CN106831292B - The separating technology of Catalyst for Oxidative Coupling of Methane reaction product - Google Patents
The separating technology of Catalyst for Oxidative Coupling of Methane reaction product Download PDFInfo
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- CN106831292B CN106831292B CN201710006765.XA CN201710006765A CN106831292B CN 106831292 B CN106831292 B CN 106831292B CN 201710006765 A CN201710006765 A CN 201710006765A CN 106831292 B CN106831292 B CN 106831292B
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
- C07C2/76—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen
- C07C2/82—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling
- C07C2/84—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling catalytic
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/40—Ethylene production
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Abstract
The present invention relates to a kind of separating technology of Catalyst for Oxidative Coupling of Methane reaction product, mainly solve the problems, such as that Recovery rate of ethylene is lower, energy consumption is higher.The present invention by using a kind of Catalyst for Oxidative Coupling of Methane reaction product separating technology, energy consumption is reduced by being highly thermally integrated many energy saving means such as technology between multiply charging, expanding machine, rectifying column and ice chest and refrigerator, can not only the reaction cycles material such as isolated ethylene product and methane, ethane, and low energy consumption, is easily industrialized.Obtained ethylene product purity reaches 99.95%, Recovery rate of ethylene reaches 99% or more, with compared with scale light hydrocarbon cracking ethylene process, the technical solution that unit ethylene energy consumption can reduce by 30% or more preferably solves the above problem, can be used in Catalyst for Oxidative Coupling of Methane.
Description
Technical field
The present invention relates to a kind of separating technologies of Catalyst for Oxidative Coupling of Methane reaction product.
Background technique
Whole world ethylene production raw materials used 70% is naphtha at present, and 25% is natural gas, and 5% is coal.Due to stone brain
Oily raw material is limited by oil supply limitation, and coal utilization process environmental issue is than more prominent, and natural gas resource especially shale
The unconventional gas resources such as gas, gas hydrates not only abundance, but also clean and environmental protection, in the long term natural gas second
Alkene has bright market prospects.It is opposite with reserves with the extensive discovery and exploitation of the following global unconventional gas resource
Abundant and cheap substitute gas Petroleum Production ethylene and its downstream product becomes more and more important, and is worth causing in the industry
Attention.
Compared to natural gas indirect reformer method, methane oxidation coupling (OCM) ethylene processed (natural gas direct translation method) only needs one
Methane can be converted to ethylene by step reaction, have very high theoretical value and economic value, very attractive.From 1982
Nian Qi successively carries out the trial-production of OCM catalyst and reaction process research both at home and abroad, had studied catalyst up to 2000 kinds or more.Closely
Nian Lai, domestic and international research and development institution constantly improves catalyst, and optimizes reactor and reaction condition, to realize with high selection
Property obtain low-carbon alkene purpose.The research and development of external methane oxidation coupling (OCM) technology are with U.S.'s Xi Luliya technology public affairs
Department is the most typical.Nano-wire catalyst, the proprietary methane oxygen of Xi Luliya technology company are accurately synthesized by using biological template
Change coupling (OCM) technology can by methane at a lower temperature high-performance catalyzed conversion become ethylene.China since the eighties,
Many research units have carried out developmental research to the catalyst and reaction technology of OCM technology, wherein Chinese Academy of Sciences Lanzhou Chemical Physics
The Na of Research Institute2WO3-Mn/SiO2Catalyst Conversion and C2 selectivity are high, and stability is good, before having good application
Scape.
The product of oxidative coupling of methane is a multiple gases mixture based on the lighter hydrocarbons such as methane, ethylene, is needed
The reaction cycles material such as ethylene product and methane, ethane is obtained to remove other components by separation process.
CN102093157A discloses the process integration process of a kind of methane direct conversion ethylene and synthesis gas, provide by
It is converted into ethylene containing methane feed, while producing the combined technique of synthesis gas.The invention is overcome over by methane
Direct ethylene processed using single product as the limitation of target, in methane high yield conversion be outside ethylene, it is also contemplated that methane into
One step utilizes, i.e., high yield conversion is synthesis gas.This method needs dedicated ethene adsorbent, separates second using pressure swing adsorption method
Alkene product.
US2015/0368167A1 discloses generation and separates the technical process of ethane and ethylene, methane oxidation coupling
(OCM) contain ethane and ethylene in reaction gas, by two rectifying columns of separative unit, obtain rich in C2, be rich in methane and richness
Containing N2Three bursts of logistics.This method process is complicated, and the tower top temperature of especially the second knockout tower reaches -210 DEG C, it is desirable to provide extremely low
The cryogen of potential temperature, equipment manufacturing costs are high, realizing industrialization, there are larger difficulties.
Summary of the invention
Lower, the higher problem of energy consumption that the technical problem to be solved by the present invention is to Recovery rate of ethylene in the prior art, mentions
For a kind of separating technology of new Catalyst for Oxidative Coupling of Methane reaction product.This method higher, energy consumption with Recovery rate of ethylene
Lower advantage.
To solve the above problems, The technical solution adopted by the invention is as follows: a kind of reaction of Catalyst for Oxidative Coupling of Methane produces
The separating technology of object, includes the following steps:
(a) enter OCM reaction member after natural gas and oxygen mix, under the action of catalyst, methane be converted into including
Second
Alkene, ethane, CO, CO2、H2O, then the reaction stream of alkynes passes through compression, removing CO2, it is compression, dry
Dry step obtains removing CO2、H2OCM reaction product after O；
(b) after ice chest A, ice chest B, ice chest C, part of lighter hydrocarbons are condensed the OCM reaction product, are formed
At least three feeding streams enter domethanizing column；
(C) after ice chest D, ice chest E are cooling, part of lighter hydrocarbons are condensed demethanizer column overhead distillate, are formed extremely
It is few
Two bursts of chargings enter lightness-removing column；
(d) lightness-removing column overhead includes H2, CO and part CH4, successively pass through ice chest C, ice chest B, ice chest A
It exchanges heat with OCM reaction product；
(e) lightness-removing column tower reactor distillate is liquid CH4, first evaporation recycling cooling capacity after by expanding machine decompression freeze using
Ice chest
E, after ice chest C, ice chest B, the heat exchange of ice chest A and OCM reaction product, OCM reaction member is returned；
(f) domethanizing column reactor distillate removes C by dethanizer3 +Component, tower top C2 +Enter ethylene after group lease making acetylene removal
After rectifying column, tower top obtains high-purity ethylene product.
In above-mentioned technical proposal, it is preferable that the removing CO2Step is using hydramine method come the CO in elimination reaction product2,
3%~5% piperazine is added to be absorbent with 15%~20%MEA or 35%~50%MDEA, in CO2In absorption tower with reaction product
Contact, removes CO therein2, obtain CO2Reaction product of the content less than 1~100ppm.
In above-mentioned technical proposal, it is preferable that OCM reaction product is cooling in ice chest A, ice chest B, ice chest C, exchanges heat therewith
Cold logistics is lightness-removing column overhead, lightness-removing column tower reactor distillate, C2Cryogen and C3Cryogen.
In above-mentioned technical proposal, it is preferable that the operating pressure of domethanizing column is 2.5~3.5MPaG, and tower top temperature is -120
~-80 DEG C.
In above-mentioned technical proposal, it is preferable that demethanizer column overhead distillate is cooling in ice chest D, ice chest E, exchanges heat therewith
Cold logistics be lightness-removing column tower reactor distillate through the cooling that throttles, expanded machine decompression refrigeration lightness-removing column tower reactor distillate.
In above-mentioned technical proposal, it is preferable that the operating pressure of lightness-removing column is 2.0~3.0MPaG, and tower top temperature is -150
~-120 DEG C.
In above-mentioned technical proposal, it is preferable that the outlet pressure of expanding machine is 0.2~1.0MPaG, the outlet streams of expanding machine
Temperature is -150~-120 DEG C.
In above-mentioned technical proposal, it is preferable that the OCM reaction product after ice chest A, ice chest B, ice chest C, 30~
70wt% lighter hydrocarbons are condensed；For demethanizer column overhead distillate after ice chest D, ice chest E are cooling, 50~90wt% lighter hydrocarbons are cold
It is solidifying.
In above-mentioned technical proposal, it is preferable that the acetylene removal step uses catalytic hydrogenation method, catalyst Pd/Al2O3Type is urged
Agent, acetylene hydrogenation generates ethane and ethylene in fixed bed reactors, obtains the product that acetylene content is less than 2ppm.
In above-mentioned technical proposal, it is preferable that catalyst Na2WO3-Mn/SiO2Catalyst.
The object of the present invention is to provide the separating technology of Catalyst for Oxidative Coupling of Methane, the technical process by multiply into
Many energy saving means such as technology are highly thermally integrated between material, expanding machine, rectifying column and ice chest and refrigerator, it can not only be isolated
The reaction cycles material such as ethylene product and methane, ethane, and low energy consumption, is easily industrialized.The present invention is by methane oxidation
Coupling reaction product is separated component by the processes such as compression, hydramine method, drying, cryogenic rectification one by one, at the same use multiply into
Many energy saving means such as technology are highly thermally integrated between material, expanding machine, rectifying column and ice chest and refrigerator reduces energy consumption, obtains
Ethylene product purity reaches 99.95%, and Recovery rate of ethylene reaches 99% or more, with compared with scale light hydrocarbon cracking ethylene process,
Unit ethylene energy consumption can reduce by 20% or more, achieve preferable technical effect.
Detailed description of the invention
Fig. 1 is the flow diagram of the method for the invention.
In Fig. 1,1 is natural gas, and 2 be pure oxygen or oxygen-enriched, 3 be reaction gas, 4 is compressed reaction gas, 5 is to remove CO2
Rear reaction gas, 6 for again after compression reaction gas, 7 be reaction gas after drying and dehydrating, 8 be through ice chest A reaction after cooling
Gas, 9 be liquid separation tank A gas phase, 10 be liquid separation tank A liquid phase, 11 be through ice chest B reaction gas after cooling, 12 liquid separation tank B gas phase,
13 be liquid separation tank B liquid phase, 14- is through ice chest C reaction gas after cooling, and 15 be demethanizer column overhead distillate (H2、N2、CH4Deng
Component), 16 be demethanizer reactor distillate (C2 +~C3 +Component), 17 to be distillated through ice chest D demethanizer column overhead after cooling
Object, 18 be liquid separation tank C gas phase, 19 be liquid separation tank C liquid phase, 20 be to be through ice chest E demethanizer column overhead distillate after cooling, 21
Lightness-removing column overhead (is rich in H2, CO and N2), 22 for lightness-removing column tower reactor distillate (be rich in CH4), 23 to throttle through pressure reducing valve
Lightness-removing column tower reactor distillate after cooling, 24 for after ice chest D heating lightness-removing column tower reactor distillate, 25 be expanded machine cooling
Rear lightness-removing column tower reactor distillate, 26 for after ice chest E heating lightness-removing column tower reactor distillate, 27 be after ice chest C heating
Lightness-removing column tower reactor distillate, 28 for after ice chest B heating lightness-removing column tower reactor distillate, 29 be de- light after ice chest A heating
Tower tower reactor distillate, 30 be through ice chest C heating after lightness-removing column overhead, 31 be through ice chest B heating after lightness-removing column
Overhead, 32 are the lightness-removing column overhead after ice chest A heating, and 33 be deethanizer overhead distillate (C2 +Group
Point), 34 be dethanizer tower reactor distillate (C3 +Component), 35 be ethylene rectifying column charging (ethylene, ethane), 36 be ethylene distillation
Column overhead distillate (ethylene product), 37 be ethylene rectifying column tower reactor distillate (ethane), 38 be CO2。
The present invention will be further described below by way of examples, but is not limited only to the present embodiment.
Specific embodiment
[embodiment 1]
Using attached technical process shown in FIG. 1, enters after natural gas and oxygen mix and Na is housed2WO3-Mn/SiO2Catalyst
Oxidative coupling of methane device, reactor outlet composition be shown in Table 1.
Table 1
Reaction gas is through compressor compresses to 1.5~2.5MPaG；Subsequently into CO2Absorption tower, using 35%MDEA plus 3%
Piperazine is absorbent, CO in the reaction product after absorption2Content is reduced to 1~10ppm (mol%)；Compressor is gone successively to add
It is pressed onto 3.0~3.5MPaG, and enters drier and removes moisture, water content is made to be reduced to 1~10ppm；Dewatered reaction product
Into ice chest A and lightness-removing column overhead, lightness-removing column tower reactor distillate, (- 40~-35 DEG C) of C3 cryogen heat exchange, it is cooled to -37
~-32 DEG C, after the separation of liquid separation tank, condensate liquid enters domethanizing column, and not solidifying gas goes successively to ice chest B and lightness-removing column tower top
Distillate, lightness-removing column tower reactor distillate, (- 81~-76 DEG C) of C2 cryogen heat exchange, are cooled to -78~-73 DEG C, by liquid separation tank point
From rear, condensate liquid enters domethanizing column, and solidifying gas goes successively to ice chest C and evaporates with lightness-removing column overhead, lightness-removing column tower reactor
Object, (- 101~-96 DEG C) of C2 cryogen heat exchange out, fully enter domethanizing column after being cooled to -98~-93 DEG C；Demethanizer column overhead
2.9~3.2MPaG of operating pressure, -98~-93 DEG C of overhead condensation temperature, tower top obtains distillate main component H2、N2、CO、CH4,
Tower reactor distillate main component C2H4、C2H6、C3H6；Demethanizer column overhead distillate enters ice chest D and lightness-removing column overhead
Heat exchange, is cooled to -102~-105 DEG C, and after the separation of liquid separation tank, condensate liquid enters lightness-removing column, and not solidifying gas goes successively to cold
Case E and lightness-removing column tower reactor distillate and (- 140~-130 DEG C) of C1 cryogen heat exchange, fully enter de- after being cooled to -125~135 DEG C
Light tower；Lightness-removing column tower top 2.2~2.5MPaG of operating pressure, -128~-135 DEG C of overhead condensation temperature, the main group of overhead
Divide H2、N2, CO, tower reactor distillate be CH4Cycle stock, CH4Content reaches 98% or more；CH4Cycle stock is depressurized to by expanding machine
After 0.5~0.8MPaG, temperature reaches -148~-140 DEG C, returns to OCM after ice chest E, ice chest C, ice chest B, ice chest A heating
Reaction member；Lightness-removing column overhead uses after ice chest C, ice chest B, ice chest A heat exchange as fuel gas；Demethanizer
Reactor distillate enters dethanizer, and tower reactor distillate is C3+Component, overhead enter acetylene reactor, acetylene therein
Hydrogenation reaction occurs and is converted to ethylene and ethane, acetylene content is made to be reduced to 1~5ppm (mol%)；Material after acetylene removal enters
Ethylene rectifying column, tower reactor distillate are ethane, return to OCM reaction member, overhead is ethylene product.Ethylene product composition
It is shown in Table 2.
Table 2.
| Component | Carbon dioxide | Methane | Acetylene | Ethylene | Ethane |
| Form mol% | < 1ppm | < 300ppm | < 2ppm | ≥99.95 | < 200ppm |
Ethylene product purity reaches polymer grade ethylene specification, and Recovery rate of ethylene reaches 99%.
It is that 540kg marks oil/ton ethylene, the comprehensive energy of Catalyst for Oxidative Coupling of Methane with scale cracking ethylene device comprehensive energy consumption
Consumption is that 360kg marks oil/ton ethylene, reduces 30% or more compared with cracking ethylene technology.
[comparative example]
Patent US2015/0368167A1 discloses a kind of process of separation of methane oxidative coupling reaction product, separated
Oxidative coupling of methane product is anti-using nano-wire catalyst (methane oxidative coupling catalyst of Siluria company exploitation)
It should obtain, main composition is shown in Table 3.
Table 3
Separation process is provided with the first knockout tower and the second knockout tower, and reaction product is divided into rich in C2 object by the first knockout tower
Flow and be rich in CH4And N2Logistics, first knockout tower 205~900kPa of operating pressure, operation temperature -162~-134 DEG C.First
Wherein setting expanding machine carries out decompression cooling to knockout tower on one feed stream.Second knockout tower will be enriched in CH4、N2Logistics is divided into
Rich in CH4Logistics and be rich in N2Logistics, second knockout tower 275~585kPa of operating pressure, operation temperature -168~-210 DEG C.It should
Patent is different from the oxidative coupling of methane product composition that this patent is separated, and separation operation condition is not also identical.
Claims (10)
1. a kind of separating technology of Catalyst for Oxidative Coupling of Methane reaction product, includes the following steps:
(a) enter OCM reaction member after natural gas and oxygen mix, under the action of catalyst, methane be converted into including ethylene,
Ethane, CO, CO2、H2O, then the reaction stream of alkynes passes through compression, removing CO2, compression, drying steps, obtain removing CO2、
H2OCM reaction product after O；
(b) after ice chest A, ice chest B, ice chest C, part of lighter hydrocarbons are condensed the OCM reaction product, form at least three strands
Charging enters domethanizing column；
(C) after ice chest D, ice chest E are cooling, part of lighter hydrocarbons are condensed demethanizer column overhead distillate, form at least two
Stock charging enters lightness-removing column；
(d) lightness-removing column overhead includes H2, CO and part CH4, production is successively reacted with OCM by ice chest C, ice chest B, ice chest A
Object heat exchange；
(e) lightness-removing column tower reactor distillate is liquid CH4, freezed by expanding machine decompression using ice chest after first evaporating recycling cooling capacity
E, after ice chest C, ice chest B, the heat exchange of ice chest A and OCM reaction product, OCM reaction member is returned；
(f) domethanizing column reactor distillate removes C by dethanizer3 +Component, tower top C2 +Enter ethylene distillation after group lease making acetylene removal
After tower, tower top obtains high-purity ethylene product.
2. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that described de-
Except CO2Step is using hydramine method come the CO in elimination reaction product2, add 3% with 15%~20%MEA or 35%~50%MDEA
~5% piperazine is absorbent, in CO2It is contacted in absorption tower with reaction product, removes CO therein2, obtain CO2Content less than 1~
The reaction product of 100ppm.
3. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that OCM reaction
Product is cooling in ice chest A, ice chest B, ice chest C, and the cold logistics to exchange heat therewith is that lightness-removing column overhead, lightness-removing column tower reactor evaporate
Object, C out2Cryogen and C3Cryogen.
4. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that demethanation
The operating pressure of tower is 2.5~3.5MPaG, and tower top temperature is -120~-80 DEG C.
5. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that demethanation
Column overhead distillate is cooling in ice chest D, ice chest E, and the cold logistics to exchange heat therewith is that the lightness-removing column tower reactor through the cooling that throttles distillates
The lightness-removing column tower reactor distillate of object, expanded machine decompression refrigeration.
6. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that lightness-removing column
Operating pressure be 2.0~3.0MPaG, tower top temperature be -150~-120 DEG C.
7. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that expanding machine
Outlet pressure be 0.2~1.0MPaG, the outlet streams temperature of expanding machine is -150~-120 DEG C.
8. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that the OCM
After ice chest A, ice chest B, ice chest C, 30~70wt% lighter hydrocarbons are condensed reaction product；Demethanizer column overhead distillate is through being subcooled
After case D, ice chest E are cooling, 50~90wt% lighter hydrocarbons are condensed.
9. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that described de-
Alkynes step uses catalytic hydrogenation method, catalyst Pd/Al2O3Type catalyst, acetylene hydrogenation generates ethane in fixed bed reactors
And ethylene, obtain the product that acetylene content is less than 2ppm.
10. the separating technology of Catalyst for Oxidative Coupling of Methane reaction product according to claim 1, it is characterised in that catalyst
For Na2WO3-Mn/SiO2Catalyst.
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| CN109678636A (en) * | 2017-10-19 | 2019-04-26 | 中国石油化工股份有限公司 | A kind of separation method and device of Catalyst for Oxidative Coupling of Methane reaction gas |
| CN109678640A (en) * | 2017-10-19 | 2019-04-26 | 中国石油化工股份有限公司 | A kind of separation method and device of Catalyst for Oxidative Coupling of Methane reaction gas |
| CN109678641A (en) * | 2017-10-19 | 2019-04-26 | 中国石油化工股份有限公司 | A kind of separation method and device of Catalyst for Oxidative Coupling of Methane reaction gas |
| WO2020073853A1 (en) * | 2018-10-08 | 2020-04-16 | 中国石油化工股份有限公司 | Method and system for separating light hydrocarbons |
| CN111004079B (en) * | 2018-10-08 | 2023-07-21 | 中国石油化工股份有限公司 | Separation method and device for reaction gas for preparing ethylene by oxidative coupling of methane |
| CN111004081B (en) * | 2018-10-08 | 2023-07-21 | 中国石油化工股份有限公司 | Separation method and device for reaction gas for preparing ethylene by oxidative coupling of methane |
| CN111747815B (en) * | 2019-03-27 | 2023-04-11 | 中国石油化工股份有限公司 | Separation method of product gas of oxidative coupling reaction of methane |
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| CN101138720A (en) * | 2007-10-19 | 2008-03-12 | 北京化工大学 | Metallic-radicle integral catalyzer for direct catalytic conversion of methyl hydride and method of preparing the same |
| CN101633595A (en) * | 2008-07-24 | 2010-01-27 | 中国石油化工股份有限公司 | Method for reclaiming ethylene in catalytic dry gas |
| CN102093157A (en) * | 2009-12-09 | 2011-06-15 | 中国科学院兰州化学物理研究所 | Joint process for preparing ethylene and synthesis gas by direct conversion of methane |
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| WO2013106771A2 (en) * | 2012-01-13 | 2013-07-18 | Siluria Technologies, Inc. | Process for separating hydrocarbon compounds |
| US9670113B2 (en) * | 2012-07-09 | 2017-06-06 | Siluria Technologies, Inc. | Natural gas processing and systems |
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| CN101138720A (en) * | 2007-10-19 | 2008-03-12 | 北京化工大学 | Metallic-radicle integral catalyzer for direct catalytic conversion of methyl hydride and method of preparing the same |
| CN101633595A (en) * | 2008-07-24 | 2010-01-27 | 中国石油化工股份有限公司 | Method for reclaiming ethylene in catalytic dry gas |
| CN102093157A (en) * | 2009-12-09 | 2011-06-15 | 中国科学院兰州化学物理研究所 | Joint process for preparing ethylene and synthesis gas by direct conversion of methane |
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