CN1401429A - Combustible gas completely oxidizing catalyst - Google Patents
Combustible gas completely oxidizing catalyst Download PDFInfo
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- CN1401429A CN1401429A CN 01125122 CN01125122A CN1401429A CN 1401429 A CN1401429 A CN 1401429A CN 01125122 CN01125122 CN 01125122 CN 01125122 A CN01125122 A CN 01125122A CN 1401429 A CN1401429 A CN 1401429A
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Abstract
A catalyst for full oxidization of combustible gas is an alumina or SiO2 carried Au-Pt-Co-K (or Na, Or Li) catalyst, in which Au, Pt and Co3O4 are primary active component and Li, Na, or K is cocatalyst. It has better catalytic activity for full oxidization of CO, H2, CO-H2 mixture and methane, so it can removing them from the O2-containing atmosphere.
Description
The present invention relates to a kind of catalyst of under relatively lower temp, effectively eliminating a small amount of or micro CO, hydrogen, carbon monoxide and hydrogen mixed gas and methane gas in the oxygen-containing atmosphere.
Noble metal catalyst is owing to have excellent catalytic activity to a lot of reactions, obtain the further investigation of catalysis circle for a long time always, and in petrochemical industry catalysis and environmental catalysis, be widely used, has good active as noble metal catalysts such as platinum, palladiums for the oxidation of hydrogen, Au catalyst can even be lower than a small amount of carbon monoxide of eliminating under the condition of room temperature in the oxygen-containing atmosphere in room temperature, also has aspect such as, petroleum refining synthetic in the catalysis of fine chemicals also to be widely applied to precious metal material.On this basis, in order to realize a plurality of functions in the catalytic reaction, people have developed bimetallic catalyst or multimetal reforming catalyst, and the various active center is promptly arranged on such catalyst, and every kind of activated centre realization function separately is to obtain better catalytic performance.
In application process, people have prepared the noble metal catalyst that supports, the noble metal of catalytic activity is supported on as having many good qualities on the carriers such as aluminium oxide, silica: noble metal mostly can be with the form of crystallite, high degree of dispersion is on the whole surface of carrier, the result, just can produce bigger active surface to used noble metal, the cost of noble metal catalyst is significantly descended; Carrier can also improve dispersing of reaction heat, stops the sintering of metal crystallite and the reduction of consequent active surface; Can also increase the service life that therefore antitoxin performance prolongs catalyst; And carrier itself also can play catalytic action sometimes, and metal and carrier can both provide the activated centre, and perhaps metal and carrier interact, and strengthens activity of such catalysts.
Golden owing to its chemical property torpescence, and be considered to be not suitable as catalysis material.But since Haruta (United States Patent 4 in 1987,698,324) etc. report is prepared high dispersion supported Au catalyst with methods such as co-precipitation, and since carbon monoxide had a good low-temperature oxidation activity, supported aurum catalyst begins to be subjected to certain concern, and in some other catalytic reaction,, show very high catalytic activity as selective oxidation, steam conversion, selective conversion nitrogen oxide, aldol condensation, alkene carbonylation, stannane coupling.This explanation gold having a high potential as catalysis material.But the Au catalyst that the metal oxide that is prepared by coprecipitation supports is generally Powdered, and inconvenience is actual to be used.
The object of the present invention is to provide a kind of catalyst, this catalyst can effectively be eliminated a small amount of or micro CO, hydrogen, carbon monoxide and hydrogen mixed gas and methane gas in the oxygen-containing atmosphere under lower temperature.
Catalyst of the present invention is characterized in that carrier is aluminium oxide or silica, and active component is gold, platinum and cobaltosic oxide, and co-catalyst is lithium, sodium or potassium.
Catalyst of the present invention is characterized in that alumina catalyst support or silica dioxide granule size are 1～4mm.
Catalyst of the present invention, the loading that it is characterized in that platinum are 0.05～4% of aluminium oxide or silica supports weight, and the loading of gold is 0.1～4% of a vehicle weight, and the loading of cobaltosic oxide is 4～30% of a vehicle weight.
Catalyst of the present invention is characterized in that the atomic ratio of platinum and gold is 0.05: 1～5: 1, is suitably 0.5: 1～2: 1.
Catalyst of the present invention, the atomic ratio that it is characterized in that platinum and cobalt is 0.0001: 1～0.04: 1, is suitably 0.0004: 1～0.02: 1, the atomic ratio of gold and cobalt is 0.0001: 1～0.04: 1, is suitably 0.0004: 1～0.02: 1.
Catalyst of the present invention is characterized in that lithium, sodium or potassium are co-catalyst, and its content is 0.1～10% of aluminium oxide or silica supports weight.
Catalyst of the present invention, the precursor of gold is salt or metal, as: gold chloride, chlorauride, gold bromide, gold potassium cyanide and gold, the precursor of platinum is salt or metal, as chloroplatinic acid and platinum, the precursor of cobaltosic oxide is salt or metal equally, as cobalt nitrate, cobalt acetate cobalt chloride and cobalt.
Catalyst of the present invention, its preparation method is dipping substep deposition-precipitation method.
The typical building-up process of dipping substep deposition-precipitation method is among the present invention: under the normal temperature, being the aluminium oxide of 0.1-4mm or silica dioxide granule with size floods 5～24h in the NaOH of 0.05～1mol/l (or potassium hydroxide, potash, sodium carbonate) solution, filter, washing a little, 20～100 ℃ of dry 24h, 200～500 ℃ of roasting 2～8h.At 20～80 ℃, under the vigorous stirring, in the aluminium oxide or silica dioxide granule less investment water gaging that obtain, add cobalt salt solution again, wherein the concentration of cobalt is 5 * 10
-2～1molCo/l stirs 1～5h, leaves standstill 3～24h, filters washing, 20～100 ℃ of dry 24h, 200～500 ℃ of roasting 2～8h.At 20～80 ℃, under the vigorous stirring, the aluminium oxide or the silica supported cobalt granule that obtain are put in the mixed solution of golden salt and platinum salt equally, wherein the concentration of golden salt is 5 * 10
-3～5 * 10
-2MolAu/l, the concentration of platinum salt is 5 * 10
-3～5 * 10
-2MolPt/l, pH is controlled to be 6～10 with the NaOH of 0.05～1mol/l (or potassium hydroxide, potash, sodium carbonate) solution, stirs 1～5h, leave standstill 3～24h, filter, washing, 20～100 ℃ of dry 24h, 200～500 ℃ of roasting 2～8h obtain required catalyst.
This catalyst can at room temperature be distinguished effectively elimination hydrogen and carbon monoxide in oxygen-containing atmosphere, eliminate hydrogen and carbon mono oxide mixture at 76-120 ℃, eliminates methane gas under 400～600 ℃ of temperature.
Support platinum, palladium, gold or platinum-palladium noble metal catalyst and compare with existing, the substantial characteristics that the present invention has are:
1. this catalyst can both show good catalytic activity to the elimination of carbon monoxide, hydrogen, carbon monoxide and hydrogen mixed gas and methane gas;
2. can be under relatively low temperature the complete oxidation of carbon monoxide, hydrogen, carbon monoxide and hydrogen mixed gas and methane gas, fully reduced energy consumption;
3. the content of active component is relatively low in this catalyst, has reduced the cost of catalyst;
4. catalyst did not need the reduction activation preliminary treatment before using;
5. the existence of steam can not reduce the catalytic activity of this catalyst to these four reactions.
6. catalyst is graininess, is convenient to actual use.
Implementation example 1:
Take by weighing alumina particle 20 grams of size for 1mm, drop in the room temperature sodium hydroxide solution of 30ml 0.1mol/l, dipping 12h filters, washing a little, 100 ℃ of dry 24h, 500 ℃ of roasting 5h.Under the strong agitation, the alumina particle that obtains is dropped in the cobalt nitrate solution of 40ml 0.6mol/l again, stir 2h, leave standstill 5h, filter 100 ℃ of dry 24h, 400 ℃ of roasting 5h of blowing air.Equally, above-mentioned alumina particle is put in the mixed solution of 50ml gold chloride and chloroplatinic acid, wherein, the concentration of gold chloride is 0.01mol/l, the concentration of chloroplatinic acid is 0.008mol/l, and control pH value is about 7, stirs 2h, leave standstill 5h, filter, washing is to not having chlorion, 100 ℃ of dry 24h, 200 ℃ of roasting 5h of blowing air obtain required catalyst.Got by icp analysis, the cobalt loading is 6.4%, and golden loading is 0.45%, and the platinum loading is 0.35%.Implementation example 2:
Step is with implementation example 1, but the alumina particle size replaces 1mm with 3.0mm, the concentration of cobalt nitrate solution replaces 0.5mol/l with 0.3mol/l, the concentration of chlorauric acid solution replaces 0.01mol/l with 0.005mol/l, the concentration of platinum acid chloride solution replaces 0.008mol/l with 0.004mol/l, obtains required catalyst.Got by icp analysis, the cobalt loading is 3.1%, and golden loading is 0.2%, and the platinum loading is 0.15%.Implementation example 3:
Step just replaces aluminium oxide with silica dioxide granule with implementation example 1, obtains required catalyst.Got by icp analysis, the cobalt loading is 4.8%, and golden loading is 0.3%, and the platinum loading is 0.25%.
Implementation example 4-7:
By implementation example 1 preparation catalyst, carbon monoxide, hydrogen, carbon monoxide and hydrogen mixed gas and methane gas are carried out activity rating.
Consist of CO:1.0% at unstripped gas; O
2: 5.0%; N
2Balance (percent by volume), gas volume air speed are 1.0 * 10
4h
-1Situation under, at room temperature reach remaining CO amount＜5ppm (example 4) in the tail gas.
Consist of H at unstripped gas
2: 1.0%; O
2: 5.0%; N
2Balance (percent by volume), gas volume air speed are 1.0 * 10
4h
-1Situation under, at room temperature reach remaining H in the tail gas
2Amount＜2ppm (example 5).
Consist of CO:1.0% at unstripped gas; H
2: 1.0%; O
2: 5.0%; N
2Balance (percent by volume), gas volume air speed are 1.0 * 10
4h
-1Situation under, be issued to remaining CO amount＜5ppm in the tail gas, H at 83 ℃
2Amount＜2ppm (example 6).
Consist of CH at unstripped gas
4: 1.0%; O
2: 5.0%; N
2Balance (percent by volume), gas volume air speed are 1.0 * 10
4h
-1Situation under, be issued to remaining CH in the tail gas at 420 ℃
4Amount＜5ppm (example 7).
Claims (9)
1. solid supported noble metal catalyst, can under lower temperature, effectively eliminate a small amount of or micro-hydrogen, carbon monoxide, hydrogen and carbon mono oxide mixture and methane gas in the oxygen-containing atmosphere, it is characterized in that carrier is aluminium oxide or silica, active component is gold, platinum and cobaltosic oxide, and co-catalyst is lithium, sodium or potassium.
2. catalyst as claimed in claim 1 is characterized in that alumina catalyst support or silica dioxide granule size are 1～4mm.
3. catalyst as claimed in claim 1, the loading that it is characterized in that platinum are 0.05～4% of aluminium oxide or silica supports weight, and the loading of gold is 0.1～4% of a vehicle weight, and the loading of cobaltosic oxide is 4～30% of a vehicle weight.
4. catalyst as claimed in claim 1 is characterized in that the atomic ratio of platinum and gold is 0.05: 1～5: 1.
5. catalyst as claimed in claim 4 is characterized in that the atomic ratio of platinum and gold is 0.5: 1～2: 1.
6. catalyst as claimed in claim 1, the atomic ratio that it is characterized in that platinum and cobalt is 0.0001: 1～0.04: 1, the atomic ratio of gold and cobalt is 0.0001: 1～0.04: 1.
7. as claim 1 or 6 described catalyst, the atomic ratio that it is characterized in that platinum and cobalt is 0.0004: 1～0.02: 1, and the atomic ratio of gold and cobalt is 0.0004: 1～0.02: 1.
8. catalyst as claimed in claim 1, the content that it is characterized in that co-catalyst are 0.1～10% of aluminium oxide or silica supports weight.
9. catalyst as claimed in claim 1, it is characterized in that this catalyst can at room temperature be distinguished in oxygen-containing atmosphere effectively eliminates hydrogen and carbon monoxide, eliminate hydrogen and carbon mono oxide mixture at 76-120 ℃, under 400～600 ℃ of temperature, eliminate methane gas.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 01125122 CN1401429A (en) | 2001-08-13 | 2001-08-13 | Combustible gas completely oxidizing catalyst |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 01125122 CN1401429A (en) | 2001-08-13 | 2001-08-13 | Combustible gas completely oxidizing catalyst |
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| CN 01125122 Pending CN1401429A (en) | 2001-08-13 | 2001-08-13 | Combustible gas completely oxidizing catalyst |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1970144B (en) * | 2006-12-13 | 2011-05-11 | 北京英泰世纪环境科技有限公司 | Combustible gas catalyst preparation method and combustible gas catalyst prepared therefrom and burner |
| CN102906233A (en) * | 2010-03-30 | 2013-01-30 | 阿肯马法国公司 | Process for selective oxidation of carbon monoxide |
| CN104014340A (en) * | 2014-05-28 | 2014-09-03 | 上海纳米技术及应用国家工程研究中心有限公司 | Supported cobaltosic oxide catalyst, and preparation method and application thereof |
-
2001
- 2001-08-13 CN CN 01125122 patent/CN1401429A/en active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1970144B (en) * | 2006-12-13 | 2011-05-11 | 北京英泰世纪环境科技有限公司 | Combustible gas catalyst preparation method and combustible gas catalyst prepared therefrom and burner |
| CN102906233A (en) * | 2010-03-30 | 2013-01-30 | 阿肯马法国公司 | Process for selective oxidation of carbon monoxide |
| CN104014340A (en) * | 2014-05-28 | 2014-09-03 | 上海纳米技术及应用国家工程研究中心有限公司 | Supported cobaltosic oxide catalyst, and preparation method and application thereof |
| CN104014340B (en) * | 2014-05-28 | 2016-08-24 | 上海纳米技术及应用国家工程研究中心有限公司 | Loaded Cobalto-cobaltic oxide catalyst and its preparation method and application |
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