CN1557694A - Method and apparatus for producing hydrogen by natural gas using two-stage fluid bed reformer - Google Patents
Method and apparatus for producing hydrogen by natural gas using two-stage fluid bed reformer Download PDFInfo
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- CN1557694A CN1557694A CNA2004100139260A CN200410013926A CN1557694A CN 1557694 A CN1557694 A CN 1557694A CN A2004100139260 A CNA2004100139260 A CN A2004100139260A CN 200410013926 A CN200410013926 A CN 200410013926A CN 1557694 A CN1557694 A CN 1557694A
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Abstract
The hydrogen producing process includes mixing natural gas and water vapor, heating to 450-550 deg.c, adding to the first fluidized bed reformer and separating with hydrogen transmitting film to obtain hydrogen and rest gas; mixing rest gas and heating to 850-950 deg.c, adding to the second fluidized bed reformer to convert into synthetic gas containing hydrogen and CO, cooling the synthetic gas to 450-550 deg.c, separating with hydrogen transmitting film to obtain hydrogen, and burning the waste gas in the waste gas circulating re-burner. The apparatus consists of the first fluidized bed reformer, the second fluidized bed reformer and the reheating combustor.
Description
One, technical field
Hydro carbons of the present invention relates to a kind of process for making hydrogen and device, relates in particular to a kind of Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming and device for producing hydrogen thereof.
Two, technical background
Along with society and expanding economy, the demand of the energy increases day by day, and human bad survival environment requires more and more higher.Thereby the mankind face the challenge of efficient, the clean secondary energy of exploitation.Hydrogen more and more is subjected to human great attention as efficient, clean secondary energy, and widespread use in all conglomeraties.In recent years, hydrogen is subjected to countries in the world government and scholar's positive regard with the act as a fuel fuel applications of battery of unrivaled advantages such as high heating value, no atmospheric pollution.Sweet natural gas is a kind of profuse petrochemical complex fuel source, and existing explored Natural Gas Reserve in World is 142.1 tcms, and prospective reserves is 250～350 tcms.Therefore, natural gas source optimization utilization is paid much attention to.Rationally, efficiently gas renormalizing being converted into secondary energy---the technology of hydrogen seems very important.Traditional hydrogen manufacturing technique has the method for steam reforming and the partial oxidation reforming method of water electrolysis method, hydro carbons, but all has big problem.Water electrolysis method efficient is low, energy dissipation; The method for steam reforming of hydro carbons needs outside heat supply, system complex, and thermo-efficiency is lower, the temperature of reaction height, water consumption is big in the reaction process, and energy consumption is higher, the wasting of resources; The partial oxidation reforming method of hydro carbons,, system complex higher except that temperature of reaction, the hydrogen purity that makes is low, is unfavorable for the comprehensive utilization of the energy.Because there are many drawbacks in traditional hydrogen manufacturing technique, countries in the world are the new hydrogen manufacturing technique of the numerous and confused development of developed country particularly.
Three, technology contents
Technical problem the invention provides a kind of low-cost Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming and device for producing hydrogen thereof that can cut down the consumption of energy.
Technical scheme
The method of the invention is a kind of Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming that is used to produce hydrogen,
The first step: the Sweet natural gas of sulphur content below 10ppm mixed with water vapour, after by waste gas circulation reignition device the gas mixture of Sweet natural gas and water vapour being heated to 450 ℃ ~ 550 ℃, in the input one-level fluid bed reformer, to make the steam/hydrocarbons ratio in the one-level fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, obtains hydrogen and residual air behind the saturating Hydrogen membrane sepn of the selection of gas mixture in being located at the one-level fluid bed reformer;
Second step: residual air is mixed with water vapour after purifying, behind reheat to 850～950 ℃ in the input secondary fluid bed reformer, to make the steam/hydrocarbons ratio in the secondary fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, residual air is reformed transforms the synthetic gas that generates hydrogen and carbon monoxide, synthetic gas is cooled to 450 ℃～550 ℃, enter the fly-ash separator dedusting again, behind the saturating Hydrogen membrane sepn of selection in being located at the one-level fluid bed reformer, obtain hydrogen, the remainder of exhaust gas of this moment then enters in the waste gas circulation reignition device and carries out perfect combustion, for the one-level fluid bed reformer provides heat.
Device of the present invention is a kind of device for producing hydrogen that is used to realize above-mentioned hydrogen production process, by the one-level fluid bed reformer, secondary fluid bed reformer and reheat combustion chamber are formed, in reheat combustion chamber, be provided with reheat combustion chamber, the residual air outlet of one-level fluid bed reformer links to each other with the air intake of reheat combustion chamber, the air outlet of reheat combustion chamber is connected with the air compartment of secondary fluid bed reformer, on the secondary fluid bed reformer, be provided with the synthetic gas air outlet, the one-level fluid bed reformer is by air compartment, the fluidisation device, built-in double jacket is selected the Hydrogen membrane separation apparatus, catalyzer and fluidized bed body are formed, air compartment, the fluidisation device, catalyzer order from bottom to top is distributed in the fluidized bed body, built-in double jacket is selected the Hydrogen membrane separation apparatus to be horizontally through fluidized bed body and is positioned at catalyzer, built-in double jacket selects the Hydrogen membrane separation apparatus to be made up of interior Membrane cover and outer Membrane cover, interior Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from inside to outside, outer Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from outside to inside, on the natural gas air intake of the air compartment of one-level fluid bed reformer, be provided with waste gas circulation reignition chamber, on waste gas circulation reignition chamber, be provided with natural gas inlet mouth and natural gas air outlet, the natural gas air outlet is connected with the natural gas air intake of the air compartment of one-level fluid bed reformer, at the indoor waste gas circulation reignition device that is provided with of waste gas circulation reignition, on waste gas circulation reignition device, be provided with the waste gas air intake that contains carbon monoxide and burn and use the air intake of natural gas, this burning selects the waste gas outlet side of the interior Membrane cover of Hydrogen membrane separation apparatus to communicate with the air intake of natural gas with built-in double jacket, the inlet end of interior Membrane cover is communicated with the synthetic gas air outlet of secondary fluid bed reformer, interior Membrane cover and outside be provided with hydrogen outlet on the cavity between the Membrane cover.
Beneficial effect 1. the present invention adopts waste gas circulation reignition technology, waste gas to hydrogen after the separated reignition that circulates, its heat is used to heat natural gas, make that complicated CO conversion, cleaning section deleted in traditional hydrogen producing technology, simplified the technological process of total system greatly, reduce cost and effectively utilized the heat of waste-gas burning, reduced energy consumption.2. the present invention utilizes the heat of the synthetic gas of secondary fluid bed reformer generation that the natural gas that need heat is heated, and has further utilized the waste heat of synthetic gas, has reduced energy consumption.3. the waste heat that utilizes hydrogen can further cut down the consumption of energy to the heating of natural gas.4. adopt built-in double jacket to select the Hydrogen membrane separation apparatus in the first step reformer, both improved the efficiency of conversion of the natural gas hydrogen preparation in the first step reformer; Simultaneously will be separated into hydrogen and waste gas from the synthetic gas of second stage reformer again, for follow-up waste gas circulation reignition provides feasibility.Since this technology need not be complicated CO conversion, cleaning section, this makes the integral device compactness, is easy to small-sized, the high efficiency of the equipment of realizing.The twin-stage reformer all adopts fluidization.Utilize special fluidisation device and rational fluidized-bed structure, make the whole evenly fluidisation of the interior solid particulate of fluidized-bed so both to have made even rapid, the sufficient reacting that conducts heat, the hydrogen manufacturing transformation efficiency improves; Simultaneously reduce gas-flow resistance again, and the wearing and tearing of solid particulate and breaking.Utilize enhancement of heat transfer technology and self-heating system, make entire system efficiency of utilization height, energy consumption low.
Four, description of drawings
Fig. 1 is the system flowchart of twin-stage fluidized-bed Sweet natural gas steam self-heating reforming hydrogen manufacturing apparatus and method of the present invention, and interchanger 3, secondary ash collector 4, one-level fluid bed reformer 5, cleaner 6, waste gas circulation reignition device 7, by-pass valve control 8, heat exchanger package 9, reheat combustion chamber 10, reheat combustion chamber 11, secondary fluid bed reformer 12, primary dust removing device 13, pressurized air A, water B, compressed natural gas C, finished hydrogen D, discharging waste gas E are wherein arranged.
Fig. 2 is the structure diagram of one-level fluid bed reformer, wherein has air compartment 14, fluidisation device 15, built-in double jacket to select Hydrogen membrane separation apparatus 16, catalyzer 17 and fluidized bed body 18, and catalyzer 21 adopts nickel-base catalyst, ruthenium-based catalyst etc.
Fig. 3 is the structure diagram of secondary fluid bed reformer, and air compartment 19, fluidisation device 20, catalyzer 21 and fluidized bed body 22 are wherein arranged.
Fig. 4 is the structural representation that the present invention selects Hydrogen membrane separation apparatus embodiment.
Five, specific embodiments
Embodiment is used to produce the Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming of hydrogen for 1 one kinds, the first step: the Sweet natural gas of sulphur content below 10ppm mixed with water vapour, after by waste gas circulation reignition device the gas mixture of Sweet natural gas and water vapour being heated to 450 ℃ ~ 550 ℃, in the input one-level fluid bed reformer, to make the steam/hydrocarbons ratio in the one-level fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, obtains hydrogen and residual air behind the saturating Hydrogen membrane sepn of the selection of gas mixture in being located at the one-level fluid bed reformer; Second step: residual air is mixed with water vapour after purifying, behind reheat to 850～950 ℃ in the input secondary fluid bed reformer, to make the steam/hydrocarbons ratio in the secondary fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, residual air is reformed transforms the synthetic gas that generates hydrogen and carbon monoxide, synthetic gas is cooled to 450 ℃～550 ℃, enter the fly-ash separator dedusting again, behind the saturating Hydrogen membrane sepn of selection in being located at the one-level fluid bed reformer, obtain hydrogen, the remainder of exhaust gas of this moment then enters in the waste gas circulation reignition device and carries out perfect combustion, for the one-level fluid bed reformer provides heat, above-mentionedly regulate one-level by system back pressure, operation steps commonly used in the prior art is adopted in the concrete operations of secondary fluid bed reformer internal pressure, in the present embodiment, Sweet natural gas, water vapour and be used for combustion-supporting air interchanger with from the synthetic gas of secondary fluid bed reformer and combustion exhaust after the discharging gas that produced carry out heat exchange, natural gas also carries out after the heat exchange carrying out heat exchange with synthetic gas from the secondary fluid bed reformer with prepared hydrogen in interchanger again.
2 one kinds of device for producing hydrogen that are used to realize above-mentioned hydrogen production process of embodiment, by one-level fluid bed reformer 5, secondary fluid bed reformer 12 and reheat combustion chamber 11 are formed, in reheat combustion chamber 11, be provided with reheat combustion chamber 10, the residual air outlet 5b of one-level fluid bed reformer 5 links to each other with the air intake 11a of reheat combustion chamber 11, the air outlet 11b of reheat combustion chamber 11 is connected with the air compartment 19 of secondary fluid bed reformer 12, on secondary fluid bed reformer 12, be provided with synthetic gas air outlet 12b, one-level fluid bed reformer 5 is by air compartment 14, fluidisation device 15, built-in double jacket is selected Hydrogen membrane separation apparatus 16, catalyzer 17 and fluidized bed body 18 are formed, air compartment 14, fluidisation device 15, catalyzer 17 order from bottom to top is distributed in the fluidized bed body 18, built-in double jacket is selected Hydrogen membrane separation apparatus 16 to be horizontally through fluidized bed body 18 and is positioned at catalyzer 17, built-in double jacket selects Hydrogen membrane separation apparatus 16 to be made up of interior Membrane cover and outer Membrane cover, interior Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from inside to outside, outer Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from outside to inside, on the natural gas air intake of the air compartment 14 of one-level fluid bed reformer 5, be provided with waste gas circulation reignition chamber 7, on waste gas circulation reignition chamber 7, be provided with natural gas inlet mouth 7a and natural gas air outlet, the natural gas air outlet is connected with the natural gas air intake of the air compartment 14 of one-level fluid bed reformer 5, in waste gas circulation reignition chamber 7, be provided with waste gas circulation reignition device 7f, on waste gas circulation reignition device 7f, be provided with the waste gas air intake that contains carbon monoxide and burn and use the air intake of natural gas, this burning selects the waste gas outlet side of the interior Membrane cover of Hydrogen membrane separation apparatus 16 to communicate with the air intake of natural gas with built-in double jacket, the inlet end of interior Membrane cover is communicated with the synthetic gas air outlet 12b of secondary fluid bed reformer 12, interior Membrane cover and outside be provided with hydrogen outlet 5c on the cavity between the Membrane cover, in the present embodiment, the synthetic gas air outlet 12b of secondary fluid bed reformer 12 is communicated with the inlet end of interior Membrane cover through the plate exterior passage way of heat exchanger package 9, be used to carry the second plate interior passageway outlet side 92b of the heat exchanger package 9 of natural gas to link to each other with the natural gas inlet mouth 7a of waste gas circulation reignition chamber 7 and the inlet mouth of reheat combustion chamber 10 respectively, the 3rd plate interior passageway outlet side 93b that is used for the heat exchanger package 9 of fluming water steam communicates with the natural gas inlet mouth 7a and the reheat combustion chamber 11 of waste gas circulation reignition chamber 7 respectively with respectively, be used to carry the 4th plate interior passageway outlet side 94b of the heat exchanger package 9 of air to communicate with waste gas circulation reignition device 7f and reheat combustion chamber 10 respectively, natural gas is transported to the second plate interior passageway inlet end of heat exchanger package 9 through the plate interior passageway of interchanger 3, hydrogen from hydrogen outlet 5c is exported through the plate exterior passage way of interchanger 3, the synthetic gas air outlet 12b of secondary fluid bed reformer 12 is communicated with the inlet end of the plate exterior passage way of heat exchanger package 9 by primary dust removing device 13, the outlet side of the plate exterior passage way of heat exchanger package 9 is communicated with the inlet end of interior Membrane cover through secondary ash collector 4, residual air from one-level fluid bed reformer 5 enters reheat combustion chamber 11 through cleaner 6, above-mentioned secondary fluid bed reformer 12 is by air compartment 19, fluidisation device 20, catalyzer 21 and fluidized bed body 22 are formed, air compartment 19, fluidisation device 20 and catalyzer 21 being located in the fluidized bed body 22 from bottom to top, catalyzer 21 adopts nickel-base catalyst, ruthenium-based catalyst etc.
Claims (8)
1, a kind of Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming that is used to produce hydrogen is characterized in that:
The first step: the Sweet natural gas of sulphur content below 10ppm mixed with water vapour, after by waste gas circulation reignition device the gas mixture of Sweet natural gas and water vapour being heated to 450 ℃ ~ 550 ℃, in the input one-level fluid bed reformer, to make the steam/hydrocarbons ratio in the one-level fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, obtains hydrogen and residual air behind the saturating Hydrogen membrane sepn of the selection of gas mixture in being located at the one-level fluid bed reformer;
Second step: residual air is mixed with water vapour after purifying, behind reheat to 850～950 ℃ in the input secondary fluid bed reformer, to make the steam/hydrocarbons ratio in the secondary fluid bed reformer be 2.5～4.0 by regulating above-mentioned steam rates, making pressure by the system back pressure adjusting is 0.15～4.0Mpa, residual air is reformed transforms the synthetic gas that generates hydrogen and carbon monoxide, synthetic gas is cooled to 450 ℃～550 ℃, enter the fly-ash separator dedusting again, behind the saturating Hydrogen membrane sepn of selection in being located at the one-level fluid bed reformer, obtain hydrogen, the remainder of exhaust gas of this moment then enters in the waste gas circulation reignition device and carries out perfect combustion, for the one-level fluid bed reformer provides heat.
2, Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming according to claim 1, it is characterized in that Sweet natural gas, water vapour and be used for combustion-supporting air interchanger with from the synthetic gas of secondary fluid bed reformer and combustion exhaust after the discharging gas that produced carry out heat exchange.
3, Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming according to claim 2 is characterized in that natural gas carries out after the heat exchange carrying out heat exchange with synthetic gas from the secondary fluid bed reformer with prepared hydrogen again in interchanger.
4, according to claim 1,2 or 3 described Sweet natural gas twin-stage fluidized-bed method for preparing hydrogen by reforming, it is characterized in that gas mixture and synthetic gas select Hydrogen membrane separation apparatus (16) separating hydrogen gas by the built-in double jacket that is located in the one-level fluid bed reformer, built-in double jacket selects Hydrogen membrane separation apparatus (16) to be made up of interior Membrane cover and outer Membrane cover, gas mixture is via the outer Membrane cover separating hydrogen gas of the outer saturating Hydrogen of selection inwards, and synthetic gas is via Membrane cover separating hydrogen gas in the saturating Hydrogen of the outside selection in lining.
5, a kind of device for producing hydrogen that is used to realize the described hydrogen production process of claim 1, by one-level fluid bed reformer (5), secondary fluid bed reformer (12) and reheat combustion chamber (11) are formed, in reheat combustion chamber (11), be provided with reheat combustion chamber (10), the residual air outlet (5b) of one-level fluid bed reformer (5) links to each other with the air intake (11a) of reheat combustion chamber (11), the air outlet (11b) of reheat combustion chamber (11) is connected with the air compartment (19) of secondary fluid bed reformer (12), on secondary fluid bed reformer (12), be provided with synthetic gas air outlet (12b), it is characterized in that one-level fluid bed reformer (5) is by air compartment (14), fluidisation device (15), built-in double jacket is selected Hydrogen membrane separation apparatus (16), catalyzer (17) and fluidized bed body (18) are formed, air compartment (14), fluidisation device (15), catalyzer (17) order from bottom to top is distributed in the fluidized bed body (18), built-in double jacket is selected Hydrogen membrane separation apparatus (16) to be horizontally through fluidized bed body (18) and is positioned at catalyzer (17), built-in double jacket selects Hydrogen membrane separation apparatus (16) to be made up of interior Membrane cover and outer Membrane cover, interior Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from inside to outside, outer Membrane cover adopts to be the saturating Hydrogen Membrane cover of selection of hydrogen direction from outside to inside, on the natural gas air intake of the air compartment (14) of one-level fluid bed reformer (5), be provided with waste gas circulation reignition chamber (7), on waste gas circulation reignition chamber (7), be provided with natural gas inlet mouth (7a) and natural gas air outlet, the natural gas air outlet is connected with the natural gas air intake of the air compartment (14) of one-level fluid bed reformer (5), in waste gas circulation reignition chamber (7), be provided with waste gas circulation reignition device (7f), on waste gas circulation reignition device (7f), be provided with the waste gas air intake that contains carbon monoxide and burn and use the air intake of natural gas, this burning selects the waste gas outlet side of the interior Membrane cover of Hydrogen membrane separation apparatus (16) to communicate with the air intake of natural gas with built-in double jacket, the inlet end of interior Membrane cover is communicated with the synthetic gas air outlet (12b) of secondary fluid bed reformer (12), interior Membrane cover and outside be provided with hydrogen outlet (5c) on the cavity between the Membrane cover.
6, device for producing hydrogen according to claim 5, the synthetic gas air outlet (12b) that it is characterized in that secondary fluid bed reformer (12) is communicated with the inlet end of interior Membrane cover through the plate exterior passage way of heat exchanger package (9), be used to carry the second plate interior passageway outlet side (92b) of the heat exchanger package (9) of natural gas to link to each other with the natural gas inlet mouth (7a) of waste gas circulation reignition chamber (7) and the inlet mouth of reheat combustion chamber (10) respectively, the 3rd plate interior passageway outlet side (93b) that is used for the heat exchanger package (9) of fluming water steam communicates with the natural gas inlet mouth (7a) and the reheat combustion chamber (11) of waste gas circulation reignition chamber (7) respectively with respectively, is used to carry the 4th plate interior passageway outlet side (94b) of the heat exchanger package (9) of air to communicate with waste gas circulation reignition device (7f) and reheat combustion chamber (10) respectively.
7, device for producing hydrogen according to claim 6 is characterized in that natural gas transports to the second plate interior passageway inlet end of heat exchanger package (9) through the plate interior passageway of interchanger (3), from the plate exterior passage way output through interchanger (3) of the hydrogen of hydrogen outlet (5c).
8, device for producing hydrogen according to claim 7, the synthetic gas air outlet (12b) that it is characterized in that secondary fluid bed reformer (12) is communicated with the inlet end of the plate exterior passage way of heat exchanger package (9) by primary dust removing device (13), the outlet side of the plate exterior passage way of heat exchanger package (9) is communicated with the inlet end of interior Membrane cover through secondary ash collector (4), enters reheat combustion chamber (11) from the residual air of one-level fluid bed reformer (5) through cleaner (6).
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| CN 200410013926 CN1234594C (en) | 2004-01-16 | 2004-01-16 | Method and apparatus for producing hydrogen by natural gas using two-stage fluid bed reformer |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100503790C (en) * | 2005-09-01 | 2009-06-24 | 中国科学院工程热物理研究所 | Method of producing chemical product by double fuel reforming chemical system |
| CN1869165B (en) * | 2005-05-23 | 2010-04-28 | 中国科学院工程热物理研究所 | Bifuel reforming multifunctional energy system and its method |
| CN101842316B (en) * | 2007-11-01 | 2012-10-03 | Sk新技术株式会社 | Hydrogen generating apparatus using steam reforming reaction |
| CN107597199A (en) * | 2017-09-13 | 2018-01-19 | 武汉凯迪工程技术研究总院有限公司 | Recirculating fluidized bed hydrocarbon reforming catalyst and its preparation method and application |
| CN115111629A (en) * | 2022-06-10 | 2022-09-27 | 北京市燃气集团有限责任公司 | Zero-carbon heat supply method |
-
2004
- 2004-01-16 CN CN 200410013926 patent/CN1234594C/en not_active Expired - Fee Related
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1869165B (en) * | 2005-05-23 | 2010-04-28 | 中国科学院工程热物理研究所 | Bifuel reforming multifunctional energy system and its method |
| CN100503790C (en) * | 2005-09-01 | 2009-06-24 | 中国科学院工程热物理研究所 | Method of producing chemical product by double fuel reforming chemical system |
| CN101842316B (en) * | 2007-11-01 | 2012-10-03 | Sk新技术株式会社 | Hydrogen generating apparatus using steam reforming reaction |
| CN107597199A (en) * | 2017-09-13 | 2018-01-19 | 武汉凯迪工程技术研究总院有限公司 | Recirculating fluidized bed hydrocarbon reforming catalyst and its preparation method and application |
| CN115111629A (en) * | 2022-06-10 | 2022-09-27 | 北京市燃气集团有限责任公司 | Zero-carbon heat supply method |
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