CN109420419B - Hydrate decomposer, mixed gas separation system and separation method - Google Patents
Hydrate decomposer, mixed gas separation system and separation method Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D29/00—Filters with filtering elements stationary during filtration, e.g. pressure or suction filters, not covered by groups B01D24/00 - B01D27/00; Filtering elements therefor
- B01D29/01—Filters with filtering elements stationary during filtration, e.g. pressure or suction filters, not covered by groups B01D24/00 - B01D27/00; Filtering elements therefor with flat filtering elements
- B01D29/03—Filters with filtering elements stationary during filtration, e.g. pressure or suction filters, not covered by groups B01D24/00 - B01D27/00; Filtering elements therefor with flat filtering elements self-supporting
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D3/00—Distillation or related exchange processes in which liquids are contacted with gaseous media, e.g. stripping
- B01D3/007—Energy recuperation; Heat pumps
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D3/00—Distillation or related exchange processes in which liquids are contacted with gaseous media, e.g. stripping
- B01D3/34—Distillation or related exchange processes in which liquids are contacted with gaseous media, e.g. stripping with one or more auxiliary substances
- B01D3/38—Steam distillation
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
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- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- General Chemical & Material Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- Gas Separation By Absorption (AREA)
Abstract
The invention discloses a hydrate decomposer, a mixed gas separation system and a separation method, wherein the hydrate decomposer comprises a slurry separation unit and a decomposition unit, and the slurry separation unit is communicated with the decomposition unit through a connecting channel; the slurry separation unit is divided into an upper part and a lower part by a filter screen clapboard component; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet, a connecting channel interface and a regenerated liquid storage tank from top to bottom. The decomposer can efficiently decompose the hydrate slurry with fluidity, and greatly reduces the energy consumption of heating decomposition of the hydrate slurry and cooling reuse of the regenerated working solution after decomposition. The invention also provides a mixed gas separation system and a method, which can ensure good fluidity of the hydrate and continuous, large-scale and long-period stable operation of a separation device by conveying materials in a hydrate slurry form and matching with the hydrate decomposer.
Description
Technical Field
The invention belongs to the field of gas, liquid and solid phase separation, and particularly relates to a hydrate decomposer, and a system and a method for separating mixed gas by using a hydrate technology.
Background
The hydrate technology is a hot point of research at home and abroad in recent years, besides being used as energy development and utilization, the gas hydrate related technology derives a plurality of new applications for gas storage and transportation, mixed gas and solution separation, sewage treatment, seawater desalination, CO2Sealing and cold storage technologies and other fields. In 2014, the eighth international gas hydrate congress called BeijingThe major society is held in developing countries for the first time, which shows that the research level of the hydrate in China has been accepted in the world, and meanwhile, the hot tide of a new round of energy development and related technical research of the hydrate in China is caused. In the application of various hydrate technologies, the mixed gas separation technology is paid much attention by virtue of the advantages of simple flow, mild conditions, flexible operation, greenness, no pollution and the like. The principle of separating the mixed gas by the hydrate technology is that the pressure difference of hydrates formed by different gases is large, and the separation of the components of the mixed gas can be realized by utilizing the pressure difference of the hydrates formed by the different gases and controlling the generation conditions. At present, hydrate separation technology is reported to be applied to the research of gas purification and purification in various fields of natural gas, flue gas, coal bed gas, synthetic gas, refinery gas, methane and the like.
The generation process of the hydrate is similar to a crystallization generation mechanism and comprises two processes of nucleation and growth, a liquid phase for separating gas by using the traditional hydrate method adopts an aqueous solution, the generated hydrate is generally in a crystallization form, the hydrate can agglomerate at a gas-liquid interface, the gas-liquid two-phase contact is hindered, the hydration speed is reduced, the mobility of the formed hydrate is poor, the formed hydrate is easy to aggregate and block, and the continuity and large-scale application of the related technology of the hydrate is directly restricted. However, many studies and patents do not consider the problem of hydrate prevalence, such as patents CN1301684A, CN1272618A, and CN101428190A, so that the industrial application of the technology is restricted. In order to solve the problem of the fluidity of the hydrate, the hydrate is processed into spherical particles and transported by the japan mitsui shipbuilding company, and a dehydration step is required, and the dehydrated hydrate is processed by a pelletizer, which makes the process complicated. Patents CN103030494A, CN101530719A, CN101554560A, CN1762929A, etc. adopt hydrate slurry form, and hydrate and solution which does not react to generate hydrate are circularly transported together to solve the fluidity problem, but the hydrate needs to be wholly heated up when being decomposed, and the temperature is wholly reduced after the gas is decomposed and released, so that energy consumption is greatly increased, and the operation cost is increased.
Disclosure of Invention
Aiming at the problems of poor fluidity and high energy consumption for hydrate decomposition of the existing hydrate method mixed gas separation technology, the invention provides the hydrate decomposer, the mixed gas separation system and the separation method, which can ensure the good fluidity of the hydrate, ensure the continuous, large-scale and long-period stable operation of a separation device and greatly reduce the problems of hydrate decomposition and high energy consumption for cooling caused by maintaining the fluidity of the hydrate.
In a first aspect, the present invention provides a hydrate decomposer, which comprises a slurry separation unit and a decomposition unit, wherein the slurry separation unit and the decomposition unit are communicated through a connecting channel; the slurry separation unit is divided into an upper part and a lower part by a filter screen partition plate assembly, the upper part is sequentially provided with a hydrate slurry inlet, a cleaning liquid inlet and a connecting channel interface from top to bottom, the lower part is a cold clear liquid storage tank, and the bottom of the storage tank is provided with a cold clear liquid outlet; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet, a connecting channel interface and a regeneration liquid storage tank from top to bottom, and the regeneration liquid storage tank is internally provided with a heat exchange unit, a stripping gas inlet and a regenerated hydrate working liquid outlet.
In the hydrate decomposer, the connecting channel is horizontally arranged or obliquely arranged at a certain angle, when the connecting channel is obliquely arranged, the connecting channel interface of the slurry separation unit is higher than the connecting channel interface of the decomposition unit, and the oblique angle forms 10-60 degrees, preferably 15-45 degrees with the horizontal plane. The lower plane of the connecting channel is arranged at 1/2-3/4 of the vertical height of the slurry separation unit.
In the hydrate decomposer, the filter screen partition plate assembly can be horizontally arranged or obliquely arranged at a certain angle, and the upper plane of the filter screen partition plate assembly and the lower plane of the connecting channel are arranged on the same plane. The filter screen clapboard component adopts any one of a filler structure, a wire mesh structure or a screen mesh structure to filter the hydrate slurry, the filtered hydrate-rich phase slurry (or particle crystallized) is conveyed to the decomposition unit, and the filtrate (cold clear liquid) enters a liquid storage tank below. The parameters of the filter screen separator assembly, such as pore size, porosity, filling thickness, etc., need to be determined according to the gas mixture system, the type of additive and what structural hydrate is formed.
In the hydrate decomposer, the hydrate slurry inlet is connected with a spraying assembly, the spraying assembly can adopt a liquid distributor known in the art, the hydrate slurry can be sprayed and uniformly distributed, and the coverage area is ensured to be the section of the whole slurry separation unit.
In the hydrate decomposer, the cleaning liquid inlet is connected with a nozzle, the nozzle can adopt any known form in the field, the cleaning liquid can be sprayed to the filter screen partition plate assembly at a high speed, the coverage area accounts for more than 70% of the area of the whole filter screen partition plate assembly, the washing and scouring effect on the filter screen partition plate assembly is realized, the nozzle is arranged at a certain inclination angle, the inclination direction faces towards the connecting channel, and the inclination angle and the vertical central line form 5-45 degrees, preferably 10-30 degrees.
In the hydrate decomposer, the liquid holding capacity of the cold clear liquid storage tank is 1/3-2/3 of the volume of the liquid storage tank.
In the hydrate decomposer, the liquid holding capacity of the regeneration liquid storage tank is 1/2-5/6 of the volume of the storage tank.
In the hydrate decomposer, a dividing wall type heat exchange device is arranged in the heat exchange unit, the hot fluid pipe running process heats the hydrate slurry in a coil pipe mode, and fins can be additionally arranged outside the coil pipe for strengthening heat exchange.
In the hydrate decomposer, a plurality of groups of baffle plates are arranged among the coil pipes of the heat exchange equipment in the decomposition unit, so that the functions of supporting the coil pipes and strengthening the heat exchange effect are achieved.
In the hydrate decomposer, the stripping gas inlet is connected with a gas distributor, the gas distributor and the cross section of the decomposition unit are maximally and uniformly distributed, so that the stripping gas is in reverse flowing contact with the hydrate-rich slurry in the decomposition unit, the gas distributor can adopt a gas distributor known in the field, the stripping gas can be recycled for the regenerated gas decomposed by the unit, and when the regenerated gas has a subsequent reprocessing process, the stripping gas can also be any gas which does not react with the subsequent processing process.
In the hydrate decomposer, a regenerated hydrate working solution outlet at the bottom of the decomposition unit is divided into two paths, one path is connected with the cleaning solution inlet through a pipeline, part of regenerated hydrate working solution discharged from the bottom of the decomposition unit is used as an internal circulation cleaning solution, and the volumetric flow rate of the regenerated hydrate working solution used as the internal circulation cleaning solution accounts for 1/5-1, preferably 1/3-1/2, of the volumetric flow rate of the total regenerated hydrate working solution.
In a second aspect, the invention provides a mixed gas separation system, which comprises a hydration reactor, a hydrate decomposer and a heat exchanger, wherein a mixed gas feeding pipeline is connected with a gas phase inlet of the hydrate reactor, a liquid phase outlet of the hydrate reactor is connected with a hydrate slurry inlet of a hydrate decomposer slurry separation unit through a pipeline, and a cold clear liquid outlet and a regenerated hydrate working liquid outlet of the hydrate decomposer are connected with a liquid phase inlet of the hydrate reactor after passing through a heat exchange device; the hydrate decomposer comprises a slurry separation unit and a decomposition unit, wherein the slurry separation unit is communicated with the decomposition unit through a connecting channel; the slurry separation unit is divided into an upper part and a lower part by a filter screen partition plate assembly, the upper part is sequentially provided with a hydrate slurry inlet, a cleaning liquid inlet and a connecting channel interface from top to bottom, the lower part is a cold clear liquid storage tank, and the bottom of the storage tank is provided with a cold clear liquid outlet; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet, a connecting channel interface and a regeneration liquid storage tank from top to bottom, and the regeneration liquid storage tank is internally provided with a heat exchange unit, a stripping gas inlet and a regenerated hydrate working liquid outlet.
In the separation system, the mixed gas feed line is provided with a compressor for ensuring that the mixed gas pressure is matched with the operation pressure of the hydration reactor.
In the separation system, a branch is led out from the hydrate decomposition gas outlet and is connected with the stripping gas inlet through a pipeline.
In the separation system, the connecting channel is horizontally arranged or obliquely arranged at a certain angle, when the connecting channel is obliquely arranged, the connecting channel interface of the slurry separation unit is higher than the connecting channel interface of the decomposition unit, and the oblique angle forms 10-60 degrees, preferably 15-45 degrees with the horizontal plane. The lower plane of the connecting channel is arranged at 1/2-3/4 of the vertical height of the slurry separation unit.
In the above separation system, the screen separator assembly is horizontally disposed or inclined at a certain angle, and the upper plane of the screen separator assembly is to be maintained to be in the same plane arrangement with the lower plane of the connecting passage. The filter screen clapboard component adopts any one of a filler structure, a wire mesh structure or a screen mesh structure to filter the hydrate slurry, the filtered hydrate-rich phase slurry (or particle crystallized) is conveyed to the decomposition unit, and the filtrate (cold clear liquid) enters a liquid storage tank below. The parameters of the filter screen separator assembly, such as pore size, porosity, filling thickness, etc., need to be determined according to the gas mixture system, the type of additive and what structural hydrate is formed.
In the separation system, the hydrate slurry inlet is connected with a spraying assembly, the spraying assembly can adopt a liquid distributor known in the field, the hydrate slurry can be sprayed and uniformly distributed, and the coverage area is ensured to be the section of the whole slurry separation unit.
In the above-mentioned piece-rate separation system, the washing liquid entry is connected with the nozzle, the nozzle can adopt the known arbitrary form in this field, can spray the washing liquid to filter screen baffle subassembly at a high speed, and the area of coverage accounts for more than 70% of whole filter screen baffle subassembly area, realizes the washing and scouring action to filter screen baffle subassembly, and the nozzle is arranged at certain inclination, and the incline direction is towards the connected passage, and inclination becomes 5 ~ 45, preferred 10 ~ 30 with perpendicular central line.
In the separation system, the liquid holding capacity of the cold clear liquid storage tank is 1/3-2/3 of the volume of the liquid storage tank.
In the separation system, the liquid holding capacity of the regeneration liquid storage tank is 1/2-5/6 of the volume of the liquid storage tank.
In the separation system, a dividing wall type heat exchange device is arranged in the heat exchange unit, the hot fluid pipe running process heats the hydrate slurry in a coil pipe mode, and fins can be additionally arranged outside the coil pipe for strengthening heat exchange.
In the separation system, a plurality of groups of baffle plates are arranged among the coil pipes of the heat exchange equipment in the decomposition unit, so that the functions of supporting the coil pipes and strengthening the heat exchange effect are achieved.
In the separation system, the stripping gas inlet is connected with a gas distributor, the gas distributor and the cross section of the decomposition unit are maximally and uniformly distributed, so that the stripping gas is in reverse flow contact with the hydrate-rich slurry in the decomposition unit, the gas distributor can adopt a gas distributor known in the field, the stripping gas can be recycled for the regenerated gas decomposed by the unit, and when the regenerated gas has a subsequent reprocessing process, the stripping gas can also be any gas which does not react with the subsequent processing process.
In the separation system, the regenerated hydrate working solution outlet at the bottom of the decomposition unit is divided into two paths, one path is connected with the cleaning solution inlet through a pipeline, the regenerated hydrate working solution discharged from the bottom of part of the decomposition unit is used as an internal circulation cleaning solution, and the volumetric flow rate of the regenerated hydrate working solution used as the internal circulation cleaning solution accounts for 1/5-1, preferably 1/3-1/2, of the volumetric flow rate of the total regenerated hydrate working solution.
In the above separation system, the hydration reactor is a device which is beneficial to gas-liquid mass transfer and has good heat transfer effect, and the form is not limited, and the hydration reactor can be one of stirring type, spray type, bubbling type, sieve plate type, packing type, supergravity or impact flow type and the like.
In a third aspect, the present invention provides a method for separating a mixture gas, comprising the steps of:
(1) the mixed gas enters a hydration reactor to react with the hydrate working solution, the components which are easy to generate the hydrate in the mixed gas react with the hydrate working solution and enter a hydrate phase to form hydrate slurry, and the components which are difficult to generate the hydrate are enriched in a gas phase and discharged out of the hydration reactor;
(2) enabling the gas-rich hydrate slurry obtained in the step (1) to enter a hydrate decomposer, processing the gas-rich hydrate slurry by a slurry separation unit of the decomposer to obtain cold clear liquid and hydrate-rich phase slurry, and enabling the cold clear liquid to enter a cold clear liquid storage tank below the cold clear liquid storage tank;
(3) enabling the hydrate-rich phase slurry obtained in the step (2) to enter a decomposition unit for treatment under the action of a cleaning solution, and enabling the slurry to be in countercurrent contact with stripping gas introduced from the bottom of the decomposition unit to decompose and release high-concentration absorbed gas, thereby obtaining regenerated hydrate working solution;
(4) and (3) mixing the cold clear liquid obtained in the step (2) with the regenerated hydrate working solution obtained in the step (3), cooling, and returning to the hydration reactor for recycling.
In the above mixed gas separation method, the operating conditions of the hydration reactor are as follows: the pressure is 0.1-5.0 Mpa, the temperature is 0-15 ℃, and the specific operation conditions need to be determined according to the treated mixed gas system and the selected additive type.
In the above mixed gas separation method, the hydrate working solution in step (1) may be an aqueous solution, or various thermodynamic and kinetic accelerators such as one or more of Sodium Dodecyl Sulfate (SDS), Sodium Dodecyl Benzene Sulfonate (SDBS), linear sodium alkyl sulfonate (LAB-SA), Alkyl Polyglycoside (APG), Tetrahydrofuran (THF), tetrabutylammonium bromide (TBAB), Cyclopentane (CP) and acetone may be added.
In the above mixed gas separation method, the hydrate working fluid in step (1) may also be an oil-water mixed emulsion, and an oil substance with good fluidity, such as one or more of kerosene, diesel oil and silicone oil, may be added to the working fluid and used in combination with a hydrophilic emulsifier.
In the above mixed gas separation method, in the hydration reactor in step (1), the hydrate slurry refers to a mixed solution of a formed hydrate and an unreacted hydrate working solution, and the volume ratio of the hydrate in the hydrate slurry is controlled to be 30-80%, preferably 50-70%.
In the above mixed gas separation method, the operating conditions of the hydrate decomposer in the step (2) are as follows: the pressure is 0.05 Mpa-3.0 Mpa, the temperature of the separation unit is 0-10 ℃, and the temperature of the decomposition unit is 10-40 ℃.
In the above mixed gas separation method, the slurry separation unit in step (2) separates the hydrate slurry into a cold clear liquid and a hydrate-rich phase slurry, the hydrate volume content in the cold clear liquid is less than 10%, and the hydrate volume content in the hydrate-rich phase slurry is more than 80%.
In the above mixed gas separation method, the stripping gas in step (2) may be any gas that does not react with the subsequent processing, such as nitrogen, inert gas, or may be a part of the cycle of the decomposed gas obtained from the decomposition unit.
In the mixed gas separation method, the cold clear liquid obtained in the step (2) and the regenerated hydrate working solution obtained in the step (3) are mixed and cooled to match the temperature of the hydration reactor in the step (1), and the mixture is returned to the hydration reactor for recycling.
In the above mixed gas separation method, the mixed gas may be a mixed gas purification (CH) of natural gas and biogas4/CO2) Decarbonization of flue gas (N)2/CO2) Coal bed methane separation (CH)4/N2) Decarbonization of synthesis gas (CO)2/H2) Refinery dry gas recovery (light hydrocarbon/H)2) Processing, and the like.
The heat in the hydrate decomposer of the method can be heated by steam, high-temperature flue gas or tail gas can be utilized, and the reaction heat and the process waste heat of peripheral devices can be utilized.
Compared with the prior art, the hydrate decomposer, the mixed gas separation system and the separation method have the following advantages:
(1) the hydrate decomposer provided by the invention is provided with a slurry separation unit and a decomposition unit, and is used for filtering and separating hydrate slurry and deeply decomposing the hydrate slurry respectively. The slurry separation unit separates the hydrate slurry into a hydrate-rich phase and a cold clear liquid phase: the hydrate content in the cold clear liquid phase is extremely low, the temperature does not need to be raised, and the lower temperature can be maintained for recycling; the hydrate in the hydrate-rich phase accounts for more than 80 percent, the decomposition unit is heated and decomposed, the high-efficiency heat exchange and stripping means are matched to enhance the decomposition of the hydrate, and the leading-out part of the regenerated working solution is used for washing and scouring the filter screen partition plate assembly of the slurry separation unit. The decomposer with the mode can efficiently decompose hydrate slurry with fluidity, has high hydrate decomposition efficiency, self-cleaning function and easy maintenance, and greatly reduces the energy consumption of heating decomposition of the hydrate slurry and cooling and recycling of working solution after decomposition.
(2) The mixed gas separation system and the method provided by the invention have mild operation conditions, can separate the mixed gas at the temperature of more than 0 ℃, have moderate operation pressure, and have the advantages of short flow, simple and flexible operation, high safety, environmental protection, no pollution and the like. The hydrate is enabled to have good fluidity by conveying materials between the hydrate reactor and the hydrate decomposer in a hydrate slurry form, and the hydrate decomposer provided by the invention is matched, so that the problem of restricting the continuity of the hydrate technology for separating the mixed gas is solved, the energy consumption cost brought by maintaining the hydrate fluidity is greatly reduced, the operation cost of the device is reduced, and the continuous, large-scale and long-period stable operation of the separation device is ensured.
Drawings
FIG. 1 is a schematic structural view of a hydrate decomposer according to the present invention.
FIG. 2 is a schematic view of a mixed gas separation system according to the present invention.
Detailed Description
The hydrate decomposer and the mixed gas separation system of the invention are described in detail with reference to the accompanying drawings and examples, but the invention is not limited thereby.
As shown in fig. 1, the present invention provides a hydrate decomposer comprising a slurry separation unit and a decomposition unit which are communicated through a connection passage 12; the slurry separation unit is divided into an upper part and a lower part by a filter screen partition plate assembly 5, the upper part is sequentially provided with a hydrate slurry inlet 1, a cleaning liquid inlet 3 and a connecting channel interface 19 from top to bottom, the lower part is a cold clear liquid storage tank 6, and the bottom of the storage tank is provided with a cold clear liquid outlet 13; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet 11, a connecting channel interface 20 and a regenerated liquid storage tank 7 from top to bottom, and the regenerated liquid storage tank 7 is sequentially provided with a heat exchange unit 10, a stripping gas inlet 8 and a regenerated hydrate working liquid outlet 14 from top to bottom. Wherein the hydrate slurry inlet 1 of the separation unit is connected with a spraying assembly 2; the inner circulation cleaning liquid inlet 3 is connected with a cleaning nozzle 4; the stripping gas inlet 8 of the deep decomposition unit is connected with a stripping gas distributor 9; one end of the heat exchange device 10 is provided with a heat medium inlet 15, and the other end is provided with a heat medium outlet 16; and a plurality of groups of baffle plates 17 are arranged among the coil pipes of the heat exchange unit in the regeneration liquid storage tank 7.
The working process of the hydrate decomposer is as follows: the hydrate slurry is introduced into the decomposer through a hydrate slurry inlet 1 of the hydrate decomposer, the hydrate slurry is sprayed downwards through a spraying assembly 2, the sprayed hydrate slurry is filtered by a filter screen partition plate assembly 5 and is divided into a hydrate-rich phase and a cold clear liquid phase, a washing nozzle 4 above the filter screen partition plate assembly 5 realizes washing and scouring of the filter screen partition plate assembly 5 through continuous spraying of an internal circulation cleaning liquid, the filtered cold clear liquid falls to a cold clear liquid reservoir 6, the cold clear liquid circulates at a cold clear liquid outlet 13 at the bottom of the reservoir to be recycled to a hydrate reactor, the hydrate-rich phase enters a regeneration liquid reservoir 7 through a connecting channel 12, the hydrate-rich phase exchanges heat with a heat exchange device 10 in the regeneration liquid reservoir 7 and sequentially passes through a channel formed by a baffling baffle 17, the hydrate-rich phase is continuously heated and decomposed and releases gas in the falling process, and simultaneously, stripping gas is introduced into the bottom of the regeneration liquid reservoir 7 through a stripping gas inlet 8, the stripping gas is uniformly distributed by a stripping gas distributor 9 and then is in countercurrent contact with the hydrate slurry, the hydrate is decomposed to release high-concentration absorbed gas, the gas is finally discharged through a hydrate decomposition gas outlet 11, the decomposed regenerated hydrate working solution is discharged through a regenerated hydrate working solution outlet 14 at the bottom of a regenerated solution reservoir 7, part of the regenerated hydrate working solution 18 is used as an internal circulation washing solution and enters a slurry separation unit to wash the filter screen partition plate assembly 5, and the rest regenerated working solution is subjected to cooling treatment and then is conveyed to a hydrate reactor.
As shown in fig. 2, the present invention further provides a mixed gas separation system, which comprises a hydration reactor 24, a hydrate decomposer 27 and a heat exchanger 29, wherein the hydrate decomposer is the hydrate decomposer shown in fig. 1; the mixed gas feeding pipeline 21 is connected with a gas phase inlet of a hydrate reactor 24, and a compressor 22 is arranged on the feeding pipeline 21; the liquid phase outlet of the hydrate reactor is connected with the hydrate slurry inlet of the hydrate decomposer 27 through a pipeline 26, and the gas phase outlet of the hydrate reactor is connected with a separation tail gas pipeline 25; a cold clear liquid outlet pipeline 28 and a regenerated working liquid outlet pipeline 31 of the hydrate decomposer are connected with inlets of a heat exchange device 29, and an outlet of the heat exchange device is connected with a liquid phase inlet of the hydrate reactor 24 through a pipeline 30; the inlet of the hydrate decomposer heat exchange unit is connected with a heat medium incoming line 33, and the outlet of the hydrate decomposer heat exchange unit is connected with a heat medium return line 34; the hydrate decomposition gas outlet is connected with a decomposition regeneration gas pipeline 32, and a branch pipeline 35 led out from the decomposition regeneration gas pipeline 32 is connected with a stripping gas inlet of the hydrate decomposer 27; the stripping gas inlet of the hydrate decomposer 27 is connected to a stripping gas line 36.
The process of treating the mixed gas by adopting the mixed gas separation system provided by the invention comprises the following steps: the mixed gas 21 enters the hydration reactor 24 after being pressurized by the compressor 22, in the hydration reactor 24, gas components which are easy to generate hydrate enter a hydrate phase (solid-liquid phase) to form slurry, and components which are not easy to generate hydrate are enriched in a gas phase and discharged through a tail gas pipeline 25, so that the separation of the mixed gas is realized. The gas-rich hydrate slurry in the hydration reactor is led via line 26 to a hydrate decomposer 27, where the slurry is first treated in a separation unit of the decomposer to obtain a cold clear liquid and a hydrate-rich phase slurry, the cold clear liquid is led to a lower cold clear liquid reservoir and discharged via line 28, and the hydrate-rich phase slurry is led to the decomposition unit. The hydrate-rich slurry in the decomposition unit is heated and is in countercurrent contact with the stripping gas introduced from the bottom of the decomposition unit, the used stripping gas is provided by an external stripping gas pipeline 36 or a branch pipeline 35 led out by regenerated gas, the hydrate slurry is decomposed to release high-concentration absorbed gas, regenerated hydrate working solution is obtained at the same time, the released gas is discharged through a decomposed regenerated gas pipeline 32, and the regenerated hydrate working solution 31 and the cold clear liquid 28 enter a heat exchange device 29 together to be cooled and then return to the hydration reactor 24 for recycling.
Example 1
The hydrate decomposer provided by the invention is selected, and the process flow shown in figure 2 is adopted to separate the coal bed gas, namely CH in the coal bed gas4The volume content is about 40 percent, and the rest is N2And O2And the like. The coal bed gas 21 passes through a compressor 22, pressurizing to 0.4Mpa, entering a hydrate reactor 24 to perform hydration reaction with hydrate working solution, controlling the generation amount of hydrate to be about 60% of the total volume of hydrate slurry under the conditions that the pressure of the hydration reactor 24 is 0.4Mpa and the temperature is 4 ℃, the hydrate working solution is aqueous solution containing THF (6% molar concentration) and SDS (300 ppm) SDS, and treating mixed gas to discharge CH (CH) in gas 25 of the hydration reactor4The content is less than 5 percent, and the requirement of safe emission (CH) is met4Explosion limit of 5% -15%); conveying the hydrate slurry 26 to a hydrate decomposer 27, wherein the condition of the hydrate decomposer 27 is that the pressure is 0.1Mpa, the hydrate slurry 26 is divided into a hydrate-rich phase accounting for 70% of the total slurry amount and a cold clear liquid phase accounting for 30% of the total slurry amount in a slurry separation unit, wherein about 9% of the hydrate content in the cold clear liquid enters a cold clear liquid storage tank, about 82% of the hydrate content in the cold clear liquid enters a regeneration liquid storage tank, the temperature of the regeneration liquid storage tank is maintained at 25 ℃ through heat exchange equipment, and CH in gas 32 released from the hydrate decomposer4The content is more than 80 percent, 1/3 of the decomposed and released gas is returned to the bottom of a regenerative liquid storage tank to be used as stripping gas 35, and the obtained high-concentration CH4The gas may be used as a fuel or further processed into a natural gas product. The process for treating the coal bed gas not only avoids the explosion risk of oxygen-enriched coal bed gas discharge, but also recovers and obtains high-concentration CH4A gas. The whole treatment process can ensure good fluidity of the hydrate in the device, and the double-tower graded decomposer is adopted to regenerate hydrate slurry, so that the energy consumption is greatly reduced.
Comparative example 1
The method is the same as that in the embodiment 1, except that the hydrate decomposer is in a conventional single-tower form, when the same treatment effect is achieved, because the double-tower hierarchical decomposer adopted in the embodiment 1 decomposes the hydrate slurry into a hydrate-rich phase and a cold clear liquid phase through the separation unit, and then only the hydrate-rich phase (the hydrate content is 82%) accounting for 70% of the total slurry is subjected to deep decomposition treatment, while the conventional decomposer adopted in the comparative example needs to integrally heat the hydrate and the slurry (the hydrate content is 60%) which does not react to generate the hydrate, and the regenerated liquid obtained after decomposing and releasing gas is integrally cooled, so that the energy consumption is greatly increased, and the operation cost is increased. Compared with the embodiment 1, the total energy consumption of the working solution for cooling after the hydrate slurry is heated and decomposed and the working solution is decomposed in the comparative example is increased by more than 40%.
Example 2
The hydrate decomposer provided by the invention is selected, and the process flow shown in figure 2 is adopted to separate the marsh gas, wherein CH is contained in the marsh gas4The volume content is about 60 percent, and the rest is CO2Mainly impurity gases. Pressurizing the marsh gas 21 to 0.4Mpa by a compressor 22, then entering a hydrate reactor 24 to perform hydration reaction with hydrate working solution, wherein the hydrate reactor 24 is under the conditions of 3.0Mpa of pressure and 3 ℃ of temperature, the hydrate working solution is an aqueous solution containing 4% of CP by volume fraction and 0.3% of TBAB by mole fraction, the reaction is controlled to control the hydrate generation amount to be about 65% of the total volume amount of hydrate slurry, and the mixed gas is treated to discharge CH in gas 25 of the hydration reactor4The content is about 90 percent; conveying the hydrate slurry 26 to a hydrate decomposer 27, wherein the condition of the hydrate decomposer 27 is that the pressure is 0.8Mpa, the hydrate slurry 26 is separated into a hydrate-rich phase accounting for 74 percent of the total slurry amount and a cold clear liquid phase accounting for 26 percent of the total slurry amount in a slurry separation unit, wherein the hydrate content in the cold clear liquid is about 8 percent and enters a cold clear liquid storage tank, the hydrate content in the hydrate-rich liquid is about 84 percent and enters a regeneration liquid storage tank, the temperature of the regeneration liquid storage tank is maintained at 22 ℃ through heat exchange equipment, and CO in gas 32 released in the hydrate decomposer21/2 with the content higher than 80 percent and decomposed and released gas returns to the bottom of the regenerated liquid storage tank to be used as the stripping gas 35, and the obtained high-concentration CO2And (5) recovering the gas. The biogas is treated by the process to respectively obtain high-concentration CH4Gas and high concentration of CO2Purifying the marsh gas and simultaneously purifying CO2Gas capture, not only obtaining high-value fuel, but also realizing CO2Emission reduction, and energy and environmental protection benefits. The process not only solves the problem of poor mobility of the hydrate and ensures the continuous, large-scale and long-period stable operation of the separation device, but also adopts the double-tower hierarchical decomposer to regenerate the hydrate slurry, thereby greatly reducing the energy consumption and further reducing the operation cost of the device.
Comparative example 2
The method is the same as that in the embodiment 2, except that the hydrate decomposer adopts a conventional single-tower form, when the same treatment effect is achieved, because the double-tower hierarchical decomposer adopted in the embodiment 1 decomposes the hydrate slurry into 74% of a hydrate-rich phase and 26% of a cold clear liquid phase through the separation unit, and then only the hydrate-rich phase accounting for 74% of the total slurry is subjected to deep decomposition treatment, while the conventional decomposer adopted in the comparative example needs to integrally heat the hydrate and the slurry which does not react to generate the hydrate, and integrally cool the regenerated liquid obtained after decomposing the released gas, so that the energy consumption is greatly increased, and the operation cost is increased. Compared with the embodiment 1, the total energy consumption of the working solution for cooling after the hydrate slurry is heated and decomposed and the hydrate slurry is decomposed in the comparative example is increased by about 35%.
Claims (35)
1. A hydrate decomposer comprises a slurry separation unit and a decomposition unit, wherein the slurry separation unit is communicated with the decomposition unit through a connecting channel; the slurry separation unit is divided into an upper part and a lower part by a filter screen partition plate assembly, the upper part is sequentially provided with a hydrate slurry inlet, a cleaning liquid inlet and a connecting channel interface from top to bottom, the lower part is a cold clear liquid storage tank, and the bottom of the storage tank is provided with a cold clear liquid outlet; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet, a connecting channel interface and a regeneration liquid storage tank from top to bottom, a heat exchange unit, a stripping gas inlet and a regeneration hydrate working liquid outlet are arranged in the regeneration liquid storage tank, the regeneration hydrate working liquid outlet is divided into two paths, and one path is connected with the cleaning liquid inlet through a pipeline.
2. A hydrate decomposer according to claim 1, wherein the connection channel is arranged horizontally or inclined at an angle such that the slurry separation unit connection channel interface is higher than the decomposition unit connection channel interface, the angle being between 10 ° and 60 ° from the horizontal.
3. A hydrate decomposer according to claim 1, wherein the connection channel is arranged horizontally or inclined at an angle such that the slurry separation unit connection channel interface is higher than the decomposition unit connection channel interface, the angle being between 15 ° and 45 ° to the horizontal.
4. A hydrate decomposer according to claim 1, wherein the lower plane of the connecting passage is disposed at a vertical height of from 1/2 to 3/4 of the slurry separation unit.
5. The hydrate decomposer according to claim 1, wherein the screen partition plate assembly is arranged horizontally or inclined at an angle, and an upper plane of the screen partition plate assembly is arranged in the same plane as a lower plane of the connecting passage.
6. The hydrate decomposer according to claim 1, wherein the screen partition plate assembly adopts any one of a packing structure, a wire mesh structure or a screen structure.
7. A hydrate decomposer according to claim 1, wherein the liquid hold-up of the cold clear liquid reservoir is from 1/3 to 2/3 of the volume of the reservoir.
8. A hydrate decomposer according to claim 1, wherein the regenerating liquid reservoir has a liquid hold up of 1/2 to 5/6 of the volume of the reservoir.
9. A hydrate decomposer according to claim 1, wherein a dividing wall type heat exchange device is arranged in the heat exchange unit, and the hot fluid pipe running process heats the hydrate slurry in a coil form.
10. A hydrate decomposer according to claim 9, wherein a plurality of sets of baffle plates are arranged between coils of the heat exchange equipment in the decomposition unit.
11. A mixed gas separation system comprises a hydration reactor, a hydrate decomposer and a heat exchanger, wherein a mixed gas feeding pipeline is connected with a gas phase inlet of the hydrate reactor, a liquid phase outlet of the hydrate reactor is connected with a hydrate slurry inlet of a hydrate decomposer slurry separation unit through a pipeline, and a cold clear liquid outlet and a regenerated hydrate working liquid outlet of the hydrate decomposer are connected with a liquid phase inlet of the hydrate reactor after passing through a heat exchange device; the hydrate decomposer comprises a slurry separation unit and a decomposition unit, wherein the slurry separation unit is communicated with the decomposition unit through a connecting channel; the slurry separation unit is divided into an upper part and a lower part by a filter screen partition plate assembly, the upper part is sequentially provided with a hydrate slurry inlet, a cleaning liquid inlet and a connecting channel interface from top to bottom, the lower part is a cold clear liquid storage tank, and the bottom of the storage tank is provided with a cold clear liquid outlet; the decomposition unit is sequentially provided with a hydrate decomposition gas outlet, a connecting channel interface and a regeneration liquid storage tank from top to bottom, and the regeneration liquid storage tank is internally provided with a heat exchange unit, a stripping gas inlet and a regenerated hydrate working liquid outlet.
12. The separation system according to claim 11, wherein a compressor is provided on the mixed gas feed line for ensuring that the mixed gas pressure matches the hydration reactor operating pressure.
13. A separation system as claimed in claim 11, wherein a branch from the hydrate splitting gas outlet is connected via a line to the stripping gas inlet.
14. A separation system as claimed in claim 11, wherein the connecting channel is arranged horizontally or inclined at an angle such that the slurry separation unit connecting channel interface is higher than the decomposition unit connecting channel interface and the angle of inclination is between 10 ° and 60 ° from the horizontal.
15. A separation system as claimed in claim 11, wherein the connecting channel is arranged horizontally or inclined at an angle such that the slurry separation unit connecting channel interface is higher than the decomposition unit connecting channel interface and the angle of inclination is between 15 ° and 45 ° to the horizontal.
16. The separation system according to claim 11 wherein the lower plane of the connecting channel is located between 1/2 and 3/4 of the vertical height of the slurry separation unit.
17. A separation system as claimed in claim 11, wherein the screen cloth baffle assembly is arranged horizontally or inclined at an angle, the upper plane of the screen cloth baffle assembly being maintained in the same planar arrangement as the lower plane of the connecting passage.
18. The separation system according to claim 11 wherein said screen spacer assembly employs any one of a packing structure, a wire mesh structure, or a screen structure.
19. A separation system as claimed in claim 11, wherein the cold clear liquid reservoir liquid hold-up is 1/3 to 2/3 of the reservoir volume.
20. A separation system as claimed in claim 11, wherein the regeneration liquid reservoir liquid hold up is 1/2 to 5/6 of the reservoir volume.
21. A separation system as claimed in claim 11, wherein a dividing wall type heat exchanger is provided in the heat exchange unit, and the hot fluid pipe passes through the coil to heat the hydrate slurry.
22. A separation system as claimed in claim 21, wherein a plurality of sets of baffles are provided between the coils of the heat exchange means within the decomposition unit.
23. The separation system according to claim 11, wherein the regenerated hydrate working solution outlet at the bottom of the decomposition unit is divided into two paths, one path is connected with the cleaning solution inlet through a pipeline, and part of the regenerated hydrate working solution discharged from the bottom of the decomposition unit is used as an internal circulation cleaning solution.
24. A method for separating a mixture gas using the separation system according to any one of claims 11 to 23, the method comprising the steps of:
(1) the mixed gas enters a hydration reactor to react with the hydrate working solution, the components which are easy to generate the hydrate in the mixed gas react with the hydrate working solution and enter a hydrate phase to form hydrate slurry, and the components which are difficult to generate the hydrate are enriched in a gas phase and discharged out of the hydration reactor;
(2) enabling the gas-rich hydrate slurry obtained in the step (1) to enter a hydrate decomposer, processing the gas-rich hydrate slurry by a slurry separation unit of the decomposer to obtain cold clear liquid and hydrate-rich phase slurry, and enabling the cold clear liquid to enter a cold clear liquid storage tank below the cold clear liquid storage tank;
(3) enabling the hydrate-rich phase slurry obtained in the step (2) to enter a decomposition unit for treatment under the action of a cleaning solution, and enabling the slurry to be in countercurrent contact with stripping gas introduced from the bottom of the decomposition unit to decompose and release high-concentration absorbed gas, thereby obtaining regenerated hydrate working solution;
(4) and (3) mixing the cold clear liquid obtained in the step (2) with the regenerated hydrate working solution obtained in the step (3), cooling, and returning to the hydration reactor for recycling.
25. The method for separating a mixed gas as claimed in claim 24, wherein the operation conditions of the hydration reactor are: the pressure is 0.1-5.0 Mpa, and the temperature is 0-15 ℃.
26. The method for separating mixed gas according to claim 24, wherein the hydrate working fluid in the step (1) is an aqueous solution, or various thermodynamic and kinetic promoters are added.
27. The method for separating mixed gas according to claim 24, wherein the hydrate working fluid in the step (1) is an oil-water mixed emulsion, and oil substances with better fluidity are added into the working fluid, and the oil substances are one or more of kerosene, diesel oil and silicone oil and are matched with a hydrophilic emulsifier for simultaneous use.
28. The method for separating mixed gas according to claim 24, wherein in the hydration reactor in the step (1), hydrate slurry refers to a mixed solution of formed hydrate and unreacted hydrate working solution, and the volume ratio of the hydrate in the hydrate slurry is controlled to be 30-80%.
29. The method for separating mixed gas according to claim 24, wherein in the hydration reactor in the step (1), hydrate slurry refers to a mixed solution of formed hydrate and unreacted hydrate working solution, and the volume ratio of the hydrate in the hydrate slurry is controlled to be 50-70%.
30. The method for separating a mixed gas according to claim 24, wherein the operating conditions of the hydrate decomposer in the step (2) are as follows: the pressure is 0.05 Mpa-3.0 Mpa, the temperature of the slurry separation unit is 0-10 ℃, and the temperature of the decomposition unit is 10-40 ℃.
31. The method for separating mixed gas according to claim 24, wherein the slurry separation unit in the step (2) separates the hydrate slurry into a cold clear liquid and a hydrate-rich phase slurry, the hydrate volume content in the cold clear liquid is less than 10%, and the hydrate volume content in the hydrate-rich phase slurry is more than 80%.
32. The method for separating a mixed gas according to claim 24, wherein the stripping gas in the step (3) is any gas which does not react with a subsequent process.
33. The method for separating a mixed gas according to claim 32, wherein the stripping gas in the step (3) is nitrogen or an inert gas.
34. The method for separating a mixed gas as claimed in claim 24, wherein the stripping gas in the step (3) is a decomposed gas obtained from the decomposing unit.
35. The method for separating the mixed gas as claimed in claim 24, wherein the cold clear liquid obtained in the step (2) is mixed with the regenerated hydrate working solution obtained in the step (3), is cooled to match the temperature of the hydration reactor in the step (1), and is returned to the hydration reactor for recycling.
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| CN111974165B (en) * | 2019-05-22 | 2022-03-18 | 中国石油大学(北京) | Method and device for removing volatile organic compounds in mixed gas by hydration |
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| DE10045586C2 (en) * | 2000-09-15 | 2002-07-18 | Alstom Power Boiler Gmbh | Process and device for cleaning smoke gases containing sulfur dioxide |
| CN100404483C (en) * | 2005-09-23 | 2008-07-23 | 中国石油大学(北京) | Hydration, pressure swing adsorption and deep cooling combined process for separating ethene cracking gas |
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| CN204022772U (en) * | 2014-08-08 | 2014-12-17 | 辽宁石油化工大学 | A kind of gas hydrate slurry liquid decomposer |
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Effective date of registration: 20230927 Address after: 100728 No. 22 North Main Street, Chaoyang District, Beijing, Chaoyangmen Patentee after: CHINA PETROLEUM & CHEMICAL Corp. Patentee after: Sinopec (Dalian) Petrochemical Research Institute Co.,Ltd. Address before: 100728 No. 22 North Main Street, Chaoyang District, Beijing, Chaoyangmen Patentee before: CHINA PETROLEUM & CHEMICAL Corp. Patentee before: DALIAN RESEARCH INSTITUTE OF PETROLEUM AND PETROCHEMICALS, SINOPEC Corp. |