CN103865564B - The integrated approach of a kind of methyl alcohol or DME synthesis gasoline - Google Patents
The integrated approach of a kind of methyl alcohol or DME synthesis gasoline Download PDFInfo
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- CN103865564B CN103865564B CN201410062786.XA CN201410062786A CN103865564B CN 103865564 B CN103865564 B CN 103865564B CN 201410062786 A CN201410062786 A CN 201410062786A CN 103865564 B CN103865564 B CN 103865564B
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Abstract
The present invention is the integrated approach of a kind of methyl alcohol or DME synthesis gasoline.Be characterised in that: methyl alcohol or dme generate the hydro carbons being rich in gasoline component after synthesis reactor, obtain C through flash tank, knockout drum, separation column after being separated
1 ~ 2hydro carbons, C
3 ~ 4hydro carbons, petroleum naphtha component, heavy gasoline components and water, wherein petroleum naphtha component is arranged outward as product, and water enters sewage treatment unit, C
1 ~ 2hydro carbons returns synthesis reactor after compressor supercharging, C
3 ~ 4hydro carbons is after aromizing again, and product directly mixes with heavy gasoline components and enters transalkylation reactor as raw material, and reaction product returns flashing tower, a small amount of C
1 ~ 2discharge as by product with heavy gasoline components.Present invention process flow process is simple, and system energy consumption is low, and with charging refined methanol for benchmark, yield of gasoline reaches 36 ~ 40%, and with charging dme for benchmark, yield of gasoline reaches 50 ~ 54%.
Description
Technical field
The invention belongs to methyl alcohol or dme deep process technology field, what be specifically related to is the integrated approach of a kind of methyl alcohol or DME synthesis gasoline.
Background technology
Methyl alcohol or DME synthesis gasoline technology develop on the basis that the methyl alcohol of Mobil company exploitation is converted into aromatic hydrocarbons on ZSM-5 molecular sieve, the gasoline synthesized by this technology is without sulphur, without nitrogen, olefin(e) centent is low, can use as high-quality gasoline blend component, this technology is for significant China.
In recent years, under the drive of coal liquifaction correlative study, domestic coal-based methanol plant investment temperature rises steadily, so that methyl alcohol production capacity increases year by year, and by the end of the end of the year 2012, domestic methyl alcohol production capacity will amount to and reached 5,200 ten thousand tons.But methyl alcohol conventional downstream development of chemical industry is slow, causes methyl alcohol production capacity of leaving unused constantly to rise, ended for the end of the year 2012, methyl alcohol leaves unused nearly 2,100 ten thousand tons/year of production capacity, and industry working rate is only 60%; On the other hand, due to the restriction of national policy, dme market is since two thousand eight always at a low ebb.Therefore, the deep process technology developing methyl alcohol or dme is extremely urgent.
According to statistics, domestic operation, to amount in the methyl alcohol built or DME synthesis gasoline apparatus production capacity and be about 2,000,000 tons/year, but, while this technology synthetic gasoline, a certain amount of liquefied gas of meeting by-product and the heavy aromatics being rich in durol, have a strong impact on the economic benefit of enterprise.
US3931349 discloses a kind of two-stage method technique of methanol synthesized gasoline, wherein first paragraph is dimethyl ether by methanol dehydration, the mixture of first paragraph methyl alcohol out, dme and water enters second segment reactor, generates liquefied gas and gasoline under ZSM-5 molecular sieve catalyst action.This technological line is the preparing gasoline by methanol technique of the classics developed by Mobil company, Mobil company is in order to promote the economic benefit of yield of gasoline and technique subsequently, a series of improving technique is proposed again, such as propose synthetic oil reactor in parallel in US4404414, and by being used for controlling the circulation gas of temperature of reaction successively by each reactor, to reduce the energy consumption of circulation gas; Propose the durol cyclically utilizing of by-product in US4035430, with the growing amount of durol in the reaction process reducing synthetic gasoline, promote the selectivity of gasoline; Propose to adopt fluidized-bed reactor, to promote the selectivity of object product in US4423274; Propose in US4665249 first by the dme separating-purifying in first paragraph dehydration reactor product, and then enter synthetic oil reactor, to promote stability and the yield of gasoline of catalyzer.
CN1923366A discloses a kind of single stage method preparing gasoline by methanol novel process, and methyl alcohol directly generates gasoline and liquefied gas through first stage reactor.This technology is researched and developed by Shanxi coalification institute, and obtains Industrial demonstration application in Yunnan coalification group.Compared with two-stage method technique, the technical process of single stage method preparing gasoline by methanol is short, invests low, thus makes the economy of MTG obtain raising, but does not mention the recycling to the by product such as liquefied gas, heavy aromatics in patent.
CN101787306A discloses a kind of refining methanol synthetic oil method and apparatus, by the means such as fractionation, crystallization by separating of oil for methanol-fueled CLC be fuel gas, liquefied gas, treated gasoline and durol.Although can be promoted the quality of each product of preparing gasoline by methanol by this technique, flow process is complicated, and system energy consumption is high.
Summary of the invention
The object of this invention is to provide a kind of less energy-consumption, flow process is simple, and there is the methyl alcohol of high yield of gasoline or the integrated approach of DME synthesis gasoline.
The present invention is the integrated approach of a kind of methyl alcohol or DME synthesis gasoline, it is characterized in that:
Methyl alcohol or dme generate the hydro carbons being rich in gasoline component after synthesis reactor, obtain C through flashing tower, knockout drum, separation column after being separated
1 ~ 2hydro carbons, C
3 ~ 4hydro carbons, petroleum naphtha component, heavy gasoline components and water, wherein petroleum naphtha component is arranged outward as product, and water enters sewage treatment unit, C
1 ~ 2hydro carbons returns synthesis reactor after compressor supercharging, C
3 ~ 4hydro carbons is after aromizing again, and product directly mixes with heavy gasoline components and enters transalkylation reactor as raw material, and reaction product returns flashing tower, a small amount of C
1 ~ 2discharge as by product with heavy gasoline components; This Technology eliminates deethanizing column and debutanizing tower, and C out at the bottom of flashing tower
5 +hydro carbons temperature is 50 ~ 300 DEG C, can enter separation column without the need to heat exchange or through simple heat exchange; C
3 ~ 4after aromatization of hydrocarbons product mixes with heavy gasoline components, temperature is 250 ~ 400 DEG C, can enter transalkylation reactor without the need to heat exchange; The temperature out of transalkylation reactor is 200 ~ 450 DEG C, can return flashing tower after simple heat exchange.Present invention process flow process is simple, and system energy consumption is low, and with charging refined methanol for benchmark, yield of gasoline reaches 36 ~ 40%, and with charging dme for benchmark, yield of gasoline reaches 50 ~ 54%.
Processing step comprises:
(1) with HZSM-5 molecular sieve for catalyzer, be 350 ~ 450 DEG C in temperature, pressure is 0.5 ~ 2.0MPa, and raw material WHSV is 0.5 ~ 2.5h
-1condition under, methyl alcohol or dme are transformed the hydrocarbon mixture generating and be rich in gasoline component through synthesis reactor;
(2) reaction product of step (1) enters flashing tower after heat exchange is cooled to 50 ~ 300 DEG C, is separated into gas-liquid two-phase, and gas phase is C
1~ C
4hydro carbons, liquid phase is C
5 +hydro carbons and water;
(3) gas-phase product that step (2) obtains obtains C again after heat exchange cooling, separation
1 ~ 2hydro carbons and C
3 ~ 4hydro carbons, the former returns synthesis reactor through compressor, and the latter enters liquid gas aromatization reaction device, and reaction conditions is temperature 400 ~ 600 DEG C, and pressure is 0.1 ~ 2.0MPa, and raw material WHSV is 0.1 ~ 2.0h
-1, catalyzer adopts the ZSM-5 molecular sieve of one or more modifications in Ga, Zn, Ce, Fe, Ni, Cr, and on catalyzer, total metal content is 0.5 ~ 7.0%;
(4) liquid product that obtains of step (2) through water-and-oil separator by C
5 +hydro carbons separates with water, and water enters sewage treatment unit, C
5 +hydro carbons sends into separation column through heat pump, fractionation obtains petroleum naphtha component and heavy gasoline components, petroleum naphtha component is arranged outward as product, heavy gasoline components directly enters transalkylation reactor after mixing with the product of liquid gas aromatization reaction device, reaction product returns flashing tower, reaction conditions is temperature 200 ~ 450 DEG C, and pressure 1.0 ~ 3.0MPa, raw material WHSV are 0.1 ~ 2.0h
-1, catalyzer adopts metal-modified Y molecular sieve, and modified metal is one or more in Mo, Co, Ni, La, Ce, and on catalyzer, total metal content is 0.5 ~ 7.0%.
According to integrated approach of the present invention, it is characterized in that:
Methyl alcohol or dme generate the hydro carbons being rich in gasoline component after synthesis reactor, obtain C through flashing tower, knockout drum, separation column after being separated
1 ~ 2hydro carbons, C
3 ~ 4hydro carbons, petroleum naphtha component, heavy gasoline components and water, wherein petroleum naphtha component is arranged outward as product, and water enters sewage treatment unit, C
1 ~ 2hydro carbons returns synthesis reactor after compressor supercharging, C
3 ~ 4hydro carbons is after aromizing again, and product directly mixes with heavy gasoline components and enters transalkylation reactor as raw material, and reaction product returns flashing tower, a small amount of C
1 ~ 2discharge as by product with heavy gasoline components.This Technology eliminates deethanizing column and debutanizing tower, and C out at the bottom of flashing tower
5 +hydro carbons temperature is 80 ~ 280 DEG C, can enter separation column without the need to heat exchange or through simple heat exchange; C
3 ~ 4after aromatization of hydrocarbons product mixes with heavy gasoline components, temperature is 300 ~ 350 DEG C, can enter transalkylation reactor without the need to heat exchange; The temperature out of transalkylation reactor is 250 ~ 400 DEG C, can return flashing tower after simple heat exchange.Present invention process flow process is simple, and system energy consumption is low, and with charging refined methanol for benchmark, yield of gasoline reaches 37 ~ 39%, and with charging dme for benchmark, yield of gasoline reaches 51 ~ 53%.
Processing step comprises:
(1) with HZSM-5 molecular sieve for catalyzer, be 380 ~ 420 DEG C in temperature, pressure is 1.0 ~ 1.8MPa, and raw material WHSV is 1.0 ~ 2.0h
-1condition under, methyl alcohol or dme are transformed the hydrocarbon mixture generating and be rich in gasoline component through synthesis reactor;
(2) reaction product of step (1) enters flashing tower after heat exchange is cooled to 80 ~ 280 DEG C, is separated into gas-liquid two-phase, and gas phase is C
1~ C
4hydro carbons, liquid phase is C
5 +hydro carbons and water;
(3) gas-phase product that step (2) obtains obtains C again after heat exchange cooling, separation
1 ~ 2hydro carbons and C
3 ~ 4hydro carbons, the former returns synthesis reactor through compressor, and the latter enters liquid gas aromatization reaction device, and reaction conditions is temperature 450 ~ 550 DEG C, and pressure is 0.1 ~ 1.0MPa, and raw material WHSV is 0.5 ~ 1.5h
-1, catalyzer adopts the ZSM-5 molecular sieve of one or more modifications in Ga, Zn, Ce, Fe, Ni, Cr, and on catalyzer, total metal content is 1.0 ~ 6.0%;
(4) liquid product that obtains of step (2) through water-and-oil separator by C
5 +hydro carbons separates with water, and water enters sewage treatment unit, C
5 +hydro carbons sends into separation column through heat pump, fractionation obtains petroleum naphtha component and heavy gasoline components, petroleum naphtha component is arranged outward as product, heavy gasoline components directly enters transalkylation reactor after mixing with the product of liquid gas aromatization reaction device, reaction product returns flashing tower, reaction conditions is temperature 250 ~ 400 DEG C, and pressure 1.2 ~ 2.0MPa, raw material WHSV are 0.5 ~ 1.5h
-1, catalyzer adopts metal-modified Y molecular sieve, and modified metal is one or more in Mo, Co, Ni, La, Ce, and on catalyzer, total metal content is 1.0 ~ 5.0%;
Accompanying drawing explanation
Fig. 1 is the process flow sheet of the integrated approach of a kind of methyl alcohol of the present invention or DME synthesis gasoline:
Wherein: E-1, E-2, E-4, E-6, E-14 interchanger, E-3 synthetic oil reactor, E-5 flashing tower, E-7, E-9 knockout drum, E-10 recycle gas compressor, E-11 liquid gas aromatization reaction device, E-12 gun barrel, E-13 high-temperature pump, E-15 separation column, E-16 transalkylation reactor.
Technical process is described as follows:
Methyl alcohol or dme enter after the gasification of E-1, E-2 interchanger through P-1, are mixed into synthetic oil reactor with the circulation gas from E-4 interchanger, and reaction product enters E-5 flashing tower after the cooling of E-4, E-1 interchanger.E-5 gaseous phase materials enters E-7 knockout drum through E-6 interchanger, and E-7 gaseous phase materials enters knockout drum E-9 after E-8 water cooler, and E-7 liquid phase material is discharged through P-4.E-9 gaseous phase materials enters E-6, E-4 interchanger after compressor E-10 supercharging, and E-9 liquid phase material enters liquid gas aromatization reaction device E-11.E-5 flashing tower liquid phase material enters gun barrel E-12, and aqueous phase is arranged outward through P-3 and entered Sewage treatment systems, and oil phase enters separation column E-15 through E-13 heat pump, E-14 interchanger, and tower top discharging is petroleum naphtha component, and discharging at the bottom of tower is heavy gasoline components.Heavy gasoline components enters E-16 transalkylation reactor after mixing with E-11 reaction product, and reaction product returns E-1 interchanger, a small amount of C
1 ~ 2discharged by P-5, P-6 with heavy gasoline components.
Embodiment
Embodiment 1
Raw material adopts refined methanol, and synthetic oil reactor adopts fixed-bed reactor, and reaction conditions is temperature 380 DEG C, pressure 1.0MPa, methyl alcohol WHSV=1.0h
-1.Liquid gas aromatization reaction device adopts fixed-bed reactor, and reaction conditions is temperature 450 DEG C, and pressure is 0.5MPa, and raw material WHSV is 1.0h
-1, catalyzer adopts Ga/Ce-ZSM-5 molecular sieve catalyst, and wherein Ga content is 1.5%, Ce content is 0.5%.Transalkylation reactor adopts fixed-bed reactor, and reaction conditions is temperature 300 DEG C, and pressure 1.2MPa, raw material WHSV are 1.0h
-1, catalyzer adopts Mo/Ni-Y molecular sieve catalyst, and wherein Mo content is 1.5%, Ni content is 1.0%.Under above processing condition, drop temperature at the bottom of E-5 flashing tower is 130 DEG C, E-15 separation column can be entered after simple heat exchange, after E-11 aromatization reactor product mixes with the discharging of E-15 Fractionator Bottom, temperature is 300 DEG C, can enter E-16 transalkylation reactor without the need to heat exchange, E-16 product can return E-5 through simple heat exchange cooling.The yield (taking methyl alcohol as base, lower same) of each product is as shown in table 1.
Embodiment 2
Raw material adopts refined methanol, and synthetic oil reactor adopts moving-burden bed reactor, and reaction conditions is temperature 400 DEG C, pressure 1.5MPa, methyl alcohol WHSV=1.5h
-1.Liquid gas aromatization reaction device adopts moving-burden bed reactor, and reaction conditions is temperature 500 DEG C, and pressure is 0.2MPa, and raw material WHSV is 0.8h
-1, catalyzer adopts Ga/Fe-ZSM-5 molecular sieve catalyst, and wherein Ga content is 3.0%, Fe content is 2.0%.Transalkylation reactor adopts fixed-bed reactor, and reaction conditions is temperature 320 DEG C, and pressure 1.8MPa, raw material WHSV are 0.7h
-1, catalyzer adopts Mo/La-Y molecular sieve catalyst, and wherein Mo content is 3.0%, La content is 0.3%.Under above processing condition, drop temperature at the bottom of E-5 flashing tower is 150 DEG C, E-15 separation column can be entered after simple heat exchange, after E-11 aromatization reactor product mixes with the discharging of E-15 Fractionator Bottom, temperature is 320 DEG C, can enter E-16 transalkylation reactor without the need to heat exchange, E-16 product can return E-5 after simple heat exchange cooling.The yield of each product is as shown in table 1.
Embodiment 3
Raw material adopts dme, and synthetic oil reactor adopts fluidized-bed reactor, and reaction conditions is temperature 420 DEG C, pressure 1.8MPa, methyl alcohol WHSV=2.0h
-1.Liquid gas aromatization reaction device adopts fluidized-bed reactor, and reaction conditions is temperature 550 DEG C, and pressure is 0.2MPa, and raw material WHSV is 1.5h
-1, catalyzer adopts Ga/Zn-ZSM-5 molecular sieve catalyst, and wherein Ga content is 3.0%, Zn content is 1.0%.Transalkylation reactor adopts fixed-bed reactor, and reaction conditions is temperature 340 DEG C, and pressure 2.0MPa, raw material WHSV are 1.2h
-1, catalyzer adopts Mo/Co-Y molecular sieve catalyst, and wherein Mo content is 3.0%, Co content is 2.0%.Under above processing condition, drop temperature at the bottom of E-5 flashing tower is 170 DEG C, E-15 separation column can be entered after simple heat exchange, after E-11 aromatization reactor product mixes with the discharging of E-15 Fractionator Bottom, temperature is 340 DEG C, can enter E-16 transalkylation reactor without the need to heat exchange, E-16 product can return E-5 after simple heat exchange cooling.The yield of each product is as shown in table 1.
Table 1 methanol/dimethyl ether produces the product composition of gasoline integrated approach
Claims (2)
1. an integrated approach for methyl alcohol or DME synthesis gasoline, is characterized in that:
Methyl alcohol or dme generate the hydro carbons being rich in gasoline component after synthesis reactor, obtain C through flashing tower, knockout drum, separation column after being separated
1 ~ 2hydro carbons, C
3 ~ 4hydro carbons, petroleum naphtha component, heavy gasoline components and water, wherein petroleum naphtha component is arranged outward as product, and water enters sewage treatment unit, C
1 ~ 2hydro carbons returns synthesis reactor after compressor supercharging, C
3 ~ 4hydro carbons is after aromizing again, and product directly mixes with heavy gasoline components and enters transalkylation reactor as raw material, and reaction product returns flashing tower, a small amount of C
1 ~ 2discharge as by product with heavy gasoline components;
Processing step comprises:
1) with HZSM-5 molecular sieve for catalyzer, be 350 ~ 450 DEG C in temperature, pressure is 0.5 ~ 2.0MPa, and raw material WHSV is 0.5 ~ 2.5h
-1condition under, methyl alcohol or dme are transformed the hydrocarbon mixture generating and be rich in gasoline component through synthesis reactor;
2) reaction product of step 1) enters flashing tower after heat exchange is cooled to 50 ~ 300 DEG C, is separated into gas-liquid two-phase, and gas phase is C
1~ C
4hydro carbons, liquid phase is C
5 +hydro carbons and water;
3) step 2) gas-phase product that obtains obtains C through heat exchange cooling, knockout drum after being separated again
1 ~ 2hydro carbons and C
3 ~ 4hydro carbons, the former returns synthesis reactor through compressor, and the latter enters liquid gas aromatization reaction device, and reaction conditions is temperature 400 ~ 600 DEG C, and pressure is 0.1 ~ 2.0MPa, and raw material WHSV is 0.1 ~ 2.0h
-1, catalyzer adopts the ZSM-5 molecular sieve of one or more modifications in Ga, Zn, Ce, Fe, Ni, Cr, and on catalyzer, total metal content is 0.5 ~ 7.0%;
4) step 2) liquid product that obtains through gun barrel by C
5 +hydro carbons separates with water, and water enters sewage treatment unit, C
5 +hydro carbons sends into separation column through heat pump, fractionation obtains petroleum naphtha component and heavy gasoline components, petroleum naphtha component is arranged outward as product, heavy gasoline components directly enters transalkylation reactor after mixing with the product of liquid gas aromatization reaction device, reaction product returns flashing tower, reaction conditions is temperature 200 ~ 450 DEG C, and pressure 1.0 ~ 3.0MPa, raw material WHSV are 0.1 ~ 2.0h
-1, catalyzer adopts metal-modified Y molecular sieve, and modified metal is one or more in Mo, Co, Ni, La, Ce, and on catalyzer, total metal content is 0.5 ~ 7.0%.
2. in accordance with the method for claim 1, it is characterized in that:
Methyl alcohol or dme generate the hydro carbons being rich in gasoline component after synthesis reactor, obtain C through flashing tower, knockout drum, separation column after being separated
1 ~ 2hydro carbons, C
3 ~ 4hydro carbons, petroleum naphtha component, heavy gasoline components and water, wherein petroleum naphtha component is arranged outward as product, and water enters sewage treatment unit, C
1 ~ 2hydro carbons returns synthesis reactor after compressor supercharging, C
3 ~ 4hydro carbons is after aromizing again, and product directly mixes with heavy gasoline components and enters transalkylation reactor as raw material, and reaction product returns flashing tower, a small amount of C
1 ~ 2discharge as by product with heavy gasoline components;
Processing step comprises:
1) with HZSM-5 molecular sieve for catalyzer, be 380 ~ 420 DEG C in temperature, pressure is 1.0 ~ 1.8MPa, and raw material WHSV is 1.0 ~ 2.0h
-1condition under, methyl alcohol or dme are transformed the hydrocarbon mixture generating and be rich in gasoline component through synthesis reactor;
2) reaction product of step 1) enters flashing tower after heat exchange is cooled to 80 ~ 280 DEG C, is separated into gas-liquid two-phase, and gas phase is C
1~ C
4hydro carbons, liquid phase is C
5 +hydro carbons and water;
3) step 2) gas-phase product that obtains again through heat exchange cooling, be separated after obtain C
1 ~ 2hydro carbons and C
3 ~ 4hydro carbons, the former returns synthesis reactor through compressor, and the latter enters liquid gas aromatization reaction device, and reaction conditions is temperature 450 ~ 550 DEG C, and pressure is 0.1 ~ 1.0MPa, and raw material WHSV is 0.5 ~ 1.5h
-1, catalyzer adopts the ZSM-5 molecular sieve of one or more modifications in Ga, Zn, Ce, Fe, Ni, Cr, and on catalyzer, total metal content is 1.0 ~ 6.0%;
4) step 2) liquid product that obtains through gun barrel by C
5 +hydro carbons separates with water, and water enters sewage treatment unit, C
5 +hydro carbons sends into separation column through heat pump, fractionation obtains petroleum naphtha component and heavy gasoline components, petroleum naphtha component is arranged outward as product, heavy gasoline components directly enters transalkylation reactor after mixing with the product of liquid gas aromatization reaction device, reaction product returns flashing tower, reaction conditions is temperature 250 ~ 400 DEG C, and pressure 1.2 ~ 2.0MPa, raw material WHSV are 0.5 ~ 1.5h
-1, catalyzer adopts metal-modified Y molecular sieve, and modified metal is one or more in Mo, Co, Ni, La, Ce, and on catalyzer, total metal content is 1.0 ~ 5.0%.
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| CN105013528B (en) * | 2015-07-24 | 2017-07-14 | 麦森能源科技有限公司 | Composite molecular sieve catalyst for preparing gasoline by methanol and preparation method thereof |
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Address after: 100010 Beijing, Chaoyangmen, North Street, No. 25, No. Patentee after: China National Offshore Oil Corporation Patentee after: CNOOC TIANJIN CHEMICAL RESEARCH & DESIGN INSTITUTE CO., LTD. Patentee after: CNOOC Energy Development Co., Ltd. Address before: 100010 Beijing, Chaoyangmen, North Street, No. 25, No. Patentee before: China National Offshore Oil Corporation Patentee before: CNOOC Tianjin Chemical Research & Design Institute Patentee before: CNOOC Energy Development Co., Ltd. |
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