CN108246249A - It is a kind of to be used to remove adsorbent of the low thermal discharge of polar molecule in material and preparation method thereof - Google Patents
It is a kind of to be used to remove adsorbent of the low thermal discharge of polar molecule in material and preparation method thereof Download PDFInfo
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- CN108246249A CN108246249A CN201810148572.2A CN201810148572A CN108246249A CN 108246249 A CN108246249 A CN 108246249A CN 201810148572 A CN201810148572 A CN 201810148572A CN 108246249 A CN108246249 A CN 108246249A
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D15/00—Separating processes involving the treatment of liquids with solid sorbents; Apparatus therefor
- B01D15/08—Selective adsorption, e.g. chromatography
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- 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
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
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- 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
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
- B01J20/08—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04 comprising aluminium oxide or hydroxide; comprising bauxite
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- 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
- B01J2220/00—Aspects relating to sorbent materials
- B01J2220/40—Aspects relating to the composition of sorbent or filter aid materials
- B01J2220/42—Materials comprising a mixture of inorganic materials
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Abstract
A kind of adsorbent for being used to remove the low thermal discharge of polar molecule in material, is made, each parts by weight of raw materials ratio is of molecular sieve, metal oxide, rare earth oxide and activated alumina：Molecular sieve 20 59.5, metal oxide 1 10, rare earth oxide 0.5 1, wherein aluminium oxide 40 64, molecular sieve are complex type molecular sieves, it is mixed by SAPO molecular sieve or SSZ molecular sieve, then with one or more in A type molecular sieve, X-type molecular sieve and Y type molecular sieve.The present invention contacts to purify alkene with adsorbent using continous way fixed bed olefin stream.Olefin feed should carry out activation procedure before being contacted with adsorbent to adsorbent, and dry nitrogen is passed through adsorbent bed heating adsorbent with certain temperature and air speed.Temperature is controlled between 250 350 degree, and air speed is less than 8000/H, and after adsorbent activates, raw material olefin material is contacted with adsorbent to be cleaned, and regeneration times are significantly increased, and service life is longer.
Description
Technical field：
The invention belongs to absorbent fields, more particularly to a kind of adsorbent for being used to remove impurity in low-carbon alkene material.
Background technology：
The dilute hydrocarbon of low-carbon（Ethylene, propylene）Basic organic chemical industry raw material is important, is occupied an important position in national economy, China
Existing ethylene, producing most of for propylene are to be produced by oil for raw material, and with the development of national economy, petroleum resources become
Shortage, and China is the country of the few oil of more coals, therefore the technology of the dilute hydrocarbon of coal low-carbon obtains the attention of people.
In production technology of the coal through the dilute hydrocarbon of methanol low-carbon, the oxidiferous impurity such as methanol/ethanol dimethyl ether can be contained,
After these impurity have to pass through purification, low-carbon alkene can be only achieved the quality level of aggregation level, inexpensive purification of light olefins and tool
There is the hot spot that low heat release flow characteristic becomes concern universal at present.
Common adsorbents are using molecular sieve as main component, to polar molecule（The dilute hydrocarbon molecule of low-carbon）There is strong absorption to make
With, amount of heat is released, the appearance of precarious position may be led to, therefore use preload technique, reduction danger.
The molecular sieve of impurity or alumina solid adsorbent in the logistics such as purification separation alkene, natural gas are frequently used for, by
It is unsaturated hydrocarbons in alkene, there is stronger polarity, impurity is also polar molecule in above-mentioned alkene, miscellaneous using molecular sieve adsorption cleaning
During matter, while alkene can be also adsorbed, adsorbent bed is caused to heat up, and then cause alkene in adsorbent surface polymerization and coking phenomenon；
When aluminium oxide makees adsorbent, though heat of adsorption is low, there are the defects of adsorption deeply and all low capacity.Chinese patent
CN201610856039.2 is improved in terms of heat of adsorption, but not good enough in terms of stability, effect still without reaching best,
The solid absorbent of low adsorption heat and depth suction-operated can not taken into account in of the same trade at present simultaneously still.
Invention content
It is difficult to have the solid absorbent that can take into account low adsorption heat and depth suction-operated simultaneously the purpose of the present invention is overcoming
The problem of, a kind of adsorbent for being used to remove the low thermal discharge of polar molecule in material is provided, activity is low, is put when adsorbing polar molecule
Heat is few, can subtract preload technique, not only reduce cost, and absorption property does not also reduce.
Technical solution is used by the present invention realizes above-mentioned purpose：One kind is used to remove the low heat release of polar molecule in material
The adsorbent of amount is made of molecular sieve, metal oxide, rare earth oxide and activated alumina, and each parts by weight of raw materials ratio is：Point
Son sieve 20-59.5, metal oxide 1-10, rare earth oxide 0.5-1, aluminium oxide 40-64, wherein molecular sieve are compound molecules
Sieve, by SAPO molecular sieve or SSZ molecular sieve, then with it is one or more mixed in A type molecular sieve, X-type molecular sieve and Y type molecular sieve
It closes.
Each parts by weight of raw materials of adsorbent is than preferred molecular sieve 35-59, metal oxide 2-8, rare earth oxide 0.5-
1, aluminium oxide 40-64.
The particle that the adsorbent is spherical, diameter is between 1-5mm.
The crystal structure of the aluminium oxide powder is γ-Al2O3, specific surface area is more than 200m2/g。
For the particle size of the raw molecule sieve between 1-4um, the content of wherein SAPO or SSZ molecular sieve accounts for absorption
The 5-10% of agent total weight.
The metal oxide uses copper oxide（CuO2）, iron oxide（Fe2O3）, tungsten oxide（WO3）Or molybdenum oxide (MoO3)
Deng.
The rare earth oxide is lanthana（La2O3）Or cerium oxide (Ce2O3) etc..
The present invention is a kind of for removing the preparation method of the purifying adsorbent of the low thermal discharge of polar molecule in material, prepares step
It is rapid as follows：
（1）Molecular sieve, alumina powder, metal oxide, rare earth oxide are sufficiently mixed by mechanical agitation；
（2）Material is added in pot forming after mixing, rotational forming, in pot forming rotation process, sprays into adhesive, graininess is made
The 15-20% that the penetrating weight of adsorbent, wherein adhesive water accounts for,
（3）Granular adsorbent is dried, and drying temperature is room temperature to 200 degrees Celsius, and drying time is 0.5 to 2 hours；
（4）Dried granular adsorbent is activated again, and activation temperature is 200 to 500 degrees Celsius, soak time 0.5
By 3 hours, finished product adsorbent is made.
The present invention is a kind of for removing the application of the purifying adsorbent of the low thermal discharge of polar molecule in material, and adsorbent is used for
Alcohol, ether, CO are removed in raw material2、The purification of water isopolarity molecular impurity, particularly preferred for removing coal through methanol olefin polymerization
The purification of impurity in material.
The present invention compared with similar products, has prominent substantive distinguishing features and significant progress, is embodied in：
（1）Another composition of adsorbent of the present invention is molecular sieve, mainly plays adsorbing contaminant.Molecular sieve is that one kind has
The water-containing crystal alumino-silicate of uniform micropore, what it is using the present invention is SAPO molecular sieve or SSZ molecular sieve, then with A type molecular sieve,
One or more mixing in X-type molecular sieve and Y type molecular sieve, wherein SSZ, SAPO molecular sieve topological structure are CHA types.Molecule
Sieve is sufficiently mixed with aluminium oxide, and the heat released during molecular sieve adsorbing contaminant is enable to disperse to be released in time, avoids molecule
Sieve adsorbent bed temperature runaway causes olefinic polymerization phenomenon.
（2）The metal oxide that the present invention adds significantly reduces thermal discharge during absorption, enhances the heat of adsorbent
Stability；Effectively reduce the carbon deposit of organic materials on the sorbent.
（3）The present invention adds micro rare earth oxide, and the stability of adsorbent has been significantly greatly increased.Hot conditions are not easy to burn
Knot and phase transformation, anti-carbon deposition ability also dramatically increase.
（4）The necessary component of adsorbent of the present invention is activated alumina, and crystal phase structure is γ-Al2O3, can be with
It is activated alumina powder available on the market, specific surface area is more than 200m2/ g, raw material are easy to get, and effect is good.
Final finished adsorbent can remove multiple pollutant in olefin feed, these olefin feeds contain：Water, titanium dioxide
The oxygenatedchemicals such as carbon, alcohol, ether, aldehyde, one kind and multiple pollutant of the sulfur-containing compounds such as hydrogen sulfide, mercaptan.
Application effect of the present invention is notable, contacts with adsorbent to purify alkene using continous way fixed bed olefin stream.Alkene
Material should carry out activation procedure before being contacted with adsorbent to adsorbent, and dry nitrogen is passed through with certain temperature and air speed
Adsorbent bed heating adsorbent.Temperature is controlled between 250-350 degree, and air speed is less than 8000/H, is activated by adsorbent
Afterwards, raw material olefin material is contacted with adsorbent is cleaned, and regeneration times are significantly increased, and service life is longer.
Description of the drawings：
Fig. 1 is the XRD diagram spectrogram of inventive samples 1#.
Specific embodiment：
With reference to example, the present invention is described in detail.
Embodiment 1
One kind is for hydrocarbon impurities purifying adsorbent, and adsorbent is by molecular sieve, metal oxide, rare earth oxide and active oxidation
Aluminium is made, each raw material weight aluminium oxide 150g, 13X molecular sieve 110g and SAPO-34 molecular sieve 10g, tungsten oxide 2g and rare earth oxygen
Compound La2O31.5g；
Preparation process is as follows：
（1）Molecular sieve, alumina powder, metal oxide, rare earth oxide are sufficiently mixed for 20 minutes by mechanical agitation；
（2）Material is added in pot forming after mixing, rotational forming, in pot forming rotation process, slowly sprays into adhesive deionization
Water 100g, is made granular adsorbent；
（3）Granular adsorbent is dried, and drying temperature is 100 degrees Celsius, and drying time is 2 hours；
（4）Dried granular adsorbent is activated again, and activation temperature is 450-480 degrees Celsius, and soak time is small for 1
When, finished product adsorbent is made（Sample 1#）.
Embodiment 2
One kind is for hydrocarbon impurities purifying adsorbent, and adsorbent is by molecular sieve, metal oxide, rare earth oxide and active oxidation
Aluminium is made, each raw material weight：Aluminium oxide 160g, 5A molecular sieve 140g, SAPO-34 molecular sieve 20g, tungsten oxide 2g, powder shape are dilute
Native oxide Ce2O32g；
Sample 2# is made with embodiment 1 in specific preparation process.
Embodiment 3
One kind is for hydrocarbon impurities purifying adsorbent, and adsorbent is by molecular sieve, metal oxide, rare earth oxide and active oxidation
Aluminium is made, each raw material weight：Aluminium oxide 200g and SSZ molecular sieve 25g, 13X molecular sieve 95g, NaY molecular sieve 60g, tungsten oxide
2g, rare earth oxide La2O32.5 g；
Sample 3# is made with embodiment 1 in specific preparation process
Embodiment 4
One kind is for hydrocarbon impurities purifying adsorbent, and adsorbent is by molecular sieve, metal oxide, rare earth oxide and active oxygen
Change aluminium to be made, each raw material weight：Aluminium oxide 120g and SSZ molecular sieve 8g, NaY molecular sieve 72g, 3 g rare earth oxides of molybdenum oxide
La2O31.5 g；
Above each raw material is sufficiently mixed, is put into water spray molding in disk rotational molding machine, 1-3mm spherical particles are chosen in screening,
It is put into electric dry oven drying, 120 degree of drying temperature, time 2 h；Then muffle furnace activates, and 460 degree of activation temperature, the time 1 is small
When；Sample 4# is made.
Embodiment 5
One kind is made for hydrocarbon impurities purifying adsorbent, adsorbent of molecular sieve, metal oxide and activated alumina, each original
Expect weight：Aluminium oxide 130g and SSZ molecular sieve 8g, 13X molecular sieve 72g, molybdenum oxide 3 g, rare earth oxide La2O31.5 g；
Above each raw material is sufficiently mixed, is put into water spray molding in disk rotational molding machine, 1-3mm spherical particles are chosen in screening,
It is put into electric dry oven drying, 120 degree of drying temperature, time 2 h；Then muffle furnace activates, and 480 degree of activation temperature, the time 1 is small
When；Sample 5# is made.
Embodiment 6
One kind is made for hydrocarbon impurities purifying adsorbent, adsorbent of molecular sieve, metal oxide and activated alumina, each original
Expect weight：Aluminium oxide 130g and SSZ molecular sieve 8g, 13X molecular sieve 72g, copper oxide 3 g, rare earth oxide La2O31.5 g；
Embodiment 7
One kind is made for hydrocarbon impurities purifying adsorbent, adsorbent of molecular sieve, metal oxide and activated alumina, each original
Expect weight：Aluminium oxide 130g and SSZ molecular sieve 8g, 13X molecular sieve 72g, iron oxide 3 g, rare earth oxide La2O31.5 g；
In addition the technique for pressing embodiment 1-7, formula do not add metal oxide, test 7 comparative examples respectively, are detected：1.
Dynamic evaluation, under actual condition state, the evaluation of adsorbent adsorbing contaminant capacity are carried out to adsorbent obtained above.
Sample of sorbent 1# 10g, 2# 10g, 4#10g is taken to be respectively charged into gas phase evaluating apparatus.In about 500/h high pure nitrogens
Under flow, 300 DEG C activate 2 hours, then cool down room temperature.Using containing trace impurity（Methanol：200ppm, dimethyl ether：200ppm、）
High pure nitrogen, with 600ml/min flow velocitys, 0.1MPa pressure under continue through adsorbent bed, the tail gas through over-molecular sieve utilizes color
The content of spectrometer checked for impurities.Investigate adsorbance of the adsorbent to impurity.
Sample of sorbent 3# 10g, 5# 10g, 6# 10g, 7# 10g is taken to be respectively charged into gas phase evaluating apparatus.In about 500/h
Under high pure nitrogen flow, 300 DEG C activate 2 hours, then cool down room temperature.Using containing trace impurity（Methanol：200ppm, dimethyl ether：
200ppm、）High pure nitrogen, with 1200ml/min flow velocitys, 0.1MPa pressure under continue through adsorbent bed, the tail through over-molecular sieve
Gas utilizes the content of chromatograph checked for impurities.Investigate adsorbance of the adsorbent to impurity.
More than testing inspection result such as table 1.
Table 1
The adsorbing contaminant capacity that can be seen that the sample that the present invention is added to metal oxide from above-mentioned detection data significantly will
It is high.
2. the evaluation of weak-exothermic reaction is carried out to the adsorbent of above-mentioned system below.
Adsorbent 1# -5# sample 10g of the present invention are taken, are packed into gas phase evaluating apparatus.Under about 500/h high pure nitrogen flows,
300 DEG C activate 2 hours, then cool down room temperature.Using containing trace impurity（Methanol：200ppm, dimethyl ether：200ppm、）High Purity Nitrogen
Gas, with 600ml/min flow velocitys, 0.1MPa pressure under continue through adsorbent bed, during by tail gas difference through over-molecular sieve
Between temperature measurement, weak-exothermic reaction of the evaluation adsorbent during adsorbing contaminant.
50 DEG C of temperature of reactor, testing result such as table 2
Table 2
| Adsorption time H | 1 | 3 | 5 | 7 | 9 |
| 1# sample exhaust temperatures DEG C | 52 | 51.5 | 52 | 50.5 | 50 |
| 2# sample exhaust temperatures DEG C | 55 | 52 | 53 | 51 | 51 |
| 3# sample exhaust temperatures DEG C | 53 | 53 | 54 | 52 | 50 |
| 4# sample exhaust temperatures DEG C | 55 | 56 | 55 | 54 | 52 |
| 5# sample exhaust temperatures DEG C | 54 | 55 | 54 | 53 | 51 |
| 6# sample exhaust temperatures DEG C | 55 | 55 | 53 | 52 | 52 |
| 7# sample exhaust temperatures DEG C | 52 | 53 | 52 | 52 | 50 |
| The similar sample exhaust temperature DEG C in market | 60 | 67 | 70 | 63 | 60 |
From data above, sample of the invention is significantly lower than market similar product heat release
3. degradation evaluates the variation of adsorbent reactivation number and adsorption capacity
By the evaluation method of sample 1#, the continuous absorption regenerations of sample 1#-5# 100 times investigate the adsorbance down ratio of adsorbent.
More than testing inspection result such as table 3
Table 3
By above-mentioned detection it is found that inventive samples adsorbance rate of descent is significantly low, service life greatly improves.
Claims (8)
1. a kind of adsorbent for being used to remove the low thermal discharge of polar molecule in material, which is characterized in that it is by molecular sieve, metal oxygen
Compound, rare earth oxide and activated alumina are made, and each parts by weight of raw materials ratio is：Molecular sieve 20-59.5, metal oxide 1-
10th, rare earth oxide 0.5-1, wherein aluminium oxide 40-64, molecular sieve are complex type molecular sieves, by SAPO molecular sieve or SSZ molecules
Sieve, then mixed with one or more in A type molecular sieve, X-type molecular sieve and Y type molecular sieve.
2. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In each parts by weight of raw materials ratio of adsorbent is：Molecular sieve 35-59, metal oxide 2-8, rare earth oxide 0.5-1, oxidation
Aluminium 40-64.
3. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In the particle that the adsorbent is spherical, diameter is between 1-5mm.
4. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In the crystal structure of the aluminium oxide powder is γ-Al2O3, specific surface area is more than 200m2/g。
5. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In, raw molecule sieve particle size between 1-4um, it is total that the content of wherein SAPO or SSZ molecular sieve accounts for adsorbent
The 5-10% of weight.
6. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In the metal oxide uses copper oxide, iron oxide, tungsten oxide or molybdenum oxide.
7. according to claim 1 a kind of for removing the adsorbent of the low thermal discharge of polar molecule in material, feature exists
In the rare earth oxide is lanthana or cerium oxide.
A kind of 8. preparation method for the purifying adsorbent for being used to remove the low thermal discharge of polar molecule in material, which is characterized in that system
Standby step is as follows：
（1）Molecular sieve, alumina powder, metal oxide, rare earth oxide are sufficiently mixed by mechanical agitation；
（2）Material is added in pot forming after mixing, rotational forming, in pot forming rotation process, sprays into adhesive, graininess is made
The 15-20% that the penetrating weight of adsorbent, wherein adhesive water accounts for,
（3）Granular adsorbent is dried, and drying temperature is room temperature to 200 degrees Celsius, and drying time is 0.5 to 2 hours；
（4）Dried granular adsorbent is activated again, and activation temperature is 200 to 500 degrees Celsius, soak time 0.5
By 3 hours, finished product adsorbent is made.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112642395A (en) * | 2019-10-11 | 2021-04-13 | 中国石油化工股份有限公司 | Molecular sieve compound and composite material as well as preparation method and application thereof |
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| CN102463101A (en) * | 2010-11-17 | 2012-05-23 | 中国石油化工股份有限公司 | Ion-exchange molecular sieve adsorbent and preparation method thereof |
| CN104383874A (en) * | 2014-12-05 | 2015-03-04 | 上海绿强新材料有限公司 | Purification adsorbent based on mesoporous molecular sieve material and preparation method and application of purification adsorbent based on mesoporous molecular sieve material |
| CN105289477A (en) * | 2015-11-19 | 2016-02-03 | 上海绿强新材料有限公司 | Adsorbent for removing impurities in olefin flow of coal chemical industry and use thereof |
| CN106423114A (en) * | 2016-09-28 | 2017-02-22 | 大连海鑫化工有限公司 | Purification adsorbent for hydrocarbon impurities, preparing method and application |
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2018
- 2018-02-13 CN CN201810148572.2A patent/CN108246249A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102463101A (en) * | 2010-11-17 | 2012-05-23 | 中国石油化工股份有限公司 | Ion-exchange molecular sieve adsorbent and preparation method thereof |
| CN104383874A (en) * | 2014-12-05 | 2015-03-04 | 上海绿强新材料有限公司 | Purification adsorbent based on mesoporous molecular sieve material and preparation method and application of purification adsorbent based on mesoporous molecular sieve material |
| CN105289477A (en) * | 2015-11-19 | 2016-02-03 | 上海绿强新材料有限公司 | Adsorbent for removing impurities in olefin flow of coal chemical industry and use thereof |
| CN106423114A (en) * | 2016-09-28 | 2017-02-22 | 大连海鑫化工有限公司 | Purification adsorbent for hydrocarbon impurities, preparing method and application |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112642395A (en) * | 2019-10-11 | 2021-04-13 | 中国石油化工股份有限公司 | Molecular sieve compound and composite material as well as preparation method and application thereof |
| WO2021068600A1 (en) * | 2019-10-11 | 2021-04-15 | 中国石油化工股份有限公司 | Molecular sieve complex, composite material and application thereof |
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