KR101660472B1 - Method of Synthetic Natural Gas Production Using Sorption-enhanced Methanation - Google Patents
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- KR101660472B1 KR101660472B1 KR1020150065411A KR20150065411A KR101660472B1 KR 101660472 B1 KR101660472 B1 KR 101660472B1 KR 1020150065411 A KR1020150065411 A KR 1020150065411A KR 20150065411 A KR20150065411 A KR 20150065411A KR 101660472 B1 KR101660472 B1 KR 101660472B1
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- C—CHEMISTRY; METALLURGY
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- 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
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Abstract
The present invention relates to a method for producing synthetic natural gas using an adsorption unit and a methanation reaction, and more particularly, to a process for producing synthetic natural gas using adsorbent and a methanation reaction. More particularly, And the carbon dioxide captured by the adsorbent is again used in a carbon dioxide methanation reaction, thereby greatly reducing the amount of carbon dioxide generated and the amount of hydrogen gas used.
The method for producing synthetic natural gas using the adsorbing part and the methanation reaction according to the present invention reduces the amount of discharged carbon dioxide and the amount of consumed hydrogen to prevent warming and is useful for producing economically synthetic natural gas.
Description
The present invention relates to a method for producing synthetic natural gas using an adsorption unit and a methanation reaction, and more particularly, to a process for producing synthetic natural gas using adsorbent and a methanation reaction. More particularly, And the carbon dioxide captured by the adsorbent is again used in a carbon dioxide methanation reaction, thereby greatly reducing the amount of carbon dioxide generated and the amount of hydrogen gas used.
Compared to fossil fuels such as petroleum and natural gas, coal has a large amount of reserves. However, when used through direct combustion, carbon dioxide and environmental pollutants such as SO x and NO x, which are major contributors to global warming, occur in large quantities. As a technology for using coal more cleanly, gasification of coal at high temperature by an indirect combustion method generates syngas containing carbon monoxide, hydrogen and carbon dioxide, and this synthesis gas is reacted with methanation ) To produce methane to produce synthetic natural gas (SNG).
The synthetic gas produced by the conventional coal gasification process is subjected to a desulfurization process, followed by a water gas shift (WGS) reaction to convert the ratio of hydrogen to carbon monoxide to methanation To the stoichiometric ratio of H 2 / CO = 3. Then, carbon dioxide, which is a byproduct produced through the water gas conversion reaction, is removed, and the thus obtained gas is subjected to a carbon monoxide methanation reaction at about 300 ° C. using a nickel-based catalyst. Methane is produced. [Korean Patent Publication No. 10-2004-00157590]
Meanwhile, Korean Patent Laid-Open No. 10-2010-0136840 discloses a process for improving the existing methanation reaction process. In the process of converting a water gas into a methanation reaction without removal of carbon dioxide, It has also been suggested that the carbon dioxide methanation reaction proceeds as well. In addition, Korean Patent Laid-Open No. 10-2011-0009839 attempts to control the high reaction heat of the methanation reaction by including a water gas conversion reaction in the middle of the methanation reaction. However, all of these processes have the disadvantage that the by-products carbon dioxide and water, which are respectively generated in the water gas conversion reaction and the methanation reaction, must be removed through an additional separation process.
The adsorbents usable for the adsorption unit and the methanation reaction proposed in the present invention include hydrotalcite and NaX zeolite. Hydrotalcite exhibits a high carbon dioxide adsorption capacity at 300 ° C, a temperature condition in which a water gas shift reaction and a methanation reaction occur well as a carbon dioxide adsorbent. Hydrotalcite has a layered structure and its basic chemical formula is [M 1-x Ⅱ M x Ⅲ (OH) 2 ] [A x / n n- ] m H 2 O, where M Ⅱ and M Ⅲ are 2 and 3 respectively Metal ion, and A is an anion present in the hydrotalcite inner layer. Representative hydrotalcites include Mg 6 Al 2 CO 3 (OH) 16 4 (H 2 O) having Mg and Al as metal ions. Hydrotalcite itself does not have a high carbon dioxide adsorbing capacity, but potassium carbonate (K 2 CO 3 ) can be added to enhance the adsorption capacity. On the other hand, zeolite is an alumino silica material composed of aluminum, silicon and oxygen, and is widely used as an adsorbent because of its unique structure of porosity. Among various zeolite materials, NaX zeolite is known to have moisture adsorption ability at high temperature (Carvill et al., 1996).
Accordingly, the present inventors have made intensive efforts to solve the above problems, and as a result, they have found that, as a result, carbon dioxide generated in a methanation reaction of a coal gas is adsorbed and removed by an adsorbent, Gas production process has been completed. As a result of simulating the synthetic natural gas production process using the above production method, it has been confirmed that the amount of carbon dioxide emission and the amount of hydrogen gas used are greatly reduced, and the present invention has been completed.
It is an object of the present invention to provide a method for producing synthetic natural gas using an adsorption part and a methanation reaction.
In order to accomplish the above object, the present invention provides a process for producing a carbon dioxide adsorbent, comprising: supplying a synthesis gas obtained by gasifying a raw material to a reactor filled with a carbon dioxide adsorbent, simultaneously performing a carbon monoxide methanation reaction and a water gas conversion reaction in the presence of a catalyst, Wherein the carbon dioxide produced in the step of adsorbing carbon dioxide is adsorbed by the carbon dioxide adsorbent, and a method for producing synthetic natural gas using the methanation reaction.
According to the present invention, there is also provided a process for producing a carbon dioxide adsorbent, comprising the steps of: (a) supplying a synthesis gas obtained by gasifying a raw material to a reactor filled with a carbon dioxide adsorbent, simultaneously performing a carbon monoxide methanation reaction and a water gas conversion reaction in the presence of a catalyst, Adsorbing carbon dioxide in the carbon dioxide adsorbent; And (b) the water (H 2 O) in which the carbon dioxide is converted to carbon dioxide in the presence of a catalyst by the water adsorbent is added to the carbon dioxide methanation reactor filled with hydrogen gas to remove the carbon dioxide from the adsorbed carbon dioxide adsorbent with methane, and the resulting And adsorbing the adsorbent on the adsorbent to produce methane, and a method for producing synthetic natural gas using the methanation reaction.
The method for producing synthetic natural gas using the adsorbing part and the methanation reaction according to the present invention reduces the amount of carbon dioxide discharged and the amount of hydrogen consumed to prevent warming and is useful for producing synthetic natural gas economically.
Figure 1 shows a conventional methanation reaction process.
Figure 2 shows the adsorption part and the methanation reaction process.
Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. In general, the nomenclature used herein is well known and commonly used in the art.
In the present invention, carbon dioxide generated in the methanation reaction of the coal gas and the biomass is adsorbed and removed by the adsorbent, and at the same time, a water gas conversion reaction is performed to supply hydrogen to the methanation reaction to produce a synthetic natural gas. The process of producing synthetic natural gas by carbon dioxide methanation reaction was simulated by separating carbon dioxide. As a result, the amount of carbon dioxide contained in the resulting synthetic natural gas is greatly reduced, and the amount of hydrogen gas used is greatly reduced.
Therefore, in one aspect of the present invention, there is provided a process for producing a carbon dioxide adsorbent, comprising the steps of: supplying a synthesis gas obtained by gasifying a raw material to a reactor filled with a carbon dioxide adsorbent, simultaneously performing a carbon monoxide methanation reaction and a water gas conversion reaction in the presence of a catalyst, And the generated carbon dioxide is adsorbed by the carbon dioxide adsorbent, and a method for producing synthetic natural gas using the methanation reaction.
In another aspect of the present invention, there is provided a process for producing a carbon dioxide adsorbent, comprising the steps of: (a) supplying a synthesis gas obtained by gasifying a raw material to a reactor filled with a carbon dioxide adsorbent, simultaneously performing a carbon monoxide methanation reaction and a water gas conversion reaction in the presence of a catalyst, Adsorbing the generated carbon dioxide with the carbon dioxide adsorbent; And (b) the water (H 2 O) in which the carbon dioxide is converted to carbon dioxide in the presence of a catalyst by the water adsorbent is added to the carbon dioxide methanation reactor filled with hydrogen gas to remove the carbon dioxide from the adsorbed carbon dioxide adsorbent with methane, and the resulting To the water adsorbent to produce methane, and a method for producing synthetic natural gas using the methanation reaction.
In the present invention, water (H 2 O) generated in the carbon monoxide methanation reaction may be used in a water gas conversion reaction, and hydrogen generated in the water gas conversion reaction may be used in a carbon monoxide methanation reaction have. In the conventional methanation reaction, water is produced as a by-product as shown in Fig. In addition, due to the continuous consumption of hydrogen, hydrogen must be continuously supplied. However, hydrogen gas has the risk of explosion, and the price is too high, raising the overall production cost. In the present invention, carbon monoxide is used in the hydrocyanation reaction using water generated in the carbon monoxide methanation reaction, and hydrogen generated at this time is used in the carbon monoxide methanation reaction so that the amount of hydrogen used can be minimized.
In the present invention, the raw material may be coal or biomass. Synthetic gas, in which coal is gasified, is often used for the production of synthetic natural gas. Most of the syngas is composed of carbon monoxide, hydrogen, and carbon dioxide. Synthetic gas contains a large amount of sulfur, so it is preferable to use it through a desulfurization process. The gas having the above composition may be used without limitation, but preferably coal or bismuth can be used as a raw material.
In the present invention, the synthesis gas may have a ratio of H 2 / CO of from 0.5 to 1.5. The synthesis gas produced by coal gasification has an H 2 / CO ratio of 0.5 to 1.5, and hydrogen is additionally supplied to meet the stoichiometric ratio of 3 in the conventional synthetic natural gas production process. In the present invention, however, the addition of hydrogen is minimized by supplying hydrogen in the water gas conversion reaction. Further, the ratio of H 2 / CO is preferably 0.5 to 1.5, and more preferably, the ratio of H 2 / CO can be 0.5 to 1.
In the present invention, the carbon dioxide adsorbent is a hydrotalcite (M 1-x II M x III (OH) 2 ] [A x / n n- ] m H 2 O), an alkali metal- , An alkaline earth metal oxide, or zirconate. The carbon dioxide adsorbent used in the present invention can be used without limitation as long as it is a carbon dioxide adsorbable material. However, since the reaction temperature of the present invention is carried out at around 300 ° C, hydrotalcite (M 1-x II M x to use a ⅲ (OH) 2] [a x / n n-] m H 2 O) or de-dihydro-impregnated with an alkali metal site, an alkaline earth metal oxide or zirconate (zirconate) are preferred. The hydrotalcite is preferably Mg 6 Al 2 CO 3 (OH) 16 4 (H 2 O) having Mg and Al as metal ions, and the alkali metal is preferably Li, Na, (K), rubidium (Rb), cesium (Cs) or francium (Fr), and the alkaline earth metal oxide may be beryllium oxide, magnesium oxide, calcium oxide, strontium oxide, barium oxide or radium oxide, nose carbonate may be a Li 2 ZrO 3, Na 2 ZrO 3, K 2
The carbon dioxide adsorbent adsorbs carbon dioxide generated in the water gas conversion reaction and promotes the reaction to convert carbon monoxide to methane according to the Recharteley's law. Accordingly, the stoichiometric ratio of H 2 / CO = A high reaction conversion ratio can be obtained even when H 2 / CO = 1 which is 3 or less. Also, since the produced water and carbon dioxide are consumed by the water gas conversion reaction and the carbon dioxide methanation reaction, the produced gas can be used as a synthetic natural gas without an additional separation process.
In the present invention, the step (a) may be performed at a temperature of 200 to 600 ° C and a pressure of 1 to 50 atm. As shown in FIG. 2, the carbon monoxide methanation reaction is a reaction in which the number of moles of gas is reduced, and therefore, a large amount of methane can be obtained when the reaction is carried out at a high pressure by the Recharterier's law. Also, since the methanation reaction is an exothermic reaction, the lower the internal temperature of the reactor, the larger the amount of methane, but the reaction is preferably carried out at a higher temperature than a certain level in order to maintain the reaction rate above a certain level. Therefore, it is preferably carried out at a temperature of 200 to 600 ° C and a pressure of 1 to 60 atm, more preferably at a temperature of 350 ° C and a pressure of 10 atm.
In the present invention, the ratio of H 2 / CO 2 supplied to the reactor in the step (b) may be 3 to 5. Carbon dioxide adsorbed by the adsorbent is used in the carbon dioxide methanation reaction with additional hydrogen supplied. At this time, since the carbon monoxide methanation reaction and the carbon dioxide methanation reaction do not occur at the same time, it is preferable to carry out the reaction separately in order to increase the yield of the synthetic natural gas. In addition, it is preferable to remove water generated in the carbon dioxide methanation reaction using a water adsorbent.
In the present invention, the water adsorbent may be zeolite X, zeolite Y, or a metal organic framework (MOF). Since the water adsorbent used in the carbon dioxide methanation reaction can be used without limitation as long as it is capable of adsorbing water, the carbon dioxide methanation reaction takes place at a high temperature of about 300 ° C. Therefore, the zeolite X, zeolite Y, or metal organic framework, MOF) is preferably used, and more preferably NaX zeolite can be used.
In the present invention, the step (b) may be performed at a temperature of 200 to 600 ° C. and a pressure of 1 to 50 atm. The carbon dioxide methanation reaction is also a reaction in which the number of moles of gas is reduced as in the case of the carbon monoxide methanation reaction, and therefore it is possible to obtain a large amount of methane when it is carried out at a high pressure by the Recharterier's law. However, since carbon monoxide is liquefied at high pressure, it is more preferable to carry out the reaction at the atmospheric pressure. Also, since the methanation reaction is an exothermic reaction, the lower the internal temperature of the reactor, the larger the amount of methane, but the reaction is preferably carried out at a higher temperature than a certain level in order to maintain the reaction rate above a certain level. Therefore, it is preferably carried out at a temperature of 200 to 600 ° C and a pressure of 1 to 50 atm, more preferably at a temperature of 275 ° C and a pressure of 1 atm.
In the present invention, the catalyst may be at least one selected from the group consisting of Ni, Fe, Cu, Co, Ru, Mo, Zn, Zr, Ti), cerium (Ce), or silicon (Si). The carbon monoxide methanation reaction and the carbon dioxide methanation reaction can be carried out using the same catalyst. The catalyst used here may be a metal compound containing nickel (Ni), iron (Fe), copper (Cu), cobalt (Co), ruthenium (Ru) or molybdenum (Mo) , Zirconium (Zr), titanium (Ti), cerium (Ce), or silicon (Si). In addition, as a supporter of these metal catalysts, Al 2 O 3 , C, MgAl 2 O 4 , SiO 2 , ZrO 2 , MgO, CeO 2 and TiO 2 can be used. The catalyst is more preferably Ni / Al 2 O 3, Ni / SiC, Ni / MgAl 2 O 4, Ni / TiO 2, Ni / SiO 2, Ni / ZrO 2,, Ni / MgO, Ni / CeO 2, Co 3 O 4, Co 4 Ni / SiO 2, Co 4 Ni / Al 2
[Example]
Hereinafter, the present invention will be described in more detail with reference to Examples. It is to be understood by those skilled in the art that these embodiments are only for illustrating the present invention and that the scope of the present invention is not construed as being limited by these embodiments.
Example 1: Process numerical simulation
In order to verify the feasibility of the adsorption part and the methanation reaction process for the synthesis of synthetic natural gas of the present invention, a numerical simulation of the process using the MATLAB program was carried out. At this time, Ni catalyst was used as the catalyst, and the reaction rate equation for the above three reactions was Xu and Froment (1989).
In the above equation, r CO , r WGS , and r CO2 are reaction formulas for the carbon monoxide methanation reaction, the water gas conversion reaction, and the carbon dioxide methanation reaction, respectively. K 1 , k 2 , and k 3 are reaction rate constants, and p i is the partial pressure of the i component on the gas phase. The equilibrium constants K 1 , K 2 , and K 3 were used in the literature values given by Twigg (1989). K i is the surface adsorption value of i component in the equilibrium state and is a value that varies with temperature.
The carbon dioxide adsorbent used was hydrotalcite with potassium carbonate (K 2 CO 3 ), and the adsorption model was used as shown in Lee et al., (2007).
Where n * is the amount of adsorbed carbon dioxide at a specific temperature T and pressure P, m is the saturation amount of carbon dioxide adsorbed on the surface of the adsorbent, and a is the reaction ratio of the adsorbent to carbon dioxide in the adsorption mechanism. P CO means partial pressure of carbon dioxide in gaseous state. K c and K R are equilibrium constants for temperature-dependent surface adsorption, K c 0 and K R 0 are constants, q c is molar isosteric heat of adsorption, and ΔH R Represents surface adsorption heat.
On the other hand, NaX zeolite was used as a water adsorbent and the model of water adsorption at 275 ° C is as follows. (B. T. Carvill et al., 1996)
Here, α, β, γ, and δ are empirically determined constants and their values are as follows.
? = 1.4877,? = 7.2868 * 10 -3 ,? = 2.9691,? = 0.1574
The reactor was modeled using the equation given above and the adsorption model. In the numerical model, it is assumed that the reactor is CSTRs in series. The reacting gases show ideal gas behavior, no diffusion in the axial direction of the reactor, no internal pressure reduction, and the porosity of the solid in the reactor is assumed to be constant . The governing equation using these assumptions is as follows.
Ideal gas law
Molar balance in the solid phase (linear driving force model)
Overall molar balance in the gas phase
Component molar balance
Energy balance
Where n t and ε denote the total number of moles of gas and the void fraction, respectively. N is the total flux of the gas, A is the cross-sectional area of the reactor, ρ b is the density of the solid, y j is the mole fraction of the j component, and R i is the reaction rate for the i reaction. On the other hand, R ads shows the adsorption rate of carbon dioxide, f cat shows the ratio of solid catalysts, and L stage and V stage indicate the length and volume of the CSTR stage, respectively. c ps and c pg are the heat capacities of the solid and gas, respectively, and η is the factor indicating the heat capacity of the heat exchanger tube and body. d c is the inner diameter of the reactor, T in and T w are the temperature of the injected gas and the temperature of the reactor wall, respectively, and U 0 is the overall heat transfer coefficient. n ads and n * ads are the carbon dioxide adsorption amount and the equilibrium adsorption amount of carbon dioxide, respectively. k ads is the mass transfer coefficient of the linear driving force model.
The above differential equation can be solved by numerical analysis using the MATLAB function ODE15s, and the result is obtained. The model parameter values used in this calculation are shown in Table 1.
[Table 1] Parameter values used in the process simulation
Example 2: Simulation of synthetic natural gas production process through process simulation
Numerical simulations of the process were performed using the equations presented above. Carbon monoxide methanation reaction was conducted at 350 ℃, 10atm, conditions of H 2 / CO = 1, was used as a reactant in the methanation reaction carbon dioxide, the high concentration of carbon dioxide adsorbed in the reaction again. The carbon dioxide methanation reaction was carried out under conditions of 275 ° C, 1 atm, and H 2 / CO 2 = 4. The process simulation results are shown in Table 2.
[Table 2] Methanation reaction product composition and reaction performance
As a result of the process simulation, the first reaction, carbon monoxide methanation reaction, produced 96.89% of high purity methane. As a result of the carbon dioxide methanation reaction using adsorbed carbon dioxide, methane purity of 93.08% was obtained and 98.82% of carbon dioxide was removed through this reaction.
Comparative Example 1: Adsorption by process simulation Methanation Reaction and general Methanation Comparison of reactions
The new adsorption part obtained from the examples and the methanation reaction process and the conventional methanation reaction and the reaction performance were compared. The reactant conversion rates and methane purity of the adsorbent and methanation reactions were averaged from the results of the carbon monoxide and carbon dioxide methanation reactions shown in Table 2 above. On the other hand, CO2 emissions were calculated as the sum of carbon dioxide from the two methanization reactions. The temperature and pressure were constant at 350 ° C and 10 atm for both the adsorption and methanation reactions and the general methanation reactions. The results are shown in Table 3.
[Table 3] Comparisons between adsorption and methanation reactions and general methanation reactions
In terms of reactant conversion rates, it can be seen that there is no significant difference between the adsorption and methanation reactions and the general methanation reaction process, but in terms of methane purity (49.40% → 94.99%) and carbon dioxide emissions after reaction (48.98% → 4.24%) It can be seen that the adsorption part and the methanation reaction process are superior to the general methanation reaction.
In the conventional methanation reaction, hydrogen was continuously supplied to perform the reaction. However, since the hydrogen used in the adsorption part and the methanation reaction of the present invention are supplied by the water gas conversion reaction, Can be reduced by 22%.
While the present invention has been particularly shown and described with reference to specific embodiments thereof, those skilled in the art will appreciate that such specific embodiments are merely preferred embodiments and that the scope of the present invention is not limited thereto will be. Accordingly, the actual scope of the present invention will be defined by the appended claims and their equivalents.
Claims (15)
(a) supplying a synthesis gas obtained by gasifying a raw material to a reactor filled with a carbon dioxide adsorbent, simultaneously performing a carbon monoxide methanation reaction and a water gas conversion reaction in the presence of a catalyst, wherein the carbon dioxide produced in the water gas conversion reaction is converted into carbon dioxide Adsorbing with an adsorbent; And
(b) the water (H 2 O) in which the carbon dioxide is converted to carbon dioxide in the presence of a catalyst to the water absorbent is put on the filled carbon dioxide methanation reactor together with hydrogen gas by separating carbon dioxide from the adsorbed carbon dioxide adsorbent with methane, and the resulting And adsorbing it on the water adsorbent to produce methane.
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| WO2011060556A1 (en) * | 2009-11-18 | 2011-05-26 | G4 Insights Inc. | Sorption enhanced methanation of biomass |
| KR20130130972A (en) * | 2012-05-23 | 2013-12-03 | 한국에너지기술연구원 | Method for high purity hydrogen generation |
| KR20140085671A (en) * | 2012-12-26 | 2014-07-08 | 재단법인 포항산업과학연구원 | Apparatus and method for producing synthetic natural gas using synthesis gas of low H2/CO ratio |
| KR20140119520A (en) * | 2013-04-01 | 2014-10-10 | 한국에너지기술연구원 | Method and Device for High Purity Hydrogen Generation with Fixed Catalyst |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2011060556A1 (en) * | 2009-11-18 | 2011-05-26 | G4 Insights Inc. | Sorption enhanced methanation of biomass |
| KR20130130972A (en) * | 2012-05-23 | 2013-12-03 | 한국에너지기술연구원 | Method for high purity hydrogen generation |
| KR20140085671A (en) * | 2012-12-26 | 2014-07-08 | 재단법인 포항산업과학연구원 | Apparatus and method for producing synthetic natural gas using synthesis gas of low H2/CO ratio |
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