CN111068464B - System and method for collecting gas containing volatile organic compounds and preparing carbon nano material - Google Patents
System and method for collecting gas containing volatile organic compounds and preparing carbon nano material Download PDFInfo
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- B01J2220/00—Aspects relating to sorbent materials
- B01J2220/40—Aspects relating to the composition of sorbent or filter aid materials
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- B01J2220/4812—Sorbents characterised by the starting material used for their preparation the starting material being of organic character
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Abstract
The system comprises an absorption/desorption subsystem, an adsorption/desorption subsystem and a carbonization subsystem, and optionally comprises a gas-liquid separation subsystem; the method for collecting the gas containing the volatile organic compounds and preparing the carbon nano material by using the system comprises the steps of firstly passing the gas containing the volatile organic compounds through an absorption/desorption subsystem to remove most of the volatile organic compounds; then the effluent is discharged after reaching the standard through an adsorption/desorption subsystem; performing desorption or desorption operation when the absorption or adsorption is close to saturation; condensing the organic matters obtained by desorption or desorption in a gas-liquid separation subsystem, and collecting liquid (recycling or retreatment); and the separated gas enters a carbonization subsystem to generate a carbon nano material at high temperature, and the tail gas of the carbonization subsystem is combined with the tail gas of an adsorption/desorption subsystem and then is discharged after reaching the standard. The invention prolongs the service cycle of the adsorbent and reduces the energy consumption; volatile organic compounds are changed into carbon nano materials, and the cost of the adsorbent is reduced.
Description
Technical Field
The invention belongs to the technical field of chemical industry and environmental protection, and particularly relates to a system and a method for collecting gas containing volatile organic compounds and preparing a carbon nano material.
Background
In the chemical production process, the material processing industry, the catering industry and the oil storage, loading and unloading process, a large amount of Volatile Organic Compounds (VOCs) are often generated, and the oil-based fuel oil has the actual current situations of strong dispersity, more components, large molecular weight difference, large physical property difference and the like. Methods for treating volatile organic compound-containing gases generally include condensation, adsorption, absorption, oxidation, and the like. Wherein, the adsorption method is commonly used for various porous materials (such as active carbon and silica gel), and has the characteristics of simple and safe process and the like. If the activated carbon material is used in the adsorption method, the cyclic use performance is poor because of the large number of micropores. Recently, mesoporous materials such as carbon nanotubes and graphene have been developed rapidly, and long-term cyclic use of adsorption and desorption can be realized. . However, carbon nanomaterials are still high in cost and are one of the obstacles that hinder their adsorption applications.
In addition, after adsorption and concentration, a part of the desorbed organic matters can be changed into a liquid phase, so that the organic matters can be conveniently separated and recycled or treated by other methods. However, most of the gas still remains as gas at normal temperature and pressure, is inconvenient to store, cannot be discharged randomly and needs to be treated continuously. Meanwhile, for the treatment of the gas containing volatile organic compounds with large flow fluctuation or concentration fluctuation, frequent switching of the adsorption/desorption devices is caused, and energy consumption is increased.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a system and a method for capturing gas containing volatile organic compounds and preparing carbon nano materials by matching an absorption method and an adsorption method, so as to solve the problem that the desorbed gaseous organic compounds are difficult to treat, increase the volatile organic compounds with large flow fluctuation or concentration fluctuation, reduce energy consumption and improve the added value of products. And the carbon nano material can be made into the adsorbent, so that the cost of the adsorbent can be greatly reduced.
In order to achieve the purpose, the invention adopts the following technical scheme:
the system for trapping the gas containing the volatile organic compounds and preparing the carbon nano material comprises an absorption/desorption subsystem 1, an adsorption/desorption subsystem 2 and a carbonization subsystem 4, wherein the system comprises or does not comprise a gas-liquid separation subsystem 3; the bottom of the absorption/desorption subsystem 1 is provided with a gas inlet 5 containing volatile organic compounds, and the top is provided with a gas outlet 6; the bottom of the adsorption/desorption subsystem 2 is provided with a gas inlet 7 containing volatile organic compounds, and the top is provided with an adsorbed gas outlet 8 and a desorbed gas outlet 9; the bottom of the gas-liquid separation subsystem 3 is provided with a condensed organic liquid outlet 11), the top is provided with an organic matter gas outlet 12, and the middle part is provided with a middle inlet 10; the bottom of the carbonization subsystem 4 is provided with a bottom inlet 13, the top of the carbonization subsystem 4 is provided with a carbonized tail gas outlet 14, and the carbonization subsystem 4 is also provided with a catalyst inlet 15 and a carbon material outlet 16; the gas outlet 6 at the top of the absorption/desorption subsystem 1 is divided into two paths, one path is communicated with the gas inlet 7 at the bottom of the absorption/desorption subsystem 2, when the gas-liquid separation subsystem 3 is included, the other path is communicated with the middle inlet 10 of the gas-liquid separation subsystem 3, and when the gas-liquid separation subsystem 3 is not included, the other path is communicated with the bottom inlet 13 of the carbonization subsystem 4; when the system comprises the gas-liquid separation subsystem 3, a desorbed gas outlet 9 at the top of the adsorption/desorption subsystem 2 is communicated with a middle inlet 10 of the gas-liquid separation subsystem 3, and an organic matter gas outlet 12 at the top of the gas-liquid separation subsystem 3 is communicated with a bottom inlet 13 of the carbonization subsystem 4; when the gas-liquid separation subsystem 3 is not included, the desorbed gas outlet 9 at the top of the adsorption/desorption subsystem 2 is communicated with the bottom inlet 13 of the carbonization subsystem 4; and a carbonized tail gas outlet 14 at the top of the carbonization subsystem 4 is communicated with an adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2.
The absorption/desorption subsystem 1 is filled with a liquid hydrocarbon absorbent, the boiling point of the liquid hydrocarbon absorbent is 200-300 ℃, and the freezing point of the liquid hydrocarbon absorbent is-50 to-10 ℃.
The adsorption/desorption subsystem 2 is filled with an easily-regenerated adsorbent which is made of one or more of carbon adsorbent, molecular sieve or alumina.
The carbon adsorbent is one or more of activated carbon, carbon fiber, carbon nanotube and graphene.
The catalyst filled in the carbonization subsystem 4 is metal and/or oxide, the metal comprises one or more of iron, cobalt, nickel, copper, manganese, zinc, platinum, molybdenum and tungsten, and the oxide comprises one or more of alumina, silica, magnesia and zirconia; the mass fraction of the metal is 0-20%; the catalyst cracks the organic matter at the temperature of 800 ℃ and the mass space velocity of the organic matter is 0.01-30h-1Generation of carbonNano material, and the obtained tail gas contains hydrogen and methane.
The method for trapping the gas containing the volatile organic compounds and preparing the carbon nano material by the system comprises the following steps:
a) the absorption/desorption subsystem 1, the adsorption/desorption subsystem 2 and the carbonization subsystem 4 are connected or not connected with the gas-liquid separation subsystem 3;
b) introducing gas containing volatile organic compounds from a gas inlet 5 of an absorption/desorption subsystem 1, after the gas passes through a liquid hydrocarbon absorbent, most of the volatile organic compounds are remained in a liquid phase, a small amount of volatile organic compounds are introduced into an adsorption/desorption subsystem 2 from a gas outlet 6 through a gas inlet 7 along with the gas, after the gas passes through an adsorbent layer of the adsorption/desorption subsystem 2, the organic compounds are adsorbed on the adsorbent, and the adsorbed gas is discharged from an adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2 or used for other purposes;
c) when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is close to saturation, the gas inlet 5 of the absorption/desorption subsystem 1 is closed, and the gas containing volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 through the gas inlet 7; meanwhile, closing a pipeline which is communicated with the adsorption/desorption subsystem 2 from the top of the absorption/desorption subsystem 1, opening a pipeline which passes through the gas-liquid separation subsystem 3 from the top of the absorption/desorption subsystem 1, carrying out heating and vacuumizing operations, desorbing dissolved matters in the liquid hydrocarbon absorbent, discharging the desorbed dissolved matters from the gas outlet 6, and feeding the desorbed dissolved matters into the middle inlet 10 of the gas-liquid separation subsystem 3; when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is desorbed, the operation of the step 1 is resumed;
d) when the adsorption layer of the adsorption/desorption subsystem 2 is close to saturation, stopping introducing the gas containing volatile organic compounds from the gas inlet 7, heating and vacuumizing the adsorption/desorption subsystem 2 to desorb the gas on the adsorbent, and discharging the gas from the desorbed gas outlet 9 at the upper part of the adsorption/desorption subsystem 2;
e) if the gas desorbed from the absorption/desorption subsystem 1 or the gas desorbed from the gas outlet 9 after the desorption from the top of the absorption/desorption subsystem 2 does not have the recycling value, the gas is directly introduced into the carbonization subsystem 4 through the bottom inlet 13 to generate the carbon nano material on the catalyst;
f) if the gas desorbed from the absorption/desorption subsystem 1 or the gas exhausted from the desorbed gas outlet 9 of the absorption/desorption subsystem 2 has a recycling value, the gas is introduced into the gas-liquid separation subsystem 3 through the middle inlet 10 to separate the organic liquid from the organic gas; the organic liquid is discharged from a condensed organic liquid outlet 11 at the bottom of the gas-liquid separation subsystem 3, so that direct recycling or continuous separation recycling is realized; the tail gas containing organic matters discharged from an organic matter gas outlet 12 at the top of the gas-liquid separation subsystem 3 enters the carbonization subsystem 4 through a bottom inlet 13 to generate carbon nano materials on the catalyst;
g) the tail gas of the carbonization subsystem 4 is discharged through a carbonized tail gas outlet 14, is mixed with the adsorbed gas of an adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2, and is discharged after reaching the standard or used for other purposes;
h) after the carbon material of the carbonation subsystem 4 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
When the sub-absorption/desorption subsystem 1 executes absorption operation, the temperature is-30-25 ℃, the absolute pressure is 120-1500KPa, and the absorption rate is 70-95%; when the desorption operation is carried out, the temperature is 50-160 ℃, the absolute pressure is 10-120KPa, and the desorption rate is 80-99%.
When the sub-gas adsorption/desorption system 2 executes the adsorption operation, the temperature is-25-20 ℃, and the absolute pressure is 100-1480 KPa; the adsorption effect is as follows: so that the content of organic matters in the gas containing volatile organic matters is less than 50ppm, C5The above compound is less than 4 ppm; when the desorption operation is carried out, the temperature is 50-250 ℃, the absolute pressure is 10-90KPa, and the desorption rate is 95-99.99%.
The main body of the gas containing volatile organic compounds is nitrogen, argon and CO2Are mixed in any proportion or H2One or two of CO are mixed in any proportion; the concentration of the organic matter is 0.05-2%, and the organic matter comprises 26-150 molecular weight.
The carbon nano-materials generated in the carbonization sub-system 4 include one or more of carbon nano-particles, carbon nano-fibers, carbon nano-tubes and graphene.
Compared with the prior art, the invention has the beneficial effects that:
(1) the absorption/desorption subsystem is additionally arranged in front of the adsorption/desorption subsystem, so that the treatment of the gas containing volatile organic compounds with large content variation can be effectively dealt with. The service cycle of the following adsorbent is prolonged by 50-80%, the desorption frequency is reduced by more than 50%, and the comprehensive energy consumption is reduced by 40-50%.
(2) The system and the method convert the volatile organic gas which is most difficult to liquefy into the carbon nano material, and can reduce the cost of the adsorbent by 80-90%. And the operation of the medium containing oxidizing property is avoided, and the process safety is greatly improved.
Drawings
FIG. 1 is a block diagram of a system including four subsystems (including subsystems (1), (2), (3) and (4))
FIG. 2 is a block diagram of the present invention without the gas-liquid separation subsystem 3
Wherein, 1, the absorption/desorption subsystem, 2, the adsorption/desorption subsystem, 3, the gas-liquid separation subsystem, 4, the carbonization subsystem, 5, the gas inlet 5; 6. the device comprises a gas outlet, 7, a gas inlet, 8, an adsorbed gas outlet, 9, a desorbed gas outlet, 10, a middle inlet, 11, a condensed organic liquid outlet, 12, an organic gas outlet, 13, a bottom inlet, 14, a carbonized tail gas outlet, 15, a catalyst inlet and 16, a carbon material outlet.
Detailed Description
The present invention will be described in detail with reference to examples.
Example 1
As shown in fig. 1, an absorption/desorption subsystem 1, an adsorption/desorption subsystem 2, a gas-liquid separation subsystem 3, and a carbonization subsystem 4 are connected in sequence;
gas containing volatile organic compounds (nitrogen as main gas, 2% of organic compounds, C)4-C10Hydrocarbon) is introduced from a gas inlet 5 containing volatile organic compounds of the absorption/desorption subsystem 1, and the boiling point of the used liquid hydrocarbon absorbent is 200-250 ℃, and the freezing point is-50-40 ℃. The absorption was carried out at-30 ℃ and at a pressure of 1500KPa (absolute pressure) and an absorption of 90%. Absorption ofThen, the gas is discharged from a gas outlet 6 and is introduced into the adsorption/desorption subsystem 2 through a gas inlet 7, the adsorption temperature is-20 ℃, the pressure is 1480KPa (absolute pressure), after passing through an adsorbent layer in the adsorption/desorption subsystem 2, the organic matters are adsorbed on an adsorbent (the mass fraction of the carbon nano tubes is 50 percent and the mass fraction of the molecular sieves is 50 percent), and the desorption rate is>99 percent, the treated gas (nitrogen, wherein the non-methane total hydrocarbon is 35ppm, the aromatic hydrocarbon is 3ppm) is discharged from the gas outlet 8 after adsorption, and the gas reaches the discharge standard;
when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is nearly saturated, the introduction of the gas containing the volatile organic compounds is stopped, and the treatment system is switched off (the gas containing the volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 for treatment). Heating the absorption/desorption subsystem 1 to 160 deg.C, and desorbing at 60KPa (absolute pressure) to desorb the dissolved substances in the absorbent at a desorption rate>95% of the gas discharged from the gas outlet 6 of the absorption/desorption subsystem 1; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6-C10Hydrocarbons with C4-C5And (4) separating the hydrocarbon. C6-C10The hydrocarbons are discharged from the condensed organic liquid outlet 11 for reuse.
When the adsorption layer of the adsorption/desorption subsystem 2 is nearly saturated, the introduction of the gas containing volatile organic compounds is stopped, and the treatment system is switched out. Heating the adsorption/desorption subsystem 2 to 250 ℃ and the desorption pressure is 60KPa (absolute pressure), so that the gas on the adsorbent is desorbed with the desorption rate of 99.99 percent and is discharged from a desorbed gas outlet 9 of the adsorption/desorption subsystem 2; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6-C10Hydrocarbons with C4-C5And (4) separating the hydrocarbon. C6-C10The hydrocarbons are discharged from the condensed organic liquid outlet 11 for reuse.
C-containing gas discharged from an organic gas outlet 12 at the top of the gas-liquid separation subsystem 34-C5The tail gas of the organic matters enters the carbonization subsystem 4 through a bottom inlet 13 and is cracked on a catalyst (20 percent of nickel-80 percent of alumina) at 800 ℃, and the mass space velocity of the organic matters is 0.01h-1To form carbon nanotubes and carbon nanofibersA mixture of vitamins; the tail gas of the carbonization subsystem 4 is mixed with the gas of the adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2 through the carbonized tail gas outlet 14, and the mixture is discharged after reaching the standard.
After the carbon material of the carbonation subsystem 3 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
Example 2
As shown in fig. 1, an absorption/desorption subsystem 1, an adsorption/desorption subsystem 2, a gas-liquid separation subsystem 3, and a carbonization subsystem 4 are connected in sequence;
volatile organic compound-containing gas (the main gases are argon and CO)2(argon gas: CO)21:1) and gasoline hydrocarbon containing 0.05% of organic matters) is introduced from a gas inlet 5 containing volatile organic matters of the absorption/desorption subsystem 1, and the boiling point of the used liquid hydrocarbon absorbent is 200-300 ℃ and the freezing point is-30-10 ℃. The absorption was carried out at 25 ℃ and 180KPa (absolute pressure) at an absorption rate of 70%. After absorption, gas is discharged from a gas outlet 6, introduced into the adsorption/desorption subsystem 2 through a gas inlet 7, the adsorption temperature is 10 ℃, the pressure is 150KPa (absolute pressure), and after passing through an adsorbent layer in the adsorption/desorption subsystem 2, organic matters are adsorbed on an adsorbent (on 20% of graphene and 80% of alumina in mass fraction), and the removal rate is high>97% of treated gas (argon and CO)2(argon gas: CO)21:1), wherein the non-methane total hydrocarbon is 40ppm, and the aromatic hydrocarbon is 4ppm) is discharged from an adsorbed gas outlet 8, and the emission reaches the standard;
when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is nearly saturated, the introduction of the gas containing the volatile organic compounds is stopped, and the treatment system is switched off (the gas containing the volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 for treatment). Heating the absorption/desorption subsystem 1 to 90 ℃, wherein the desorption pressure is 120KPa (absolute pressure), so that dissolved matters in the absorbent are desorbed, the desorption rate is 95 percent, and the dissolved matters are discharged from a gas outlet 6 of the absorption/desorption subsystem 1; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6Above hydrocarbons with C4-C5And (4) separating the hydrocarbon. C6From the above hydrocarbons condensing intoAnd discharging the machine liquid from an outlet 11 for recycling.
When the adsorption layer of the adsorption/desorption subsystem 2 is nearly saturated, the introduction of the gas containing volatile organic compounds is stopped, and the treatment system is switched out. The adsorption/desorption subsystem 2 is heated to 100 ℃, the desorption pressure is 85KPa (absolute pressure), so that the gas on the adsorbent is desorbed, and the desorption rate>95 percent of the gas is discharged from a gas outlet 9 after desorption of the adsorption/desorption subsystem 2; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6Above hydrocarbons with C4-C5And (4) separating the hydrocarbon. C6The above hydrocarbons are discharged from the condensed organic liquid outlet 11 and recycled.
C-containing gas discharged from an organic gas outlet 12 at the top of the gas-liquid separation subsystem 34-C5The tail gas of the organic matters enters a carbonization subsystem 4 through a bottom inlet 13 and is treated in a catalyst (1 percent of Mo-1 percent of Co-18 percent of Fe-80 percent of SiO) at the temperature of 450 DEG C2) The mass space velocity of the organic matter is 0.01h-1Generating a mixture of carbon nanofibers and carbon nanoparticles; the tail gas of the carbonization subsystem 4 is mixed with the gas of the adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2 through the carbonized tail gas outlet 14, and the mixture is discharged after reaching the standard.
After the carbon material of the carbonation subsystem 3 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
Example 3
As shown in fig. 1, an absorption/desorption subsystem 1, an adsorption/desorption subsystem 2, a gas-liquid separation subsystem 3, and a carbonization subsystem 4 are connected in sequence;
introducing gas containing volatile organic compounds (the main gas is hydrogen, and the organic compounds are a mixture of propane, cyclohexene, cyclohexane, cyclohexanol and cyclohexanone in any proportion of 1%) from a gas inlet 5 containing the volatile organic compounds of the absorption/desorption subsystem 1, and introducing a liquid hydrocarbon absorbent, wherein the boiling point of the liquid hydrocarbon absorbent is 250-300 ℃, and the freezing point of the liquid hydrocarbon absorbent is-20-10 ℃. The absorption operating temperature was 20 ℃ and the pressure 1000KPa (absolute pressure), and the absorption efficiency was 70%. After absorption, gas is discharged from a gas outlet 6 and is introduced into the adsorption/desorption subsystem 2 through a gas inlet 7, the adsorption temperature is minus 10 DEG CThe pressure is 800KPa (absolute pressure), organic matters are adsorbed on the adsorbent (on the carbon nano tube with the mass fraction of 60 percent and the molecular sieve with the mass fraction of 40 percent) after passing through the adsorbent layer in the adsorption/desorption subsystem 2, and the desorption rate is>99% of treated gas (hydrogen gas, 20ppm of total hydrocarbons, C)6Compound 4ppm) is discharged from the post-adsorption gas outlet 8 for its use;
when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is nearly saturated, the introduction of the gas containing the volatile organic compounds is stopped, and the treatment system is switched off (the gas containing the volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 for treatment). Heating the absorption/desorption subsystem 1 to 50 ℃, wherein the desorption pressure is 90KPa (absolute pressure), so that dissolved matters in the absorbent are desorbed, the desorption rate is 80 percent, and the dissolved matters are discharged from a gas outlet 6 of the absorption/desorption subsystem 1; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6Compounds with C3And (4) separating the hydrocarbon. C6The compounds are discharged from the condensed organic liquid outlet 11 for reuse.
When the adsorption layer of the adsorption/desorption subsystem 2 is nearly saturated, the introduction of the gas containing volatile organic compounds is stopped, and the treatment system is switched out. Heating the adsorption/desorption subsystem 2 to 150 deg.C, and desorbing at 90KPa (absolute pressure) to desorb the gas on the adsorbent with desorption rate>95 percent of the gas is discharged from a gas outlet 9 after desorption of the adsorption/desorption subsystem 2; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6Compounds with C3And (4) separating the hydrocarbon. C6The compound is discharged from the condensed organic liquid outlet 11 for reuse.
C-containing gas discharged from an organic gas outlet 12 at the top of the gas-liquid separation subsystem 33Hydrocarbon tail gas, entering the carbonization subsystem 4 through the bottom inlet 13, is in the catalyst (1% W-1% Pt-8% Ni-90% Al) at 700 DEG C2O3) The mass space velocity of the organic matter is 1h-1Generating a mixture of carbon nanotubes and graphene; the tail gas of the carbonization subsystem 4 is mixed with the gas of the gas outlet 8 after the absorption at the top of the absorption/desorption subsystem 2 through the carbonized tail gas outlet 14 and is discharged for use.
After the carbon material of the carbonation subsystem 3 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
Example 4
As shown in fig. 1, an absorption/desorption subsystem 1, an adsorption/desorption subsystem 2, a gas-liquid separation subsystem 3, and a carbonization subsystem 4 are connected in sequence;
the gas containing volatile organic compounds (the main gas is CO)2. The content of volatile organic compounds is 0.8 percent, and is C4-C5Mixture of isoparaffin, pyridine and xylene in any proportion) is introduced from a gas inlet 5 containing volatile organic compounds of the absorption/desorption subsystem 1, the boiling point of the liquid hydrocarbon absorbent is 200-240 ℃, and the freezing point is-50 to-35 ℃. The absorption was carried out at 10 ℃ and at a pressure of 500KPa (absolute pressure) and an absorption of 80%. After absorption, the gas is discharged from the gas outlet 6, introduced into the adsorption/desorption subsystem 2 through the gas inlet 7, the adsorption temperature is 0 ℃, the pressure is 400KPa (absolute pressure), after passing through the adsorbent layer in the adsorption/desorption subsystem 2, the organic matters are adsorbed on the adsorbent (on 80% carbon nano tubes and 20% active carbon by mass fraction), and the treated gas (CO)2Wherein the non-methane total hydrocarbons are 20ppm, C5The above compounds 2ppm) are discharged from an adsorbed gas outlet 8 and discharged after reaching the standard;
when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is nearly saturated, the introduction of the gas containing the volatile organic compounds is stopped, and the treatment system is switched off (the gas containing the volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 for treatment). Heating the absorption/desorption subsystem 1 to 120 ℃, wherein the desorption pressure is 50KPa (absolute pressure), so that dissolved matters in the absorbent are desorbed, the desorption rate is 98 percent, and the dissolved matters are discharged from a gas outlet 6 of the absorption/desorption subsystem 1; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6And the above compounds and C4-C5And (4) separating the hydrocarbon. C6And the above compounds are discharged from the condensed organic liquid outlet 11 for reuse.
When the adsorption layer of the adsorption/desorption subsystem 2 is nearly saturated, the introduction of the volatile organic compounds is stoppedAnd switching out of the processing system. Heating the adsorption/desorption subsystem 2 to 120 ℃, wherein the desorption pressure is 50KPa (absolute pressure), so that the gas on the adsorbent is desorbed, the desorption rate is 97%, and the desorbed gas is discharged from a gas outlet 9 of the adsorption/desorption subsystem 2; enters the gas-liquid separation subsystem 3 through the middle inlet 10 of the gas-liquid separation subsystem 3. Condensing at-20 deg.C to carry out C6Compounds with C4-C5And (4) separating isoparaffin. C6The compound is discharged from the condensed organic liquid outlet 11 for reuse.
C-containing gas discharged from an organic gas outlet 12 at the top of the gas-liquid separation subsystem 34-C5The isoparaffin tail gas enters the carbonization subsystem 4 through a bottom inlet 13 and is treated in a catalyst (8 percent of Ni-2 percent of Cu-30 percent of MgO-60 percent of SiO) at the temperature of 650 DEG C2) The mass space velocity of the organic matter is 30h-1Generating a mixture of carbon nanotubes and graphene; the tail gas of the carbonization subsystem 4 is mixed with the gas of the adsorbed gas outlet 8 at the top of the adsorption/desorption subsystem 2 through the carbonized tail gas outlet 14, and the mixture is discharged after reaching the standard.
After the carbon material of the carbonation subsystem 4 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
Example 5
As shown in fig. 2, an absorption/desorption subsystem system 1, an adsorption/desorption subsystem 2, and a carbonization subsystem 4 are connected in sequence;
the gas containing volatile organic compounds (the main gas is H)2And CO (H)2: CO is 2: 1) 1% of butane, octane, methyl tert-butyl ether, benzene, thiophene and organic matters with the boiling point of 120-. The absorption was carried out at 5 ℃ and at a pressure of 120K Pa (absolute pressure) and at an absorption rate of 85%. After absorption, gas is discharged from a gas outlet 6, introduced into the adsorption/desorption subsystem 2 through a gas inlet 7, the adsorption temperature is 0 ℃, the pressure is 100KPa (absolute pressure), and after passing through an adsorbent layer in the adsorption/desorption subsystem 2, organic matters are adsorbed in an adsorbent (the mass fraction of carbon is 50%)Fibers, 30% carbon nanotubes and 20% activated carbon), treated gas (H)2And CO (H)2: CO is 2: 1) wherein the non-methane total hydrocarbons are 15ppm, C5The above compound 4ppm) is discharged from the post-adsorption gas outlet 8 for its use;
when the liquid hydrocarbon absorbent of the absorption/desorption subsystem 1 is nearly saturated, the introduction of the gas containing the volatile organic compounds is stopped, and the treatment system is switched off (the gas containing the volatile organic compounds is directly introduced into the adsorption/desorption subsystem 2 for treatment). Heating the absorption/desorption subsystem 1 to 150 ℃, wherein the desorption pressure is 10KPa (absolute pressure), so that dissolved matters in the absorbent are desorbed, the desorption rate is 94 percent, and the dissolved matters are discharged from a gas outlet 6 of the absorption/desorption subsystem 1; enters the carbonization subsystem (4) through the bottom inlet 13;
when the adsorption layer of the adsorption/desorption subsystem 2 is nearly saturated, the introduction of the gas containing volatile organic compounds is stopped, and the treatment system is switched out. Heating the adsorption/desorption subsystem 2 to 250 ℃, wherein the desorption pressure is 10KPa (absolute pressure), so that the gas on the adsorbent is desorbed, the desorption rate is 98%, and the gas is discharged from a desorbed gas outlet 9 of the adsorption/desorption subsystem 2; enters the carbonization subsystem (4) through the bottom inlet 13;
the two streams of material entering the carbonisation sub-system (4) are carried out in the presence of a catalyst (5% Mn-45% SiO) at 800 DEG C2-25％MgO-25％Al2O3) The mass space velocity of the organic matter is 1.5h-1Generating a mixture of carbon nanoparticles and graphene; the tail gas of the carbonization subsystem 4 is mixed with the gas of the gas outlet 8 after the absorption at the top of the absorption/desorption subsystem 2 through the carbonized tail gas outlet 14 and is discharged for use.
After the carbon material of the carbonation subsystem 4 reaches a predetermined volume, it is removed through the carbon material outlet 16 and the catalyst is replenished through the catalyst inlet 15.
Claims (9)
1. A system for collecting gas containing volatile organic compounds and preparing carbon nanomaterials is characterized in that: comprises an absorption/desorption subsystem (1), an adsorption/desorption subsystem (2) and a carbonization subsystem (4), and comprises or does not comprise a gas-liquid separation subsystem (3); the bottom of the absorption/desorption subsystem (1) is provided with a gas inlet (5) containing volatile organic compounds, and the top is provided with a gas outlet (6); the bottom of the adsorption/desorption subsystem (2) is provided with a gas inlet (7) containing volatile organic compounds, and the top is provided with an adsorbed gas outlet (8) and a desorbed gas outlet (9); the bottom of the gas-liquid separation subsystem (3) is provided with a condensed organic liquid outlet (11), the top is provided with an organic gas outlet (12), and the middle is provided with a middle inlet (10); the bottom of the carbonization subsystem (4) is provided with a bottom inlet (13), the top of the carbonization subsystem is provided with a carbonized tail gas outlet (14), and the carbonization subsystem (4) is also provided with a catalyst inlet (15) and a carbon material outlet (16); the gas outlet (6) at the top of the absorption/desorption subsystem (1) is divided into two paths, one path is communicated with the gas inlet (7) at the bottom of the adsorption/desorption subsystem (2), when the gas-liquid separation subsystem (3) is included, the other path is communicated with the middle inlet (10) of the gas-liquid separation subsystem (3), and when the gas-liquid separation subsystem (3) is not included, the other path is communicated with the bottom inlet (13) of the carbonization subsystem (4); when the system comprises the gas-liquid separation subsystem (3), a desorbed gas outlet (9) at the top of the adsorption/desorption subsystem (2) is communicated with a middle inlet (10) of the gas-liquid separation subsystem (3), and an organic matter gas outlet (12) at the top of the gas-liquid separation subsystem (3) is communicated with a bottom inlet (13) of the carbonization subsystem (4); when the gas-liquid separation subsystem (3) is not included, a desorbed gas outlet (9) at the top of the adsorption/desorption subsystem (2) is communicated with a bottom inlet (13) of the carbonization subsystem (4); a carbonized tail gas outlet (14) at the top of the carbonization subsystem (4) is communicated with an adsorbed gas outlet (8) at the top of the adsorption/desorption subsystem (2);
the absorption/desorption subsystem (1) is filled with a liquid hydrocarbon absorbent;
the catalyst filled in the carbonization subsystem (4) is metal and/or oxide, the metal comprises one or more of iron, cobalt, nickel, copper, manganese, zinc, platinum, molybdenum and tungsten, and the oxide comprises one or more of alumina, silicon oxide, magnesium oxide and zirconium oxide; the mass fraction of the metal is 0-20%; the catalyst cracks the organic matter at the temperature of 800 ℃ and the mass space velocity of the organic matter is 0.01-30h-1Generating carbon nano materials, wherein the components of the obtained tail gas are hydrogen and methane;
the desorption rate of the sub-absorption/desorption subsystem (1) is 80-99%, and the desorption rate of the sub-gas absorption/desorption subsystem (2) is 95-99.99%.
2. The system for capturing volatile organic compound-containing gas and producing carbon nanomaterial according to claim 1, wherein: the liquid hydrocarbon absorbent has a boiling point of 200-300 ℃ and a freezing point of-50-10 ℃.
3. The system for capturing volatile organic compound-containing gas and producing carbon nanomaterial according to claim 1, wherein: the adsorption/desorption subsystem (2) is filled with an easily-regenerated adsorbent which is made of one or more of carbon adsorbent, molecular sieve or alumina.
4. The system for capturing volatile organic compound-containing gas and producing carbon nanomaterial according to claim 3, wherein: the carbon adsorbent is one or more of activated carbon, carbon fiber, carbon nanotube and graphene.
5. The method for capturing volatile organic compound-containing gas and producing carbon nanomaterial by the system of any one of claims 1 to 4, comprising the steps of:
a) the absorption/desorption subsystem (1), the adsorption/desorption subsystem (2) and the carbonization subsystem (4) are connected or not connected with the gas-liquid separation subsystem (3);
b) introducing gas containing volatile organic compounds from a gas inlet (5) of an absorption/desorption subsystem (1), after the gas passes through a liquid hydrocarbon absorbent, most of the volatile organic compounds are remained in a liquid phase, a small amount of volatile organic compounds are introduced into the absorption/desorption subsystem (2) from a gas outlet (6) through a gas inlet (7) along with the gas, after the gas passes through an adsorbent layer of the absorption/desorption subsystem (2), the organic compounds are adsorbed on the adsorbent, and the gas after adsorption is discharged from an adsorbed gas outlet (8) at the top of the absorption/desorption subsystem (2) or used for the gas;
c) when the liquid hydrocarbon absorbent of the absorption/desorption subsystem (1) is close to saturation, the gas inlet (5) of the absorption/desorption subsystem (1) is closed, and the gas containing volatile organic compounds is directly introduced into the adsorption/desorption subsystem (2) through the gas inlet (7); simultaneously, closing a pipeline which is introduced into the adsorption/desorption subsystem (2) from the top of the adsorption/desorption subsystem (1);
d) heating and vacuumizing the absorption/desorption subsystem (1) to desorb dissolved matters in the liquid hydrocarbon absorbent, and discharging the dissolved matters from a gas outlet (6) at the top of the absorption/desorption subsystem (1); if the gas desorbed from the absorption/desorption subsystem (1) does not have recycling value, the gas is directly introduced into the carbonization subsystem (4) through a bottom inlet (13) to generate the carbon nano material on the catalyst;
if the organic liquid has recycling value, the organic liquid is introduced into the gas-liquid separation subsystem (3) through the middle inlet (10) to separate the organic liquid from the organic gas; organic liquid is discharged from a condensed organic liquid outlet (11) at the bottom of the gas-liquid separation subsystem (3) to realize direct recycling or continuous separation recycling; tail gas containing organic matters discharged from an organic matter gas outlet (12) at the top of the gas-liquid separation subsystem (3) enters the carbonization subsystem (4) through a bottom inlet (13) to generate carbon nano materials on a catalyst;
e) when the liquid hydrocarbon absorbent of the absorption/desorption subsystem (1) is desorbed, the operation of the step b) is recovered;
f) when the adsorption layer of the adsorption/desorption subsystem (2) is nearly saturated, stopping introducing the gas containing volatile organic compounds from the gas inlet (7), heating and vacuumizing the adsorption/desorption subsystem (2) to desorb the gas on the adsorbent, and discharging the gas from a desorbed gas outlet (9) at the upper part of the adsorption/desorption subsystem (2); if the gas desorbed from the desorbed gas outlet (9) has no recycling value, the gas is directly introduced into the carbonization subsystem (4) through the bottom inlet (13) to generate the carbon nano material on the catalyst;
if the organic liquid has recycling value, the organic liquid is introduced into the gas-liquid separation subsystem (3) through the middle inlet (10) to separate the organic liquid from the organic gas; organic liquid is discharged from a condensed organic liquid outlet (11) at the bottom of the gas-liquid separation subsystem (3) to realize direct recycling or continuous separation recycling; tail gas containing organic matters discharged from an organic matter gas outlet (12) at the top of the gas-liquid separation subsystem (3) enters the carbonization subsystem (4) through a bottom inlet (13) to generate carbon nano materials on a catalyst;
g) the tail gas of the carbonization subsystem (4) is discharged through a carbonized tail gas outlet (14), and is mixed with the gas after adsorption of an adsorbed gas outlet (8) at the top of the adsorption/desorption subsystem (2) to be discharged after reaching the standard or used for the purpose;
h) after the carbon material in the carbonation subsystem (4) reaches a predetermined volume, it is removed through the carbon material outlet (16) and the catalyst is replenished through the catalyst inlet (15).
6. The method of claim 5, wherein: when the sub-absorption/desorption subsystem (1) executes absorption operation, the temperature is-30-25 ℃, the absolute pressure is 120-1500KPa, and the absorption rate is 70-95%; when desorption is carried out, the temperature is 50-160 ℃ and the absolute pressure is 10-120 KPa.
7. The method of claim 5, wherein: when the sub-gas adsorption/desorption system (2) executes the adsorption operation, the temperature is-25-20 ℃, and the absolute pressure is 100-1480 KPa; the adsorption effect is as follows: so that the content of organic matters in the gas containing volatile organic matters is less than 50ppm, C5The above compound is less than 4 ppm; when the desorption operation is carried out, the temperature is 50-250 ℃ and the absolute pressure is 10-90 KPa.
8. The method of claim 5, wherein: the main body of the gas containing volatile organic compounds is nitrogen, argon and CO2Are mixed in any proportion or H2One or two of CO are mixed in any proportion; the concentration of the organic matter is 0.05-2%, and the organic matter comprises 26-150 molecular weight.
9. The method of claim 5, wherein: and the carbon nano-materials generated in the carbonization subsystem (4) comprise one or more of carbon nano-particles, carbon nano-fibers, carbon nano-tubes and graphene.
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