CN1309079A - Catalyst for preparing synthetic gas by reforming methane and CO2 - Google Patents
Catalyst for preparing synthetic gas by reforming methane and CO2 Download PDFInfo
- Publication number
- CN1309079A CN1309079A CN00135648A CN00135648A CN1309079A CN 1309079 A CN1309079 A CN 1309079A CN 00135648 A CN00135648 A CN 00135648A CN 00135648 A CN00135648 A CN 00135648A CN 1309079 A CN1309079 A CN 1309079A
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- Prior art keywords
- catalyst
- synthetic gas
- molecular sieve
- preparing synthetic
- methane
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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
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
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Abstract
A catalyst for preparing synthetic gas by reforming methane and CO2 is prepared from mesoporous molecular sieve MCM-41 as carrier and Ni (3-13 wt.%) as active component by impregnation method. Its advantages are less carried metal amount and high conversion and yield at low temp.
Description
The present invention relates to a kind of methane and CO 2 reformation catalyst for preparing synthetic gas and preparation method thereof.
Sweet natural gas (main component methane) transforms preparing synthetic gas and provides cheap raw material for C-1 chemistry industry, for solving energy shortage, shortage of resources and environment protection important meaning is arranged.Many important technological processs,, synthol synthetic as F-T, synthetic ammonia all need to have the synthetic gas of different ratios.Now existing nearly 10% Sweet natural gas is used to make Chemicals in the world, and wherein the throughput of methyl alcohol has surpassed annual 2200 ten thousand tons, and the Ammonia Production ability also surpasses annual 100000000 tons, wherein accounts for 80% and 76% of ultimate production respectively by gas production.
Make inertia micro-molecular gas CH
4And CO
2Activation is also carried out the orientation conversion, and its key is to select suitable catalyzer.Being used for this catalyst for reaction at present mainly is loading type Rh, Ru, Pt, Ir, Ni, Co grade in an imperial examination VIII family metal catalyst.Noble metal catalyst has the catalytic activity height, carbon distribution is few or the advantage of carbon distribution not, and regrettably noble metal catalyst costs an arm and a leg, and high temperature easily runs off and sintering.Therefore, develop that non-precious metal catalyst is used for methane and CO 2 reforming reaction is a valuable job.
The purpose of this invention is to provide a kind of have the at a lower temperature methane of higher catalytic activity and the Catalysts and its preparation method of CO 2 reformation preparing synthetic gas.
Support of the catalyst of the present invention is mesoporous molecular sieve MCM-41, its specific surface area 1000 ± 200m
2/ g, active ingredient is made up of 3%～13% (weight) Ni.
Catalyzer of the present invention adopts immersion process for preparing, it is characterized in that elder generation is immersed in the saline solution of nickel on the mesoporous molecular sieve MCM-41, after 100～120 ℃ of dryings, again through 500～800 ℃ of roasting 4-8 hours, use 600～800 ℃ of following reduction activations of hydrogen at last, make catalyzer.
The corresponding salt of the used nickel of catalyzer of the present invention is a nickelous nitrate, and the employing fixed bed is a reactor, and gas hourly space velocity is 8400mlg
-1h
-1, normal pressure is reaction down, under 700 ℃, and CH
4And CO
2Transformation efficiency all can reach more than 90%.
Embodiment 1: adopting mesoporous molecular sieve MCM-41 is carrier, take by weighing 2.0g mesoporous molecular sieve MCM-41, be dissolved in 10 ml distilled waters with the 0.2973g nickelous nitrate, this nitrate solution is immersed among the mesoporous molecular sieve MCM-41, stir, drying is 2 hours under 100～120 ℃, again through 500～800 ℃ of roasting 4-8 hours, promptly obtains finished catalyst.
Get 0.3g30～this catalyzer of 50 orders and place the quartz tube reactor of φ 6mm.Feed 1: 1 CH
4And CO
2Reaction gas, its air speed are 8400mlg
-1h
-1, temperature programming successive reaction under normal pressure.Reaction result is listed in table 1.
The transformation efficiency of methane and carbonic acid gas and yield under table 1. differing temps
| Temperature (℃) | X CH4(％) | X CO2(％) | Y CO(％) | Y H2(％) |
| ????500 | ????24.2 | ????34.5 | ????29.4 | ????32.0 |
| ????550 | ????44.2 | ????54.1 | ????49.2 | ????51.6 |
| ????600 | ????65.5 | ????73.6 | ????69.6 | ????71.6 |
| ????650 | ????83.2 | ????87.7 | ????85.5 | ????86.7 |
| ????700 | ????92.3 | ????94.2 | ????93.3 | ????93.9 |
| ????750 | ????97.0 | ????97.8 | ????97.4 | ????97.6 |
| ????800 | ????98.5 | ????98.8 | ????98.6 | ????98.7 |
X
CH4: CH
4Transformation efficiency X
CO2: CO
2Transformation efficiency Y
CO: CO yield Y
H2: H
2Yield
Embodiment 2: adopting mesoporous molecular sieve MCM-41 is carrier, takes by weighing 2.0g mesoporous molecular sieve MCM-41, is dissolved in 10 ml distilled waters with the 0.6936g nickelous nitrate, and following step is with embodiment 1.
Get 0.3g30～this catalyzer of 50 orders, adopt reaction unit and the reaction conditions of embodiment 1.Reaction result is listed in table 2.
The transformation efficiency of methane and carbonic acid gas and yield under table 2. differing temps
X
CH4: CH
4Transformation efficiency X
CO2: CO
2Transformation efficiency Y
CO: CO yield Y
H2: H
2Yield embodiment 3: adopting mesoporous molecular sieve MCM-41 is carrier, takes by weighing 2.0g mesoporous molecular sieve MCM-41, is dissolved in 10 ml distilled waters with the 1.0904g nickelous nitrate, and following step is with embodiment 1.
| Temperature (℃) | X CH4(％) | X CO2(％) | Y CO(％) | Y H2(％) |
| ????500 | ????30.5 | ????22.8 | ????26.6 | ????34.4 |
| ????550 | ????51.2 | ????45.7 | ????48.4 | ????53.9 |
| ????600 | ????69.3 | ????67.9 | ????68.6 | ????70.0 |
| ????650 | ????83.5 | ????83.6 | ????83.6 | ????83.4 |
| ????700 | ????92.1 | ????94.4 | ????93.3 | ????90.9 |
| ????750 | ????97.2 | ????98.1 | ????97.7 | ????96.8 |
| ????800 | ????98.7 | ????99.3 | ????99.0 | ????98.5 |
Get 0.3g30～this catalyzer of 50 orders, adopt reaction unit and the reaction conditions of embodiment 1.Reaction result is listed in table 3.
The transformation efficiency of methane and carbonic acid gas and yield under table 3. differing temps
| Temperature (℃) | X CH4(％) | X CO2(％) | Y CO(％) | Y H2(％) |
| ????500 | ????31.4 | ????24.6 | ????28.0 | ????34.9 |
| ????550 | ????53.0 | ????47.5 | ????50.3 | ????55.8 |
| ????600 | ????70.9 | ????71.9 | ????71.4 | ????70.5 |
| ????650 | ????83.9 | ????87.8 | ????85.9 | ????82.1 |
| ????700 | ????92.6 | ????94.2 | ????93.4 | ????91.8 |
| ????750 | ????98.2 | ????98.8 | ????98.5 | ????98.0 |
| ????800 | ????99.0 | ????99.4 | ????99.2 | ????98.8 |
X
CH4: CH
4Transformation efficiency X
CO2: CO
2Transformation efficiency Y
CO: CO yield Y
H2: H
2Yield
Embodiment 4: adopting mesoporous molecular sieve MCM-41 is carrier, takes by weighing 2.0g mesoporous molecular sieve MCM-41, is dissolved in 10 ml distilled waters with the 1.2880g nickelous nitrate, and following step is with embodiment 1.
Get 0.3g30～this catalyzer of 50 orders, adopt reaction unit and the reaction conditions of embodiment 1.Reaction result is listed in table 4.
The transformation efficiency of methane and carbonic acid gas and yield under table 4. differing temps
| Temperature (℃) | X CH4(％) | X CO2(％) | Y CO(％) | Y H2(％) |
| ????500 | ????30.5 | ????22.8 | ????26.6 | ????34.4 |
| ????550 | ????51.2 | ????45.7 | ????48.4 | ????53.9 |
| ????600 | ????69.3 | ????67.9 | ????68.6 | ????70.0 |
| ????650 | ????83.5 | ????83.6 | ????83.6 | ????83.4 |
| ????700 | ????93.3 | ????93.5 | ????93.4 | ????93.1 |
| ????750 | ????97.2 | ????96.9 | ????97.1 | ????97.4 |
| ????800 | ????98.3 | ????97.9 | ????98.1 | ????98.5 |
X
CH4: CH
4Transformation efficiency X
CO2: CO
2Transformation efficiency Y
CO: CO yield Y
H2: H
2Yield
Claims (2)
1. methane and CO 2 reformation catalyst for preparing synthetic gas is characterized in that carrier selects mesoporous molecular sieve MCM-41 for use, and active ingredient is made up of the oxide compound of the nickel of 3%-13% weight.
2. Preparation of catalysts method as claimed in claim 1, it is characterized in that nickelous nitrate is dissolved in the distilled water, dry under 100～120 ℃ behind the immersion MCM-41,500～800 ℃ of following roastings, use 600～800 ℃ of following reduction activations of hydrogen at last, make catalyzer.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN00135648A CN1309079A (en) | 2000-12-14 | 2000-12-14 | Catalyst for preparing synthetic gas by reforming methane and CO2 |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN00135648A CN1309079A (en) | 2000-12-14 | 2000-12-14 | Catalyst for preparing synthetic gas by reforming methane and CO2 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1309079A true CN1309079A (en) | 2001-08-22 |
Family
ID=4596794
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN00135648A Pending CN1309079A (en) | 2000-12-14 | 2000-12-14 | Catalyst for preparing synthetic gas by reforming methane and CO2 |
Country Status (1)
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|---|---|
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6680006B2 (en) * | 2001-12-17 | 2004-01-20 | Natural Resources Canada | Conversion of natural gas to synthesis gas using nickel catalyst |
| CN1297345C (en) * | 2004-01-13 | 2007-01-31 | 厦门大学 | Solid catalyst for preparing epoxy phenylethane by epoxidation of styrene and preparation method |
| CN100388975C (en) * | 2005-09-29 | 2008-05-21 | 北京化工大学 | Metal carrier catalyst for producing synthetic gas by methane carbon dioxide reformation and its production |
| CN102745648A (en) * | 2011-04-22 | 2012-10-24 | 太原理工大学 | Preparation method of catalyst for producing synthetic gas by methane and carbon dioxide reformation |
| CN102886272A (en) * | 2012-04-26 | 2013-01-23 | 华东理工大学 | Supported catalyst, preparation method and application thereof |
| CN103191744A (en) * | 2013-04-17 | 2013-07-10 | 中国科学院新疆理化技术研究所 | Modified vermiculite supported nickel catalyst and preparation method thereof |
-
2000
- 2000-12-14 CN CN00135648A patent/CN1309079A/en active Pending
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6680006B2 (en) * | 2001-12-17 | 2004-01-20 | Natural Resources Canada | Conversion of natural gas to synthesis gas using nickel catalyst |
| CN1297345C (en) * | 2004-01-13 | 2007-01-31 | 厦门大学 | Solid catalyst for preparing epoxy phenylethane by epoxidation of styrene and preparation method |
| CN100388975C (en) * | 2005-09-29 | 2008-05-21 | 北京化工大学 | Metal carrier catalyst for producing synthetic gas by methane carbon dioxide reformation and its production |
| CN102745648A (en) * | 2011-04-22 | 2012-10-24 | 太原理工大学 | Preparation method of catalyst for producing synthetic gas by methane and carbon dioxide reformation |
| CN102886272A (en) * | 2012-04-26 | 2013-01-23 | 华东理工大学 | Supported catalyst, preparation method and application thereof |
| CN102886272B (en) * | 2012-04-26 | 2014-12-24 | 华东理工大学 | Supported catalyst, preparation method and application thereof |
| CN103191744A (en) * | 2013-04-17 | 2013-07-10 | 中国科学院新疆理化技术研究所 | Modified vermiculite supported nickel catalyst and preparation method thereof |
| CN103191744B (en) * | 2013-04-17 | 2015-07-08 | 中国科学院新疆理化技术研究所 | Modified vermiculite supported nickel catalyst and preparation method thereof |
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