CN104134811A - Reforming hydrogen preparing device capable of recycling pressure swing absorption desorption gas and technique thereof - Google Patents
Reforming hydrogen preparing device capable of recycling pressure swing absorption desorption gas and technique thereof Download PDFInfo
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- CN104134811A CN104134811A CN201410356317.9A CN201410356317A CN104134811A CN 104134811 A CN104134811 A CN 104134811A CN 201410356317 A CN201410356317 A CN 201410356317A CN 104134811 A CN104134811 A CN 104134811A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
- H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
- H01M8/0618—Reforming processes, e.g. autothermal, partial oxidation or steam reforming
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
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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
- 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
- Y02E60/50—Fuel cells
Abstract
The invention relates to a reforming hydrogen preparing device capable of recycling pressure swing absorption desorption gas and a technique thereof. The hydrogen preparing device integrates multiple areas of a combustible gas mixture buffer area, a desorption gas recycling and transforming area, a catalytic combustion transition area, a second air & combustible gas reaction area, a reformed raw material mixing area, a natural gas reforming & hydrogen preparing area, a reformed raw gas buffer area, etc. The raw material required by the reforming hydrogen preparation can enter the natural gas reforming & hydrogen preparing device directly at room temperature, the natural gas is reformed to prepare hydrogen and the pressure swing absorption desorption gas is recycled, transformed and utilized in the natural gas reforming & hydrogen preparing device. By this technique, the water pipe management is intensified, and a gas product with the hydrogen density reaching more than 99.9% can be obtained. In addition, hydrogen can be provided for fuel batteries, and the device and the battery system are capable of providing power and heat for users jointly. Both natural gas and alcohol & hydrocarbon hydrogen-containing compounds such as methanol and ethanol can be used as the raw material for the hydrogen preparing technique.
Description
Technical field
The present invention relates to a kind of reforming hydrogen production device and the technique that can recycle pressure-variable adsorption resolution gas, especially relate to a kind of hydrogen making by natural gas reformation device and the technique that can recycle pressure-variable adsorption resolution gas of focusing on promoting hydrogen making by natural gas reformation device integrated level, strengthening thermal management and water route management, raising total system energy efficiency.
Background technology
Enter 21 century, energy security and environmental protection have become the problem of globalization, resolve the energy sustainable development strategic issue of China, are the important steps that realizes Chinese society sustainable economic development.For the oil-poor energy resource structure of China's many coals weak breath, the energy development strategic requirement of Future in China improves energy efficiency, and the clean fossil energy that uses, readjusts the energy structure, and increases alternative energy source, realizes the sustainable development of the energy.Hydrogen Energy does not produce any disposal of pollutants in the time utilizing, and is the ideal chose of following clean energy resource carrier, brings into play main flow effect by likely being smoothly transitted to by fossil energy at human society in the sustainable end-around carry that does not finally rely on fossil energy.
Hydrogen is the abundantest element, but that natural hydrogen exists is few, must consume a large amount of energy and will after hydrogenous material decomposition, just can obtain hydrogen, therefore finds a kind of low energy consumption, high efficiency hydrogen production process is trend of the times.The abundantest hydrogenous material is water (H
2o), be exactly secondly various fossil fuel (coal, oil, natural gas) and various biomass etc.The production of hydrogen, purify, transport and store and all need to have corresponding capital construction, need a large amount of investments, relate to multiple links, and links technological difficulties, economy and the fail safe etc. that relate to all exist some bottleneck problems need to go to improve to solve.China's natural gas resource is mainly distributed in the remote districts such as western part, the northwestward, causes the costs such as its compression, transport, storage, utilization higher.At present, in order to realize the economic utilization of natural gas, conventionally natural gas is processed as initial feed, conversion of natural gas is become to CO and H
2(being synthesis gas), this is also a comparatively desirable hydrogen producing technology route.
Pressure-variable adsorption (Pressure Swing Adsorption, PSA) gas Separation & Purification technology developed rapidly in the sixties in last century, had become at present a kind of production technology of chemical engineering industry and unit process independently.Because PSA Gas Separation Technology is to rely on the variation of pressure to realize absorption and regeneration, thereby reproduction speed is fast, energy consumption is low, belongs to energy-saving gas separation.And this technical process is simple, stable operation, impurity once can be removed and obtains high purity product for the gaseous mixture containing plurality of impurities, development in recent years is very fast, and wherein the development of pressure-variable adsorption making pure hydrogen technology especially attracts people's attention.
The present invention just considers from hydrogen manufacturing total system, to improve system capacity efficiency as object, provides a kind of improved hydrogen production reaction technique, comprises that hydrogen making by natural gas reformation device, water knockout drum, pressure-swing absorption apparatus and pressure-variable adsorption resolution gas reclaim converter etc.Adopt catalytic combustion technology that the fuel gas in resolution gas is all reclaimed and change into efficient heat and offer natural gas hydrogen preparation reaction, finally reaching the object that improves system capacity efficiency.
Distributed heat chp system (Combined Heat and Power, CHP) has that energy cascade utilization efficiency is high, electric power supply is reliable, good in economic efficiency, advantages of environment protection; Supplement as the organic of traditional energy system, significant to alleviating China's terminal energy sources severe challenge that electric and hot production and supply faces.Along with the continuous progress of Hydrogen Energy and fuel cell technology, the cogeneration system based on fuel cell technology becomes the important development direction that distributed heat CCHP is new just gradually.
Proton Exchange Membrane Fuel Cells (PEMFC), taking hydrogen as fuel, is converted into electric energy by the electrode reaction between the hydrogen of anode and the oxygen of negative electrode by chemical energy, has the advantages such as energy conversion efficiency is high, simple in structure, environmental pollution is little.Adopt fossil feedstock reforming hydrogen producing technology and proton exchange film fuel battery system associating, in fixed or Mobile fuel battery power supply system or fuel cell cogeneration system, be widely applied.But in the rich reformed gas that fossil feedstock reforming hydrogen producing technology provides, residual CO is very large on the anode impact of PEMFC, conventionally requires CO concentration below 30ppm.
For CO residual in hydrogen-rich reformed gas, traditional method is to adopt chemical reaction method, finally can control CO concentration at 3-30ppm, but this kind of technology path brings technical difficult point can to whole system handling of goods and materials and energy management, comprise the technology such as reactor design, design of heat exchanger and thermal management etc., simultaneously very high to CO catalyst for selective oxidation performance requirement, especially to catalyst at CO and H
2between competitive reaction selectivity require very highly, also to be strict with the long-time stability (3000-10000h) of catalyst simultaneously, the noble metal such as Pt, Pd is comparatively effective as catalyst activity component in addition, but has the problem of Financial cost aspect.
Patent documentation (CN101054160A, US6793698 B1, EP1094031 A1) discloses a kind of reforming hydrogen-preparation reactor, but simple in structure, energy utilization rate is low, and the residual gas of resolving gas cannot make full use of, and reformation hydrogen production efficiency is not high.In addition, there are differences of balance combustion reaction rate and reformation hydrogen production reaction rate, this reforming hydrogen-preparation reactor can not be realized stable the carrying out of two kinds of different chemicals reactions.
Natural gas hydrogen production plant provided by the invention and process using pressure-swing absorption apparatus substitute CO shift-converter and CO purification reactor, directly hydrogen-rich reformed tail gas is carried out to separating-purifying, with respect to adopting chemical reaction method to eliminate CO, adopt the pressure-swing absorption apparatus technique H that directly purifies
2, have that energy consumption is low, flow process is simple, H
2the advantages such as purity is high, device operating flexibility is large and environmental benefit is good.Can be fuel cell system provides the H of high-quality
2raw material, constitutes jointly distributed heat chp system with fuel cell system, simultaneously by the H in pressure-swing absorption apparatus resolution gas and anode of fuel cell tail gas
2recycled, improved the H of whole system
2the rate of recovery, and then the energy consumption of reduction system, the energy efficiency of raising system.
Summary of the invention
The invention provides a kind of reforming hydrogen production device and the technique that can recycle pressure-variable adsorption resolution gas, especially recycle hydrogen making by natural gas reformation device and the technique of pressure-variable adsorption resolution gas, first pass through reforming hydrogen production device, by hydrocarbon (hydro carbons, alcohol compound, particularly natural gas etc.) be converted into hydrogen-rich gas, adopt afterwards pressure-swing absorption apparatus separating-purifying to obtain the hydrogen of high-quality.The high-quality hydrogen producing can store or supply with user and use, and also can generate electricity by feed fuels battery system; Reclaim the hydrogen in pressure-swing absorption apparatus resolution gas simultaneously, be translated into effective energy and act in hydrogen generating system, and then improve the energy efficiency of system.
Can recycle a reforming hydrogen production device for pressure-variable adsorption resolution gas, the central area of described device comprises that fuel gas mixing buffering area (A), resolution gas reclaim zone of transformation (B), catalytic combustion transition region (C) successively; The outside of the central area of described device is followed successively by second reaction zone (D), reformer feed mixed zone (E), reformation hydrogen production Second Region (G) of reformation hydrogen production the firstth district (F), air and fuel gas; The bottom of described device is provided with hydrogen feedstock buffering area (H); Wherein said fuel gas mixing buffering area (A) is provided with fuel gas entrance (a) and air intake (b), the second reaction zone (D) that fuel gas and air reclaim zone of transformation (B), catalytic combustion transition region (C), air and fuel gas by fuel gas mixing buffering area (A), resolution gas after mixing successively, reacted combustion tail gas is discharged by combustion tail gas outlet (c); Hydrogen feedstock buffering area (H) is provided with hydrogen feedstock entrance (f) and hydrogen feedstock diversion cavity (107), wherein hydrogen feedstock diversion cavity (107) stretches in reformer feed mixed zone (E), the raw water that hydrogen feedstock enters at reformer feed mixed zone (E) and raw water entrance (d) by hydrogen feedstock diversion cavity (107) after hydrogen feedstock buffering area (H) mixes, enter successively again reformation hydrogen production the firstth district (F) and reformation hydrogen production Second Region (G), after heat exchanger heat exchange, discharged by product gas outlet (e); Product gas outlet (e) is connected with pressure-swing absorption apparatus; Pressure-swing absorption apparatus connects fuel gas entrance (a) by resolution gas recovery channel; Described resolution gas reclaims the interior filling in second reaction zone (D) combustion catalyst of zone of transformation (B), fuel gas; Described catalytic combustion transition region (C) is loaded the heat-storing material of large thermal capacitance.
Reformer feed is natural gas, can be also methyl alcohol or ethanol, and reformer feed is that hydrogen-containing compound or the mixture of alcohols or hydro carbons can be realized the present invention.Described reformation hydrogen production Second Region (G) is connected with product gas outlet (e) by the heat exchanger (106) being arranged in hydrogen feedstock buffering area (H).The described pipeline being arranged in hydrogen feedstock buffering area (H) is S shape or helical form.Described hydrogen feedstock diversion cavity (107) is provided with and is down " protruding " shape hydrogen feedstock discharge end, and the bottom surface of this hydrogen feedstock discharge end and side face region are provided with hydrogen feedstock discharge orifice.Described combustion catalyst is palladium system, platinum group or their alloy catalyst.Fuel gas entrance and air intake place are provided with gas distributor.In fuel gas mixing buffering area (A), be provided with fuel gas redistributor (105).Between product gas outlet (e) and pressure-swing absorption apparatus, water knockout drum is set.
This reforming hydrogen production device also comprises water circulation system, and described water circulation system comprises multiple water knockout drums, hydrotreater, cyclic water tank successively, and cyclic water tank connects reformer feed water inlet (d).Described combustion tail gas outlet (c) is connected with heat exchanger, and heat exchanger connects water knockout drum.It is front through heat exchanger preheating that air enters air intake (b).Described fuel gas is natural gas, coal gas, or the gaseous mixture of the pressure-variable adsorption resolution gas of natural gas or coal gas and recovery.Gas material storage-tank pipeline connects natural gas via desulfurizer, and then pipeline is divided into two-way, and wherein a road connects fuel gas entrance (a); Another road natural gas straight connects hydrogen feedstock entrance (f) in succession.Pressure-swing absorption apparatus connecting fuel battery system, the tail gas that anode of fuel cell produces is carried and is connected fuel gas entrance (a) through pipeline.On the pipeline of connection fuel gas entrance (a), be equipped with temperature control adjusting valve and flame arrester; Regulate temperature control adjusting valve by temperature feedback controlled adjuster.
The process for making hydrogen of reforming hydrogen production device described in a kind of claim 1, fuel gas is after mix fuel gas mixing buffering area (A), in resolution gas reclaims the second reaction zone (D) of zone of transformation (B), catalytic combustion transition region (C), air and fuel gas and air generation catalyst combustion reaction, and for reformation hydrogen production reaction provides heat, combustion tail gas is discharged through combustion tail gas outlet (c); Hydrogen feedstock enters hydrogen feedstock buffering area (H) through hydrogen feedstock entrance (f), after heat exchange, enter hydrogen feedstock diversion cavity (107), the raw water entering at reformer feed mixed zone (E) and raw water entrance (d) mixes, after heat exchange, preheating, in reformation hydrogen production the firstth district (F), reformation hydrogen production Second Region (G) carry out reforming reaction and generate hydrogen-rich reformate gas, reformate gas enters pressure-swing absorption apparatus, and hydrogen is carried out to separating-purifying; After pressure-swing absorption apparatus separating-purifying, remaining resolution gas reclaims by resolution gas recovery channel, and as combustible gas input fuel gas entrance.
In the time of reformation hydrogen production initial operating stage, fuel gas is natural gas; When after reformation hydrogen production stable operation, after pressure-swing absorption apparatus separating-purifying, remaining resolution gas reclaims by resolution gas recovery channel, and as combustible gas input fuel gas entrance (a).Gas material storage tank provides natural gas, after desulfurizer desulfurization, is divided into two-way, and wherein a road natural gas enters fuel gas entrance (a), and another road natural gas straight connects unstripped gas entrance (f) in succession.The high-purity hydrogen of separating offers fuel cell system, and the tail gas that anode of fuel cell produces returns to fuel gas entrance (a) as fuel gas utilization.On the pipeline of connection fuel gas entrance (a), be equipped with temperature control adjusting valve and flame arrester; Regulate temperature control adjusting valve by temperature feedback controlled adjuster, realize the real-time matching of natural gas, resolution gas and anode of fuel cell tail gas feed rate, ensure the stable operation of reformation hydrogen production reaction.
The reformate gas of preparation is discharged by product gas outlet (e), enter the gas product water knockout drum that product gas outlet (e) is connected with pressure-swing absorption apparatus, after hydrotreater purified treatment, be delivered to cyclic water tank as raw water at the water obtaining in gas product water knockout drum.The combustion tail gas of combustion tail gas outlet (c) enters fraction water device water-dividing after heat exchanger, and the water producing in combustion process is discharged by water knockout drum bottom, enters hydrotreater and processes rear direct circulation recovery tank; Fuel battery negative pole tail gas enters point water in cathode exhaust gas water knockout drum and be delivered to cyclic water tank as raw water after hydrotreater carries out purified treatment.Fuel gas and mixed reformer feed reverse flow, ensured the utilance of heat.
The invention provides a kind of reforming hydrogen production device and the technique that can recycle pressure-variable adsorption resolution gas, both solved the emission problem of pressure-variable adsorption resolution gas in hydrogen production process, can recycle again pressure-variable adsorption resolution gas, use it for reformation hydrogen production process; The water generating in part reformation hydrogen production raw water and pressure-variable adsorption resolution gas recycling process can cycling and reutilization, has effectively saved water resources; Be recoverable pressure-variable adsorption resolution gas in this reforming hydrogen production device inside, simplified Hydrogen making technological process, improved hydrogen production efficiency.
Reforming hydrogen production device and the technique that can recycle pressure-variable adsorption resolution gas provided by the invention, in the time recycling pressure-variable adsorption resolution gas, adopt catalytic combustion technology, compared with direct burning, catalytic combustion temperature is lower, ratio of combustion is more complete, extremely friendly to environment.
The reforming hydrogen production device that can recycle pressure-variable adsorption resolution gas provided by the invention, in order to improve hydrogen production efficiency, this reforming hydrogen production device inner integrated fuel gas mixing buffering area A, resolution gas reclaims zone of transformation B, catalytic combustion transition region C, the second reaction zone D of air and fuel gas, reformer feed Mixed Zone E, reformation hydrogen production the first district F, multiple main region such as reformation hydrogen production Second Region G and reformer feed gas buffering area H, by the reasonable distribution of the cold fluid and hot fluid in adjacent area, simultaneously by the partition heat exchange between adjacent area, reduce the heat transmission resistance of endothermic process and exothermic process, improve the compactedness of reforming hydrogen production device.
The reforming hydrogen production device that can recycle pressure-variable adsorption resolution gas provided by the invention, by fuel gas mixing buffering area A is set in reforming hydrogen production device, can avoid due to the heat supply entrance a of reforming hydrogen production device and the fluctuation of air intake b place gas pressure and the pressure of whole hydrogen generating system is exerted an influence, thus the stable operation of assurance device.After fuel gas mixes, fuel gas redistributor 105 is set, can ensure that fuel gas fully mixes with air and evenly enters resolution gas recovery zone of transformation B, the appearance of the focus of avoiding well burning.Because resolution gas reclaims combustion rate in zone of transformation B and the reformation hydrogen production reaction rate in adjacent hydrogen making by natural gas reformation the first district F differs larger, therefore at catalytic combustion transition region C, the heat-storing material that a large amount of thermal capacitances are larger is set, in order to the difference of balance combustion reaction rate and reformation hydrogen production reaction rate, thereby ensure stable the carrying out that two kinds of different chemicals react.
The reforming hydrogen producing process that can recycle pressure-variable adsorption resolution gas provided by the invention, by pressure-swing absorption apparatus, reformation gas product is carried out to separating-purifying, can provide more than 99.9% hydrogen of purity for user, while can all be reclaimed pressure-swing absorption apparatus resolution gas and be converted into effective energy and be acted on reforming hydrogen production device, has greatly improved the energy efficiency of system.
The reforming hydrogen producing process that can recycle pressure-variable adsorption resolution gas provided by the invention, can with fuel cell system cogeneration, and provide heat.Hydrogen in anode of fuel cell tail gas can reclaim completely, and is converted into effective energy and acts on hydrogen making by natural gas reformation device, and then has improved the energy efficiency of system.
The reforming hydrogen producing process that can recycle pressure-variable adsorption resolution gas provided by the invention, not only can adopt natural gas is hydrogen feedstock, also can extensively adopt the hydrogen-containing compound of the multiple alcohols such as methyl alcohol, ethanol, town gas, liquefied gas and hydro carbons as hydrogen feedstock.
brief description of the drawings
Fig. 1 is hydrogen making by natural gas reformation device and the inner experiment flow figure that can recycle pressure-variable adsorption resolution gas;
Fig. 2 is the cut-away view that can recycle the hydrogen making by natural gas reformation device of pressure-variable adsorption resolution gas;
Fig. 3 is the flow chart that can recycle the hydrogen making by natural gas reformation technique of pressure-variable adsorption resolution gas;
Fig. 4 is the flow chart of the hydrogen making by natural gas reformation technique that can recycle pressure-variable adsorption resolution gas of combining with fuel cell system.
Embodiment
Taking natural gas as hydrogen feedstock, the present invention is further described.
Hydrogen making by natural gas reformation device (Fig. 1), has mainly comprised that fuel gas mixing buffering area A, resolution gas reclaim multiple major functions regions such as second reaction zone D, reformer feed mixed zone E, hydrogen making by natural gas reformation the first district F, hydrogen making by natural gas reformation Second Region G and the reformer feed gas buffering area H of zone of transformation B, catalytic combustion transition region C, air and fuel gas.First pass into respectively a certain amount of pressure-variable adsorption resolution gas and air that needs recycling by heat supply entrance a and the air intake b of hydrogen making by natural gas reformation device, both reclaim the second reaction zone D of zone of transformation B, catalytic combustion transition region C, air and fuel gas successively by fuel gas mixing buffering area A, resolution gas after mixing, combustion tail gas is discharged system by combustion tail gas outlet c.Hydrogen making by natural gas reformation needed raw material gas is entered by the unstripped gas entrance f of hydrogen making by natural gas reformation device, the hydrogen making by natural gas reformation needed raw material water entering at reformer feed mixed zone E with by the raw water entrance d of hydrogen making by natural gas reformation device after reformer feed gas buffering area H mixes, enter successively again hydrogen making by natural gas reformation the first district F and hydrogen making by natural gas reformation Second Region G, chemical reaction process by hydrogen making by natural gas reformation produces reformate gas, finally discharges system by the product gas outlet e of hydrogen making by natural gas reformation device.
Hydrogen making by natural gas reformation device of the present invention has adopted flow process as described below (Fig. 2) in the time of stable operation, first passed into the pressure-variable adsorption resolution gas of a certain amount of recovery by the heat supply entrance a of hydrogen making by natural gas reformation device, pressure-variable adsorption resolution gas enters fuel gas distributor 104 through fuel gas buffering area 101, evenly enter the mixed zone A of air and fuel gas, air enters air cushioning district 102 by the air intake b of hydrogen making by natural gas reformation device simultaneously, entered again the mixed zone A of air and fuel gas by air sparger 103, in the A of the mixed zone of air and fuel gas, air and fuel gas fully mix, and process fuel gas redistributor 105 enters the conversion zone of air and fuel gas, be that resolution gas reclaims zone of transformation B in the first half of this conversion zone, in reclaiming zone of transformation B, resolution gas is filled with the catalyst that air and fuel gas generation chemical reaction is had to catalytic action, catalyst is palladium system, platinum group or their alloy catalyst, make air and fuel gas under the effect of catalyst, do not need external heat, under pressurized conditions, carry out catalyst combustion reaction, emit a large amount of heat simultaneously.The latter half that reacted high-temperature gas directly enters the conversion zone of air and fuel gas is catalytic combustion transition region C, at the larger heat-storing material of this position filling thermal capacitance.Reacted high-temperature gas is after heat-storing material layer, temperature slightly declines and enters the second reaction zone D of air and fuel gas, in this region, combustion catalyst is housed, it is identical with the catalyst in resolution gas recovery zone of transformation B, ensure after air and the second reaction zone D of fuel gas by air and fuel gas, fuel gas is all converted into carbon dioxide and water, and discharges system by combustion tail gas outlet c.
The required water of hydrogen making by natural gas reformation is entered by the raw water entrance d of hydrogen making by natural gas reformation device, raw water is first by entering reformer feed mixed zone E after liquid distributor 108 uniform distributions, the required natural gas of hydrogen making by natural gas reformation enters reformer feed gas buffering area H by the unstripped gas entrance f of hydrogen making by natural gas reformation device simultaneously, carry out heat exchange at this and the reformation hydrogen production gas product of the hydrogen making by natural gas reformation device internal exchanger 106 of flowing through, natural gas after preheating is evenly sprayed and enters reformer feed mixed zone E by unstripped gas mozzle 107, near unstripped gas mozzle 107 outlets in the E of reformer feed mixed zone, natural G&W can acutely mix, mixed natural G&W flows to bottom from the middle part of reformer feed mixed zone E, and finally enter hydrogen making by natural gas reformation the first district F, be filled with hydrogen making by natural gas reformation catalyst in this region, under the catalytic action of catalyst, natural G&W generates rich hydrogen production gas by reaction, rich hydrogen production gas enters hydrogen making by natural gas reformation Second Region G, in this region, reformer feed can be converted into hydrogen-rich mixed gas completely, and undertaken being flowed out by the product gas outlet e of hydrogen making by natural gas reformation device after heat exchange by hydrogen making by natural gas reformation device internal exchanger 106 and unstripped gas.
Hydrogen making by natural gas reformation device of the present invention, in the time of stable operation, has been realized the Proper Match of energy well between inner different logistics.First the reformer feed gas being entered by the unstripped gas entrance f of hydrogen making by natural gas reformation device carry out heat exchange by the gas product of hydrogen making by natural gas reformation device internal exchanger 106 and reformation hydrogen production in reformer feed gas buffering area H, by adjustment operation parameter, can ensure that the temperature of the gas product of reformation hydrogen production reduces and meet the demand of subsequent processing, meanwhile, unstripped gas can be preheating to higher temperature, and mix with raw water near 107 outlets of unstripped gas mozzle, directly part heat is passed to raw water efficiently.Unstripped gas and raw water are mixed into after hydrogen making by natural gas reformation the first district F, under effect at catalyst, carry out hydrogen making by natural gas reformation reaction at this region unstripped gas and raw water, because this reaction needed is drawn a large amount of heat, this part heat all comes from the catalyst combustion reaction of the interior air of adjacent area and fuel gas.In order to ensure the high efficient heat exchanging between the endothermic reaction and exothermic reaction, the material that material in hydrogen making by natural gas reformation the first district F and adjacent resolution gas reclaim zone of transformation B and catalytic combustion transition region C adopts counter-current flow mode, ensure the fastest rate of heat transfer, avoided reacting in catalyticing combustion process the generation of focus.The required water of hydrogen making by natural gas reformation is entered by the raw water entrance d of hydrogen making by natural gas reformation device, the same counter-current flow mode that adopts of catalytic combustion tail gas of the raw water of lower temperature higher temperature in the second reaction zone D of reformer feed mixed zone E and air and fuel gas, between raw water and catalytic combustion tail gas, heat exchange fully also makes the temperature of the combustion tail gas after catalyst combustion reaction significantly decline, and has substantially reached the desired temperature of discharge.
The flow process of the hydrogen making by natural gas reformation technique that can recycle pressure-variable adsorption resolution gas of the present invention as shown in Figure 3, mainly comprises combustion of natural gas exothermic reaction logistics branch road, hydrogen making by natural gas reformation reaction logistics branch road, pressure-swing absorption apparatus resolution gas returned logistics branch road, temperature feedback controlled adjuster branch road, water returned logistics branch road and supplies user's hot water branch road.
Combustion of natural gas exothermic reaction logistics branch road: gas material storage tank 301 provides natural gas, after digester 302 desulfurization, be divided into two-way, wherein a road natural gas via is crossed temperature control adjusting valve 303 and flame arrester 304 and is entered in hydrogen making by natural gas reformation device 309 in fuel gas mixing buffering area A, air in while raw air storage tank 306 enters heat exchanger 307 and carries out preheating, enter in hydrogen making by natural gas reformation device 309 in fuel gas mixing buffering area A through flame arrester 308 afterwards, carry out oxidation reaction with natural gas, liberated heat is supplied with the gas renormalizing reaction in hydrogen making by natural gas reformation device 309.The interior combustion tail gas of hydrogen making by natural gas reformation device 309 enters heat exchanger 307 and carries out heat exchange with raw air, enter afterwards heat exchanger 310, the cold water providing with water tank 313 carries out secondary heat exchange, and combustion tail gas temperature is down to below 500C, enters afterwards after 311 points of water of water knockout drum emptying.Natural gas flame arrester 304 and air flame arrester 308 are set in combustion reaction raw material pipeline, prevent combustion mixture tempering, with the safety of safeguards system.
Hydrogen making by natural gas reformation reaction logistics branch road: gas material storage tank 301 provides natural gas, after digester 302 desulfurization, be divided into two-way, wherein a road natural gas straight taps in hydrogen making by natural gas reformation device 309 in reformer feed gas buffering area H, the raw water simultaneously being provided by water tank 313 directly enters in hydrogen making by natural gas reformation device 309 in the E of reformer feed mixed zone,, after heat exchange, preheating, carry out reforming reaction with natural gas and generate hydrogen-rich reformed gas in hydrogen making by natural gas reformation device 309 inside.Reformation tail gas enters water knockout drum 314 after the heat exchanger of hydrogen making by natural gas reformation device 309 inside and unstripped gas heat exchange, reformed gas after point water enters pressure-swing absorption apparatus 315, hydrogen is carried out to separating-purifying, and the high-purity hydrogen of separating stores or supplies with terminal use 316 and uses.
Pressure-swing absorption apparatus resolution gas returned logistics branch road: the resolution gas priority process temperature control adjusting valve 318 of pressure-swing absorption apparatus and flame arrester 319 enter in hydrogen making by natural gas reformation device 309 and react with air in fuel gas mixing buffering area A, and liberated heat is supplied with the reformation hydrogen production endothermic reaction in hydrogen making by natural gas reformation device 309.In the time of hydrogen generating system initial operating stage, the fuel of combustion reaction is taking natural gas as main, when after system stable operation, the reformed gas that in hydrogen making by natural gas reformation device 309, reformation hydrogen production reaction generates is after pressure-swing absorption apparatus 315 separating-purifyings, remaining resolution gas returns in fuel gas mixing buffering area A, and pressure-swing absorption apparatus resolution gas is all reclaimed.In ensureing that reformation hydrogen production reaction is carried out smoothly, the feed rate that regulates natural gas temperature control adjusting valve 303 and pressure-swing absorption apparatus resolution gas temperature control adjusting valve 318 to control natural gas and resolution gas by temperature feedback controlled adjuster 305 monitor temperatures and according to real time temperature distributes.Pressure-swing absorption apparatus resolution gas is changed into effective energy and for reformation hydrogen production reaction, take full advantage of the energy of pressure-swing absorption apparatus resolution gas, and then improved the energy efficiency of system hydrogen making by natural gas reformation device 309 is interior.On resolution gas returned logistics pipeline, resolution gas flame arrester 319 is set, prevents combustion mixture tempering, with the safety of safeguards system.
Temperature feedback controlled adjuster branch road: in the time of system stable operation, ensureing under the prerequisite that hydrogen making by natural gas reformation device 309 interior reforming reactions are carried out smoothly, regulate natural gas temperature control adjusting valve 303 and pressure-swing absorption apparatus resolution gas temperature control adjusting valve 318 by temperature feedback controlled adjuster 305 monitor temperatures and according to real time temperature, the feed rate of controlling natural gas and resolution gas distributes, and pressure-swing absorption apparatus 315 resolution gas are made full use of.The increasing of loading along with hydrogen making by natural gas reformation device 309, hydrogen output raises gradually, and the flow of pressure-swing absorption apparatus resolution gas strengthens gradually, and then the inlet amount of regulation and control combustion material natural gas continues to reduce, the input variable that is overall system energy reduces, and then has improved the energy efficiency of system.
Water returned logistics branch road: in hydrogen making by natural gas reformation device 309, combustion reaction tail gas enters water knockout drum 311 and divides water after heat exchanger 307 and heat exchanger 310 heat exchange, emptying afterwards.The cold water that in water knockout drum 311, separation obtains enters hydrotreater 317 and carries out purified treatment, and the water obtaining can loop back in water tank 313, has improved the utilization ratio of water in system.The cold water that in hydrogen making by natural gas reformation device 309, reformation hydrogen production reaction end gas obtains in water knockout drum 314 after point water simultaneously enters equally hydrotreater 317 and carries out purified treatment, the water obtaining can loop back in water tank 313, further improves the utilization ratio of water in system.
Supply user's hot water branch road: water tank 313 provides a road cold water after the abundant heat exchange of combustion reaction tail gas in heat exchanger 310 and hydrogen making by natural gas reformation device 309, and the hot water obtaining enters in hot water storage tank 312 and stores, and can provide domestic hot-water for user.
The hydrogen making by natural gas reformation device that can recycle pressure-variable adsorption resolution gas of the present invention and technique can with fuel cell system cooperation, electric energy and heat energy are provided, technological process as shown in Figure 4, mainly comprises combustion of natural gas exothermic reaction logistics branch road, hydrogen making by natural gas reformation reaction logistics branch road, pressure-swing absorption apparatus resolution gas returned logistics branch road, anode of fuel cell tail gas recycle logistics branch road, temperature feedback controlled adjuster branch road, water returned logistics branch road and supplies user's hot water branch road.
Combustion of natural gas exothermic reaction logistics branch road: gas material storage tank 401 provides natural gas, after digester 402 desulfurization, be divided into two-way, wherein a road natural gas via is crossed temperature control adjusting valve 403 and flame arrester 404 and is entered in hydrogen making by natural gas reformation device 409 in fuel gas mixing buffering area A, air in while raw air storage tank 406 enters heat exchanger 407 and carries out preheating, enter in hydrogen making by natural gas reformation device 409 in fuel gas mixing buffering area A through flame arrester 408 afterwards, carry out oxidation reaction with natural gas, liberated heat is supplied with the gas renormalizing reaction in hydrogen making by natural gas reformation device 309.The interior combustion tail gas of hydrogen making by natural gas reformation device 409 enters heat exchanger 407 and carries out heat exchange with raw air, enter afterwards heat exchanger 410, the cold water providing with water tank 413 carries out secondary heat exchange, and combustion tail gas temperature is down to below 50oC, enters afterwards after 411 points of water of water knockout drum emptying.Natural gas flame arrester 404 and air flame arrester 408 are set in combustion reaction raw material pipeline, prevent combustion mixture tempering, with the safety of safeguards system.
Hydrogen making by natural gas reformation reaction logistics branch road: provide natural gas in gas material storage tank 401, after digester 402 desulfurization, be divided into two-way, wherein a road natural gas straight taps in hydrogen making by natural gas reformation device 409 in reformer feed gas buffering area H, the raw water simultaneously being provided by water tank 413 directly enters in hydrogen making by natural gas reformation device 409 in the E of reformer feed mixed zone,, after heat exchange, preheating, carry out reforming reaction with natural gas and generate hydrogen-rich reformed gas in hydrogen making by natural gas reformation device 409 inside.Reformation tail gas enters water knockout drum 414 after the heat exchanger of hydrogen making by natural gas reformation device 409 inside and raw water heat exchange, reformed gas after point water enters pressure-swing absorption apparatus 415, hydrogen is carried out to separating-purifying, the high-purity hydrogen of separating offers fuel cell system 416, by fuel cell power generation and offer user use.
Pressure-swing absorption apparatus resolution gas returned logistics branch road: the resolution gas priority process temperature control adjusting valve 419 of pressure-swing absorption apparatus and flame arrester 420 enter in hydrogen making by natural gas reformation device 409 and react with air in fuel gas mixing buffering area A, and liberated heat is supplied with the reformation hydrogen production endothermic reaction occurring in hydrogen making by natural gas reformation device 409.In the time of hydrogen generating system initial operating stage, the fuel of combustion reaction is taking natural gas as main, when after system stable operation, the reformed gas that in hydrogen making by natural gas reformation device 409, reformation hydrogen production reaction produces is after pressure-swing absorption apparatus 415 separating-purifyings, remaining resolution gas returns in fuel gas mixing buffering area A, and pressure-swing absorption apparatus resolution gas is all reclaimed.In ensureing that reformation hydrogen production reaction is carried out smoothly, the feed rate that regulates natural gas temperature control adjusting valve 403 and pressure-swing absorption apparatus resolution gas temperature control adjusting valve 419 to control natural gas and resolution gas by temperature feedback controlled adjuster 405 monitor temperatures and according to real time temperature distributes.Pressure-swing absorption apparatus resolution gas is changed into effective energy and for reformation hydrogen production reaction, take full advantage of the energy of pressure-swing absorption apparatus resolution gas, and then improved the energy efficiency of system hydrogen making by natural gas reformation device 409 is interior.On resolution gas returned logistics pipeline, resolution gas flame arrester 420 is set, prevents combustion mixture tempering, with the safety of safeguards system.
Anode of fuel cell tail gas recycle logistics branch road: in anode of fuel cell tail gas, hydrogen content is about more than 20% and (depends on fuel-cell fuel utilance), recycles this part hydrogen the energy efficiency that is conducive to improve whole system.Anode of fuel cell tail gas priority process temperature control adjusting valve 421 and flame arrester 422 enter in hydrogen making by natural gas reformation device 409 and react with air in fuel gas mixing buffering area A, and liberated heat is supplied with the reformation hydrogen production endothermic reaction occurring in hydrogen making by natural gas reformation device 409.In ensureing that hydrogen making by natural gas reformation device 409 interior reforming reactions are carried out smoothly, the feed rate that regulates natural gas temperature control adjusting valve 403 and anode of fuel cell tail gas temperature control adjusting valve 421 to control natural gas and anode of fuel cell tail gas by temperature feedback controlled adjuster 405 monitor temperatures and according to real time temperature distributes.Along with the increasing that hydrogen making by natural gas reformation device 409 is loaded, hydrogen output raises gradually, and the amounts of hydrogen of feed fuels battery increases gradually, and anode of fuel cell exhaust flow strengthens gradually, and then the inlet amount of regulation and control combustion material natural gas continues to reduce.In hydrogen making by natural gas reformation device, 409 change into effective energy by anode of fuel cell tail gas and for reformation hydrogen production reaction, take full advantage of the energy of anode of fuel cell tail gas, and then improved the energy efficiency of system.On anode of fuel cell tail gas recycle logistics pipeline, anode exhaust gas flame arrester 422 is set, prevents combustion mixture tempering, with the safety of safeguards system.
Temperature feedback controlled adjuster branch road: in the time of system stable operation, ensureing under the prerequisite that hydrogen making by natural gas reformation device 409 interior reforming reactions are carried out smoothly, regulate natural gas temperature control adjusting valve 403, pressure-swing absorption apparatus resolution gas temperature control adjusting valve 419 and anode of fuel cell tail gas temperature control adjusting valve 421 by temperature feedback controlled adjuster 405 monitor temperatures and according to real time temperature, the feed rate of controlling natural gas, resolution gas and anode exhaust gas distributes, and pressure-swing absorption apparatus resolution gas and anode exhaust gas are made full use of.The increasing of loading along with hydrogen making by natural gas reformation device 409, hydrogen output raises gradually, the flow of pressure-swing absorption apparatus resolution gas strengthens gradually, anode of fuel cell tail gas hydrogen content raises gradually, the inlet amount of regulation and control combustion material natural gas continues to reduce, the input variable that is overall system energy reduces, and then has improved the energy efficiency of system.
Water returned logistics branch road: in hydrogen making by natural gas reformation device 409, combustion reaction tail gas enters water knockout drum 411 and divides water after heat exchanger 407 and heat exchanger 410 heat exchange, emptying afterwards.The cold water that in water knockout drum 411, separation obtains enters hydrotreater 418 and carries out purified treatment, and the water obtaining can loop back in water tank 413, has improved the utilization ratio of water in system.In hydrogen making by natural gas reformation device 409, reformation hydrogen production reaction end gas is through water knockout drum 414, and the cold water obtaining after point water enters hydrotreater 418 and carries out purified treatment, and the water obtaining can loop back in water tank 413, has improved the utilization ratio of water in system.Fuel battery negative pole tail gas enters in water knockout drum 417 cold water obtaining after point water and enters equally hydrotreater 418 and carry out purified treatment, and the water obtaining can loop back in water tank 413, further improves the utilization ratio of water in system.Air in fuel battery negative pole tail gas can reclaim to compress and add in raw air storage tank 406 simultaneously.
Supply user's hot water branch road: water tank 413 provides a road cold water after the abundant heat exchange of combustion reaction tail gas in heat exchanger 410 and hydrogen making by natural gas reformation device 409, and the hot water obtaining enters in hot water storage tank 412 and stores, and can provide domestic hot-water for user.
More than show and described general principle of the present invention and principal character and advantage of the present invention.The technical staff of the industry should understand; the present invention is not restricted to the described embodiments; that in above-described embodiment and specification, describes just illustrates principle of the present invention; without departing from the spirit and scope of the present invention; the present invention also has various changes and modifications, and these changes and improvements all fall in the claimed scope of the invention.The claimed scope of the present invention is defined by appending claims and equivalent thereof.
Claims (24)
1. can recycle a reforming hydrogen production device for pressure-variable adsorption resolution gas, the central area of described device comprises that fuel gas mixing buffering area (A), resolution gas reclaim zone of transformation (B), catalytic combustion transition region (C) successively; The outside of the central area of described device is followed successively by second reaction zone (D), reformer feed mixed zone (E), reformation hydrogen production Second Region (G) of reformation hydrogen production the firstth district (F), air and fuel gas; The bottom of described device is provided with hydrogen feedstock buffering area (H); Wherein said fuel gas mixing buffering area (A) is provided with fuel gas entrance (a) and air intake (b), the second reaction zone (D) that fuel gas and air reclaim zone of transformation (B), catalytic combustion transition region (C), air and fuel gas by fuel gas mixing buffering area (A), resolution gas after mixing successively, reacted combustion tail gas is discharged by combustion tail gas outlet (c); Hydrogen feedstock buffering area (H) is provided with hydrogen feedstock entrance (f) and hydrogen feedstock diversion cavity (107), wherein hydrogen feedstock diversion cavity (107) stretches in reformer feed mixed zone (E), the raw water that hydrogen feedstock enters at reformer feed mixed zone (E) and raw water entrance (d) by hydrogen feedstock diversion cavity (107) after hydrogen feedstock buffering area (H) mixes, enter successively again reformation hydrogen production the firstth district (F) and reformation hydrogen production Second Region (G), after heat exchanger (106) heat exchange, discharged by product gas outlet (e); Product gas outlet (e) is connected with pressure-swing absorption apparatus; Pressure-swing absorption apparatus connects fuel gas entrance (a) by resolution gas recovery channel; Described resolution gas reclaims the interior filling in second reaction zone (D) combustion catalyst of zone of transformation (B), fuel gas; Described catalytic combustion transition region (C) is loaded the heat-storing material of large thermal capacitance.
2. device according to claim 1, is characterized in that, described reformation hydrogen production Second Region (G) is connected with product gas outlet (e) by the heat exchanger (106) being arranged in hydrogen feedstock buffering area (H).
3. device according to claim 2, is characterized in that, described in the heat exchanger (106) that is arranged in hydrogen feedstock buffering area (H) be S shape or spiral helicine pipeline.
4. device according to claim 1, is characterized in that, described hydrogen feedstock diversion cavity (107) is provided with and is down " protruding " shape hydrogen feedstock discharge end, and the bottom surface of this hydrogen feedstock discharge end and side face region are provided with hydrogen feedstock discharge orifice.
5. device according to claim 1, is characterized in that, described combustion catalyst is palladium system, platinum group or their alloy catalyst.
6. device according to claim 1, is characterized in that, fuel gas entrance and air intake place are provided with gas distributor.
7. device according to claim 1, is characterized in that, is provided with fuel gas redistributor (105) in fuel gas mixing buffering area (A).
8. device according to claim 1, is characterized in that, between product gas outlet (e) and pressure-swing absorption apparatus, water knockout drum is set.
9. device according to claim 1, is characterized in that, hydrogen feedstock is hydrogen-containing compound or the mixture of alcohols or hydro carbons.
10. device according to claim 1, is characterized in that, hydrogen feedstock is natural gas, methyl alcohol or ethanol.
11. devices according to claim 1, is characterized in that, also comprise water circulation system, and described water circulation system comprises water knockout drum, hydrotreater, cyclic water tank successively, and cyclic water tank connects raw water entrance (d).
12. devices according to claim 11, is characterized in that, described combustion tail gas outlet (c) is connected with heat exchanger, and heat exchanger connects water knockout drum.
13. devices according to claim 12, is characterized in that, it is front through heat exchanger preheating that air enters air intake (b).
14. devices according to claim 1, is characterized in that, described fuel gas is natural gas, coal gas, or the gaseous mixture of the pressure-variable adsorption resolution gas of natural gas or coal gas and recovery.
15. devices according to claim 1, is characterized in that, gas material storage-tank pipeline connects natural gas via desulfurizer, and then pipeline is divided into two-way, and wherein a road connects fuel gas entrance (a); Another road natural gas straight connects hydrogen feedstock entrance (f) in succession.
16. devices according to claim 1, is characterized in that, pressure-swing absorption apparatus connecting fuel battery system, and the tail gas that anode of fuel cell produces is carried and is connected fuel gas entrance (a) through pipeline.
17. according to the device described in claim 1 or 15 or 16, it is characterized in that, on the pipeline of connection fuel gas entrance (a), is equipped with temperature control adjusting valve and flame arrester; Regulate temperature control adjusting valve by temperature feedback controlled adjuster.
The process for making hydrogen of reforming hydrogen production device described in 18. 1 kinds of claims 1, fuel gas is after mix fuel gas mixing buffering area (A), in resolution gas reclaims the second reaction zone (D) of zone of transformation (B), catalytic combustion transition region (C), air and fuel gas and air generation catalyst combustion reaction, and for reformation hydrogen production reaction provides heat, combustion tail gas is discharged through combustion tail gas outlet (c); Hydrogen feedstock enters hydrogen feedstock buffering area (H) through hydrogen feedstock entrance (f), after heat exchange, enter hydrogen feedstock diversion cavity (107), the raw water entering at reformer feed mixed zone (E) and raw water entrance (d) mixes, after heat exchange, preheating, in reformation hydrogen production the firstth district (F), reformation hydrogen production Second Region (G) carry out reforming reaction and generate hydrogen-rich reformate gas, reformate gas enters pressure-swing absorption apparatus, and hydrogen is carried out to separating-purifying; After pressure-swing absorption apparatus separating-purifying, remaining resolution gas reclaims by resolution gas recovery channel, and as combustible gas input fuel gas entrance.
19. techniques according to claim 18, is characterized in that, in the time of reformation hydrogen production initial operating stage, fuel gas is natural gas; When after reformation hydrogen production stable operation, after pressure-swing absorption apparatus separating-purifying, remaining resolution gas reclaims by resolution gas recovery channel, and as combustible gas input fuel gas entrance (a).
20. techniques according to claim 19, is characterized in that, gas material storage tank provides natural gas, after desulfurizer desulfurization, be divided into two-way, wherein a road natural gas enters fuel gas entrance (a), and another road natural gas straight connects unstripped gas entrance (f) in succession.
21. techniques according to claim 20, is characterized in that, the high-purity hydrogen of separating offers fuel cell system, and the tail gas that anode of fuel cell produces returns to fuel gas entrance (a) as fuel gas utilization.
22. according to the technique described in claim 19-21 any one, it is characterized in that, on the pipeline of connection fuel gas entrance (a), is equipped with temperature control adjusting valve and flame arrester; Regulate temperature control adjusting valve by temperature feedback controlled adjuster, realize the real-time matching of natural gas, resolution gas and anode of fuel cell tail gas feed rate, ensure the stable operation of reformation hydrogen production reaction.
23. techniques according to claim 22, it is characterized in that, the reformate gas of preparation is discharged by product gas outlet (e), enter the gas product water knockout drum that product gas outlet (e) is connected with pressure-swing absorption apparatus, after hydrotreater purified treatment, be delivered to cyclic water tank as raw water at the water obtaining in gas product water knockout drum.
24. techniques according to claim 22, it is characterized in that, the combustion tail gas of combustion tail gas outlet (c) enters fraction water device water-dividing after heat exchanger, and the water producing in combustion process is discharged by water knockout drum bottom, enters hydrotreater and processes rear direct circulation recovery tank; Fuel battery negative pole tail gas enters point water in cathode exhaust gas water knockout drum and be delivered to cyclic water tank as raw water after hydrotreater carries out purified treatment.
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Effective date of registration: 20160621 Address after: Linjiang Industrial Zone, Linjiang New District, Haimen, Jiangsu Patentee after: Nantong Zhengta Gas Co.,Ltd. Address before: 100022, D, block SOHO, 2608, Jianguo Road, 88, Beijing, Chaoyang District Patentee before: BEIJING ZTAIR GROUP LTD. |