CN104134811B - A kind of reforming hydrogen production device and technique can recycling pressure-variable adsorption resolution gas - Google Patents
A kind of reforming hydrogen production device and technique can recycling pressure-variable adsorption resolution gas Download PDFInfo
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- 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
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Abstract
The present invention relates to reforming hydrogen production device and the technique of recoverable pressure-variable adsorption resolution gas, multiple zoness of different such as the second reaction zone of fuel gas mixing buffering area, resolution gas recovery zone of transformation, catalytic combustion transition region, air and fuel gas, reformer feed mixed zone, hydrogen making by natural gas reformation district and reformer feed gas buffering area integrate by this device for producing hydrogen; The raw material that reformation hydrogen production needs at room temperature can directly enter hydrogen making by natural gas reformation device; The recovery of hydrogen making by natural gas reformation and pressure-variable adsorption resolution gas and trans-utilization all complete in hydrogen making by natural gas reformation device inside.This process for making hydrogen enhances water route management, and H2 concentration can be provided to reach the gas product of more than 99.9%; This process for making hydrogen can be fuel cell with hydrogen gas, simultaneously and fuel cell system combine for customer power supply, heat supply; The raw material of this process for making hydrogen not only can adopt natural gas, also can adopt the alcohols such as methyl alcohol, ethanol and hydro carbons hydrogen-containing compound.
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 emphasis and promote hydrogen making by natural gas reformation device integrated level, strengthening thermal management and water route management, the hydrogen making by natural gas reformation device can recycling pressure-variable adsorption resolution gas improving total system energy efficiency and technique.
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 realizing Chinese society sustainable economic development.For the energy resource structure that China's many coals weak breath is oil-poor, the energy development strategic requirement in China future improves energy efficiency, cleanly uses fossil energy, readjusts the energy structure, increases alternative energy source, realize the sustainable development of the energy.Hydrogen Energy does not produce any disposal of pollutants when utilizing, and is the ideal chose of following clean energy resource carrier, plays main flow effect by likely smoothly transitting to final dependence in the sustainable end-around carry of fossil energy at human society by fossil energy.
Hydrogen is the abundantest element, but natural hydrogen exists few, must consume after hydrogenous material decomposes by a large amount of energy and just can obtain hydrogen, therefore find 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 secondly exactly various fossil fuel (coal, oil, natural gas) and various biomass etc.The production of hydrogen, purify, transport and store and all need corresponding capital construction, need a large amount of investments, relate to multiple link, and all to there are some bottleneck problem needs in technological difficulties, economy and fail safe etc. that links relates to go to improve and 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, usually natural gas is processed as initial feed, conversion of natural gas is become CO and H
2(i.e. synthesis gas), this is also an ideal hydrogen producing technology route.
Pressure-variable adsorption (PressureSwingAdsorption, PSA) gas separaion and purification technique developed rapidly in the sixties in last century, had become a kind of production technology and the independently unit process of chemical engineering industry at present.Because PSA Gas Separation Technology relies on the change of pressure to realize absorption and regeneration, thus reproduction speed is fast, energy consumption is low, belongs to energy-saving gas separation.Further, this technical process is simple, stable operation, impurity once can be removed obtain high purity product for the gaseous mixture containing plurality of impurities, and 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 for the purpose of system energy efficiency, provides a kind of hydrogen production reaction technique of improvement, comprises hydrogen making by natural gas reformation device, water knockout drum, pressure-swing absorption apparatus and pressure-variable adsorption resolution gas and reclaims converter etc.Adopt catalytic combustion technology all to be reclaimed by the fuel gas in resolution gas and change into efficient heat and be supplied to natural gas hydrogen preparation reaction, finally reaching the object improving system energy efficiency.
Distributed heat chp system (CombinedHeatandPower, CHP) has that energy cascade utilization efficiency is high, electric power supply is reliable, good in economic efficiency, advantages of environment protection; Supplementing as the organic of traditional energy system, is that the severe challenge that production and supply that is electric and heat faces is significant to alleviating China's terminal energy sources.Along with the continuous progress of Hydrogen Energy and fuel cell technology, the cogeneration system based on fuel cell technology becomes the new important development direction of distributed heat CCHP just gradually.
Proton Exchange Membrane Fuel Cells (PEMFC) take hydrogen as fuel, by the electrode reaction between the hydrogen of anode and the oxygen of negative electrode, chemical energy is converted into electric energy, has the advantages such as energy conversion efficiency is high, structure is simple, environmental pollution is little.Adopt fossil feedstock reforming hydrogen producing technology and proton exchange film fuel battery system associating, be widely applied in fixed or Mobile fuel battery power supply system or fuel cell cogeneration system.But the anode impact of CO residual in the rich reformed gas that provides of fossil feedstock reforming hydrogen producing technology on PEMFC is very large, usually requires that CO concentration is at below 30ppm.
For CO residual in hydrogen-rich reformed gas, traditional method adopts 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 etc. such as reactor design, design of heat exchanger and thermal management, simultaneously very high to CO catalyst for selective oxidation performance requirement, especially to catalyst at CO and H
2between competitive reaction selectivity require very high, also will be strict with the long-time stability (3000-10000h) of catalyst, the noble metal such as Pt, Pd is comparatively effective as catalyst activity component in addition, but there is the problem of Financial cost aspect simultaneously.
Patent documentation (CN101054160A, US6793698B1, EP1094031A1) discloses a kind of reforming hydrogen-preparation reactor, but structure is simple, and 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 realize stable the carrying out of two kinds of different chemicals reactions.
Natural gas hydrogen production plant provided by the invention and technique adopt pressure-swing absorption apparatus to substitute CO shift-converter and CO purification reactor, directly separating-purifying is carried out to hydrogen-rich reformed tail gas, eliminate CO relative to employing chemical reaction method, adopt pressure-swing absorption apparatus technique directly to purify H
2, have that energy consumption is low, flow process be simple, H
2the advantages such as purity is high, device operating flexibility is large and environmental benefit is good.Can be the H that fuel cell system provides 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 reducing system, improve the energy efficiency of 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 hydrogen making by natural gas reformation device and the technique of pressure-variable adsorption resolution gas is recycled, first reforming hydrogen production device is passed through, by hydrocarbon (hydro carbons, alcohol compound, particularly natural gas etc.) be converted into hydrogen-rich gas, adopt pressure-swing absorption apparatus separating-purifying to obtain the hydrogen of high-quality afterwards.The high-quality hydrogen produced can store or supply user and use, and also can be used for and generates electricity to fuel cell 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 fuel gas mixing buffering area (A) successively, resolution gas reclaims zone of transformation (B), catalytic combustion transition region (C); The outside of the central area of described device is followed successively by reformation hydrogen production first district (F), the second reaction zone (D) of air and fuel gas, reformer feed mixed zone (E), reformation hydrogen production second district (G); 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), reclaimed the second reaction zone (D) of zone of transformation (B), catalytic combustion transition region (C), air and fuel gas after fuel gas and air mix successively by fuel gas mixing buffering area (A), resolution gas, reacted combustion tail gas exports (c) by combustion tail gas and discharges; 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 is entered at reformer feed mixed zone (E) and feed water inlet (d) by hydrogen feedstock diversion cavity (107) after hydrogen feedstock buffering area (H) mixes, enter reformation hydrogen production first district (F) and reformation hydrogen production second district (G) more successively, 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) loads the heat-storing material of large thermal capacitance.
Reformer feed is natural gas, also can be methyl alcohol or ethanol, and reformer feed is that the hydrogen-containing compound of alcohols or hydro carbons or mixture can realize the present invention.Described reformation hydrogen production second district (G) is connected with product gas outlet (e) by the heat exchanger (106) be arranged in hydrogen feedstock buffering area (H).The described pipeline be arranged in hydrogen feedstock buffering area (H) is S shape or helical form.Described hydrogen feedstock diversion cavity (107) is provided with in falling " convex " shape hydrogen feedstock discharge end, and bottom surface and the side face region of this hydrogen feedstock discharge end 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.Fuel gas redistributor (105) is provided with in fuel gas mixing buffering area (A).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 drum, 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 connects fuel gas entrance (a) through Cemented filling.The pipeline of connection fuel gas entrance (a) is equipped with temperature control adjusting valve and flame arrester; Temperature control adjusting valve is regulated by temperature feedback control adjuster.
The process for making hydrogen of reforming hydrogen production device described in a kind of claim 1, fuel gas is after the mixing of fuel gas mixing buffering area (A), with air generation catalyst combustion reaction in the second reaction zone (D) that resolution gas reclaims zone of transformation (B), catalytic combustion transition region (C), air and fuel gas, and providing heat for reformation hydrogen production reaction, combustion tail gas is discharged through combustion tail gas outlet (c); Hydrogen feedstock enters hydrogen feedstock buffering area (H) through hydrogen feedstock entrance (f), hydrogen feedstock diversion cavity (107) is entered after heat exchange, in the raw water mixing that reformer feed mixed zone (E) and feed water inlet (d) enter, after heat exchange, preheating, in reformation hydrogen production first district (F), reformation hydrogen production second district (G) carries out reforming reaction and generates hydrogen-rich reformate gas, reformate gas enters pressure-swing absorption apparatus, carries out separating-purifying to hydrogen; After pressure-swing absorption apparatus separating-purifying, remaining resolution gas is reclaimed by resolution gas recovery channel, and as combustible gas input fuel gas entrance.
When 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 is reclaimed 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 separated is supplied to fuel cell system, and the tail gas that anode of fuel cell produces returns fuel gas entrance (a) and utilizes as fuel gas.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 control 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 obtained 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 produced in combustion process is discharged by bottom water knockout drum, enters direct circulation recovery tank after hydrotreater process; Fuel battery negative pole tail gas enters point water in cathode exhaust gas water knockout drum to carry out being delivered to cyclic water tank as raw water after purified treatment through hydrotreater.Fuel gas and mixed reformer feed reverse flow, ensure that 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, and pressure-variable adsorption resolution gas can have been recycled again, and used it for reformation hydrogen production process; The water generated in partial conversion hydrogen feedstock water and pressure-variable adsorption resolution gas recycling process can cycling and reutilization, has effectively saved water resources; At this reforming hydrogen production device inside and recoverable pressure-variable adsorption resolution gas, simplify Hydrogen making technological process, improve hydrogen production efficiency.
Reforming hydrogen production device and the technique can recycling pressure-variable adsorption resolution gas provided by the invention, adopt catalytic combustion technology when recycling pressure-variable adsorption resolution gas, compared with directly burning, catalytic combustion temperature is lower, ratio of combustion is comparatively complete, extremely friendly to environment.
The reforming hydrogen production device can recycling pressure-variable adsorption resolution gas provided by the invention, in order to improve hydrogen production efficiency, fuel gas mixing buffering area A is integrated with in this reforming hydrogen production device inside, 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 first district F, multiple main region such as reformation hydrogen production second district 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 septate heat transfer 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 can recycling pressure-variable adsorption resolution gas provided by the invention, by arranging fuel gas mixing buffering area A 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 had an impact, thus the stable operation of assurance device.After fuel gas mixing, fuel gas redistributor 105 is set, can ensures that fuel gas and air fully mix and evenly enter resolution gas and reclaim zone of transformation B, avoid the appearance of burning focus well.Because the combustion rate in resolution gas recovery zone of transformation B and the reformation hydrogen production reaction rate in adjacent hydrogen making by natural gas reformation first district F differ larger, therefore at catalytic combustion transition region C, the heat-storing material that a large amount of thermal capacitance is larger is set, in order to the difference of balance combustion reaction rate and reformation hydrogen production reaction rate, thus ensure stable the carrying out of two kinds of different chemicals reactions.
The reforming hydrogen producing process can recycling pressure-variable adsorption resolution gas provided by the invention, by pressure-swing absorption apparatus, separating-purifying is carried out to reformation gas product, the hydrogen of purity more than 99.9% can be provided for user, pressure-swing absorption apparatus resolution gas all can be reclaimed and is converted into effective energy simultaneously and act on reforming hydrogen production device, substantially increase the energy efficiency of system.
The reforming hydrogen producing process can recycling 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 improves the energy efficiency of system.
The reforming hydrogen producing process can recycling pressure-variable adsorption resolution gas provided by the invention, natural gas not only can be adopted to be hydrogen feedstock, also can extensively to adopt the hydrogen-containing compound of the multiple alcohols such as methyl alcohol, ethanol, town gas, liquefied gas and hydro carbons as hydrogen feedstock.
Accompanying drawing explanation
Fig. 1 is hydrogen making by natural gas reformation device and the Internal Experiment flow chart that can recycle pressure-variable adsorption resolution gas;
Fig. 2 is the cut-away view of the hydrogen making by natural gas reformation device can recycling pressure-variable adsorption resolution gas;
Fig. 3 is the flow chart of the hydrogen making by natural gas reformation technique can recycling pressure-variable adsorption resolution gas;
Fig. 4 is the flow chart can recycling the hydrogen making by natural gas reformation technique of pressure-variable adsorption resolution gas of combining with fuel cell system.
Embodiment
Be hydrogen feedstock with natural gas, the present invention is further described.
Hydrogen making by natural gas reformation device (Fig. 1), mainly include fuel gas mixing buffering area A, second reaction zone D, reformer feed mixed zone E that resolution gas reclaims zone of transformation B, catalytic combustion transition region C, air and fuel gas, multiple main functional areas such as hydrogen making by natural gas reformation first district F, hydrogen making by natural gas reformation second district G and reformer feed gas buffering area H.First a certain amount of pressure-variable adsorption resolution gas that need recycle and air is passed into respectively by the heat supply entrance a of hydrogen making by natural gas reformation device and air intake b, reclaimed the second reaction zone D of zone of transformation B, catalytic combustion transition region C, air and fuel gas after both mixing successively by fuel gas mixing buffering area A, resolution gas, combustion tail gas exports c by combustion tail gas and discharges system.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, after reformer feed gas buffering area H reformer feed mixed zone E and entered by the feed water inlet d of hydrogen making by natural gas reformation device hydrogen making by natural gas reformation needed raw material water mixing, enter hydrogen making by natural gas reformation first district F and hydrogen making by natural gas reformation second district G more successively, produce reformate gas by the chemical reaction process of hydrogen making by natural gas reformation, finally discharge 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 have employed flow process as described below (Fig. 2) when stable operation, first the pressure-variable adsorption resolution gas of a certain amount of recovery is passed into 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, the mixed zone A of air and fuel gas is entered again by air sparger 103, in the mixed zone A of air and fuel gas, air and fuel gas fully mix, and the conversion zone of air and fuel gas is entered through fuel gas redistributor 105, be that resolution gas reclaims zone of transformation B in the first half of this conversion zone, reclaim in zone of transformation B at resolution gas and be filled with catalyst air and fuel gas generation chemical reaction being 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, catalyst combustion reaction is carried out under pressurized conditions, release a large amount of heat simultaneously.Reacted high-temperature gas directly enters the latter half and the catalytic combustion transition region C of the conversion zone of air and fuel gas, at the heat-storing material that this position filling thermal capacitance is larger.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 built with combustion catalyst, it is identical with the catalyst that resolution gas reclaims in zone of transformation B, ensure that air and fuel gas are by after the second reaction zone D of air and fuel gas, fuel gas is all converted into carbon dioxide and water, and exports c discharge system by combustion tail gas.
Water needed for hydrogen making by natural gas reformation is entered by the feed water inlet d of hydrogen making by natural gas reformation device, first raw water enters reformer feed mixed zone E by after liquid distributor 108 uniform distribution, natural gas simultaneously needed for 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, heat exchange is carried out at this and the reformation hydrogen production gas product flowing through hydrogen making by natural gas reformation device internal exchanger 106, natural gas after preheating is evenly sprayed by unstripped gas mozzle 107 and enters reformer feed mixed zone E, near unstripped gas mozzle 107 in the E of reformer feed mixed zone exports, natural gas and water can acutely mix, mixed natural gas and water flow from the middle part lower portion of reformer feed mixed zone E, and finally enter hydrogen making by natural gas reformation first district F, hydrogen making by natural gas reformation catalyst is filled with in this region, under the catalytic action of catalyst, natural gas and water generate rich hydrogen production gas by reaction, rich hydrogen production gas enters hydrogen making by natural gas reformation second district G, in this region, reformer feed can be converted into hydrogen-rich mixed gas completely, and flowed out by the product gas outlet e of hydrogen making by natural gas reformation device after carrying out 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, when stable operation, achieves the Proper Match of energy well between inner different logistics.First the reformer feed gas 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 meets the demand of subsequent processing, meanwhile, unstripped gas can be preheating to higher temperature, and mix with raw water near unstripped gas mozzle 107 exports, directly partial heat is passed to raw water efficiently.After unstripped gas and raw water are mixed into hydrogen making by natural gas reformation first district F, hydrogen making by natural gas reformation reaction is carried out under effect at catalyst at this region unstripped gas and raw water, because this reaction needed draws a large amount of heat, this partial heat all comes from the catalyst combustion reaction of air and fuel gas in adjacent area.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 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, avoid in catalyticing combustion process the generation of reacting focus.Water needed for hydrogen making by natural gas reformation is entered by the feed water inlet d of hydrogen making by natural gas reformation device, the 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 is same adopts counter-current flow mode, the temperature of the combustion tail gas after sufficient heat exchange also makes catalyst combustion reaction between raw water and catalytic combustion tail gas significantly declines, and substantially reaches the temperature required by discharge.
The flow process can recycling the hydrogen making by natural gas reformation technique of 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 control adjuster branch road, Water Sproading logistics branch road and for 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 to be entered in hydrogen making by natural gas reformation device 309 in fuel gas mixing buffering area A, air simultaneously in raw air storage tank 306 enters heat exchanger 307 and carries out preheating, to enter in hydrogen making by natural gas reformation device 309 in fuel gas mixing buffering area A through flame arrester 308 afterwards, oxidation reaction is carried out with natural gas, gas renormalizing reaction in liberated heat supply hydrogen making by natural gas reformation device 309.Hydrogen making by natural gas reformation device 309 combustion tail gas enters heat exchanger 307 and carries out heat exchange with raw air, enter heat exchanger 310 afterwards, the cold water provided with water tank 313 carries out secondary heat exchange, makes combustion tail gas temperature be down to below 500C, emptying after entering water knockout drum 311 points of water afterwards.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 to tap in hydrogen making by natural gas reformation device 309 in reformer feed gas buffering area H, the raw water simultaneously provided by water tank 313 directly to enter in hydrogen making by natural gas reformation device 309 in the E of reformer feed mixed zone, in hydrogen making by natural gas reformation device 309 inside after heat exchange, preheating, carry out reforming reaction with natural gas and generate hydrogen-rich reformed gas.Reformation tail gas enters water knockout drum 314 after the heat exchanger and unstripped gas heat exchange of hydrogen making by natural gas reformation device 309 inside, reformed gas after point water enters pressure-swing absorption apparatus 315, carry out separating-purifying to hydrogen, the high-purity hydrogen separated stores or supplies terminal use 316 and uses.
Pressure-swing absorption apparatus resolution gas returned logistics branch road: the resolution gas of pressure-swing absorption apparatus successively enters in hydrogen making by natural gas reformation device 309 through temperature control adjusting valve 318 and flame arrester 319 and reacts with air in fuel gas mixing buffering area A, the reformation hydrogen production endothermic reaction in liberated heat supply hydrogen making by natural gas reformation device 309.When hydrogen generating system initial operating stage, the fuel of combustion reaction is based on natural gas, 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-purifying, remaining resolution gas returns in fuel gas mixing buffering area A, is all reclaimed by pressure-swing absorption apparatus resolution gas.While the reaction of guarantee reformation hydrogen production is carried out smoothly, to be distributed according to the feed rate that real time temperature 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 control adjuster 305 monitor temperature.In hydrogen making by natural gas reformation device 309, pressure-swing absorption apparatus resolution gas changed into effective energy and be used for reformation hydrogen production reaction, taking full advantage of the energy of pressure-swing absorption apparatus resolution gas, and then improve the energy efficiency of system.Resolution gas returned logistics pipeline arranges resolution gas flame arrester 319, prevents combustion mixture tempering, with the safety of safeguards system.
Temperature feedback control adjuster branch road: when system stable operation, under the prerequisite that reforming reaction is carried out smoothly in guarantee hydrogen making by natural gas reformation device 309, by temperature feedback control adjuster 305 monitor temperature and according to real time temperature adjustment natural gas temperature control adjusting valve 303 and pressure-swing absorption apparatus resolution gas temperature control adjusting valve 318, the feed rate controlling natural gas and resolution gas distributes, and is made full use of by pressure-swing absorption apparatus 315 resolution gas.Along with the increasing of hydrogen making by natural gas reformation device 309 load, 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, namely the input variable of overall system energy reduces, and then improves the energy efficiency of system.
Water Sproading logistics branch road: in hydrogen making by natural gas reformation device 309, combustion reaction tail gas enters water knockout drum 311 and carries out a point water after heat exchanger 307 and heat exchanger 310 heat exchange, emptying afterwards.Be separated the cold water obtained in water knockout drum 311 to enter hydrotreater 317 and carry out purified treatment, the water obtained can loop back in water tank 313, improves 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 hydrotreater 317 equally and carries out purified treatment, the water obtained can loop back in water tank 313, the utilization ratio of water in further raising system.
For 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 with hydrogen making by natural gas reformation device 309, and the hot water obtained enters in hot water storage tank 312 and stores, and can provide domestic hot-water for user.
Of the present invention can recycle pressure-variable adsorption resolution gas hydrogen making by natural gas reformation device 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 control adjuster branch road, Water Sproading 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 to be entered in hydrogen making by natural gas reformation device 409 in fuel gas mixing buffering area A, air simultaneously in raw air storage tank 406 enters heat exchanger 407 and carries out preheating, to enter in hydrogen making by natural gas reformation device 409 in fuel gas mixing buffering area A through flame arrester 408 afterwards, oxidation reaction is carried out with natural gas, gas renormalizing reaction in liberated heat supply hydrogen making by natural gas reformation device 309.Hydrogen making by natural gas reformation device 409 combustion tail gas enters heat exchanger 407 and carries out heat exchange with raw air, enter heat exchanger 410 afterwards, the cold water provided with water tank 413 carries out secondary heat exchange, makes combustion tail gas temperature be down to below 50oC, emptying after entering water knockout drum 411 points of water afterwards.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 to tap in hydrogen making by natural gas reformation device 409 in reformer feed gas buffering area H, the raw water simultaneously provided by water tank 413 directly to enter in hydrogen making by natural gas reformation device 409 in the E of reformer feed mixed zone, in hydrogen making by natural gas reformation device 409 inside after heat exchange, preheating, carry out reforming reaction with natural gas and generate hydrogen-rich reformed gas.Reformation tail gas enters water knockout drum 414 after the heat exchanger and raw water heat exchange of hydrogen making by natural gas reformation device 409 inside, reformed gas after point water enters pressure-swing absorption apparatus 415, separating-purifying is carried out to hydrogen, the high-purity hydrogen separated is supplied to fuel cell system 416, by fuel cell power generation and be supplied to user use.
Pressure-swing absorption apparatus resolution gas returned logistics branch road: the resolution gas of pressure-swing absorption apparatus successively enters in hydrogen making by natural gas reformation device 409 through temperature control adjusting valve 419 and flame arrester 420 and reacts with air in fuel gas mixing buffering area A, the reformation hydrogen production endothermic reaction occurred in liberated heat supply hydrogen making by natural gas reformation device 409.When hydrogen generating system initial operating stage, the fuel of combustion reaction is based on natural gas, 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-purifying, remaining resolution gas returns in fuel gas mixing buffering area A, is all reclaimed by pressure-swing absorption apparatus resolution gas.While the reaction of guarantee reformation hydrogen production is carried out smoothly, to be distributed according to the feed rate that real time temperature 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 control adjuster 405 monitor temperature.In hydrogen making by natural gas reformation device 409, pressure-swing absorption apparatus resolution gas changed into effective energy and be used for reformation hydrogen production reaction, taking full advantage of the energy of pressure-swing absorption apparatus resolution gas, and then improve the energy efficiency of system.Resolution gas returned logistics pipeline arranges resolution gas flame arrester 420, 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 was about for more than 20% (depending on fuel-cell fuel utilance), recycles the energy efficiency being conducive to improving whole system by this part hydrogen.Anode of fuel cell tail gas successively enters in hydrogen making by natural gas reformation device 409 through temperature control adjusting valve 421 and flame arrester 422 and reacts with air in fuel gas mixing buffering area A, the reformation hydrogen production endothermic reaction occurred in liberated heat supply hydrogen making by natural gas reformation device 409.While in guarantee hydrogen making by natural gas reformation device 409, reforming reaction is carried out smoothly, to be distributed according to the feed rate that real time temperature 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 control adjuster 405 monitor temperature.Along with the increasing of hydrogen making by natural gas reformation device 409 load, hydrogen output raises gradually, and the amounts of hydrogen of supply fuel cell 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, anode of fuel cell tail gas is changed into effective energy and is used for reformation hydrogen production reaction by 409, takes full advantage of the energy of anode of fuel cell tail gas, and then improves the energy efficiency of system.Anode of fuel cell tail gas recycle logistics pipeline arranges anode exhaust gas flame arrester 422, prevents combustion mixture tempering, with the safety of safeguards system.
Temperature feedback control adjuster branch road: when system stable operation, under the prerequisite that reforming reaction is carried out smoothly in guarantee hydrogen making by natural gas reformation device 409, by temperature feedback control adjuster 405 monitor temperature and according to real time temperature adjustment 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, the feed rate controlling natural gas, resolution gas and anode exhaust gas distributes, and pressure-swing absorption apparatus resolution gas and anode exhaust gas is made full use of.Along with the increasing of hydrogen making by natural gas reformation device 409 load, 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, namely the input variable of overall system energy reduces, and then improves the energy efficiency of system.
Water Sproading logistics branch road: in hydrogen making by natural gas reformation device 409, combustion reaction tail gas enters water knockout drum 411 and carries out a point water after heat exchanger 407 and heat exchanger 410 heat exchange, emptying afterwards.Be separated the cold water obtained in water knockout drum 411 to enter hydrotreater 418 and carry out purified treatment, the water obtained can loop back in water tank 413, improves 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 obtained after point water enters hydrotreater 418 and carries out purified treatment, and the water obtained can loop back in water tank 413, improves the utilization ratio of water in system.Fuel battery negative pole tail gas enters the cold water obtained after point water in water knockout drum 417 and enters hydrotreater 418 equally and carry out purified treatment, and the water obtained can loop back in water tank 413, the utilization ratio of water in further raising system.Air simultaneously in fuel battery negative pole tail gas can carry out recovery compression and add in raw air storage tank 406.
For 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 with hydrogen making by natural gas reformation device 409, and the hot water obtained enters in hot water storage tank 412 and stores, and can provide domestic hot-water for user.
More than show and describe 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; what describe in above-described embodiment and specification 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.Application claims protection range 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 fuel gas mixing buffering area (A) successively, resolution gas reclaims zone of transformation (B), catalytic combustion transition region (C); The outside of the central area of described device is followed successively by reformation hydrogen production first district (F), the second reaction zone (D) of air and fuel gas, reformer feed mixed zone (E), reformation hydrogen production second district (G); 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), reclaimed the second reaction zone (D) of zone of transformation (B), catalytic combustion transition region (C), air and fuel gas after fuel gas and air mix successively by fuel gas mixing buffering area (A), resolution gas, reacted combustion tail gas exports (c) by combustion tail gas and discharges; 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 is entered at reformer feed mixed zone (E) and feed water inlet (d) by hydrogen feedstock diversion cavity (107) after hydrogen feedstock buffering area (H) mixes, enter reformation hydrogen production first district (F) and reformation hydrogen production second district (G) more successively, 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) loads the heat-storing material of large thermal capacitance.
2. device according to claim 1, is characterized in that, described reformation hydrogen production second district (G) is connected with product gas outlet (e) by the heat exchanger (106) be arranged in hydrogen feedstock buffering area (H).
3. device according to claim 2, is characterized in that, described in the heat exchanger (106) be 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 in falling " convex " shape hydrogen feedstock discharge end, and bottom surface and the side face region of this hydrogen feedstock discharge end 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, arranges water knockout drum between product gas outlet (e) and pressure-swing absorption apparatus.
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, described water circulation system comprises water knockout drum, hydrotreater, cyclic water tank successively, and cyclic water tank connects feed water inlet (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 connects fuel gas entrance (a) through Cemented filling.
17. devices according to claim 1 or 15 or 16, is characterized in that, the pipeline connecting fuel gas entrance (a) is equipped with temperature control adjusting valve and flame arrester; Temperature control adjusting valve is regulated by temperature feedback control adjuster.
The process for making hydrogen of reforming hydrogen production device described in 18. 1 kinds of claims 1, fuel gas is after the mixing of fuel gas mixing buffering area (A), with air generation catalyst combustion reaction in the second reaction zone (D) that resolution gas reclaims zone of transformation (B), catalytic combustion transition region (C), air and fuel gas, and providing heat for reformation hydrogen production reaction, combustion tail gas is discharged through combustion tail gas outlet (c); Hydrogen feedstock enters hydrogen feedstock buffering area (H) through hydrogen feedstock entrance (f), hydrogen feedstock diversion cavity (107) is entered after heat exchange, in the raw water mixing that reformer feed mixed zone (E) and feed water inlet (d) enter, after heat exchange, preheating, in reformation hydrogen production first district (F), reformation hydrogen production second district (G) carries out reforming reaction and generates hydrogen-rich reformate gas, reformate gas enters pressure-swing absorption apparatus, carries out separating-purifying to hydrogen; After pressure-swing absorption apparatus separating-purifying, remaining resolution gas is reclaimed by resolution gas recovery channel, and as combustible gas input fuel gas entrance.
19. techniques according to claim 18, is characterized in that, when 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 is reclaimed 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 separated is supplied to fuel cell system, and the tail gas that anode of fuel cell produces returns fuel gas entrance (a) and utilizes as fuel gas.
22. techniques according to any one of claim 19-21, is characterized in that, the pipeline connecting fuel gas entrance (a) is equipped with temperature control adjusting valve and flame arrester; Regulate temperature control adjusting valve by temperature feedback control 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 obtained 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 produced in combustion process is discharged by bottom water knockout drum, enters direct circulation recovery tank after hydrotreater process; Fuel battery negative pole tail gas enters point water in cathode exhaust gas water knockout drum to carry out being delivered to cyclic water tank as raw water after purified treatment through hydrotreater.
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| CN111082102B (en) * | 2019-12-23 | 2020-12-29 | 上海重塑能源科技有限公司 | Water knockout drum |
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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. |