CN106268645B - A kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane - Google Patents
A kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane Download PDFInfo
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- CN106268645B CN106268645B CN201610861224.0A CN201610861224A CN106268645B CN 106268645 B CN106268645 B CN 106268645B CN 201610861224 A CN201610861224 A CN 201610861224A CN 106268645 B CN106268645 B CN 106268645B
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- 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
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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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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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C11/00—Aliphatic unsaturated hydrocarbons
- C07C11/02—Alkenes
- C07C11/04—Ethylene
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C7/00—Purification; Separation; Use of additives
- C07C7/12—Purification; Separation; Use of additives by adsorption, i.e. purification or separation of hydrocarbons with the aid of solids, e.g. with ion-exchangers
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C9/00—Aliphatic saturated hydrocarbons
- C07C9/02—Aliphatic saturated hydrocarbons with one to four carbon atoms
- C07C9/06—Ethane
Abstract
The invention discloses a kind of preparation methods of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane.This method mainly includes the following steps: the preparation of (1) carbon material；(2) preparation of the carbon-based adsorbent material of Fluorin doped.The carbon-based adsorbent material of Fluorin doped prepared by the present invention not only has the feature of Preferential adsorption ethane, but also all has very high adsorption capacity to ethane and ethylene；Compared with the π complexing adsorbent reported at present, heat of adsorption is low, stable structure, has a good application prospect in terms of adsorbing separation ethane and ethylene.
Description
Technical field
The present invention relates to ethylene and ethane adsorption and separation material field, and in particular to one kind has Preferential adsorption ethane characteristic
The carbon-based adsorption and separation material of Fluorin doped preparation method.
Background technique
Ethylene is a kind of important industrial chemicals, is not only widely used in manufacture polymer, and also can be used as synthesis, other have
The intermediate of machine synthesis.The whole world produces the ethylene and propylene more than 200,000,000 tons every year, wherein ethylene (C2H4) it is simplest alkene,
It is also the industrial maximum chemical products of production scale.Industrially to obtain high-purity ethylene main path mostly come from by
Alkene and alkane separation in cracking gas come out.Since the relative volatility of ethylene and ethane differs very little, industrial at present point
It is usually that high pressure, low-temperature fractionating tower is applied to be separated from ethylene and ethane, this is the lock out operation extremely to consume energy, behaviour
The production cost of ethylene of 75-85% is occupied as cost.In order to reduce energy consumption, production cost of ethylene is reduced, people also exist always
Research and development can carry out the new method of separation ethylene and ethane at normal temperatures and pressures.The method reported in the past 10 years mainly has reversible chemical
Complexometry, membrane separation process, absorption method.And absorption method due to that can be separated under normal temperature and pressure conditions, it is considered to be most work
The new method of the separation alkene and alkane of industry application prospect.Adsorbent is its key in adsorption separation method, its performance will certainly
The efficiency and energy consumption of this fixed separation process.
Report, which can be applied to ethylene and the adsorbent of ethane separation, in recent years mainly has zeolite, active carbon and metal organic
Framework material (MOFs) etc..Way more classical at present is main by the way that Cu (I) and Ag (I) are supported on high-specific surface area
On carrier, by the ethylene in pi bond complexing Preferential adsorption ethylene-ethane gaseous mixture, the separation of ethylene and ethane is realized.Example
Such as, Tiscornia etc. uses AgNO3Ag (I)/ETS-10 adsorbent is made in solution modification ETS-10 porous material, not only preferential to inhale
Attached propylene, and to the adsorption capacity of propylene 311K up to 1.02mmol/g (Tiscornia Ines, Irusta Silvia,
Pradanos Pedro,Tellez Carlos,Coronas Joaquin,Santamaria Jesus.Preparation and
characterization of titanosilicate Ag-ETS-10for propylene and propane
adsorption[J].J.Phys.Chem.C,2007,111:4702-4709)；Li et al. has synthesized Ag+Porous virtue after functionalization
Fragrant framework material, and confirm due to Ag+π complexing material promotes the adsorption capacity of ethylene from 2.95mmol/g
4.1mmol/g is arrived, simultaneous selection also increases 125 (Li B, Zhang Y, Krishna R, Yao K, Han from 0.88
Y,Wu Z,et al.Introduction of pi-complexation into porous aromatic framework
for highly selective adsorption of ethylene over ethane.J Am Chem Soc.2014；
136(24):8654-60.).Although these π complexing adsorbents have the absorption of the characteristic and high ethylene/ethane of ethylene adsorption
Selectivity, but they have obvious deficiency: and (1) pi bond is a kind of weak chemical bond, and absorption binding force will be significantly stronger than physical absorption work
Firmly, this causes the energy consumption of desorption relatively high；(2) in cracking gas, ethylene contents account for major part, ethylene in usual cracking gas
Ratio with ethane is 15:1, if industrially using the adsorbent adsorbing separation ethylene and ethane of Preferential adsorption ethylene, is just meaned
The ethylene of high-purity can be just obtained in desorption process.In industrial processes, usually using decompression desorption or lazy
Property gas purging desorption method, the adsorption process of this Preferential adsorption ethylene is intended to additional desorption process, at least
Four adsorption desorption circulations are needed, such operating process can must increase additional energy consumption.
Based on the above reasons, if adsorbent can be (small in gaseous mixture by physisorption Preferential adsorption ethane
Part forms), then target product ethylene obtains after being directly over adsorption process, and this absorbing process will greatly simplify
Production technology and reduction energy consumption.Therefore, develop can the adsorbent of Preferential adsorption ethane have become an important project.Zhu etc.
People has probed into ball type active carbon to the absorption property of ethylene and ethane at 298K, it is found that active carbon is to ethylene at 15kPa
2mmol/g (Zhu W., Groen J.C., Miltenburg A.v., et are each about with the adsorbance of ethane
al.Comparison of adsorption behaviour of light alkanes and alkenes on Kureha
Activated carbon [J] .Carbon, 2005,43 (7): 1416-1423.), almost without selectivity.Byoung-Uk
Choi et al. reports merchandise active carbon to the absorption property of ethylene and ethane, as a result, it has been found that active carbon under low pressure can Preferential adsorption
Ethane, when 293K and pressure are 15kPa, active carbon is 0.73mmol/g to the adsorbance of ethane, and ethylene absorption amount is
0.6mmol/g(Byoung-Uk Choi D.-K.C.Adsorption Equilibria of Methane,Ethane,
Ethylene,Nitrogen,and Hydrogen onto Activated Carbon[J].J Chem Eng Data,2003,
48:603-607.), these adsorbances are relatively low, no industrial application value.In recent years, MOFs material emerges in multitude, and causes people
Probe into the concern of its aspect of performance in terms of alkene and alkane separation.Bergh etc. and Gucuyener etc. report ZIF-7 is by " exhaling
Inhale effect " realize Preferential adsorption ethane, and under the conditions of 100kPa, 25 DEG C, ZIF-7 is about 2mmol/g to ethane adsorbance
(van den Bergh J.,Gucuyener C.,Pidko E.A.,et al.Understanding the anomalous
alkane selectivity of ZIF-7in the separation of light alkane/alkene mixtures
[J].Chemistry,2011,17(32):8832-8840.)(Canan Guyener J.v.d.B.Ethane/Ethene
Separation Turned on Its Head:Selective Ethane Adsorption on the Metal-
Organic Framework ZIF-7through a Gate-Opening Mechanism[J].2010,132:17704-
17706.).Pires and Pillai etc. reports that IRMOF-8 has the characteristic of Preferential adsorption ethane, and in 100kPa, 25 DEG C of items
Under part, the ethane adsorption capacity of IRMOF-8 is 4.0mmol/g, but the selectivity factor of ethylene/ethane lower than 2 (Pires J,
Pinto ML,Saini VK.Ethane selective IRMOF-8and its significance in ethane-
ethylene separation by adsorption.ACS applied materials&interfaces.2014；6
(15):12093-9.)(Pillai RS,Pinto ML,Pires J,Jorge M,Gomes JR.Understanding Gas
adsorption selectivity in IRMOF-8using molecular simulation.ACS applied
materials&interfaces.2015；7(1):624-37.).Recently, Liang etc. has synthesized a kind of double ligand MOF material Nis
(bdc) adsorbance of (ted) 0.5, ethane of material under the conditions of 100kPa, 273K reach 6.93mmol/g, and low in pressure
When 100kPa, the selectivity factor of the ethylene/ethane of the material is 2-7.8 (Liang W., Xu F., Zhou X., et
al.Ethane selective adsorbent Ni(bdc)(ted)0.5with high uptake and its
significance in adsorption separation of ethane and ethylene[J].Chemical
Engineering Science,2016,148:275-281.).These MOFs adsorbents are primarily present high production cost, absorption
The problems such as capacity is low or stability is poor, limits its industrial applications.
In face of these there are problem, the present invention provides one kind have Preferential adsorption ethane characteristic, again to ethane with compared with
The preparation method of high adsorption capacity and the carbon-based adsorbent material of the Fluorin doped of stable structure.
Summary of the invention
During being used for adsorbing separation ethylene and ethane for existing porous material, there are energy consumptions
Greatly, adsorbance and the problems such as not high selectivity, providing a kind of has Preferential adsorption ethane, higher ethane and ethylene selectivity special
The preparation method of the carbon-based adsorption and separation material of the Fluorin doped of sign.
The invention is realized by the following technical scheme.
A kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane, comprising the following steps:
(1) preparation of carbon material: by glucide preparation glucide aqueous solution soluble in water, after carrying out carburizing reagent,
It is dry by reaction product deionized water centrifuge washing, obtain carbon material；
(2) it the preparation of the carbon-based adsorbent material of Fluorin doped: is fully ground, obtains after obtained carbon material is mixed with potassium hydroxide
To solid mixture；Polytetrafluoroethylene (PTFE) is added into solid mixture again to be mixed, is uniformly mixed and is placed in tube furnace,
It is reacted after heat temperature raising under atmosphere of inert gases, obtains the carbon-based adsorbent material of crude Fluorin doped；By crude Fluorin doped
Carbon-based adsorbent material is wash with distilled water, dry, obtains the carbon-based adsorbent material of Fluorin doped of the Preferential adsorption ethane.
Further, in step (1), the glucide includes one or more of starch and starch sugar.
Further, in step (1), the concentration of the glucide aqueous solution is 0.0125g/ml-0.4g/ml.
Further, in step (1), the temperature of the carburizing reagent is 140-220 DEG C, reaction time 4-24h.
Further, in step (2), the mass ratio of the carbon material and potassium hydroxide is 1:1-1:6.
Further, in step (2), the mass ratio of the polytetrafluoroethylene (PTFE) and carbon material is 1:1-20:1.
Further, in step (2), the atmosphere of inert gases is argon gas, nitrogen or argon-nitrogen mixed gas.
Further, in step (2), the heating rate of the heat temperature raising is 2-10 DEG C/min.
Further, in step (2), the temperature of the reaction is 550-850 DEG C, reaction time 0.5-4h.
Compared with prior art, the invention has the following beneficial effects:
(1) the carbon-based adsorbent material of Fluorin doped prepared by the present invention has the feature of obvious Preferential adsorption ethane, to ethane and
Ethylene not only all has higher adsorption capacity, but also ethane with higher and ethylene absorption selectivity；
(2) the carbon-based adsorbent material stable structure of Fluorin doped prepared by the present invention, potential good adsorbing separation ethane and second
The application prospect of alkene；
(3) operation of the present invention is simple, easy to accomplish, favorable reproducibility.
Detailed description of the invention
Fig. 1 is the N of the carbon-based carbon material of Fluorin doped of Examples 1 to 4 preparation2Suction-desorption isotherm；
Fig. 2 is the infrared spectrum of the carbon-based carbon material of Fluorin doped of Examples 1 to 4 preparation；
Fig. 3 a, Fig. 3 b, Fig. 3 c and Fig. 3 d are that the ethylene of the carbon-based carbon material of Fluorin doped of Examples 1 to 4 preparation and ethane are inhaled
Attached thermoisopleth.
Specific embodiment
Below in conjunction with specific embodiment, the present invention is further elaborated, but the present invention is not limited to following embodiments.
The polytetrafluoroethylene (PTFE) that embodiment of the present invention uses is raw material band.
The present invention is using the ASAP2020 specific surface area and pore analysis instrument of U.S. Micro company production to prepared fluorine
The pore structure of doped carbon adsorbing material is characterized.
Embodiment 1
(1) starch of 4g is dissolved in the water of 40ml, at 180 DEG C carry out carburizing reagent 10h, obtained product spend from
It is dried after sub- water centrifuge washing, obtains crude carbon material；
(2) 0.3g carbon material is mixed with KOH by 1:4 mass ratio, and be fully ground, it is mixed in the solid that grinding obtains
It closes addition 0.3g raw material band in object and is mixed (mass ratio of raw material band and carbon material is 1:1), the material dress after mixing
It in porcelain boat, is put into high temperature process furnances, and control heating rate is 5 DEG C/min, carry out table after rising to 800 DEG C under nitrogen atmosphere
Face adulterates fluorine and reacts 1h, is cleaned with distilled water to the carbon-based adsorbent material of crude Fluorin doped after cooling, dry, obtains fluorine and mixes
Miscellaneous carbon-based adsorbent material, is named as carbon 1#.
Embodiment 2
(1) starch of 2g is dissolved in the water of 50ml, carries out carburizing reagent for 24 hours at 140 DEG C, centrifuge separation obtains
It is dried after product deionized water centrifuge washing, obtains crude carbon material；
(2) 0.3g carbon material is mixed with KOH by 1:1 mass ratio, and be fully ground, obtain solid mixing in grinding
1.8g raw material band is added in object and is mixed (mass ratio of raw material band and carbon material is 6:1), the material after mixing is mounted in
Porcelain boat is put into high temperature process furnances, and controlling heating rate under argon atmosphere is 2 DEG C/min, carries out surface after rising to 550 DEG C
It adulterates fluorine and reacts 3h, the carbon-based adsorbent material of crude Fluorin doped is cleaned with distilled water after cooling, it is dry, obtain Fluorin doped
Carbon-based adsorbent material is named as carbon 2#.
Embodiment 3
(1) starch of 1g is dissolved in the water of 80ml, carburizing reagent 4h, centrifuge separation, obtained production is carried out at 180 DEG C
It is dried after object deionized water centrifuge washing, obtains crude carbon material；
(2) 0.3g carbon material is mixed with KOH by 1:5 mass ratio, and be fully ground, it is mixed in the solid that grinding obtains
It closes addition 6g raw material band in object and is mixed (mass ratio of raw material band and carbon material is 20:1), the material after mixing is mounted in
Porcelain boat is put into high temperature process furnances, and controlling heating rate under argon-nitrogen gaseous mixture atmosphere is 10 DEG C/min, rises to 850
Surface doping fluorine is carried out after DEG C and reacts 0.5h, and the carbon-based adsorbent material of crude Fluorin doped is cleaned with distilled water after cooling,
It is dry, the carbon-based adsorbent material of Fluorin doped is obtained, carbon 3# is named as.
Embodiment 4
(1) starch of 8g is dissolved in the water of 20ml, carries out carburizing reagent for 24 hours at 220 DEG C, centrifuge separation obtains
It is dried after product deionized water centrifuge washing, obtains crude carbon material；
(2) 0.3g carbon material is mixed with KOH by 1:6 mass ratio, and be fully ground, it is mixed in the solid that grinding obtains
It closes addition 2.1g raw material band in object and is mixed (mass ratio of raw material band and carbon material is 7:1), the material dress after mixing
It in porcelain boat, is put into high temperature process furnances, and control heating rate is 3 DEG C/min, carry out table after rising to 750 DEG C under nitrogen atmosphere
Face adulterates fluorine and reacts 4h, is cleaned with distilled water to the carbon-based adsorbent material of crude Fluorin doped after cooling, dry, obtains fluorine and mixes
Miscellaneous carbon-based carbon material, is named as carbon 4#.
Fig. 1 is the N of the carbon-based adsorbent material of Fluorin doped made from Examples 1 to 42Suction-desorption isotherm, according to thermoisopleth meter
Calculate the specific surface area and Kong Rong for obtaining material, the specific surface area and hole of the carbon-based adsorbent material of Fluorin doped of Examples 1 to 4 preparation
The results are shown in Table 1 for structural characterization.
The specific surface area and pore structure of the carbon-based adsorbent material of Fluorin doped prepared by table 1
As shown in Table 1, the BET specific surface area of the carbon-based adsorbent material of the Fluorin doped of preparation is 1152-2585m2/ g, total pore volume
Range is 0.46-1.46cm3/ g, Micropore volume 0.39-0.73cm3/ g illustrates that the carbon-based adsorbent material of Fluorin doped of preparation has
High specific surface area and big hole appearance and more micropore.
Fig. 2 is the infrared spectrogram of the carbon-based adsorbent material of Fluorin doped of Examples 1 to 4 preparation, as shown in Figure 2, main in figure
It will be there are three absorption peak, wherein in 3500cm-1The peak at place is the hydroxyl peak in carboxyl, 1600cm-1The peak at place is carboxylate radical
Peak, and in 1000cm-1Neighbouring peak is then mainly the peak of fluorohydrocarbon (C-F), illustrates the present invention successfully by Fluorin doped to carbon materials
Expect surface, makes carbon material surface that there is F element abundant.
Fig. 3 a, Fig. 3 b, Fig. 3 c and Fig. 3 d are that the carbon-based adsorbent material of Fluorin doped of Examples 1 to 4 preparation is distinguished at 298K
To the adsorption isotherm of ethylene and ethane, by Fig. 3 a, Fig. 3 b, Fig. 3 c and Fig. 3 d it is found that all material to the adsorption isotherm of ethane
Line is all higher than the adsorption isotherm to ethylene, hence it is evident that show the feature with Preferential adsorption ethane, and adsorption capacity is all higher,
Wherein the adsorbance of ethane is 5~6mmol/g, and the adsorbance of ethylene is 4.5~5mmol/g.
The carbon-based adsorbent material of Fluorin doped of Examples 1 to 4 preparation and the Preferential adsorption ethane adsorbent reported at present exist
It is as shown in table 2 to the comparing result of the adsorbance of ethylene and ethane under 100kPa.
Comparing result of the table 2 to the adsorbance of ethylene and ethane
As shown in Table 2, the carbon-based adsorbent material of Fluorin doped of Examples 1 to 4 preparation is high to the adsorbance of ethylene and ethane
In the adsorbent with Preferential adsorption ethane feature reported at present, and there is higher ethane selectivity.Also need to refer to
It is that the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane prepared by the present invention has than similar MOFs material preferably to stablize
Property and lower cost, have better application prospect.
Claims (8)
1. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane, which is characterized in that comprise the steps of:
(1) preparation of carbon material: will be anti-after carrying out carburizing reagent by glucide preparation glucide aqueous solution soluble in water
Product deionized water centrifuge washing is answered, it is dry, obtain carbon material；
(2) preparation of the carbon-based adsorbent material of Fluorin doped: being fully ground after obtained carbon material is mixed with potassium hydroxide, consolidate
Body mixture；Polytetrafluoroethylene (PTFE) is added into solid mixture again to be mixed, is uniformly mixed and is placed in tube furnace, in inertia
It is reacted after heat temperature raising under atmosphere, obtains the carbon-based adsorbent material of crude Fluorin doped；Crude Fluorin doped is carbon-based
Adsorbent material is wash with distilled water, dry, obtains the carbon-based adsorbent material of Fluorin doped of the Preferential adsorption ethane.
2. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is that in step (1), the glucide includes one or more of starch and starch sugar.
3. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (1), the concentration of the glucide aqueous solution is 0.0125g/ml-0.4g/ml.
4. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (1), the temperature of the carburizing reagent is 140-220 DEG C, reaction time 4-24h.
5. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (2), the mass ratio of the carbon material and potassium hydroxide is 1:1-1:6.
6. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (2), the mass ratio of the polytetrafluoroethylene (PTFE) and carbon material is 1:1-20:1.
7. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (2), the atmosphere of inert gases is argon gas, nitrogen or argon-nitrogen mixed gas.
8. a kind of preparation method of the carbon-based adsorbent material of Fluorin doped of Preferential adsorption ethane according to claim 1, special
Sign is, in step (2), the heating rate of the heat temperature raising is 2-10 DEG C/min；The temperature of the reaction is 550-850
DEG C, reaction time 0.5-4h.
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| CN107442084A (en) * | 2017-07-26 | 2017-12-08 | 华南理工大学 | A kind of poly-dopamine pitch base composite porous carbon adsorbing material of Preferential adsorption ethane and preparation method and application |
| CN108311109B (en) * | 2018-02-26 | 2021-01-19 | 华南理工大学 | Molasses-based adsorption material and preparation method and application thereof |
| CN114763260B (en) * | 2021-01-14 | 2023-09-05 | 中国科学院广州能源研究所 | Fluorine-doped hollow carbon sphere with high pore volume and preparation method and application thereof |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS61126036A (en) * | 1984-11-26 | 1986-06-13 | Hidefumi Hirai | Purification and separation of olefinic hydrocarbon |
| CN101091907A (en) * | 2007-04-19 | 2007-12-26 | 浙江大学 | Preparation of multistage natural adsorbent for treating organic waste gas, and method of use |
| CN103738958A (en) * | 2014-02-14 | 2014-04-23 | 中国矿业大学 | Preparation method for fluorine-doped graphene material |
| CN104525121A (en) * | 2014-12-03 | 2015-04-22 | 浙江大学 | Adsorbent for olefin/alkane mixed gas separation and preparation method and application thereof |
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| US8282709B2 (en) * | 2010-06-29 | 2012-10-09 | The Governors Of The University Of Alberta | Removal of ethane from natural gas at high pressure |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS61126036A (en) * | 1984-11-26 | 1986-06-13 | Hidefumi Hirai | Purification and separation of olefinic hydrocarbon |
| CN101091907A (en) * | 2007-04-19 | 2007-12-26 | 浙江大学 | Preparation of multistage natural adsorbent for treating organic waste gas, and method of use |
| CN103738958A (en) * | 2014-02-14 | 2014-04-23 | 中国矿业大学 | Preparation method for fluorine-doped graphene material |
| CN104525121A (en) * | 2014-12-03 | 2015-04-22 | 浙江大学 | Adsorbent for olefin/alkane mixed gas separation and preparation method and application thereof |
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