is prepared
A) it prepares metal composite oxide: weighing six nitric hydrate cerium of 3.1912g respectively, 0.3281g eight is hydrated oxychlorination Zirconium and 0.8157g ferric chloride hexahydrate, add to stirring and dissolving in deionized water, are slowly added to NaOH extremely precipitating completely, followed by After continuous stirring 2h, mixed solution is stood into half an hour, supernatant liquor is removed, successively washs 2~3 with deionized water and dehydrated alcohol It is secondary, suction filtration processing is carried out each time after washing, at 110 DEG C after dry 12h, place the product in tube furnace, in air atmosphere With 500 DEG C of calcining 3h, heating rate is 4 DEG C/min, and after being cooled to room temperature, grind into powder is to get cerium zirconium iron composition metal oxygen Compound.
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing.
C) it prepares denitrating catalyst: support body material being taken to be added to absolute ethanol, ultrasonic disperse 1h obtains suspension, then takes matter Amount is that the cerium zirconium iron metal composite oxide of support body material 2% adds in suspension, and ultrasonic disperse 30min then will mixing Liquid is placed at 110 DEG C dry 12h to get denitrating catalyst.
Embodiment 4: cerium oxide ferrozirconium composite titanium vanadium system denitrating catalyst is prepared
A) it prepares metal composite oxide: weighing six nitric hydrate cerium of 3.9073g respectively, 0.3283g eight is hydrated oxychlorination Zirconium and 1.4528g ferric chloride hexahydrate, add to stirring and dissolving in deionized water, are slowly added to NaOH extremely precipitating completely, followed by After continuous stirring 2h, mixed solution is stood into half an hour, supernatant liquor is removed, successively washs 2~3 with deionized water and dehydrated alcohol It is secondary, suction filtration processing is carried out each time after washing, at 110 DEG C after dry 12h, place the product in tube furnace, in air atmosphere With 500 DEG C of calcining 3h, heating rate is 4 DEG C/min, and after being cooled to room temperature, grind into powder is to get cerium zirconium iron composition metal oxygen Compound.
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing.
C) it prepares denitrating catalyst: support body material being taken to be added to absolute ethanol, ultrasonic disperse 1h obtains suspension, then takes matter Amount is that the cerium zirconium iron metal composite oxide of support body material 2% adds in suspension, and ultrasonic disperse 30min then will mixing Liquid is placed at 110 DEG C dry 12h to get denitrating catalyst.
Embodiment 5: cerium oxide ferrozirconium composite titanium vanadium system denitrating catalyst is prepared
A) it prepares metal composite oxide: weighing six nitric hydrate cerium of 3.9120g respectively, 0.3221g eight is hydrated oxychlorination Zirconium and 2.3139g ferric chloride hexahydrate, add to stirring and dissolving in deionized water, are slowly added to NaOH extremely precipitating completely, followed by After continuous stirring 2h, mixed solution is stood into half an hour, supernatant liquor is removed, successively washs 2~3 with deionized water and dehydrated alcohol It is secondary, suction filtration processing is carried out each time after washing, at 110 DEG C after dry 12h, place the product in tube furnace, in air atmosphere With 500 DEG C of calcining 3h, heating rate is 4 DEG C/min, and after being cooled to room temperature, grind into powder is to get cerium zirconium iron composition metal oxygen Compound.
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass Fiber, and stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, product obtains support body material after drying, calcination processing.
C) it prepares denitrating catalyst: support body material being taken to be added to absolute ethanol, ultrasonic disperse 1h obtains suspension, then takes matter Amount is that the cerium zirconium iron metal composite oxide of support body material 2% adds in suspension, and ultrasonic disperse 30min then will mixing Liquid is placed at 110 DEG C dry 12h to get denitrating catalyst.
The test of embodiment 6:X ray diffraction data
Metal composite oxide obtained in Examples 1 to 5 is subjected to X-ray diffraction characterization, it is specific as shown in Figure 1.Figure Middle eg.1~eg.5 respectively corresponds metal composite oxide obtained in Examples 1 to 5.
Embodiment 7: denitration activity test
The resulting denitrating catalyst of Example 1~5 is placed in tubular type SCR reactor respectively, is simulated in mixed gas, NO, NH3And O2/ Ar flow velocity is 90mL/min, and the flow velocity of pure argon is 30mL/min, and the temperature range of test is 90~250 DEG C, while being compared using support body material as blank test and Examples 1 to 5.The concentration of reactor outlet gas by The detection of POT400-NOX portable detector, specific denitration efficiency are as shown in Figure 2.Eg.1~eg.5 respectively corresponds implementation in figure Denitrating catalyst obtained in example 1~5, supporter indicate blank test, i.e. support body material.
After the temperature range of above-mentioned test method is is changed to 270~450 DEG C by Fig. 3, catalyst obtained by Examples 1 to 5 Denitration efficiency, the same Fig. 2 of mask method.
As shown in Figure 1, the diffraction maximum of embodiment 3 is most weak, illustrates that its crystallinity is worst, can be with thus in catalytic process More active sites are provided, the progress of catalysis reaction is conducive to.In conjunction with the denitration efficiency under Fig. 2 and Fig. 3 condition of different temperatures Curve is it is found that the temperature window width of efficient catalytic is related with the ingredient proportion of three kinds of metal soluble-salts, Fe in mixed solution3 +:(Zr4++Ce3+) mass values close to 0.5 when, the catalytic efficiency of catalyst is stronger, it might even be possible to denitration under cryogenic Efficiency is up to 100%, and hot conditions are still able to maintain 90% or more denitration efficiency.

Claims (8)

1. a kind of wide temperature range denitrating catalyst of cerium oxide ferrozirconium composite titanium vanadium system, it is characterised in that: the denitrating catalyst includes The metal oxide of cerium, zirconium and iron.
2. a kind of preparation method of the wide temperature range denitrating catalyst of cerium oxide ferrozirconium composite titanium vanadium as described in claim 1 system, tool Steps are as follows for body:
A) it prepares metal composite oxide: taking the soluble-salt of three kinds of cerium, zirconium and iron metals, add deionized water stirring and dissolving, then Sodium hydroxide is slowly added to precipitating completely, 0.5~4h is persistently stirred, calcines to obtain cerium zirconium iron metal composite oxide after dry；
B) it prepares support body material: taking Detitanium-ore-type TiO2, ammonium hydroxide, stearic acid, SiO2、WO3, ammonium metavanadate and glass fibre, And stirred evenly in kneading machine, polyoxyethylene and carboxymethyl cellulose are added, continues to stir, until water content is less than 27%, Product obtains support body material after drying, calcination processing；
C) prepare denitrating catalyst: by support body material, ultrasonic disperse is handled in dehydrated alcohol, obtains suspension, then by cerium zirconium iron Metal composite oxide is added in suspension, is dried after ultrasonic disperse, obtains cerium zirconium iron metal composite oxide denitration catalyst Agent.
3. the preparation method of denitrating catalyst according to claim 2, it is characterised in that: three kinds of metals in the step a) Soluble-salt be respectively six nitric hydrate ceriums, chlorine hydrate zirconium oxide and ferric chloride hexahydrate.
4. the preparation method of denitrating catalyst according to claim 2 or 3, it is characterised in that: in the step a), six water The molar ratio for closing cerous nitrate and chlorine hydrate zirconium oxide is 5~15:1.
5. the preparation method of denitrating catalyst according to claim 2, it is characterised in that: in the step a), mixed liquor Supernatant liquor is stood and is removed, is successively washed 2~3 times with deionized water and dehydrated alcohol, carries out suction filtration processing each time after washing, Products therefrom dry 8 at 100~130 DEG C~for 24 hours, then after calcining, cooling, milled processed the oxidation of cerium zirconium iron composition metal Object.
6. the preparation method of denitrating catalyst according to claim 5, it is characterised in that: in the step a), calcining Condition is: in air atmosphere, the product after drying being put into tube furnace, rises to 200 with the heating rate of 5~20 DEG C/min After~500 DEG C, 2~5h is calcined.
7. the preparation method of denitrating catalyst according to claim 2, it is characterised in that: in the step c), cerium zirconium iron Metal composite oxide additional amount is the 0.5~5% of support body material quality.
8. the preparation method of denitrating catalyst according to claim 2, it is characterised in that: in the step c), at drying Reason be dry 8 under the conditions of 100~130 DEG C~for 24 hours.
CN201811187778.2A 2018-10-12 2018-10-12 Wide temperature range denitrating catalyst of a kind of cerium oxide ferrozirconium composite titanium vanadium system and preparation method thereof Pending CN109225244A (en)

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