CN101372312A - Method for preparing hydrogen by coal gasification - Google Patents
Method for preparing hydrogen by coal gasification Download PDFInfo
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- CN101372312A CN101372312A CN 200810200992 CN200810200992A CN101372312A CN 101372312 A CN101372312 A CN 101372312A CN 200810200992 CN200810200992 CN 200810200992 CN 200810200992 A CN200810200992 A CN 200810200992A CN 101372312 A CN101372312 A CN 101372312A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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Abstract
The invention relates to a method for preparing hydrogen by coal gasification. The method for preparing hydrogen includes the following steps: (1) thermal cracking of coal is carried out under the condition of isolating from air and at the temperature of 900 DEG C to essentially obtain coal thermal cracking gas, tarre and coal coke, and the coal thermal cracking gas and the tarre are removed to obtain the coal coke; (2) at the temperature below 800 DEG C, a gasifying agent is used for gasifying the coal coke obtained from the step (1) to obtain coal coke gas, and the obtained coal coke gas is purified to obtain a target object. In the invention, a 'two-stage type' gasifying method is adopted for gasifying coal, and the obtained coal coke gas (the coal coke gas contains about 70v/v% of hydrogen, less than 3v/v% of carbon monoxide and no methane) is used as the 'raw material gas' for preparing hydrogen. Therefore, a methane catalytic reforming technique and a carbon monoxide conversion process in a post treatment process can be omitted, and a beforehand desulfuration process required in these techniques can also be omitted, that is to say, pure hydrogen can be prepared only after the processes of removing acidic gas and purifying a little residual gas.
Description
Technical field
The present invention relates to a kind of preparation method of hydrogen, specifically, relate to a kind of method by preparing hydrogen by coal gasification.
Background technology
The critical process of coal hydrogen manufacturing is the coal gasification process.Existing coal gasification technology (or device) comprising: strange (Lurgi) moving-bed gasification stove in Shandong, Winkler (Winkler) fluidized-bed gasification furnace, with the Kopper-Totzek and the Shell airflow bed gasification furnace of dry feed, and with the Texaco of wet method charging with by the airflow bed gasification furnace of units such as Hua Tong East China University of Science exploitation etc.
Gaseous product by above-mentioned coal gasification technology (or device) gained contains hydrogen, carbon monoxide, carbonic acid gas, methane, nitrogen and a small amount of hydrogen sulfide etc., and the content of hydrogen is very low.Therefore, if will make the higher hydrogen of purity, need conversion and sepn process tediously long through step and that processing condition are harsh.
Lin, Shi-Ying etc. disclose a kind of, having in the presence of the material of absorbing carbon dioxide (mainly being CaO, MgO or ferric oxide), be higher than 600 ℃ in pressure greater than 200 normal atmosphere, temperature by carbonaceous material (comprising coal) and supercritical water and make hydrogen (EP 1001002 A2) through the thermochemistry cracking.Though this method has improved the purity of hydrogen, the defective of its existence is: the coal tar transformation efficiency is lower, and methane content higher (methane will generate carbon monoxide again in the catalytic reforming switching process) in the gaseous product.
People such as Mondal have proposed to use ferric oxide and calcium oxide mixture as catalyst gasification hydrogen-producing method (Mondal K.etal.Ind.Eng.Chem.Chem.Res.2005,44,5508.), the processing condition of this method comparatively harsh (requiring under the condition of higher temperature (870 ℃), to carry out), and generate carbon monoxide and methane content higher (carbon monoxide about 30%) in the gas (product).
Given this, this area presses for a kind of hydrogen preparation method of efficient, highly selective.
Summary of the invention
The object of the invention is, provides a kind of and can carry out gasification reaction fast, again can highly selective generate hydrogen (hydrogen content height in gaseous product, carbon monoxide content is low and do not contain methane), by the method for preparing hydrogen by coal gasification.Can omit conversion postprocessing working procedures such as methyl hydride catalyzed reformation and carbon monoxide thus, reduce the cost of coal hydrogen manufacturing significantly.
Pyrolysis of coal is the fast speed reaction process, and it mainly is that the cracking of part ature of coal generates products such as pyrolysis of coal gas (gaseous product contains carbon monoxide, carbonic acid gas, hydrogen, methane and other light gas), coal tar and coal tar.If as hydrogen feedstock, contain light hydrocarbon gases such as methane because of it with coal pyrolysis gas, need by complicated shift conversion step, it is low to transform efficiency.
Given this, the present invention proposes the coal pyrolysis gas that methane and other light gas (relative) content is higher first and (is comprised in said generation gas: hydrogen, carbon monoxide and carbonic acid gas by char gasification gained generation gas, do not contain other light gas such as methane, and the content of hydrogen is higher) separate, thereby reach the purpose of omitting or simplifying postprocessing working procedures complicated in existing thermo-cracking carbonaceous material (as the coal etc.) hydrogen producing technology, increase substantially the hydrogen manufacturing efficiency.
The said method by preparing hydrogen by coal gasification of the present invention, it comprises the steps:
(1) at secluding air and not being higher than under 900 ℃ of conditions, the thermo-cracking coal, main pyrolysis of coal gas, tar and coal tar divide and remove pyrolysis of coal gas and tar gets coal tar;
(2) be not higher than under 800 ℃ of conditions, getting coal tar gas by the coal tar of step (1) gained with vaporized chemical (as water vapour) gasification, after gained coal tar gas is purified target compound (pure hydrogen).
The present invention adopts " two-section type " gasification process gasification of coal, gained coal tar gas (the about 70v/v% of hydrogen content in this coal tar gas, carbon monoxide content can be lower than 3v/v%, does not contain methane).In its gaseous constituent carbon monoxide and methane content all be lower than work off one's feeling vent one's spleen after conventional methane reforming and the carbon monodixe conversion in the content of corresponding gas, therefore, get " unstripped gas " of gas with this catalytic gasification legal system, in postprocessing working procedures, can omit methyl hydride catalyzed reforming process and carbon monodixe conversion operation as hydrogen manufacturing.Promptly as long as after removing sour gas operation and small amount of residual gas sweetening operation, just can make pure hydrogen.
In an optimal technical scheme of the present invention, coal thermo-cracking temperature is 500 ℃～900 ℃ in the step (1);
In another optimal technical scheme of the present invention, in step (1), add the existing additive that is used for the pyrolysis of coal process, as (but being not limited to): calcium hydroxide, lime are or/and Wingdale etc.The present invention recommends to use calcium hydroxide.Gross weight with the mixture be made up of coal and additive serves as to calculate benchmark (100wt%), and content of additive is 5wt%～20wt%.
In another optimal technical scheme of the present invention, the gasification temperature of coal tar is 700 ℃～750 ℃ in step (2).
In another optimal technical scheme of the present invention, in step (2), add sylvite (as gasifying catalyst).Gross weight with the mixture be made up of coal tar and sylvite (catalyzer) serves as to calculate benchmark (100wt%), and the content of sylvite is 5wt%～20wt%.
Description of drawings
Fig. 1. the said process flow diagram of the present invention by the preparing hydrogen by coal gasification method.
Fig. 2. raw coal first, raw coal first+lime carbonate or the hot cracked products distribution figure of raw coal first+calcium hydroxide;
Wherein: black matrix is a coal tar; The fork body is a tar; Empty body is a gas.
Fig. 3. the hot cracked gained gaseous product distribution of raw coal first, raw coal first+lime carbonate or raw coal+calcium hydroxide figure.
Fig. 4. the distribution plan of each component in the hot cracked gained tar of raw coal first, raw coal first+lime carbonate or raw coal+calcium hydroxide;
Wherein: right oblique line is represented benzene; Empty body is represented toluene; Left side oblique line is represented dimethylbenzene.
Fig. 5. at 750 ℃ and the efficiency of carbon conversion of the main carbonaceous gas of generation of different coal tar steam gasifications is arranged under catalyzer (10% salt of wormwood) existence condition;
Wherein: △---by raw coal first pyrolysis gained coal tar; ▲---by the mixture pyrolysis gained coal tar of raw coal first+calcium hydroxide; Mouthful---by raw coal second pyrolysis gained coal tar; ■---by the mixture pyrolysis gained coal tar of raw coal second+calcium hydroxide.
Fig. 6 is at 750 ℃ and the composition distribution plan of different coal tar steam gasification gained gases is arranged under catalyzer (10% salt of wormwood) existence condition.
Embodiment
As shown in Figure 1: the said method by preparing hydrogen by coal gasification of the present invention, it comprises the steps:
(1) pyrolysis of coal system coal tar:
Coal and additive (as: calcium hydroxide, lime are or/and Wingdale etc.) are mixed, and be placed in the pyrolysis reactor (as existing moving-bed or fixed-bed pyrolysis stove etc.), under secluding air and 500 ℃～900 ℃ conditions, pyrolysis 15 minutes-60 minutes, main pyrolysis of coal gas, tar and the coal tar of getting, branch removes pyrolysis of coal gas and tar (pyrolysis of coal gas and tar are separated out with the volatile matter form, separate with coal tar) gets coal tar;
Adding an amount of calcium class additive main purpose in thermal cracking processes is: coal is carried out pre-modification, improve the reactive behavior and the utilization ratio of catalyzer in the follow-up char gasification process.In actually operating, can form according to used raw coal mineral, whether decision needs additive and addition thereof.Among Fig. 5, the difference of coal sample second and coal sample first is that coal sample second contains more acid mineral substance, so the treatment effect of calcium class additive is more remarkable.Generally speaking: add the additive of appropriate amount, can not cause the operational problem of thermo-cracking and gasifying process.But too much additive can reduce gasification efficiency.Therefore, in the present invention, the content of additive in the mixture of being made up of coal and additive should be controlled at 5wt%～20wt% and be advisable.
(2) char gasification prepares target compound:
To move into vapourizing furnace by the coal tar of step (1) gained and gasify (being vaporized chemical with water vapour), vapor pressure is a normal pressure (1atm) or a little more than normal pressure; Gasification temperature (T) is not higher than 800 ℃ (T≤800 ℃).
Sylvite is a kind of ideal gasifying catalyst, and it has flowability under heating condition.The sylvite catalyzer can wiring solution-forming, sprays in the stove with liquid form.When the content of sylvite (catalyzer) in the mixture of forming by coal tar and sylvite (catalyzer) during less than 5wt%, the catalytic gasification DeGrain; When the increase along with the sylvite catalyst levels, gasification reaction speed also improves thereupon.But add sylvite too much, can cause the coal tar effective processing capacity of unit volume vapourizing furnace to descend.Therefore in the present invention, serve as calculating benchmark (100wt%) with the gross weight of the mixture formed by coal tar and sylvite (catalyzer), the content of sylvite should be controlled to be 5wt%～20wt%.
When gasification temperature (T) is higher than 800 ℃, can increase the difficulty of outside heat supply on the one hand, may cause the volatilization of part sylvite on the other hand.Therefore, gasification temperature should not be above 800 ℃.The preferred gasification temperature of the present invention is 700 ℃～750 ℃.
Said vapourizing furnace can be selected existing moving-bed gasification stove or fluidized-bed gasification furnace for use.When selecting fluidized-bed gasification furnace for use, not easy-to-use air is as fluidizing agent, and should select for use high-temperature vapor proper as fluidized gas.
In addition, hot coal Jiao who is obtained by pyrolysis preferably takes the insulation measure, or hot coal Jiao is directly sent into vapourizing furnace, avoids process of cooling to bring thermosteresis, and hot coal Jiao also provides partial gasification institute heat requirement simultaneously.
After char gasification finished, ash content was discharged from vapourizing furnace in sylvite catalyzer and the coal, and the active sylvite in the coal ash can adopt water-soluble method to reclaim and recycle.In the gaseous product that the coal tar catalytic gasification produces, hydrogen content very high (about 70v/v%), carbon monoxide content lower (being no more than 3v/v%) and do not contain methane (other is a carbon dioxide).This gaseous product need not pass through methane vapor reforming and carbon monodixe conversion reaction process, and the method for using by existing industrial production removes CO
2Gas behind gas purification, promptly obtains pure hydrogen then.
The present invention is further elaborated below by embodiment, and its purpose only is better to understand content of the present invention.Therefore, the cited case does not limit protection scope of the present invention.
Embodiment
The method of " two-section type " gasification hydrogen manufacturing
(1) thermo-cracking of raw coal (first section operation):
The mixture (wherein the content of calcium hydroxide is 10wt%) of raw coal, raw coal and calcium hydroxide or the mixture (wherein the content of lime carbonate is 10wt%) of raw coal and lime carbonate are placed the fixed-bed pyrolysis reactor respectively, in [that is: under normal pressure (1atm) and the secluding air condition] under the identical condition, pyrolysis is carried out in heating, the thermo-cracking temperature is 500 ℃～900 ℃, and the distribution of its thermal cracking products as shown in Figure 2.
Wherein gaseous fraction is separated out from the reactor volatilization, and gaseous fraction adopts gas-chromatography to carry out quantitative analysis, the results are shown in Figure 3;
Tar product is collected with cold-trap, tar content weighting method analysis, and benzene, toluene and dimethylbenzene chromatogram ration analysis the results are shown in Figure 4 in the tar;
Coal tar is collected in reactor, and weighing obtains the coal tar productive rate, and coal tar is used for gasified raw material.
(2) char gasification hydrogen manufacturing (second section operation):
Be less than or equal under 800 ℃ the condition (preferred 700 ℃～750 ℃), to place fixed-bed gasification furnace respectively by four kinds of coal tars of step (1) gained, at catalyst-free or have under catalyzer (salt of wormwood) existence condition, feed water vapour and gasify, with online gas Chromatographic Determination gasification rate and gas composition (result as shown in Figure 5 and Figure 6).As seen from the figure, main hydrogen of gaseous product and carbonic acid gas, it is extremely low to contain carbon monoxide and methane, with this gas is unstripped gas, as long as with traditional absorption process with carbon dioxide separation and remove on a small quantity other gas, can make pure hydrogen, can omit methane reforming and carbon monodixe conversion operation, also the desulfurization process that can must carry out in advance owing to having sulfur poisoning in these technologies.
Comparative Examples 1
The method of " one-part form " gasification hydrogen manufacturing
In fixed-bed reactor same as the previously described embodiments, with raw coal directly as gasified raw material, do not add any catalyzer and in same steam atmosphere, be warming up to about 1000 ℃ (conventional non-catalyzed gasification is temperature required), and insulation under this temperature condition after 60 minutes with the composition of gas Chromatographic Determination gained gas, it the results are shown in Table 1.
Comparative Examples 2
The method of " one-part form " gasification hydrogen manufacturing
Equally, in fixed-bed reactor same as the previously described embodiments, with the mixture of raw coal and salt of wormwood (in said mixture, the content of salt of wormwood is 10wt%) be gasified raw material, in same steam atmosphere, be warming up to 700 ℃～750 ℃, and being incubated the composition of gas Chromatographic Determination gained gas after 60 minutes, it the results are shown in Table 1.
Table 1
As known from Table 1: do not adding catalyzer, in (industrial use minimum temperature) gained gas, hydrogen content is lower under 1000 ℃, and carbon monoxide content is very high, contains methane simultaneously; And in the catalytic gasification gained gas, though the hydrogen body burden is very high, carbon monoxide is very low, but still contains certain methane, and it can not be out in the cold.
Do not detect methane (seeing Fig. 6 for details) in 3v/v% and the gas and adopt the method gained gas of the present invention's said " two-section type " gasification hydrogen manufacturing, its hydrogen content to be lower than up to 70v/v%, carbon monoxide content.
Claims (7)
1. the method by preparing hydrogen by coal gasification is characterized in that, said preparation hydrogen method comprises the steps:
(1) at secluding air and not being higher than under 900 ℃ of conditions, the thermo-cracking coal, main pyrolysis of coal gas, tar and coal tar divide and remove pyrolysis of coal gas and tar gets coal tar;
(2) be not higher than under 800 ℃ of conditions, getting coal tar gas by the coal tar of step (1) gained with vaporized chemical gasification, after gained coal tar gas is purified target compound.
2. the method for preparing hydrogen as claimed in claim 1 is characterized in that, wherein said vaporized chemical is a water vapour.
3. the method for preparing hydrogen as claimed in claim 1 or 2 is characterized in that, wherein coal thermo-cracking temperature is 500 ℃～900 ℃ in the step (1).
4. the method for preparing hydrogen as claimed in claim 3, it is characterized in that, wherein adding the existing additive that is used for the pyrolysis of coal process in step (1), serves as the calculating benchmark with the gross weight of the mixture is made up of coal and additive, and content of additive is 5wt%～20wt%.
5. the method for preparing hydrogen as claimed in claim 4 is characterized in that, wherein said additive is that calcium hydroxide, lime are or/and Wingdale.
6. the method for preparing hydrogen as claimed in claim 5 is characterized in that, the gasification temperature of coal tar is 700 ℃～750 ℃ in the step (2).
7. the method for preparing hydrogen as claimed in claim 6 is characterized in that, adds sylvite in step (2), serves as the calculating benchmark with the gross weight of the mixture is made up of coal tar and sylvite, and the content of sylvite is 5wt%～20wt%.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101899339A (en) * | 2009-05-27 | 2010-12-01 | 新奥科技发展有限公司 | Method for preparing high methane content gas from coal |
| CN102585912A (en) * | 2012-02-04 | 2012-07-18 | 王俊 | Method for continuous industrial production of coal gas by multi-chamber microwave heating |
| CN102585947A (en) * | 2011-12-14 | 2012-07-18 | 新奥科技发展有限公司 | Method and device for preparing methane-containing gas by using coal |
| CN103060012A (en) * | 2012-12-29 | 2013-04-24 | 中国科学院工程热物理研究所 | Gasification method for classification conversion of hydrocarbon components of coal |
| CN105158107A (en) * | 2015-07-30 | 2015-12-16 | 山东电力研究院 | Method for determining content of coal pyrolysis resultant |
| CN105964242A (en) * | 2016-06-06 | 2016-09-28 | 湖北华威斯新能源科技有限公司 | Novel coal gasification catalyst and preparation method and application thereof |
| CN106076436A (en) * | 2016-06-06 | 2016-11-09 | 湖北华威斯新能源科技有限公司 | The method of lump coal load coal gasification catalyst |
| CN108531218A (en) * | 2017-03-01 | 2018-09-14 | 何巨堂 | Hydrogen-consuming process produces the combined method of the hydrogen manufacturing of the hydrogen rich gas hydrocarbon gas and the gasification of carbonaceous solids material |
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2008
- 2008-10-10 CN CN 200810200992 patent/CN101372312A/en active Pending
Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101899339B (en) * | 2009-05-27 | 2014-03-12 | 新奥科技发展有限公司 | Method for preparing high methane content gas from coal |
| CN101899339A (en) * | 2009-05-27 | 2010-12-01 | 新奥科技发展有限公司 | Method for preparing high methane content gas from coal |
| CN102585947B (en) * | 2011-12-14 | 2016-05-04 | 新奥科技发展有限公司 | A kind of method and apparatus that is contained the gas of methane by coal preparation |
| CN102585947A (en) * | 2011-12-14 | 2012-07-18 | 新奥科技发展有限公司 | Method and device for preparing methane-containing gas by using coal |
| CN102585912A (en) * | 2012-02-04 | 2012-07-18 | 王俊 | Method for continuous industrial production of coal gas by multi-chamber microwave heating |
| CN102585912B (en) * | 2012-02-04 | 2014-05-28 | 王俊 | Method for continuous industrial production of coal gas by multi-chamber microwave heating |
| CN103060012A (en) * | 2012-12-29 | 2013-04-24 | 中国科学院工程热物理研究所 | Gasification method for classification conversion of hydrocarbon components of coal |
| CN105158107A (en) * | 2015-07-30 | 2015-12-16 | 山东电力研究院 | Method for determining content of coal pyrolysis resultant |
| CN105964242A (en) * | 2016-06-06 | 2016-09-28 | 湖北华威斯新能源科技有限公司 | Novel coal gasification catalyst and preparation method and application thereof |
| CN106076436A (en) * | 2016-06-06 | 2016-11-09 | 湖北华威斯新能源科技有限公司 | The method of lump coal load coal gasification catalyst |
| CN105964242B (en) * | 2016-06-06 | 2018-08-07 | 湖北华威斯新能源科技有限公司 | A kind of coal gasification catalyst and its preparation method and application |
| CN106076436B (en) * | 2016-06-06 | 2018-08-07 | 湖北华威斯新能源科技有限公司 | The method that lump coal loads coal gasification catalyst |
| CN108531218A (en) * | 2017-03-01 | 2018-09-14 | 何巨堂 | Hydrogen-consuming process produces the combined method of the hydrogen manufacturing of the hydrogen rich gas hydrocarbon gas and the gasification of carbonaceous solids material |
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