CN104017620A - Process method for co-production of liquid ammonia and liquefied natural gas by using carbonized furnace gas - Google Patents

Process method for co-production of liquid ammonia and liquefied natural gas by using carbonized furnace gas Download PDF

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CN104017620A
CN104017620A CN201410212201.8A CN201410212201A CN104017620A CN 104017620 A CN104017620 A CN 104017620A CN 201410212201 A CN201410212201 A CN 201410212201A CN 104017620 A CN104017620 A CN 104017620A
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gas
furnace gas
charing furnace
ammonia
production
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CN201410212201.8A
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CN104017620B (en
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董永波
王新明
高航
郭海洋
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榆林科大高新能源研究院有限公司
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Abstract

The invention relates to a process method for co-production of a liquid ammonia and liquefied natural gas by using a carbonized furnace gas. At present, utilization of the carbonized furnace gas is not enough in enterprises, thereby causing harm to the environment and violating environment-friendly meanings of energy conservation and emission reduction. The process method comprises the steps of subjecting the carbonized furnace gas to filtration, compression and deoxidation so as to separate nitrogen from the carbonized furnace gas; synthesizing ammonia in an ammonia converter after being pressurized with hydrogen and furture obtaining the liquid ammonia; then regulating a volume ratio of hydrogen to carbon monoxide by adopting a wide temperature and sulfur-resistant transformation process; converting organic sulfur into hydrogen sulfide; then carrying out desulfuration and decarbonization treatment; carrying out a multi-stage methanation reaction to obtain a gas mixture with methane as a main component; removing water and carbon dioxide by using molecular sieve; and liquefying to obtain methane with a purity of higher than 99.5%. The process method prepares the liquefied natural gas by using carbon monoxide and hydrogen in the carbonized furnace gas and co-produces liquid ammonia by using nitrogen in the carbonized furnace gas, so that useful components in the carbonized furnace gas of enterprises can be utilized reasonably.

Description

The processing method of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas

Technical field

the invention belongs to Sweet natural gas production technical field, be specifically related to the processing method of a kind of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas.

Background technology

Charing furnace gas is that to utilize high-quality jurassic period non-caking coal and weakly caking coal be raw material, in charring furnace, by destructive distillation, produces the hydrocarbon gas that is rich in producing in blue charcoal process.While utilizing charring furnace destructive distillation to produce blue charcoal, 1 ton of blue charcoal of every production remove charring furnace reuse and blue charcoal dry outside, can obtain 400-500Nm 3charring furnace gas, this gas heating value is 7500kJ/ Nm 3.End the whole nation in 2013 and produce altogether 7,000 ten thousand tons of left and right of blue charcoal, wherein 4,000 ten thousand tons, Shaanxi, 2,000 ten thousand tons, Xinjiang, the Inner Mongol and Ningxia are 1,000 ten thousand tons, and charing furnace gas can supply 280-350 hundred million Nm outward 3.Enterprise is abundant not for the utilization of charing furnace gas at present, not only environment is worked the mischief, and has run counter to the relevant policies that national energy-saving reduces discharging, and has affected the development of whole industry simultaneously.

In charing furnace gas, each component content scope is as following table:

In this gas, also contain the impurity such as coal tar, dust granules, sulfide and moisture simultaneously.Its medium sulphide content comprises hydrogen sulfide, sulfurous gas, sulphur carbonoxide, thiomethyl alcohol, thiophene etc.

The Jin You small part enterprise that utilizes for charing furnace gas passes through the approach such as scoria lime stone, smelting magnesium and generating at present, and most of enterprise does not recycle, and has the problems such as and environmental pollution low to charing furnace gas utilization ratio.From charing composition of fumes, in this gas, contain more valuable, available composition as N 2, CO, H 2, by charing furnace gas being produced to the processing method of natural gas liquids coproduction liquefied ammonia, be not only conducive to environment protection, improve energy-saving and emission-reduction, simultaneously can enterprise added value of product, bring considerable benefit.

Summary of the invention

The processing method that the object of this invention is to provide a kind of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas, can effectively solve enterprise to the low technical problem of charing furnace gas utilization ratio by this processing method, improves the value added of product.

The technical solution adopted in the present invention is:

The processing method of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas, is characterized in that:

By following steps, realized:

Step 1: filter:

Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;

Step 2: compression:

Adopt reciprocation compressor or radial compressor, charring furnace air pressure is reduced to 0.01-5.0Mpa;

Step 3: deoxidation:

Utilize dehydrogenation catalyst, it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction;

Step 4: nitrogen separation:

Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%;

Step 5: wide temperature sulfur-resisting transformation:

Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are (3.2-3.5): 1, and make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously;

Step 6: desulfurization and decarburization:

The method that adopts N methyldiethanol amine, Polyethylene glycol dimethyl ether or methyl alcohol to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction;

Step 7: methanation:

Utilize nickel-base catalyst, adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic employing of methane is multistage passes through methanation process or band circulation adiabatic methanation process without circulation primary, controlling methanation reaction temperature and be 250-700 ℃, pressure is 1-10Mpa, reaction heat is for the production of steam, for step 5;

Step 8: separation:

Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm;

Step 9: liquefaction:

Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy;

Step 10: liquefied ammonia is synthetic:

Inputting hydrogen in step 4 gained nitrogen, the compressed 20-30Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.

In step 1, load coke or gac in strainer, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.

In step 3, dehydrogenation catalyst is selected from Fe/Al 2o 3, Fe-Mo/Al 2o 3, Co-Mo/Al 2o 3.

In step 7, nickel-base catalyst is selected from Ni/Al 2o 3, Ni/Al 2o 3-MgO.

The present invention has the following advantages:

By the processing method of a kind of charing furnace gas preparing liquefied natural gas coproduction liquefied ammonia provided by the invention, can make the useful component in enterprise's charing furnace gas rationally be utilized, carbon monoxide and hydrogen are synthesized and are formed natural gas liquids by methanation, and nitrogen is produced for the synthesis of ammonia.The situation that can effectively slow down China's many ground natural gas supply deficiency after enforcement improves enterprise to charing furnace gas utilization ratio simultaneously, realizes energy-saving and emission-reduction, enriched product industrial chain, promote enterprise product added value, increased business economic, realized enterprise's cleaner production.

Embodiment

Below in conjunction with embodiment, the present invention will be described in detail.

The processing method of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas involved in the present invention, the regional high-quality jurassic period non-caking coals such as Shi Yi China Factory, Shenmu, Shanxi, Fugu and Changji, Hami and the Inner Mongol, Ningxia and the weakly caking coal that utilize are raw material, in charring furnace, by destructive distillation, produce the hydrocarbon charing furnace gas that is rich in producing in blue charcoal process, generally before production technique is implemented, need raw material charing furnace gas to carry out Components identification.In charing furnace gas, each component content scope is as following table:

In this gas, also contain the impurity such as coal tar, dust granules, sulfide and moisture simultaneously.Its medium sulphide content comprises hydrogen sulfide, sulfurous gas, sulphur carbonoxide, thiomethyl alcohol, thiophene etc.

Specifically by following steps, realized:

Step 1: filter:

Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;

In strainer, load coke or gac, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.

Step 2: compression:

Adopt reciprocation compressor or radial compressor, charring furnace air pressure is reduced to 0.01-5.0Mpa.

Step 3: deoxidation:

Utilize dehydrogenation catalyst (to be selected from Fe/Al 2o 3, Fe-Mo/Al 2o 3, Co-Mo/Al 2o 3, all with Al 2o 3for carrier), it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction.

Step 4: nitrogen separation:

Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%.

Step 5: wide temperature sulfur-resisting transformation:

Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are (3.2-3.5): 1, and make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously.

Step 6: desulfurization and decarburization:

The method that adopts N methyldiethanol amine, Polyethylene glycol dimethyl ether or methyl alcohol to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction.

Step 7: methanation:

Utilize nickel-base catalyst (to be selected from Ni/Al 2o 3, Ni/Al 2o 3-MgO, the former is with Al 2o 3for carrier, the latter is with Al 2o 3-MgO is carrier), adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic employing of methane is multistage passes through methanation process or band circulation adiabatic methanation process without circulation primary, controlling methanation reaction temperature and be 250-700 ℃, pressure is 1-10Mpa, reaction heat is for the production of steam, for step 5.

Step 8: separation:

Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm.

Step 9: liquefaction:

Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy.

Step 10: liquefied ammonia is synthetic:

Inputting hydrogen in step 4 gained nitrogen, the compressed 20-30Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.

Embodiment 1:

The raw material charing furnace gas chief component of the present embodiment specifically sees the following form: (tolerance 40000Nm 3/ h, 40 ℃ of temperature)

In gas, also contain the impurity such as coal tar, dust granules, sulfide and moisture simultaneously.Its medium sulphide content comprises hydrogen sulfide, sulfurous gas, sulphur carbonoxide, thiomethyl alcohol, thiophene etc.

Step 1: filter:

Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;

In strainer, load coke, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.

Step 2: compression:

Adopt reciprocation compressor, charring furnace air pressure is reduced to 0.01Mpa.

Step 3: deoxidation:

Utilize dehydrogenation catalyst (Fe/Al 2o 3, with Al 2o 3for carrier), it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction.

Step 4: nitrogen separation:

Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%.

Step 5: wide temperature sulfur-resisting transformation:

Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are 3.2:1, make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously.

Step 6: desulfurization and decarburization:

The method that adopts N methyldiethanol amine to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction.

Step 7: methanation:

Utilize nickel-base catalyst (Ni/Al 2o 3, with Al 2o 3for carrier), adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic employing of methane is multistage passes through methanation process without circulation primary, controlling methanation reaction temperature and be 250 ℃, pressure is 1Mpa, and reaction heat is for the production of steam, for step 5.

Step 8: separation:

Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm.

Step 9: liquefaction:

Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy.Can obtain 5.854 tons/h of natural gas liquids.

Step 10: liquefied ammonia is synthetic:

Inputting hydrogen in step 4 gained nitrogen, the compressed 20Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.Can produce 25.728 tons/h of liquefied ammonia.

Embodiment 2:

The raw material charing furnace gas chief component of the present embodiment specifically sees the following form: (tolerance 40000Nm 3/ h, 40 ℃ of temperature)

In gas, also contain the impurity such as coal tar, dust granules, sulfide and moisture simultaneously.Its medium sulphide content comprises hydrogen sulfide, sulfurous gas, sulphur carbonoxide, thiomethyl alcohol, thiophene etc.

Step 1: filter:

Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;

In strainer, load coke, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.

Step 2: compression:

Adopt reciprocation compressor, charring furnace air pressure is reduced to 2.5Mpa.

Step 3: deoxidation:

Utilize dehydrogenation catalyst (Fe-Mo/Al 2o 3, with Al 2o 3for carrier), it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction.

Step 4: nitrogen separation:

Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%.

Step 5: wide temperature sulfur-resisting transformation:

Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are 3.3:1, make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously.

Step 6: desulfurization and decarburization:

The method that adopts Polyethylene glycol dimethyl ether to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction.

Step 7: methanation:

Utilize nickel-base catalyst (Ni/Al 2o 3, with Al 2o 3for carrier), adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic employing of methane is multistage passes through methanation process without circulation primary, controlling methanation reaction temperature and be 500 ℃, pressure is 5Mpa, and reaction heat is for the production of steam, for step 5.

Step 8: separation:

Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm.

Step 9: liquefaction:

Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy.Can obtain 7.29 tons/h of natural gas liquids.

Step 10: liquefied ammonia is synthetic:

Inputting hydrogen in step 4 gained nitrogen, the compressed 25Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.Can produce 12.328 tons/h of liquefied ammonia.

Embodiment 3:

The raw material charing furnace gas chief component of the present embodiment specifically sees the following form: (tolerance 40000Nm 3/ h, 40 ℃ of temperature)

In gas, also contain the impurity such as coal tar, dust granules, sulfide and moisture simultaneously.Its medium sulphide content comprises hydrogen sulfide, sulfurous gas, sulphur carbonoxide, thiomethyl alcohol, thiophene etc.

Step 1: filter:

Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;

In strainer, load gac, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.

Step 2: compression:

Adopt radial compressor, charring furnace air pressure is reduced to 5.0Mpa.

Step 3: deoxidation:

Utilize dehydrogenation catalyst (Co-Mo/Al 2o 3, with Al 2o 3for carrier), it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction.

Step 4: nitrogen separation:

Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%.

Step 5: wide temperature sulfur-resisting transformation:

Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are 3.5:1, make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously.

Step 6: desulfurization and decarburization:

The method that adopts methyl alcohol to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction.

Step 7: methanation:

Utilize nickel-base catalyst (Ni/Al 2o 3-MgO, with Al 2o 3-MgO is carrier), adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic band circulation adiabatic methanation process that adopts of methane, controlling methanation reaction temperature and be 700 ℃, pressure is 10Mpa, and reaction heat is for the production of steam, for step 5.

Step 8: separation:

Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm.

Step 9: liquefaction:

Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy.Can obtain 3.268 tons/h of natural gas liquids.

Step 10: liquefied ammonia is synthetic:

Inputting hydrogen in step 4 gained nitrogen, the compressed 30Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.Can produce 18.76 tons/h of liquefied ammonia.

It is cited that content of the present invention is not limited to embodiment, and the conversion of any equivalence that those of ordinary skills take technical solution of the present invention by reading specification sheets of the present invention, is claim of the present invention and contains.

Claims (4)

1. the processing method of charing furnace gas liquefied ammonia co-production of liquefied processed Sweet natural gas, is characterized in that:
By following steps, realized:
Step 1: filter:
Charing furnace gas, by strainer, is removed to the non-pneumatic impurity in gas, rough purification charing furnace gas;
Step 2: compression:
Adopt reciprocation compressor or radial compressor, charring furnace air pressure is reduced to 0.01-5.0Mpa;
Step 3: deoxidation:
Utilize dehydrogenation catalyst, it is 0.5% that the amount of oxygen in charing furnace gas is reduced to volume fraction;
Step 4: nitrogen separation:
Adopt vacuum pressure varying adsorption technology to isolate the nitrogen in charing furnace gas, making nitrogen amount in charing furnace gas be reduced to volume fraction is 1%;
Step 5: wide temperature sulfur-resisting transformation:
Add water vapour, adopt wide temperature sulfur resistant conversion process, the hydrogen in adjusting charing furnace gas and the volume ratio of carbon monoxide are (3.2-3.5): 1, and make the organosulfur in charing furnace gas be transformed into hydrogen sulfide simultaneously;
Step 6: desulfurization and decarburization:
The method that adopts N methyldiethanol amine, Polyethylene glycol dimethyl ether or methyl alcohol to wash, makes the sour gas scale of construction in charing furnace gas be down to 0.1ppm, and it is 0.3% that carbonic acid gas is down to volume fraction;
Step 7: methanation:
Utilize nickel-base catalyst, adopt multistage methanation reaction, obtain take methane as main gaseous mixture, the synthetic employing of methane is multistage passes through methanation process or band circulation adiabatic methanation process without circulation primary, controlling methanation reaction temperature and be 250-700 ℃, pressure is 1-10Mpa, reaction heat is for the production of steam, for step 5;
Step 8: separation:
Use molecular sieve to remove to take moisture and the carbonic acid gas of methane in main gaseous mixture, amount of moisture is down to lppm, and amount of carbon dioxide is down to 50ppm;
Step 9: liquefaction:
Adopt azeotrope cryogenic liquefying technology to obtain being greater than the methane of 99. 5% purity, after re-heat, send into liquefying plant and liquefy;
Step 10: liquefied ammonia is synthetic:
Inputting hydrogen in step 4 gained nitrogen, the compressed 20-30Mpa that is pressurized to catalyzes and synthesizes ammonia in ammonia synthesis converter, and through water-cooled, ammonia is cold is cooled to-15 ℃, isolates liquefied ammonia wherein, unreacted gas returns to ammonia synthesis converter cyclic production.
2. the processing method of charing furnace gas according to claim 1 liquefied ammonia co-production of liquefied processed Sweet natural gas, is characterized in that:
In step 1, load coke or gac in strainer, filter outlet is installed wire cloth, and separated space is left in bottom, and air-flow is outflow filter from bottom to top.
3. the processing method of charing furnace gas according to claim 2 liquefied ammonia co-production of liquefied processed Sweet natural gas, is characterized in that:
In step 3, dehydrogenation catalyst is selected from Fe/Al 2o 3, Fe-Mo/Al 2o 3, Co-Mo/Al 2o 3.
4. the processing method of charing furnace gas according to claim 3 liquefied ammonia co-production of liquefied processed Sweet natural gas, is characterized in that:
In step 7, nickel-base catalyst is selected from Ni/Al 2o 3, Ni/Al 2o 3-MgO.
CN201410212201.8A 2014-05-20 2014-05-20 The processing method of charing furnace gas liquefied ammonia co-production of liquefied Sweet natural gas CN104017620B (en)

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