CN104830391A - Methanation device and process for synthesizing high-quality natural gas produced by coal - Google Patents

Methanation device and process for synthesizing high-quality natural gas produced by coal Download PDF

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CN104830391A
CN104830391A CN201510247498.6A CN201510247498A CN104830391A CN 104830391 A CN104830391 A CN 104830391A CN 201510247498 A CN201510247498 A CN 201510247498A CN 104830391 A CN104830391 A CN 104830391A
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methanation
gas
auxiliary
adiabatic
reactor
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CN201510247498.6A
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Chinese (zh)
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张新波
高振
马磊
宋鹏飞
郑珩
王秀林
何洋
姚辉超
杨宽辉
周婵
易竖棚
张勃
刘玉成
张瑜
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西南化工研究设计院有限公司
中海石油气电集团有限责任公司
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Priority to CN201510247498.6A priority Critical patent/CN104830391A/en
Publication of CN104830391A publication Critical patent/CN104830391A/en

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Abstract

The invention relates to a methanation device and process for synthesizing high-quality natural gas produced by coal. The methanation device is a multi-grade circulation external heat-transfer methanation device and is characterized in that a first grade device is a primary methanation device and a second grade device is an auxiliary methanation device; the primary methanation device and the auxiliary methanation device are connected; a gas circulating system is arranged between the primary methanation device and the auxiliary methanation device; the methanation device further comprises a heat recycling system; the primary methanation device is used for introducing a raw material gas; the auxiliary methanation device is used for introducing carbon dioxide; the methanation process is mainly used for adding a carbon dioxide gas in a working section of the auxiliary methanation device without increasing the thermal load of a primary methanation process; the system is easy to control, the methane product is high, the whole methanation process is guaranteed to be lightly affected by the front process, and the product quality is stable.

Description

A kind of methanation device and technique of synthesizing high-quality coal preparing natural gas
Technical field
The present invention relates to a kind of methanation device and technique of synthesizing high-quality coal preparing natural gas, the chemical technology field be specifically related to being waste synthetic natural gas with coal or biomass carries out technological operation, after low-temperature rectisol gas, synthetic gas is as raw material, and the methanation reaction process of the carbon dioxide preparation synthetic natural gas of the cleaning that low-temperature rectisol flash distillation parses is supplemented at methanation workshop section latter half, belong to chemical technology field.
Background technology
The breach of domestic natural gas supply strengthens just year by year, and external dependence degree is especially in the gesture of rising fast.According to relevant data prediction, to the year two thousand twenty, domestic natural gas breach will reach 1000 billion cubic meters.2011, Natural Gas In China external dependence degree reached 24%, compared with 2010 12.8%, in the situation that is doubled and redoubled.This objectively increases the demand dynamics to Unconventional forage and alternative Sweet natural gas, and except shale gas exploitation puts more effort, coal preparing natural gas is also sent to great expectations in country's " 12 " strategy.
Coal preparing natural gas project obtains H by operations such as gasification after purification, sulfur-resisting transformation, low-temperature rectisols 2the synthetic gas that/CO ratio is suitable enters methanation reaction workshop section and produces synthetic natural gas.Under the reality of the oil-poor weak breath of the rich coal of China, utilize coal preparing natural gas, there is great economy and social value.To Sustainable development, there is effect.
The technique of coal preparing natural gas can be divided into gasification transformation technology and direct synthetic natural gas technology.Both differences are mainly gasification transformation technology first by feed coal pressurized gasification, the synthetic gas obtained owing to gasifying does not reach the requirement of methanation, therefore needs to improve H2/CO than carrying out methanation (gas converting unit and methanation unit are merged into a part and carried out by some technique) more simultaneously through gas converting unit.Direct synthetic natural gas technology then directly can obtain available Sweet natural gas.Gasification transformation technology can be divided into comparatively traditional two-step approach methanation process and gas converting unit and methanation unit be merged into the single stage method methanation process that a part carries out simultaneously.The technology of direct synthetic natural gas mainly contains catalysis gasification technique and hydrogasification technique.Wherein catalysis gasification technique is a kind of technology utilizing catalyzer one-step synthesis coal-based gas in pressurization fluidisation vapourizing furnace.Plus hydrogenated technique is by coal dust and hydrogen Homogeneous phase mixing post-heating, direct production hydrogen-rich gas.
Producing synthesis gas from coal composition is comparatively complicated, wherein containing CH 4, CO, CO 2etc. component, reaction process relative complex.The operation such as sulfur-resisting transformation, low-temperature rectisol is at adjustment H 2all can there is the delayed of certain degree when/CO ratio, affect the quality of product on the one hand; Cause the waste of carbon resource and fully effectively cannot utilize the hydrogen in synthetic gas on the other hand.
There is following problem in current methanation process:
1, in gas product, hydrogen content is higher, and gas product calorific value is lower;
2, in unstripped gas, hydrogen-carbon ratio regulating measure is too complicated, regulates dumb.
Summary of the invention
The object of the present invention is to provide a kind of methanation reaction process producing synthetic natural gas, it supplements carbonic acid gas position by improving, then in conjunction with circulation gas technique; Improved gas-circulating system by shunting, cold shock and other means, flow process more conventional benefit carbon methanation process is more simple, methanator thermal load is low more easily regulates.
The technical problem to be solved in the present invention is for solving in current coal synthetic natural gas process, and because hydrogen-carbon ratio regulates difficulty, gas product is difficult to reach the target that methane purity is high, calorific value is high, is difficult to production quality gas.By improving carbon dioxide position, being very easy to reach desired product quality, saving investment for rear workshop section is separated simultaneously.Have that hydrogen utilization ratio is high, good product quality, adjustment be simple, the feature of follow-up equipment less investment.
The present invention is achieved through the following technical solutions:
A kind of methanation device synthesizing high-quality coal preparing natural gas, described methanation device is move hot methanation device outside multiple stage circulation, 1st grade is main methanation device, 2nd grade is auxiliary methanation device later, described main methanation device is connected with auxiliary methanation device, be provided with cycle gas system between described main methanation device and auxiliary methanation device, described methanation device also comprises heat recovery system; Described main methanation device passes into unstripped gas, and described auxiliary methanation device passes into carbonic acid gas.
As preferably, described methanation device is 2 grades, and the 1st grade is main methanation device, and the 2nd grade is auxiliary methanation device; Described main methanation device comprises the adiabatic methanation reactor of more than 2, and described auxiliary methanation device comprises the adiabatic methanation reactor of more than 1; Connect between described adiabatic methanation reactor.
As preferably, described main methanation device comprises the first adiabatic methanation reactor, the second adiabatic methanation reactor and the 3rd hot methanator, and described auxiliary methanation device comprises adiabatic methanation reactor one and adiabatic methanation reactor two.
Preferred further, the ratio that described first adiabatic methanation reactor, the second adiabatic methanation reactor and the 3rd hot methanator pass into unstripped gas is regulated by each methanator temperature out.
A methanation process for device synthesis high-quality coal preparing natural gas described above, is characterized in that, comprise the following steps:
(1) unstripped gas carried out purifying and carry out pre-treatment;
(2) unstripped gas after step (1) being processed passes into main methanation device and carries out methanation;
(3) carry out after recovery of heat from last adiabatic methanation reactor of main methanation device a part of high-temperature gas out through heat recovery system, mix with the unstripped gas entering first adiabatic methanation reactor after cycle gas system compression; Mix with the carbon dioxide of purification after a part of high-temperature gas enters auxiliary methanation device after recovery of heat in addition and carry out auxiliary methanation reaction.
(4) water outlet and gas product is separated from auxiliary methanation device gas cooling out.
As preferably, described carbon dioxide is parsed by low-temperature rectisol, is preheated to the light-off temperature of methanation catalyst in methanation device.
As preferably, after the preheating of described carbonic acid gas resolution gas, its hydrogen sulfide content is reduced to below 20ppb and enters auxiliary methanation device again and carry out methanation reaction.
Preferred further, the amount passing into auxiliary methanation device carbonic acid gas should make the adiabatic methanation reactor inlet gaseous fraction (H of auxiliary methanation device 2-CO 2)/(CO+CO 2) ratio should within the scope of 3.00-3.02.
Compared with prior art, the invention has the beneficial effects as follows: the present invention, by auxiliary methanation workshop section mend carbon technology, can reduce hydrogen content in gas product, improve gas product calorific value, obtain exit gas carbon dioxide content lower than 1%, hydrogen content lower than 2% high-quality synthetic natural gas.More existing supplementary carbon dioxide process, this technique is by optimizing carbonic acid gas position, hydrogen-carbon ratio in convenient adjustment reaction process, raising methanation reaction efficiency, main methanation operation (high-temperature methanation section) thermal load that reduces, optimization methanation workshop section heat utilization rate, reduce recycle gas compressor, carbon dioxide compressor energy consumption simultaneously.
1, more current coal synthetic natural gas technique, in this handicraft product, methane content is high, hydrogen content is low, and gas product calorific value is higher.
2, more general mend carbon technology, this technique is easy to regulate and methanator thermal load is relatively low, recycle gas compressor energy consumption is little.
3, owing to optimizing feed carbon dioxide position, carbon dioxide compressor less investment; Due to product, to fill methane content high, and subsequent product is easier to be separated, and follow-up each operation investment is less.
Figure of description
Fig. 1 is the process flow diagram of embodiment 1 in the present invention;
Fig. 2 is the process flow diagram of comparative example 1 in the present invention;
Fig. 3 is the process flow diagram of comparative example 2 in the present invention;
Reference numeral: 1-first adiabatic methanation reactor, 2-second adiabatic methanation reactor, the hot methanator of 3-the 3rd, 4-adiabatic methanation reactor one, 5-adiabatic methanation reactor two.
Embodiment
Below in conjunction with embodiment, foregoing invention content of the present invention is described in further detail.But this should be interpreted as that the scope of the above-mentioned theme of the present invention is only limitted to following embodiment.Without departing from the idea case in the present invention described above, according to ordinary skill knowledge and customary means, make various replacement and change, all should comprise within the scope of the invention.
A kind of methanation device synthesizing high-quality coal preparing natural gas, described methanation device is move hot methanation device outside multiple stage circulation, 1st grade is main methanation device, 2nd grade is auxiliary methanation device later, described main methanation device is connected with auxiliary methanation device, be provided with cycle gas system between described main methanation device and auxiliary methanation device, described methanation device also comprises heat recovery system; Described main methanation device passes into unstripped gas, and described auxiliary methanation device passes into carbonic acid gas.
A kind of methanation process synthesizing high-quality coal preparing natural gas, the step of this technique is: first by the total sulfur content that allows to methanation catalyst through superfinishing cleaner fine de-sulfur of synthetic gas after purification, and react entering methanation reaction operation after its preheating, multiple-stage adiabatic methanator is adopted to carry out multistage methanation reaction, wherein first step methanation reaction adopts >=2 adiabatic methanation reactors, to reduce single tower load, subsequent stages methanation reaction adopts adiabatic methanation reactor to react; Described multistage methanator is the methanation reaction of >=2 grades.
Obtain fresh synthetic gas and enter methanation reaction operation, first entered by synthetic gas gas in main methanation workshop section in each adiabatic reactor respectively, main methanation operation adopts series-parallel connection to arrange.Useless pot is utilized to reclaim reaction heat.The first high-temperature gas out generating 600-650 DEG C from last adiabatic reactor all mixes with the live gas entering the first adiabatic methane reactor after waste heat boiler carries out recovery of heat rear section gas converting heat to 180 DEG C after recycle gas compressor compression.Another strand of gas except circulation gas enters auxiliary methanation workshop section after recovery of heat, carbon dioxide any reactor inlet of auxiliary methanation workshop section with on a reactor outlet synthetic gas mix enter this auxiliary methane reactor after heat recuperation.
Present method can solve the excessive and problem not easily regulated of hydrogen in gas product, and the present invention adopts multistage methanation reaction, first utilizes main methanation adiabatic reactor to carry out methanation reaction to reduce CO+CO 2component concentration, more also supplement carbonic acid gas by auxiliary methanator, be convenient to the hydrogen made full use of in unstripped gas, improve methanation content in product.
Water coal slurry pressure gasification after low-temperature rectisol, coal generating gas synthesis gas compositional range following (vol% is butt):
H 2:74-75,CH 4:0.25-1,CO:20.0-24.0,CO 2:0-1.0,N 2:1-1.5
The gas below existed in citing adopts typical coal generating gas gaseous fraction, and all ratio or percentage compositions of relating to, all calculate with gas volume.
Embodiment 1:
Methanation device is 2 grades, and the 1st grade is main methanation device, and the 2nd grade is auxiliary methanation device; Described main methanation device comprises 3 adiabatic methanation reactors, and described auxiliary methanation device comprises 2 adiabatic methanation reactors; Connect between described adiabatic methanation reactor.
Main methanation device comprises the first adiabatic methanation reactor 1, second adiabatic methanation reactor 2 and the 3rd hot methanator 3, and described auxiliary methanation device comprises adiabatic methanation reactor 1 and adiabatic methanation reactor 25.
The present embodiment utilizes gas maked coal to prepare the methanation process of natural gas liquids as shown in Figure 1:
See Fig. 1, first unstripped gas is passed through purifying treatment.
Table 1 synthetic gas butt on average forms (vol%)
Title H 2 CO CO 2 N 2 CH 4 C 2H 4 C 3H 6 O 2
75.45 23.24 0.19 0.90 0.25 - - -
More than that typical case forms as methanation unstripped gas through the water coal slurry pressure gasification gas of purification.
Low-temperature rectisol resolves CO 2gas composition is as shown in table 2.
Table 2 CO 2component table
Composition CO 2 N 2 H 2S
Content V% >99 - <0.1ppm
Synthetic gas coal gas 1000Nm 3/ h, at 3.6MPa (G), under 320 DEG C of conditions, divide three strands and enter main methanation operation first adiabatic methane reactor 1, second adiabatic methanation reactor 2, the 3rd adiabatic methanation reactor 3 respectively for 29:31:40 by volume, and adopt recycle gas compressor that the section port band of gas is entered the first adiabatic methanation reactor inlet.The temperature out that circulation gas and the ratio entering the first adiabatic methanation reactor virgin gas control as required adjusts.
Work off one's feeling vent one's spleen and enter lower 2 grades of adiabatic methanation reactors, proceed reaction, supplement a certain amount of CO by low-temperature rectisol 2, supplement CO 2for low-temperature rectisol flash distillation obtains, wherein H 2s content is lower than 0.1ppm.According to processing requirement, supplement 11Nm 3/ h CO 2, after reaction.Finally obtain gas concentration lwevel and be less than 1%, density of hydrogen is less than the synthetic natural gas product of the high methane concentration of 2%.
Gas product output is as shown in table 3:
Table 3 embodiment 1 gas product butt on average forms (vol%)
Title H 2 CO CO 2 N 2 CH 4 C 2H 4 C 3H 6
1.64 28.6ppm 0.24 3.43 94.70 - -
Comparative example 1:
This comparative example adopts the feed gas composition identical with embodiment 1, adopts similar operational path, but does not add carbonic acid gas
Gas product output is as shown in table 4:
Table 4 comparative example gas product butt on average forms (vol%)
Title H 2 CO CO 2 N 2 CH 4 C 2H 4 C 3H 6 O 2
16.88 - - 3 79.90 - - -
Compare embodiment 1, in comparative example 1, H 2volume fraction still contains close to 17%.If adopt the mode of sulfur-resisting transformation and low-temp methanol washing process adjustment to change hydrogen-carbon ratio, need to consume more regulation time, cause quality product to fluctuate, even quality product occurs defective.Mend carbon technology can complete the adjustment of hydrogen-carbon ratio by relatively stable and easy-operating mode, flexible operation degree is high, little on technical process impact.
Comparative example 2:
This example is the comparative example of embodiment 1:
In the present embodiment, gaseous fraction condition, temperature, pressure are all identical with embodiment 1, and difference is, this comparative example adopts and supplements CO in methanation charging place 2technique.
Through reaction conditions similarly to Example 1, finally reach following gas product component
Table 5 comparative example 5 gas product butt on average forms (vol%)
Title H 2 CO CO 2 N 2 CH 4 C 2H 4 C 3H 6
1.64 28.6ppm 0.24 3.43 94.70 - -
Can obviously be found out by comparative example 2: comparatively embodiment 1, quality product does not change.
But because carbonic acid gas coal addition position is different, for maintaining main methanator temperature-stable.Namely embodiment 1 and comparative example 2 middle outlet temperature one show the state reaching Controlling System temperature-stable.Systemic circulation tolerance can compare.Equally, synthesizing tolerance is 1000Nm 3/ h.Main methanation first reactor outlet temperature maintains 640 DEG C.
Table 6 systemic circulation tolerance contrasts
Embodiment 1 Comparative example 2
Circulating flow rate (Nm 3/h) 780 815
Can find out, because coal addition position is different, identical for maintaining main methanation temperature, comparative example 2 needs increase by 4.49% circulating flow rate, and energy consumption is corresponding increase also.
CO 2flash off in low-temperature rectisol, through CO 2compressor enters methanation system.Consider system pressure drop, supplement CO 2position is more close to methanation work area back segment, and the compression ratio of needs is lower.According to practical experience, the pressure drop of usual coal preparing natural gas project methanation system is 0.70MPa.Wherein, the pressure drop of main methanation part is about 0.30MPa.CO 2select to add at work area back segment, can by CO 2top hole pressure decline 0.25-0.3MPa.

Claims (8)

1. one kind is synthesized the methanation device of high-quality coal preparing natural gas, it is characterized in that: described methanation device is move hot methanation device outside multiple stage circulation, 1st grade is main methanation device, 2nd grade is auxiliary methanation device later, described main methanation device is connected with auxiliary methanation device, be provided with cycle gas system between described main methanation device and auxiliary methanation device, described methanation device also comprises heat recovery system; Described main methanation device passes into unstripped gas, and described auxiliary methanation device passes into carbonic acid gas.
2. the methanation device of synthesis high-quality coal preparing natural gas according to claim 1, is characterized in that: described methanation device is 2 grades, and the 1st grade is main methanation device, and the 2nd grade is auxiliary methanation device; Described main methanation device comprises the adiabatic methanation reactor of more than 2, and described auxiliary methanation device comprises the adiabatic methanation reactor of more than 1; Connect between described adiabatic methanation reactor.
3. the methanation device of synthesis high-quality coal preparing natural gas according to claim 2, it is characterized in that: described main methanation device comprises the first adiabatic methanation reactor, the second adiabatic methanation reactor and the 3rd hot methanator, and described auxiliary methanation device comprises adiabatic methanation reactor one and adiabatic methanation reactor two.
4. the methanation device of synthesis high-quality coal preparing natural gas according to claim 3, is characterized in that: the ratio that described first adiabatic methanation reactor, the second adiabatic methanation reactor and the 3rd hot methanator pass into unstripped gas is regulated by each methanator temperature out.
5. a methanation process for the device synthesis high-quality coal preparing natural gas as described in any one of Claims 1-4, is characterized in that, comprise the following steps:
(1) unstripped gas carried out purifying and carry out pre-treatment;
(2) unstripped gas after step (1) being processed passes into main methanation device and carries out methanation;
(3) carry out after recovery of heat from last adiabatic methanation reactor of main methanation device a part of high-temperature gas out through heat recovery system, mix with the unstripped gas entering first adiabatic methanation reactor after cycle gas system compression; Mix with the carbon dioxide of purification after a part of high-temperature gas enters auxiliary methanation device after recovery of heat in addition and carry out auxiliary methanation reaction;
(4) water outlet and gas product is separated from auxiliary methanation device gas cooling out.
6. the methanation process of synthesis high-quality coal preparing natural gas according to claim 5, is characterized in that: described carbon dioxide is parsed by low-temperature rectisol, is preheated to the light-off temperature of methanation catalyst in methanation device.
7. the methanation process of synthesis high-quality coal preparing natural gas according to claim 6, is characterized in that: after the preheating of described carbonic acid gas resolution gas, its hydrogen sulfide content is reduced to below 20ppb and enters auxiliary methanation device again and carry out methanation reaction.
8. the methanation process of synthesis high-quality coal preparing natural gas according to claim 4, is characterized in that: the amount passing into auxiliary methanation device carbonic acid gas should make the adiabatic methanation reactor inlet gaseous fraction (H of auxiliary methanation device 2-CO 2)/(CO+CO 2) ratio should within the scope of 3.00-3.02.
CN201510247498.6A 2015-05-15 2015-05-15 Methanation device and process for synthesizing high-quality natural gas produced by coal CN104830391A (en)

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CN105385478A (en) * 2015-12-08 2016-03-09 大唐国际化工技术研究院有限公司 Method and apparatus for producing synthetic natural gas
CN107868686A (en) * 2017-11-15 2018-04-03 太原理工大学 A kind of energy-saving method without circulation coal synthetic natural gas full methanation

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Application publication date: 20150812