CN113828274B - BaSrNaLSX preparation method for adsorbing carbon dioxide under low pressure - Google Patents
BaSrNaLSX preparation method for adsorbing carbon dioxide under low pressure Download PDFInfo
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- CN113828274B CN113828274B CN202111172063.1A CN202111172063A CN113828274B CN 113828274 B CN113828274 B CN 113828274B CN 202111172063 A CN202111172063 A CN 202111172063A CN 113828274 B CN113828274 B CN 113828274B
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- carbon dioxide
- ion exchange
- molecular sieve
- barium
- strontium
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 138
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 69
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 69
- 238000002360 preparation method Methods 0.000 title abstract description 10
- 239000002808 molecular sieve Substances 0.000 claims abstract description 57
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 57
- 238000005342 ion exchange Methods 0.000 claims abstract description 42
- 229910001427 strontium ion Inorganic materials 0.000 claims abstract description 36
- 229910001422 barium ion Inorganic materials 0.000 claims abstract description 26
- WOIHABYNKOEWFG-UHFFFAOYSA-N [Sr].[Ba] Chemical compound [Sr].[Ba] WOIHABYNKOEWFG-UHFFFAOYSA-N 0.000 claims abstract description 15
- PWYYWQHXAPXYMF-UHFFFAOYSA-N strontium(2+) Chemical compound [Sr+2] PWYYWQHXAPXYMF-UHFFFAOYSA-N 0.000 claims abstract description 15
- 238000001179 sorption measurement Methods 0.000 claims description 55
- 239000000463 material Substances 0.000 claims description 2
- FKNQFGJONOIPTF-UHFFFAOYSA-N Sodium cation Chemical group [Na+] FKNQFGJONOIPTF-UHFFFAOYSA-N 0.000 claims 1
- 229910001415 sodium ion Inorganic materials 0.000 claims 1
- 239000002994 raw material Substances 0.000 abstract description 8
- 238000000034 method Methods 0.000 abstract description 2
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 8
- 150000001768 cations Chemical class 0.000 description 6
- 229910052712 strontium Inorganic materials 0.000 description 5
- 239000007864 aqueous solution Substances 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000011148 porous material Substances 0.000 description 4
- 239000012266 salt solution Substances 0.000 description 4
- 229910052788 barium Inorganic materials 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 239000003463 adsorbent Substances 0.000 description 2
- 159000000009 barium salts Chemical class 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- -1 strontium cations Chemical class 0.000 description 2
- 159000000008 strontium salts Chemical class 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical group [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910001424 calcium ion Inorganic materials 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/16—Alumino-silicates
- B01J20/18—Synthetic zeolitic molecular sieves
- B01J20/186—Chemical treatments in view of modifying the properties of the sieve, e.g. increasing the stability or the activity, also decreasing the activity
-
- 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
- B01D53/02—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 by adsorption, e.g. preparative gas chromatography
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/30—Processes for preparing, regenerating, or reactivating
- B01J20/3085—Chemical treatments not covered by groups B01J20/3007 - B01J20/3078
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
Abstract
The invention discloses a preparation method of BaSrNaLSX for adsorbing carbon dioxide under low pressure. The method mainly uses an LSX molecular sieve as a raw material, and makes the ion exchange degree of the Bax/2Sry/2NazLSX molecular sieve meet the following requirements through pure barium ion, pure strontium ion or two kinds of barium strontium ion exchange: (1) The barium ion exchange degree x is 0.7-1 when pure barium ion exchange (y=0), wherein x+z=1, (2) the strontium ion exchange degree y is 0.7-1 when pure strontium ion exchange (x=0), wherein y+z=1; (3) When barium strontium ions are exchanged (x >0, y > 0), 0.7.ltoreq.x+y.ltoreq.1, where x+y+z=1. The optimal molecular sieve can absorb 8.4 to 12.8 weight percent of carbon dioxide at the temperature of 25 ℃ and the low pressure of the carbon dioxide (2 to 6 torr).
Description
Technical Field
The invention relates to a preparation method of a BaSrNaLSX molecular sieve for adsorbing carbon dioxide under low partial pressure (the partial pressure of carbon dioxide is 2-6 torr), belonging to the field of inorganic adsorption materials.
Background
When the carbon dioxide content in the air exceeds a certain concentration, the air can harm the comfort and health of human bodies for a certain time. No significant changes have been found when humans live for medium and long periods of time in an air environment with carbon dioxide concentrations less than 8000 ppm. The average pore diameter of the LSX molecular sieve is 0.74nm, and after metal cations such as barium and strontium are exchanged, the number and the position occupation of the cations in the space skeleton are different, so that attractive force and pore diameter are different. The static equilibrium adsorption capacity of the molecular sieve for carbon dioxide is saturated when the adsorption is carried out under the partial pressure of carbon dioxide of a higher pressure (250 mm Hg), which is mainly related to the capacity of molecular sieve pores, but the adsorption capacity of carbon dioxide is closely related to the pore diameter of the molecular sieve and the positions and the quantity of cations in a cage when the adsorption is carried out under the partial pressure of low carbon dioxide.
The patent CN201610218602.3 discloses a preparation method of a molecular sieve adsorbent for air separation, which prepares an X-type molecular sieve with high strength and high adsorption capacity through binder conversion, mainly utilizes a vacuum adsorption instrument to research the carbon dioxide equilibrium saturated adsorption capacity of the molecular sieve at 0 ℃/250mmgh, and does not research the adsorption capacity of the molecular sieve on carbon dioxide under low pressure.
The patent CN201811513475.5 discloses a preparation method of a binderless LSX molecular sieve, which prepares a pure sodium binderless LSX molecular sieve by binderless zeolite, and the carbon dioxide adsorption capacity can reach 9.5-10.2% when the carbon dioxide partial pressure is 4-5 torr at 25 ℃.
Patent CN201811076483.8 discloses a preparation method of a high-performance TC-5A molecular sieve adsorbent, which develops a TC-5A binderless molecular sieve through calcium ion exchange, and the carbon dioxide adsorption capacity can reach 6% when the carbon dioxide partial pressure is 4torr at 25 ℃, but the influence of the strontium barium ion content in the X molecular sieve on the carbon dioxide adsorption capacity is not illustrated.
The presently disclosed patent mainly describes the adsorption capacity of carbon dioxide by molecular sieves at high partial pressures and the adsorption capacity of carbon dioxide by sodium type x molecular sieves or 5A type molecular sieves at low partial pressures. The cation with different contents is distributed differently in the positions of the hexagonal column cage, the beta cage and the octahedral zeolite cage of the LSX molecular sieve. Because the barium and strontium cations are divalent cations, the ionic radius is larger,
the device has higher polarizability and stronger adsorption acting force on carbon dioxide; when the content of the barium strontium ions is low, the barium strontium ions are mainly located near the hexagonal column, the cations are not exposed after dehydration, the gas molecules are shielded, and the adsorption effect is weak; when the content is higher, the barium strontium ions can be positioned near the six-membered ring of the beta cage (position II), and the adsorption force of the barium strontium ions positioned at the position II on gas molecules is larger. The patent can adjust the aperture of LSX type molecular sieve by changing the exchange degree of barium and strontium ions, control the position distribution of barium and strontium cations in the cage and improve the adsorption capacity of carbon dioxide under the low pressure of carbon dioxide (2-6 torr).
Disclosure of Invention
The invention aims to provide a preparation method of BaSrNaLSX for adsorbing carbon dioxide under low pressure. The preparation method of the BaSrNaLSX molecular sieve for adsorbing carbon dioxide under low partial pressure mainly uses the LSX molecular sieve as a raw material, and adjusts the ion exchange degree of barium and strontium ions through ion exchange, changes the quantity and the position of the barium and strontium ions in a space framework, and improves the adsorption capacity of the molecular sieve for carbon dioxide under the low pressure of carbon dioxide (2-6 torr).
In order to achieve the above purpose, the invention adopts the following technical scheme: a BaSrNaLSX preparation method for adsorbing carbon dioxide under low pressure mainly uses LSX molecular sieve as raw material, and makes the ion exchange degree of Bax/2Sry/2NazLSX molecular sieve meet the following requirements by pure barium ion, pure strontium ion or barium strontium ion exchange: (1) The barium ion exchange degree x is 0.7-1 when pure barium ion exchange (y=0), wherein x+z=1, (2) the strontium ion exchange degree y is 0.7-1 when pure strontium ion exchange (x=0), wherein y+z=1; (3) When barium strontium ions are exchanged (x >0, y > 0), 0.7.ltoreq.x+y.ltoreq.1, where x+y+z=1. After drying and roasting, carrying out carbon dioxide adsorption capacity test on the sample by adopting an adsorption instrument, wherein the carbon dioxide adsorption capacity of the molecular sieve is 8.4wt% or less and 9.9wt% or less when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 2 torr; when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 4torr, the adsorption capacity of the molecular sieve to the carbon dioxide is not more than 11 weight percent and not more than 11.6 weight percent; when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 6torr, the adsorption capacity of the molecular sieve to the carbon dioxide is not more than 12.3wt percent and not more than 12.8wt percent.
The raw material LSX molecular sieve can be powder, a non-binder molecular sieve and a molecular sieve containing a binder.
The barium-strontium ion exchange can be carried out by exchanging barium ions first and then exchanging strontium ions; or exchanging strontium ions and then barium ions; the barium ion and the strontium ion can be exchanged at the same time.
The beneficial effects of the invention are as follows:
the invention adjusts the exchange degree of barium and strontium ions by carrying out the exchange of barium and strontium ions on the LSX molecular sieve, and obviously improves the adsorption capacity of the molecular sieve on carbon dioxide under the low pressure of carbon dioxide (2-6 torr).
Drawings
FIG. 1 adsorption amount of carbon dioxide by barium ion exchange sample at 25℃and carbon dioxide partial pressure of 2-6 torr
FIG. 2 shows the adsorption amount of carbon dioxide at 25℃and carbon dioxide partial pressure of 2-6 torr for a strontium ion-exchanged sample.
Detailed Description
The principles and features of the present invention are described below with reference to the drawings, the illustrated embodiments are provided for illustration only and are not intended to limit the scope of the present invention.
The method mainly uses an LSX molecular sieve as a raw material, and uses barium ions and strontium ions to exchange in an aqueous solution, so that the ion exchange degree of the Bax/2Sry/2NazLSX molecular sieve meets the following requirements: (1) The barium ion exchange degree x is 0.7-1 when pure barium ion exchange (y=0), wherein x+z=1, (2) the strontium ion exchange degree y is 0.7-1 when pure strontium ion exchange (x=0), wherein y+z=1; (3) When barium strontium ions are exchanged (x >0, y > 0), 0.7.ltoreq.x+y.ltoreq.1, where x+y+z=1. After drying and roasting, carrying out carbon dioxide adsorption capacity test on the sample by adopting an adsorption instrument, wherein the carbon dioxide adsorption capacity of the molecular sieve is 8.4wt% or less and 9.9wt% or less when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 2 torr; when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 4torr, the adsorption capacity of the molecular sieve to the carbon dioxide is not more than 11 weight percent and not more than 11.6 weight percent; when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 6torr, the adsorption capacity of the molecular sieve to the carbon dioxide is not more than 12.3wt percent and not more than 12.8wt percent.
Example 1 influence of different barium ion exchange degrees on adsorption of carbon dioxide on molecular sieves
The LSX molecular sieve is used as a raw material, barium salt solution is adopted in aqueous solution for ion exchange, the barium ion exchange degree is respectively 0.5, 0.7, 0.85 and 1, then an adsorption instrument is adopted, and the adsorption quantity of a sample to carbon dioxide under the low pressure (2-6 torr) of the carbon dioxide is tested, and the specific result is shown in Table 1.
TABLE 1 influence of different barium ion exchange degrees on adsorption of carbon dioxide by molecular sieves at different pressures
As is clear from Table 1, the adsorption amount of carbon dioxide by the molecular sieve at low pressure (2 to 6 torr) is highest when the barium ion exchange degree is 0.7 to 1, and most preferably 0.85 to 1.
Example 2 Effect of different strontium ion exchange degrees on adsorption of carbon dioxide on molecular sieves
The LSX molecular sieve is used as a raw material, a strontium salt solution is adopted in an aqueous solution for ion exchange, the strontium ion exchange degrees are respectively 0.4, 0.7, 0.85 and 1, then an adsorption instrument is adopted, and the adsorption amount of a sample to carbon dioxide under the low pressure (2-6 torr) of the carbon dioxide is tested, and the specific results are shown in Table 2.
TABLE 2 influence of different strontium ion exchange degrees on adsorption of carbon dioxide by molecular sieves at different pressures
As is clear from Table 2, the molecular sieve has the highest adsorption amount of carbon dioxide at low pressure (2-6 torr) when the ion exchange degree of strontium is 0.7-1, and most preferably 0.85-1.
Example 3 Effect of the sum of different barium strontium ion exchange degrees on adsorption of carbon dioxide on molecular sieves
The LSX molecular sieve is used as a raw material, a barium salt solution, a strontium salt solution or a barium-strontium mixed solution is adopted in an aqueous solution to carry out ion exchange, the specific ion exchange degree is shown in table 3, then an adsorption instrument is adopted to test the adsorption quantity of a sample to carbon dioxide under the low pressure (2-6 torr) of the carbon dioxide, and the specific result is shown in table 3.
TABLE 3 influence of different barium ion and strontium ion exchange degrees on adsorption of carbon dioxide by molecular sieves at different pressures
As can be seen from Table 3, the adsorption amount of carbon dioxide at low pressure (2-6 torr) of the molecular sieve can be improved by using two ion exchange molecular sieve samples of barium ion and strontium ion.
While only the preferred embodiments of the present invention have been described above, it should be noted that it will be apparent to those skilled in the art that various changes and modifications can be made herein without departing from the general inventive concept, and these should also be regarded as the scope of the invention, which is not to be limited to the effects of the invention in its practice or the application of the patent.
Claims (2)
1. The application of mixed barium-strontium ion exchange molecular sieve in adsorbing carbon dioxide at low pressure adopts LSX molecular sieve as material and adopts two kinds of barium-strontium ion exchange, when the barium ion exchange degree is 0.5, the strontium ion exchange degree is 0.2 and the sodium ion exchange degree is 0.3, the prepared molecular sieve has high carbon dioxide adsorption capacity at 25 deg.c and carbon dioxide pressure of 2-4 torr.
2. The use according to claim 1, wherein the molecular sieve is prepared at a temperature of 25 ℃ and a carbon dioxide pressure of 2 and 4torr with a maximum adsorption of 8.8wt% to 11.3wt%.
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| CN113828274B true CN113828274B (en) | 2023-12-08 |
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| Low-pressure performance evaluation of CO2, H2O andCH4 on Li-LSX as a superior adsorbent for air prepurification;Franklin E. Epiepang et al;《Chemical Engineering Science》;第147卷;第2.2-2.3节，第3.1节，图1 * |
| 微孔—介孔复合分子筛的合成及其对CO2吸附性能的研究;马燕辉;《中国优秀硕士学位论文全文数据库工程科技Ⅰ辑》;B014-167 * |
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