CN108722492A - One kind being suitable for smokeless catalytic coal gasifaction catalyst and preparation method thereof - Google Patents
One kind being suitable for smokeless catalytic coal gasifaction catalyst and preparation method thereof Download PDFInfo
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- CN108722492A CN108722492A CN201710265874.3A CN201710265874A CN108722492A CN 108722492 A CN108722492 A CN 108722492A CN 201710265874 A CN201710265874 A CN 201710265874A CN 108722492 A CN108722492 A CN 108722492A
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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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/26—Catalysts comprising hydrides, coordination complexes or organic compounds containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/02—Fixed-bed gasification of lump fuel
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L10/00—Use of additives to fuels or fires for particular purposes
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L9/00—Treating solid fuels to improve their combustion
- C10L9/10—Treating solid fuels to improve their combustion by using additives
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/093—Coal
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
- C10J2300/0986—Catalysts
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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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Abstract
One kind being suitable for smokeless catalytic coal gasifaction catalyst and preparation method thereof.It is mixed using more than one organic sodium or sylvite as surfactant and anthracite coal sill, using incipient impregnation in inorganic sodium solution, anion surfactant of the catalyst with lipophilic group improves the binding ability with coal surface, sodium ion is set to obtain full and uniform dispersion on the surface of coal, organic salt generates a large amount of holes in pyroreaction, to improve coal gasification efficiency, methane content in product gas is improved, the effective rate of utilization of active component is improved.Catalyst coal when reaction proceeds to 300 minutes is changed into gas-phase product conversion ratio and reaches 87.5%, and methane accumulation production quantity reaches 11.8mmolg‑1, the content of product wherein methane reaches 24.4%, shows excellent methane performance processed.
Description
Technical field
The invention belongs to catalysis technical fields, are related to a kind of suitable for smokeless catalytic coal gasifaction catalyst and its preparation side
Method.
Background technology
The utilization of coal in China is based on directly burning, and not only energy utilization rate is very low, but also causes dust, acid rain, big
Measure greenhouse gases CO2Pollution problems, the Coal Gasification Technologies such as discharge play an important role in terms of efficient, clean utilization coal resources,
But traditional coal gasification course reaction temperature is high, generates gas purification difficulty, energy consumption is big, to equipment requirement height.
Anthracite (English name anthracite) is commonly called as anthracite or anthracite.It is the maximum coal of degree of coalification.Anthracite is solid
Determine carbon content height, volatile producibility is low, and density is big, and hardness is big, and burning point is high, and when burning does not smolder.Black is hard, there is metal light
Pool.Will not be stained with fat friction, fracture at conchoidal, when burning, flame is short and few cigarette.Noncoking.General phosphorus content 90% with
On, volatile matter is below 10%.Anthracite shows relatively high gasification reactivity, according to anthracitic Industrial Analysis as a result, nothing
Why bituminous coal shows high gasification reactivity, due principally to the coal there is high-moisture, low ash content, high-carbon content and height to wave
The characteristics of hair divides.
Alkali carbonate to the apparent catalytic action of coal gasification early in nineteen twenty-one by propositions such as Taylor, in view of soda
Be widely present and it is more cheap and easy to get, for a long time in relation to sodium carbonate catalytic gasification research carried out a large amount of reports.Especially
The salt of the carbonate of potassium, sodium, alkaline-earth metal and transition metal is all the good catalyst of catalytic gasification.The catalytic gasification of coal is one
The typical gas-solid heterogeneous reaction of kind, vapor-phase reactant will react on the coal surface for being loaded with catalyst with carbon, catalyst
Activity depends on the specific surface area of coal and its dispersion degree on coal surface.Sodium carbonate(Potassium)Alkali metal and carbon shape are removed on coal surface
Outside activated centre at oxide on surface group, can also change the pore structure on coal surface, and under gasification temperature into one
Step melting diffusion can make the activity of coal be improved.Exxonmobil companies of the U.S. are with K2CO3As catalyst, have developed with
The pressurised fluidized bed catalysis gasification technique of coal for the purpose of substitute natural gas is produced, K is added2CO3After catalyst, in same reaction
In, efficiency of carbon con version greatly improves, reaction rate also improve about 4 times (Energy Research, 1980,4:137-
147).Compared with single component catalyst, multicomponent catalyst has higher gasification efficiency, is paid high attention to recently by researcher.
Akyurtlu etc. is with K2SO4And FeSO4Mixture be catalyst gasification research, reaction condition are carried out to Pittsburgh's HVA coal tars
For:K/Fe molar ratios are 9, temperature is 850 DEG C, the atomic ratio of pressure 0.1MPa, metal/carbon is 0.02, content of metal is
5.1~7.3g/100g carbon, carbon particle size be 53 μm~106 μm, reaction gas H2O/H2Or H2O/N2(H2O content is
30%), charcoal percent conversion can reach 100%, and under same reaction conditions, K is used alone2CO3As catalyst, charcoal percent conversion
Only 89%(Fuel Processing Technology, 1995,43:71-86).Sheth etc. uses three-way catalyst respectively
Li2CO3-Na2CO3-K2CO3, binary catalyst Na2CO3-K2CO3, monolithic catalyst K2CO3Gasification kinetics research is carried out to coal,
It was found that the activation energy of catalytic gasification is less than the activation energy of binary catalyst and monolithic catalyst catalytic gasification, this is
Due in gasification temperature(700 DEG C~900 DEG C)Under, three-way catalyst is in a liquid state, and binary catalyst and monolithic catalyst K2CO3
For solid-state.Since catalyst exists with liquid, good fluidity, it is easier to be diffused into reaction system, the active sites of coal are corresponding
Increase, therefore activity is relatively high(Fuel, 2004, 83:557-572).But sodium carbonate(Potassium)Coal surface excess or
Accumulation easilys lead to mutually cohering under molten state and slagging, to be had adverse effect on to catalytic gasification process.Therefore,
It is badly in need of a kind of not easy in inactivation of exploitation, methanation effect is good, is more easy to evenly dispersed base metal catalysts, realizes catalytic coal gasifaction skill
Art industrialization bottleneck is broken through.
Invention content
Goal of the invention:Patent of the present invention provides a kind of suitable for smokeless catalytic coal gasifaction catalyst and preparation method thereof, energy
It is simple enough to provide a kind of catalyst preparation process, environmentally protective, catalyst is uniformly dispersed, the good catalyst of catalytic activity.
Technical scheme of the present invention:Suitable for smokeless catalytic coal gasifaction catalyst, it is characterised in that in the catalyst
Including inorganic sodium, surfactant and coal sill, the mass fraction of metal species in the catalyst in inorganic sodium is
1%-5%, the mass fraction of metal species in the catalyst in surfactant is 1%-5%, remaining ingredient is mainly coal base material
Material.
Usually, the inorganic sodium is one kind or more in sodium carbonate, sodium bicarbonate, sodium nitrate, sodium phosphate.
The surfactant is Organic Sodium Salt or sylvite, preferably neopelex, enuatrol, detergent alkylate
One kind or more in potassium sulfonate, potassium oleate and polyacrylamide sylvite.
The preparation method suitable for smokeless catalytic coal gasifaction catalyst, it is characterised in that:A. inorganic sodium, surface
Activating agent is configured to solution A and solution B respectively;B. it is 0.150 ~ 0.425mm by anthracite crushing grinding to grain size;C. by coal
Base is added in solution B and is stirred, and forms mixed liquor C;D. by mixed liquor C incipient impregnations in solution A;E. it will impregnate
Solution be baked to particle powdery with infrared lamp, it is dry, be ground up, sieved.
Used in water conductivity be less than 5 μ s/cm.
The mixing time is 1 ~ 4h, and temperature is 40 ~ 80 DEG C, and dip time is 8 ~ 24 h.
The significant advantage that the present invention is showed is shown as:The 1, present invention adds surfactant, with lipophilic group
Anion surfactant improves the binding ability with coal surface, and sodium ion is made to obtain full and uniform point on the surface of coal
It dissipates;2. reducing the migration or conglomeration generated by non-uniform temperature using infrared lamp baking, catalyst is made to have higher dispersion
Degree;3. binary composition has lower fusing point, easily it is changed into liquid, it can be in rapid osmotic to the hole of coal sill.
The catalyst prepared using this method, excellent gasification is shown during fixed bed smokeless catalytic coal gasifaction
Can, show excellent methane performance processed.
Specific implementation mode
Embodiment 1
By 0.58gNa2CO3、3.48gC18H29NaO3S is dissolved in 40 ml deionized waters, then extremely by 5g anthracites crushing grinding
Grain size is 0.150 ~ 0.425mm, is added to C18H29NaO3In S solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor is soaked in equal volume
Stain is in Na2CO3In solution, 10h is impregnated, particle powdery is baked to infrared lamp, into oven drying, is ground up, sieved spare, be labeled as
S-1.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 2
By 0.58g Na2CO3、2.14gC18H29KO3S is dissolved in 40 ml deionized waters, then extremely by 5g anthracites crushing grinding
Grain size is 0.150 ~ 0.425mm, is added to C18H29KO3In S solution, 1h is stirred, temperature is 80 DEG C, by mixed liquor incipient impregnation
In Na2CO3In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-
2.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 3
By 0.58g Na2CO3、3.04gC18H33O2Na is dissolved in 40 ml deionized waters, then extremely by 5g anthracites crushing grinding
Grain size is 0.150 ~ 0.425mm, is added to C18H33O2In Na solution, 1h is stirred, temperature is 80 DEG C, by mixed liquor incipient impregnation
In Na2CO3In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-
3.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 4
By 0.58g Na2CO3、3.2gC18H33O2K is dissolved in 40 ml deionized waters, then by 5g anthracites crushing grinding to grain
Diameter is 0.150 ~ 0.425mm, is added to C18H33O2In K solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor incipient impregnation is existed
Na2CO3In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-4.
Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 5
By 0.58g Na2CO3、0.028g(C3H3KO2)nIt is dissolved in 40 ml deionized waters, then extremely by 5g anthracites crushing grinding
Grain size is 0.150 ~ 0.425mm, is added to (C3H3KO2)nIn solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor is soaked in equal volume
Stain is in Na2CO3In solution, 10h is impregnated, particle powdery is baked to infrared lamp, into oven drying, is ground up, sieved spare, be labeled as
S-5.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 6
By 0.82gNaHCO3、3.2g C18H33O2K is dissolved in 40 ml deionized waters, then by 5g anthracites crushing grinding to grain
Diameter is 0.150 ~ 0.425mm, is added to C18H33O2In K solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor incipient impregnation is existed
NaHCO3In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-
6.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 7
By 0.93g NaNO3、3.2gC18H33O2K is dissolved in 40 ml deionized waters, then by 5g anthracites crushing grinding to grain size
For 0.150 ~ 0.425mm, it is added to C18H33O2In K solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor incipient impregnation is existed
NaNO3In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-7.
Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Embodiment 8
By 0.60gNa3PO4、3.2gC18H33O2K is dissolved in 40 ml deionized waters, then by 5g anthracites crushing grinding to grain size
For 0.150 ~ 0.425mm, it is added to C18H33O2In K solution, 1h is stirred, temperature is 80 DEG C, and mixed liquor incipient impregnation is existed
Na3PO4In solution, impregnate 10h, be baked to particle powdery with infrared lamp, into oven drying, be ground up, sieved it is spare, be labeled as S-8.
Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is shown in Table 2 respectively.
Comparative example
By 0.58gNa2CO3Be dissolved in 40 ml deionized waters, then by 5g anthracites crushing grinding to grain size be 0.150 ~
0.425mm is added to Na2CO3In solution, 1h is stirred, temperature is 80 DEG C, and particle powdery is baked to infrared lamp, dry into baking oven
It is dry, be ground up, sieved it is spare, be labeled as S-9.Coal is changed into the conversion ratio and CH of gas-phase product on the catalyst4Production quantity is distinguished
It is shown in Table 2.
Catalyst performance evaluation
Evaluation condition:700 DEG C of gasification temperature, vapor pressure 3.5Mpa, initial ratio of water to coal 2g/gmin-1, carrier gas(Ar gas)Stream
Fast 1L/min.Fixed bed reactors internal diameter is 32 mm, high 800 mm.Product gas enters knockout drum and carries out gas-liquid separation, after separation
Gas dehumidify through drier, collect after wet flow indicator measures, then by airbag, finally analyzed in every time by GC
Product gas composition and content.Concrete analysis data are shown in Table 2.
2 reaction time of table 300min coal gasifications conversion ratio, methane-generated quantity and methane content
As seen from the data in Table 2:In catalytic coal gasification, under same experimental condition, prepared according to the method for the present invention
Catalyst performance is better than the sodium carbonate catalyst of comparative example, and wherein S-2 catalyst coal gasification is converted into the conversion of gas-phase product
Rate highest, in reaction time 300min, conversion ratio reaches 87.5%, and methane accumulation production quantity reaches 11.8mmolg-1, product its
The content of middle methane reaches 24.4%, shows excellent methane performance processed.
Claims (7)
1. one kind being suitable for smokeless catalytic coal gasifaction catalyst, it is characterised in that include inorganic sodium, table in the catalyst
Face activating agent and coal sill, the mass fraction of metal species in the catalyst in inorganic sodium is 1%-5%, surfactant
In metal species mass fraction in the catalyst be 1%-5%, remaining ingredient is mainly coal sill.
2. catalyst as described in claim 1, it is characterised in that the inorganic sodium is sodium carbonate, sodium bicarbonate, nitric acid
One kind or more in sodium, sodium phosphate.
3. catalyst as described in claim 1, it is characterised in that the surfactant is Organic Sodium Salt or sylvite.
4. catalyst as claimed in claim 3, it is characterised in that the surfactant is neopelex, oleic acid
One kind or more in sodium, Potassium dodecylbenzenesulfonate, potassium oleate and polyacrylamide sylvite.
5. being suitable for the preparation method of smokeless catalytic coal gasifaction catalyst as described in claim 1, it is characterised in that:A. by nothing
Machine sodium salt, surfactant are configured to water solution A and aqueous solution B respectively;B. by anthracite crushing grinding to grain size be 0.150 ~
0.425mm;C. coal sill is added in solution B and is stirred, form mixed liquor C;D. mixed liquor C incipient impregnations are existed
In solution A;E. the solution impregnated is baked to particle powdery with infrared lamp, drying is ground up, sieved.
6. the preparation method of catalyst as claimed in claim 5, it is characterised in that the conductivity of water used is less than 5 μ s/cm.
7. method for preparing catalyst as claimed in claim 5, it is characterised in that mixing time is 1 ~ 4h, and temperature is 40 ~ 80 DEG C,
Dip time is 8 ~ 24 h.
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN110075931A (en) * | 2019-04-26 | 2019-08-02 | 新奥科技发展有限公司 | A kind of catalyst carrying method of coal gasification |
CN115838174A (en) * | 2022-12-22 | 2023-03-24 | 杭州星科元祥能源有限公司 | Preparation for improving activity of carbonaceous reducing agent coal, preparation method and use method |
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CN101747978A (en) * | 2009-12-31 | 2010-06-23 | 陈其厚 | Clean fired coal saving agent |
CN101805652A (en) * | 2010-04-22 | 2010-08-18 | 熊晓明 | Coal-fired multi-phase catalysis additive |
CN106540730A (en) * | 2015-09-16 | 2017-03-29 | 中国石油化工股份有限公司 | A kind of natural gas catalyst manufactured by coal and preparation method thereof |
CN106563505A (en) * | 2016-02-04 | 2017-04-19 | 太原理工大学 | Catalyst for coal gasification, preparation method and application thereof |
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CN101294111A (en) * | 2008-06-17 | 2008-10-29 | 陈其厚 | Sulfureous fixing, dust laying coal-saving agent |
CN101747978A (en) * | 2009-12-31 | 2010-06-23 | 陈其厚 | Clean fired coal saving agent |
CN101805652A (en) * | 2010-04-22 | 2010-08-18 | 熊晓明 | Coal-fired multi-phase catalysis additive |
CN106540730A (en) * | 2015-09-16 | 2017-03-29 | 中国石油化工股份有限公司 | A kind of natural gas catalyst manufactured by coal and preparation method thereof |
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
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CN110075931A (en) * | 2019-04-26 | 2019-08-02 | 新奥科技发展有限公司 | A kind of catalyst carrying method of coal gasification |
CN115838174A (en) * | 2022-12-22 | 2023-03-24 | 杭州星科元祥能源有限公司 | Preparation for improving activity of carbonaceous reducing agent coal, preparation method and use method |
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Application publication date: 20181102 |