CN104194850A - Method of producing natural gas by coupling coke oven gas and producer gas and production device - Google Patents
Method of producing natural gas by coupling coke oven gas and producer gas and production device Download PDFInfo
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- CN104194850A CN104194850A CN201410224925.4A CN201410224925A CN104194850A CN 104194850 A CN104194850 A CN 104194850A CN 201410224925 A CN201410224925 A CN 201410224925A CN 104194850 A CN104194850 A CN 104194850A
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Abstract
The invention relates to a method of producing natural gas by coupling coke oven gas and producer gas and a production device adopting the method for production of the natural gas. According to the method, the coke oven gas and the producer gas are adopted as raw materials; the ratio of the coke oven gas to the producer gas is calculated based on requirements on the ratio of H2, CO, and CO2 for methanation and according to the contents of the H2, the CO and the CO2 in the coke oven gas and the producer gas which are adopted as the raw materials; the coke oven gas and the producer gas which are adopted as the raw materials are fed into a methanation device according to the ratio and subjected to methanation; and nitrogen in the gas after the methanation is removed to form the natural gas formed by methane. The production device comprises the methanation device and a nitrogen separation device which are connected to each other. The method and the production device effectively utilize the component difference of the two raw material gases, achieve component complementation of the two kinds of coal gas and allow the gas after the methanation to meet requirements on the natural gas, thus simplifying the production process, reducing the production cost, avoiding environment pollution and increasing economic benefit.
Description
Technical field
The present invention relates to the production of Sweet natural gas, be specially a kind of coke-oven gas and producer gas coupling and produce the method for Sweet natural gas and adopt the method to produce the production equipment of Sweet natural gas.
Background technology
Coke-oven gas is that coking industry is at the byproduct that generates the generation of coke process, coking coal is heated to 1000 ℃ of left and right and carries out high temperature carbonization under isolated air conditions, by thermolysis and coking effect, produce coke, coke-oven gas and other coking chemistry products, calorific value of gas in belonging to through the coal gas purifying, thermal value is 17500kJ/Nm
3left and right, coal per ton approximately produces coke-oven gas 300-400 m
3, account for the 16%-20% of shove charge ature of coal amount, its main component is hydrogen and methane, separablely go out for the hydrogen of chemosynthesis and replace the methane of Sweet natural gas, but the technique of preparing hydrogen and Sweet natural gas by separate mode is comparatively complicated, cost is higher, actual popularization has larger difficulty, directly as fuel, because calorific value is relatively low, being unsuitable for long distance carries, except coking equipment consumes a small part on the spot, remaining most of coke-oven gas needs separately to find a way out, otherwise can only burn in vain even directly emptying by point " day lamp ", cause a large amount of wastings of resources and contaminate environment, therefore the comprehensive utilization of coke-oven gas becomes the key of the coking enterprise survival and development, some large-scale coking enterprises have been built coke-oven gas methanol project processed at present, but coke-oven gas methyl alcohol technical sophistication processed, invest larger, and domestic methyl alcohol production capacity surplus, economic benefit is difficult to guarantee, particularly relatively little for medium and small coal chemical enterprise industrial scale, coke-oven gas output is few, prepare methyl alcohol and lack especially cost advantage.
For improving the utility value of coke-oven gas, people have also proposed a kind of Sweet natural gas (Artificial Natural Gas) being comprised of methane that coke-oven gas is prepared into by technology for methanation processing, the Main Function of methanation is by hydrogen reducing, to be methane by the carbon monoxide in coke-oven gas and dioxide, because the content of hydrogen in coke-oven gas is very high, in gas after methanation process, still there is a large amount of hydrogen, still need to carry out the separation of hydrogen, be not only thus still more complicated of technological process, production cost is higher, and the economic benefit of by-product hydrogen is also undesirable, affected this technology utilization and extention in practice.
Summary of the invention
In order to overcome the above-mentioned defect of prior art, the invention provides a kind of method that Sweet natural gas is produced in coke-oven gas and producer gas coupling, also provide and adopted the production equipment of preparing in this way Sweet natural gas, this method and apparatus can effectively utilize the component difference of two kinds of unstripped gass, hydrogen in coke-oven gas is fully used in methanation, make carbon monoxide and carbonic acid gas in producer gas also all be changed simultaneously, to make full use of various resources, simplify production technique, reduce and produce cost, increase economic efficiency.
The technical solution adopted in the present invention is:
A kind of method that Sweet natural gas is produced in coke-oven gas and producer gas coupling, take coke-oven gas and producer gas as raw material, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation is processed carries out separation, remove nitrogen wherein, form the Sweet natural gas being formed by methane.
A production equipment for Sweet natural gas is produced in coke-oven gas and producer gas coupling, comprises interconnective methanation device and nitrogen tripping device, take coke-oven gas and producer gas as raw material, according to the required H of methanation reaction
2, CO and CO
2proportion requirement between three, according to H in the coke-oven gas as raw material and producer gas
2, CO and CO
2content, calculate the proportioning between coke-oven gas and producer gas, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation reaction enters nitrogen tripping device and carries out gas delivery, isolate nitrogen wherein, form the Sweet natural gas being formed by methane.
Beneficial effect of the present invention is:
Owing to take coke-oven gas and producer gas as raw material, and according to the addition of the required proportion requirement configuration coke-oven gas of methanation reaction and producer gas, realized thus this complementation of two kinds of coal gas on composition, with carbon monoxide and the carbonic acid gas in hydrogen reduction producer gas unnecessary in coke-oven gas, make two kinds of carbon in coal gas, hydrogen composition all participates in methanation reaction, substantially there is not remaining hydrogen and carbon monoxide and carbonic acid gas, make the Related Component in coke-oven gas and producer gas all be converted to methane, simplified thus technique, lowered cost, the utilization of resources that has improved coke-oven gas and producer gas is worth, the wasting of resources and the pollution to environment have been avoided.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet of production method of the present invention;
Fig. 2 is the structural representation of production equipment of the present invention;
Fig. 3 is the structural representation of the another kind of embodiment of production equipment of the present invention.
Embodiment
The present invention adopts coke-oven gas after purification and producer gas to be mixed in proportion to prepare Sweet natural gas, utilize these two kinds of coal gas difference of composition separately, according to the due proportionlity of methanation reaction, carry out the configuration of these two kinds of coal gas, thereby various compositions can both fully be reacted in methanation, prepare the Sweet natural gas that purity is higher.
Wherein, coke-oven gas is the byproduct of coking, and its composition, content (volume percent) and calorific value can see the following form:
The preparation of producer gas generally can make by hard coal, bituminous coal, brown coal, and generally, the composition of producer gas prepared by Coal rank, content (volume percent) and calorific value can see the following form:
In the process of methanation reaction, what participate in reaction is mainly hydrogen, carbon monoxide and carbonic acid gas, but other Multiple components also participate in reaction simultaneously, because of content lower, impact on methanation reaction is less, conventionally in calculating, can not consider, the product of methanation reaction is methane and water, and the principal reaction formula that relates to the methanation reaction of carbon monoxide and carbonic acid gas is:
C0 + 3H
2 = CH
4 + H
20 + 206kJ/mol (1)
C0
2 + 4H
2 = CH
4 + 2H
20 + 165kJ/mol (2)
The present invention utilizes above-mentioned methanation reaction mode, by suitable ratio, allocate, make the hydrogen in coke-oven gas and producer gas, carbon monoxide and carbonic acid gas are substantially gone up and are all participated in methanation reaction, thus need to be after reaction separating hydrogen gas in gas, do not need to add in addition hydrogen source yet, methanation degree after reaction in gas is high, except the restriction because of in actual process, substantially there is not carbon monoxide and carbonic acid gas, and the content of hydrogen also can near zero or in the situation that meeting Sweet natural gas and requiring the hydrogen of slightly certain surplus, to realize the optimization of technological process.
Referring to Fig. 1, the method that Sweet natural gas is produced in coke-oven gas provided by the invention and producer gas coupling, take coke-oven gas and producer gas as raw material, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation is processed carries out separation, remove nitrogen wherein, form the Sweet natural gas being formed by methane.
Consider that other component contents that participate in reaction are very little, can be according to the required H of methanation reaction in reality
2, CO and CO
2proportion requirement between three, according to H in the coke-oven gas as raw material and producer gas
2, CO and CO
2content, calculate the proportioning between coke-oven gas and producer gas so that after completing methanation reaction, in gas not or there is no remaining H
2, CO and CO
2, but in actual production, because of technical factor, still the consideration based on economically, all without reaching theoretic complete reaction, needs only remaining H
2, CO and CO
2composition Control within the range of permission.
Conventionally, for making methanation reaction towards favourable direction, make to be substantially devoid of in the gas after methanation CO and CO
2; on can the theoretical ratio of complete reaction, appropriateness increases the addition of coke-oven gas; appropriateness improves the ratio that applies hydrogen in methanation reaction; according to the requirement to methane concentration in Sweet natural gas at present; the addition of coke-oven gas can adopt in the gas making after methanation addition when hydrogen richness is 0.25-0.8%, can effectively improve CO and CO thus
2turnover ratio, make to remain CO and CO
2concentration meets the required standard of Sweet natural gas and is conducive to fast reaction speed, guarantees the reliability of technique and the impact resistance of system.
Conventionally, the coke-oven gas of described effect raw material and producer gas should adopt coke-oven gas (clean coke-oven gas) and the producer gas (clean producer gas) after purifying, to be suitable for methanation, process, for example, can adopt prior art to remove the impurity such as tar wherein, benzene, naphthalene, sulfide, the product of wherein separating in scavenging process can be used as industrial chemicals after suitable treatment process.
Conventionally, described producer gas can make with hard coal, bituminous coal or brown coal, owing to take the ratio difference of Coal rank various compositions in the producer gas that raw material makes, so should calculate respectively or set according to the raw materials used coal of producer gas described as the coke-oven gas of raw material and the proportioning of producer gas.
For example, generally, when described producer gas be hard coal make producer gas time, coke-oven gas consumption is preferably 79-82% with respect to the volume percent of two kinds of total consumptions of coal gas, when described producer gas is the producer gas making with bituminous coal, coke-oven gas consumption is preferably 80-83% with respect to the volume percent of two kinds of total consumptions of coal gas, when described producer gas is for take brown coal during as producer gas that raw material makes, coke-oven gas consumption is preferably 78-81% with respect to the volume percent of two kinds of total consumptions of coal gas.Under said ratio, can obtain methanation substantially completely, after methanation, in gas, there is no remaining carbon monoxide and carbonic acid gas, the ratio of remaining hydrogen meets prepares Sweet natural gas requirement, and speed of response is fast, efficiency is high, process stabilizing, good reliability, the fluctuation of the content of the various compositions of permission raw material coal gas in common scope.
Because methanation is a kind of strong exothermal reaction, be easy to occur sintering of catalyst and coking problem, therefore suitably controlling reaction process is to affect the important factor that methanation reaction can carry out smoothly, the present invention preferably adopts three grades of mutual series connection or complete as described methanation device more than the methanation equipment of three grades, mode by this multistage methanation realizes and completes described methanation reaction, in first step methanation equipment, only send into all or most of (conventionally can for more than 80%) described producer gas carries out methanation reaction, in follow-up methanation equipment, send into the gas after previous stage methanation equipment reaction and be used as the described coke-oven gas of raw material or send into the gas after previous stage methanation equipment reaction and be used as the described coke-oven gas of raw material and the remainder of described producer gas, conventionally described coke-oven gas can be divided into many parts and send into respectively first step methanation equipment at different levels afterwards, make the first step every grade of methanation equipment afterwards have coke-oven gas to add, the residue producer gas not joining in first step methanation equipment can disposablely join in certain follow-up one-level methanation equipment, to simplify operation process.Adopt aforesaid way, can pass through the supply of hydrogen in restriction methanation equipment at different levels to control methanation reaction degree and reaction process, avoid in one-level methanation equipment, producing too much reaction heat arbitrarily, in described methanation equipment at different levels, add amount or the proportionlity of unstripped gas (coke-oven gas and/or producer gas) should be according to methanation reaction intensity or gas outlet temperature in this equipment, avoid too high temperature, generally, within temperature out should be controlled at 650 ° of C, development along with catalyst technology, also can there is being suitable for the catalyzer of working under higher temperature, also can gas outlet temperature be limited in higher scope according to catalyzer and other factors thus.Employing is by controlling the mode of hydrogen amount control methanation reaction for the mode of controlling methanation reaction by controlling carbon monoxide concentration or carbon monoxide and concentration of total carbon dioxide, can guarantee to control under the prerequisite of effect, without circulation gas or significantly reduce the consumption of circulation gas, reduce thus the processing power requirement to relevant methanation equipment, and significantly reduce the power consumption because of gas circulation generation.
For example, described methanation device is three grades of methanation equipment of series connection mutually, whole producer gases is sent into first step methane equipment and carry out methanation reaction, the hydrogen own with producer gas carries out methanation to the part carbon monoxide in producer gas and carbonic acid gas, in second stage methanation equipment, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment, send into gas after second stage methanation equipment reaction and the producer gas of residue 60% and carry out methanation reaction.
And for example, described methanation device is the methanation equipment that level Four is connected mutually, 80% producer gas is sent into first step methane equipment and carry out methanation reaction, the hydrogen own with producer gas carries out methanation to the part carbon monoxide in producer gas and carbonic acid gas, in second stage methanation equipment, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment, send into the gas after second stage methanation equipment reaction, the producer gas of 20% coke-oven gas and residue 20% carries out methanation reaction, the gas of sending in fourth stage methanation equipment after third stage methanation equipment reaction carries out methanation reaction with the coke-oven gas of residue 40%.
The form of described each methanation equipment, processing power, treatment process and operating method can be according to prior aries, and methanation reaction degree can be limited with the level of response that in respective reaction system, hydrogen amount is allowed.
Conventionally, in the situation that described methanation device consists of one or more levels methanation equipment, reply is lowered the temperature through the gas after methanation equipment reaction, for example, to adapt to the requirement (requirement of one-level methanation reaction or other subsequent techniques after) of subsequent technique.Described cooling can adopt the heat change method of existing conventional heat change method or other any suitable and recycle the heat that cooling discharges, for example, by heat exchange, produce the steam of use value and/or unstripped gas is heated to certain temperature to adapt to processing requirement.
Under prior art background, the characteristic based on catalyzer and the optimal control to reaction process, the inlet temperature of described each methanation equipment and temperature out are preferably controlled at respectively 250-300 ° of C and 400-500 ° of C.
Owing to having added a certain amount of producer gas, in gas after methanation reaction, contain a certain proportion of nitrogen, the gas of conventionally tackling after methanation reaction completes carries out gas delivery, by wherein contained nitrogen separation out, gas after separation of nitrogen mainly comprises methane, can according to practical situation through purifying treatment or without purifying treatment as natural gas motorcar, for example, send into natural-gas transfer pipeline or send into natural gas storage tank, also can further prepare LNG etc.
Referring to Fig. 2 and Fig. 3, the production equipment of Sweet natural gas is produced in coke-oven gas provided by the invention and producer gas coupling, adopted above-mentioned each technical scheme that relates to method, described production equipment comprises interconnective methanation device and nitrogen tripping device 40, take coke-oven gas and producer gas as raw material, according to the required H of methanation reaction
2, CO and CO
2proportion requirement between three, according to H in the coke-oven gas as raw material and producer gas
2, CO and CO
2content, calculate the proportioning between coke-oven gas and producer gas, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation reaction enters nitrogen tripping device and carries out gas delivery, isolate nitrogen wherein, form the Sweet natural gas that mainly comprises methane.After the separation of nitrogen tripping device, the Sweet natural gas and the nitrogen that generate can be used as corresponding resource, by Sweet natural gas output tube 41 and nitrogen output tube 42, send respectively, can further purify as required, also can directly send into storing device or gas equipment.
Described methanation device can adopt three grades of mutual series connection or more than the methanation equipment of three grades, in first step methanation equipment, only send into all or part of described producer gas and carry out methanation reaction, in follow-up methanation equipment, send into the gas after previous stage methanation equipment reaction and be used as the described coke-oven gas of raw material or send into the gas after previous stage methanation equipment reaction and be used as the described coke-oven gas of raw material and the remainder of described producer gas, conventionally described coke-oven gas can be divided into many parts and send into respectively first step methanation equipment at different levels afterwards, make the first step every grade of methanation equipment afterwards have coke-oven gas to add, the residue producer gas not joining in first step methanation equipment can disposablely join in certain follow-up one-level methanation equipment, to simplify operation process.
For example, described methanation device is three grades of methanation equipment 31,32,33 of series connection mutually, whole producer gases is sent into first step methane equipment 31 and carry out methanation reaction, in second stage methanation equipment 32, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment 33, send into gas after second stage methanation equipment reaction and the producer gas of residue 60% and carry out methanation reaction.
And for example, described methanation device is the methanation equipment 31 that level Four is connected mutually, 32, 33, 34, 80% producer gas is sent into first step methane equipment 31 and carry out methanation reaction, in second stage methanation equipment 32, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment 33, send into the gas after second stage methanation equipment reaction, the producer gas of 20% coke-oven gas and residue 20% carries out methanation reaction, the gas of sending in fourth stage methanation equipment 34 after third stage methanation equipment reaction carries out methanation reaction with the coke-oven gas of residue 40%.
Conventionally, should described in each, after methanation equipment, be provided with the heat exchanger for lowering the temperature to the gas of getting rid of from described methanation equipment.
Production equipment of the present invention can also be provided with coke oven gas purifying device 10 and producer gas refining plant 20, described coke oven gas purifying device and producer gas refining plant are positioned at the preorder of described methanation device, coke-oven gas and producer gas are sent into described methanation device as the unstripped gas of methanation reaction after described coke oven gas purifying device and the purification of producer gas refining plant again, by coke oven gas pipe 11 and producer gas pipeline 21, respectively coke-oven gas and producer gas are sent into cleaner separately, coke-oven gas after purifying and producer gas are sent into corresponding methanation equipment by clean coke oven gas pipe 12 and clean producer gas pipeline 22.
The proportionlity of the gas the present invention relates to is volume ratio, described volume ratio is the volume ratio of being converted under unified standard state, when relate to same unstripped gas several times/multistage add fashionable, described each/every grade of per-cent adding (or volume percent) for this gas in the add-on of this time/this grade the volume percent with respect to the total consumption of this gas.In gas of the present invention, the content of various compositions is this composition with respect to volume (or dividing potential drop) per-cent of this gas.
Claims (10)
1. the method that Sweet natural gas is produced in a coke-oven gas and producer gas coupling, it is characterized in that take that coke-oven gas and producer gas are as raw material, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation is processed carries out separation, remove nitrogen wherein, form the Sweet natural gas being formed by methane.
2. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 1 and producer gas coupling, is characterized in that according to the required H of methanation reaction
2, CO and CO
2proportion requirement between three, according to H in the coke-oven gas as raw material and producer gas
2, CO and CO
2content, calculate the proportioning between coke-oven gas and producer gas.
3. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 2 and producer gas coupling, the addition that it is characterized in that appropriateness increase coke-oven gas in the theoretical ratio of methanation complete reaction, appropriateness improves the ratio that applies hydrogen in methanation reaction, the addition when addition of coke-oven gas adopts and makes in the gas after methanation that hydrogen richness is 0.25-0.8%.
4. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 3 and producer gas coupling, it is characterized in that the described coke-oven gas as raw material and producer gas adopt clean coke-oven gas and the clean producer gas after purifying, remove the impurity such as tar wherein, benzene, naphthalene, sulfide.
5. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 1 and producer gas coupling, it is characterized in that described producer gas is with hard coal, bituminous coal or brown coal make, according to the raw materials used coal of producer gas, calculate respectively or set described as the coke-oven gas of raw material and the proportioning of producer gas, when described producer gas be hard coal make producer gas time, coke-oven gas consumption is 79-82% with respect to the volume percent of two kinds of total consumptions of coal gas, when described producer gas is the producer gas making with bituminous coal, coke-oven gas consumption is 80-83% with respect to the volume percent of two kinds of total consumptions of coal gas, when described producer gas is for take brown coal during as producer gas that raw material makes, coke-oven gas consumption is 78-81% with respect to the volume percent of two kinds of total consumptions of coal gas.
6. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 1 and producer gas coupling, it is characterized in that adopting three grades of mutual series connection or realizing and complete described methanation reaction more than the methanation equipment of three grades, in first step methanation equipment, only send into whole or most of described producer gas and carry out methanation reaction, in follow-up methanation equipment, send into the gas after previous stage methanation equipment reaction and be used as the described coke-oven gas of raw material or the remainder of described coke-oven gas and described producer gas, wherein said coke-oven gas is divided into many parts and sends into respectively first step methanation equipment at different levels afterwards.
7. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 6 and producer gas coupling, it is characterized in that described methanation device is three grades of methanation equipment of series connection mutually, whole producer gases is sent into first step methane equipment and carry out methanation reaction, in second stage methanation equipment, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment, send into gas after second stage methanation equipment reaction and the producer gas of residue 60% and carry out methanation reaction.
8. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 6 and producer gas coupling, it is characterized in that described methanation device is the methanation equipment that level Four is connected mutually, 80% producer gas is sent into first step methane equipment and carry out methanation reaction, in second stage methanation equipment, send into gas after first step methanation equipment reaction and 40% coke-oven gas and carry out methanation reaction, in third stage methanation equipment, send into the gas after second stage methanation equipment reaction, the producer gas of 20% coke-oven gas and residue 20% carries out methanation reaction, the gas of sending in fourth stage methanation equipment after third stage methanation equipment reaction carries out methanation reaction with the coke-oven gas of residue 40%.
9. the method that Sweet natural gas is produced in coke-oven gas as claimed in claim 1 and producer gas coupling, it is characterized in that described methanation device consists of one or more levels methanation equipment, to lowering the temperature through the gas after described methanation equipment reaction, to adapt to the requirement of subsequent technique, described cooling adopts heat change method and recycles the heat that cooling discharges, gas after methanation reaction is completed carries out gas delivery, by wherein contained nitrogen separation out, gas after separation of nitrogen mainly comprises methane, through purifying treatment or without purifying treatment as Sweet natural gas.
10. a production equipment for Sweet natural gas is produced in coke-oven gas and producer gas coupling, it is characterized in that comprising interconnective methanation device and nitrogen tripping device, take coke-oven gas and producer gas as raw material, according to the required H of methanation reaction
2, CO and CO
2proportion requirement between three, according to H in the coke-oven gas as raw material and producer gas
2, CO and CO
2content, calculate the proportioning between coke-oven gas and producer gas, by sending into methanation device as the coke-oven gas of raw material and producer gas, carry out methanation processing in proportion, gas after methanation reaction enters nitrogen tripping device and carries out gas delivery, isolate nitrogen wherein, form the Sweet natural gas being formed by methane.
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| CN105296034A (en) * | 2015-11-03 | 2016-02-03 | 中海石油气电集团有限责任公司 | Method for preparing LNG from coke oven gas by supplementing carbon dioxide to improve device security and yield |
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