CN113828274A - Preparation method of BaSrNaLSX for adsorbing carbon dioxide under low pressure - Google Patents
Preparation method of BaSrNaLSX for adsorbing carbon dioxide under low pressure Download PDFInfo
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- CN113828274A CN113828274A CN202111172063.1A CN202111172063A CN113828274A CN 113828274 A CN113828274 A CN 113828274A CN 202111172063 A CN202111172063 A CN 202111172063A CN 113828274 A CN113828274 A CN 113828274A
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- carbon dioxide
- barium
- strontium
- ion exchange
- molecular sieve
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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 claims 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
- 238000001179 sorption measurement Methods 0.000 claims abstract description 55
- 238000005342 ion exchange Methods 0.000 claims abstract description 42
- 229910001427 strontium ion Inorganic materials 0.000 claims abstract description 31
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims abstract description 19
- 229910001422 barium ion Inorganic materials 0.000 claims abstract description 19
- 229910052788 barium Inorganic materials 0.000 claims abstract description 15
- WOIHABYNKOEWFG-UHFFFAOYSA-N [Sr].[Ba] Chemical compound [Sr].[Ba] WOIHABYNKOEWFG-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910052712 strontium Inorganic materials 0.000 claims abstract description 13
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims abstract description 12
- 150000002500 ions Chemical group 0.000 claims abstract description 9
- 239000002994 raw material Substances 0.000 claims abstract description 9
- PWYYWQHXAPXYMF-UHFFFAOYSA-N strontium(2+) Chemical group [Sr+2] PWYYWQHXAPXYMF-UHFFFAOYSA-N 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 4
- 150000001768 cations Chemical class 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 239000007864 aqueous solution Substances 0.000 description 4
- 239000011148 porous material Substances 0.000 description 4
- 239000012266 salt solution Substances 0.000 description 4
- 239000011230 binding agent Substances 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
- -1 barium and strontium Chemical class 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
- 239000000463 material Substances 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 239000011734 sodium Substances 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
- 229940006465 strontium cation Drugs 0.000 description 1
Images
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. Mainly takes an LSX molecular sieve as a raw material, and the ion exchange degree of the Bax/2Sry/2NazLSX molecular sieve meets the following requirements through ion exchange of pure barium ions, pure strontium ions or barium strontium ions: (1) the ion exchange degree x of barium is 0.7-1 when pure barium is ion exchanged (y = 0), wherein x + z =1, (2) the ion exchange degree y of strontium is 0.7-1 when pure strontium is ion exchanged (x = 0), wherein y + z =1; (3) when barium strontium ion exchange is carried out (x >0, y > 0), 0.7 is less than or equal to x + y is less than or equal to 1, wherein x + y + z = 1. The adsorption capacity of the optimal molecular sieve to carbon dioxide can reach 8.4-12.8 wt% at 25 ℃ and low pressure (2-6 torr) of carbon dioxide.
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 the carbon dioxide is 2-6 torr), and belongs to the field of inorganic adsorbing materials.
Background
When the carbon dioxide content in the air exceeds a certain concentration, the comfort and health of the human body can be damaged after a certain time. No significant change has been found when humans live for medium and long periods of life 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 exchange of metal cations such as barium and strontium, the number and position occupation of the cations in a space framework are different, so that the attraction and the pore diameter are different. When adsorption is carried out under a high (250 mm Hg) carbon dioxide partial pressure, the molecular sieve reaches saturation of the carbon dioxide static equilibrium adsorption capacity which is mainly related to the pore volume of the molecular sieve, but when adsorption is carried out under a low carbon dioxide partial pressure, the carbon dioxide adsorption capacity is closely related to the pore diameter of the molecular sieve, and the position and the quantity of cations in a cage.
Patent CN201610218602.3 is a method for preparing molecular sieve adsorbent for air separation, which prepares X-type molecular sieve with high strength and high adsorption capacity by binder conversion, mainly utilizes vacuum adsorption apparatus to study carbon dioxide equilibrium saturation adsorption capacity of molecular sieve at 0 ℃/250mmgh, and does not study adsorption capacity of molecular sieve to carbon dioxide under low pressure.
Patent CN201811513475.5 is a preparation method of a binderless LSX molecular sieve, which prepares a pure sodium type binderless LSX molecular sieve by binderless zeolite, and the carbon dioxide adsorption capacity can reach 9.5-10.2% at 25 ℃ and a carbon dioxide partial pressure of 4-5 torr.
Patent CN201811076483.8 is a preparation method of a high performance TC-5A molecular sieve adsorbent, which develops a TC-5A binder-free molecular sieve through calcium ion exchange, and when the carbon dioxide partial pressure is 4torr at 25 ℃, the carbon dioxide adsorption capacity can reach 6%, but the influence of the strontium barium ion content in the X molecular sieve on the carbon dioxide adsorption capacity is not elucidated.
The presently published patents mainly address the adsorption capacity of carbon dioxide by molecular sieves at high partial pressures and the adsorption capacity of carbon dioxide by sodium x molecular sieves or 5A molecular sieves at low partial pressures. The cations with different contents are distributed differently at the positions of the hexagonal column cages, the beta cages and the octahedral zeolite cages of the LSX type molecular sieve. Because the barium and strontium cations are divalent cations and have larger ionic radius,
the material has higher polarizability and stronger adsorption acting force on carbon dioxide; when the content of barium strontium ions is low, the barium strontium ions are mainly positioned near the hexagonal prism, cations are not exposed after dehydration, a shielding effect is realized on gas molecules, and an adsorption effect is weak; when the content is higher, the barium strontium ions can be positioned near the beta cage six-membered ring (position II), and the barium strontium ions positioned at the position II have larger adsorption action on gas molecules. This patent is through changing barium, strontium ion exchange degree, and adjustable LSX type molecular sieve aperture controls barium strontium cation position distribution in the cage, improves the adsorption capacity to carbon dioxide under carbon dioxide low pressure (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 takes an LSX molecular sieve as a raw material, adjusts the ion exchange degree of barium and strontium through ion exchange, changes the number and positions of barium and strontium ions in a space framework, and improves the adsorption capacity of the molecular sieve to the carbon dioxide under the low pressure (2-6 torr) of the carbon dioxide.
In order to achieve the purpose, the invention adopts the technical scheme that: a BaSrNaLSX preparation method for adsorbing carbon dioxide under low pressure mainly takes an LSX molecular sieve as a raw material, and the ion exchange degree of the Bax/2Sry/2NazLSX molecular sieve meets the following requirements through pure barium ion, pure strontium ion or barium strontium ion exchange: (1) the ion exchange degree x of barium is 0.7-1 when pure barium is ion exchanged (y = 0), wherein x + z =1, (2) the ion exchange degree y of strontium is 0.7-1 when pure strontium is ion exchanged (x = 0), wherein y + z =1; (3) when barium strontium ion exchange is carried out (x >0, y > 0), 0.7 is less than or equal to x + y is less than or equal to 1, wherein x + y + z = 1. After drying and roasting, testing the carbon dioxide adsorption capacity of the sample by using an adsorption instrument, wherein when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 2torr, the adsorption capacity of the molecular sieve to the carbon dioxide is more than or equal to 8.4wt% and less than or equal to 9.9 wt%; 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 more than or equal to 11 weight percent and less than or equal to 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 more than or equal to 12.3 weight percent and less than or equal to 12.8 weight percent.
The raw material LSX molecular sieve can be powder, a molecular sieve without a binder and a molecular sieve containing a binder.
The barium and strontium ion exchange can be carried out by exchanging barium ions first and then exchanging strontium ions; strontium ions can be exchanged first, and then barium ions can be exchanged; barium ions may also be exchanged simultaneously with strontium ions.
The invention has the beneficial effects that:
according to the invention, barium and strontium ion exchange is carried out on the LSX molecular sieve, so that the barium and strontium ion exchange degree is adjusted, and the adsorption capacity of the molecular sieve to carbon dioxide under the low pressure (2-6 torr) of the carbon dioxide is obviously improved.
Drawings
FIG. 1 shows that the barium ion exchange sample adsorbs carbon dioxide at 25 ℃ and a carbon dioxide partial pressure of 2-6 torr
In FIG. 2, the strontium ion exchange sample has a carbon dioxide adsorption capacity of 2-6 torr at 25 ℃.
Detailed Description
The principles and features of the present invention are described below in conjunction with the following drawings, which are set forth to illustrate, but are not to be construed to limit the scope of the invention.
Mainly takes an LSX molecular sieve as a raw material, and barium ions and strontium ions are exchanged in an aqueous solution to ensure that the ion exchange degree of the Bax/2Sry/2NazLSX molecular sieve meets the following requirements: (1) the ion exchange degree x of barium is 0.7-1 when pure barium is ion exchanged (y = 0), wherein x + z =1, (2) the ion exchange degree y of strontium is 0.7-1 when pure strontium is ion exchanged (x = 0), wherein y + z =1; (3) when barium strontium ion exchange is carried out (x >0, y > 0), 0.7 is less than or equal to x + y is less than or equal to 1, wherein x + y + z = 1. After drying and roasting, testing the carbon dioxide adsorption capacity of the sample by using an adsorption instrument, wherein when the adsorption temperature is 25 ℃ and the carbon dioxide partial pressure is 2torr, the adsorption capacity of the molecular sieve to the carbon dioxide is more than or equal to 8.4wt% and less than or equal to 9.9 wt%; 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 more than or equal to 11 weight percent and less than or equal to 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 more than or equal to 12.3 weight percent and less than or equal to 12.8 weight percent.
Example 1 Effect of different barium ion exchange degrees on carbon dioxide adsorption on molecular sieves
The LSX molecular sieve is used as a raw material, barium salt solution is adopted in an aqueous solution for ion exchange, the barium ion exchange degrees are respectively 0.5, 0.7, 0.85 and 1, then an adsorption instrument is adopted, and the adsorption capacity 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 1.
TABLE 1 influence of different barium ion exchange degrees on adsorption of carbon dioxide on molecular sieves at different pressures
As can be seen from Table 1, when the degree of exchange of barium ion is 0.7 to 1, preferably 0.85 to 1, the molecular sieve has the highest adsorption amount of carbon dioxide at low pressure (2 to 6 torr).
EXAMPLE 2 Effect of different strontium ion exchange degrees on carbon dioxide adsorption 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, the adsorption capacity 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 2.
TABLE 2 influence of different strontium ion exchange degrees on adsorption of carbon dioxide by molecular sieves at different pressures
As can be seen from Table 2, when the strontium ion exchange degree is 0.7 to 1, preferably 0.85 to 1, the adsorption amount of the molecular sieve to carbon dioxide is the highest at low pressure (2 to 6 torr).
EXAMPLE 3 Effect of the summation of different barium strontium ion exchange degrees on the adsorption of carbon dioxide by 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 for ion exchange, the specific ion exchange degree is shown in table 3, then an adsorption instrument is adopted, the adsorption capacity 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 3.
TABLE 3 influence of different exchange degrees of barium ion and strontium ion on adsorption of carbon dioxide by molecular sieves under different pressures
As can be seen from Table 3, the adsorption amount of the molecular sieve to carbon dioxide under low pressure (2-6 torr) can be improved by exchanging the molecular sieve sample with two ions, namely barium ion and strontium ion.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various changes and modifications can be made without departing from the overall concept of the invention, and these should be considered as the protection scope of the present invention, which will not affect the effect of the implementation of the present invention and the practicability of the patent.
Claims (5)
1. A preparation method of BaSrNaLSX for adsorbing carbon dioxide under low pressure is characterized in that an LSX molecular sieve is used as a raw material, and the molecular sieve with high carbon dioxide adsorption capacity at 25 ℃ and low carbon dioxide pressure (2-6 torr) is prepared through ion exchange of pure barium ions, pure strontium ions or barium-strontium ions.
2. The method according to claim 1, wherein the ion exchange degree of barium is 0.7 to 1, and the optimal ion exchange degree is 0.85 to 1 when pure barium is ion exchanged.
3. The method of claim 1, wherein the strontium ion exchange degree is 0.7 to 1, and the optimal exchange degree is 0.85 to 1 when pure strontium is ion exchanged.
4. The method of claim 1, wherein the ion exchange of barium and strontium is performed so that the sum of the ion exchange degrees of barium and strontium is not less than 0.7 and the sum of the ion exchange degrees of barium and strontium is not more than 1.
5. The molecular sieve of claim 1, wherein the molecular sieve has a maximum adsorption capacity of 9.9wt% at 25 ℃ under a low pressure of carbon dioxide (2 torr) and a maximum adsorption capacity of 12.8wt% at 25 ℃ under a low pressure of carbon dioxide (6 torr).
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