CN101058404B - Biomass castoff supercritical water fluid bed partial oxidation hydrogen-preparation device and method - Google Patents
Biomass castoff supercritical water fluid bed partial oxidation hydrogen-preparation device and method Download PDFInfo
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Abstract
The invention discloses an oxidizing and gasifying hydrogen-making device and method of hypercritical water fluid-bed part of the biological waste, which is characterized by the following: adopting hypercritical water fluid-bed reactor to prevent slagging and blocking problem in the pipe flow reactor; using high-pressure separator to generate high-pressure water to adsorb carbon dioxide in the gas product; realizing the separation of the hydrogen from the carbon dioxide; making the separated high-density carbon dioxide concentrate to be disposed and do resoursing usage conveniently; compacting the device structure; simplifying and conveniencing the operation; improving the gasifying rate of the biological waste with less pollution in the liquid product; realizing the oxidizing and gasifying fusion in the reactor; improving the biological mass transmitting rate and system energy transmitting efficiency; transmitting the biological waste into high-quality hydrogen through the method; reducing the environmental pollution; realizing the dual goals to harness pollution and make hydrogen.
Description
Technical field
The invention belongs to the energy clean utilization field of renewable resources and waste, particularly a kind of biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen production plant and method.
Technical background
Along with the consumption gradually of fossil energy with move towards exhausted day by day, it is extremely urgent to seek new substitute energy.Biomass are utilized in the process CO to environment as a kind of rich in natural resources on the earth at it
2Clean quantity discharged is " zero ", and therefore, the Wood Adhesives from Biomass utilization causes people's extensive concern.
Thermochemistry gasification is considered to the biomass of tool commercial promise and utilizes technology, yet traditional biomass thermal chemistry gasification technology need carry out drying to biomass, and this process need consumes lot of energy.The supercritical water gasification hydrogen production technology can directly be handled the biomass of high water capacity, need not the drying process of high energy consumption, and have characteristics such as hydrogen content height in vaporization rate height, the gaseous product, it is one of biomass gasifying hydrogen making technology of tool potentiality, in nearly twenty or thirty year, the biomass supercritical water gasification hydrogen production technology is rapidly developed.
Research institution has developed the supercritical water gasification hydrogen production apparatus and method of a series of biomass waste both at home and abroad.The Modell of MIT carries out biomass supercritical water gasification hydrogen production research at first, and to the application of this kind hydrogen production process patent (US4113446).The Antal professor of University of Hawaii studies high-concentration raw material and organic waste in the pipe flow reactor, has realized biomass and organic being gasified totally thereof.At home, power engineering polyphasic flow National Key Laboratory of Xi'an Communications University, be engaged in biomass supercritical water gasification hydrogen production experiment and theoretical investigation for a long time, invented " the continuous supercritical water gasification hydrogen-producing method and apparatus of organic solid-state material " and applied for patent, this patent of invention (ZL02114529.6) has solved the key technical problems such as the heterogeneous continuous pipe flow mixing transfusion of high pressure of organic solid-state raw materials such as biomass, has realized the supercritical water continuous gasification hydrogen manufacturing of organic solid-state raw materials such as biomass in the fluid-guiding type reactor.On this basis, improve by further improvement, this seminar has invented " coal and biomass co-overcritical water catalysis-gasification hydrogen production plant and method " again and has applied for patent, this patent of invention (ZL200510041633.8) part has solved that reaction raw materials is rapidly heated and a difficult problem such as product gas part enrichment, has realized coal and biomass co-overcritical water catalysis-gasification hydrogen manufacturing.
At present, the research of the gasification hydrogen production plant in supercritical water of biomass waste and method still exists a following main difficult problem to have to be solved:
(1) when reaction not exclusively, or flow and transmission, reaction conditions are not coupled, design when unreasonable, wall slagging scorification obstruction appears in pipe flow reactor that the biomass supercritical water gasification process is used easily, thereby causes the failure of biomass waste continuous gasification;
(2) gasification reaction need absorb a large amount of heats, adopts the indirect heating method to be difficult for realizing the biomass required condition that is rapidly heated that is gasified totally, and makes that simultaneously the total system energy conversion efficiency is low;
(3) also have greatly gas such as carbonic acid gas in the reaction product except that hydrogen, product hydrogen also needs further purification processes before use.
Summary of the invention
One object of the present invention is to provide a kind of device of biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen-producing.This apparatus structure compactness, simple, easy to operate.Device has adopted supercritical water fluid bed reactor, has prevented the slagging scorification blockage problem that occurs in the pipe flow reactor.Adopt high-pressure separator in the device, utilize the carbonic acid gas in system's mesohigh water absorption gaseous product, realization hydrogen separates with carbonic acid gas, and isolated high concentration carbon dioxide is convenient to focus on and recycling simultaneously.
Another object of the present invention provides a kind of method of biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen-producing, makes biomass waste vaporization rate height, and it is few to contain pollutent in the product liquid.Simultaneously, in reactor, realize the coupling of oxidation and gasification, improved the energy conversion efficiency of Wood Adhesives from Biomass rate and system greatly.
The technical solution used in the present invention is: a kind of biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen production plant comprises storage tank, first feeder and second feeder, reactor, interchanger, preheater, water cooler, first back pressure valve, second back pressure valve, the 3rd back pressure valve, high-pressure separator, light pressure separator, first wet test meter, second wet test meter, first high pressure plunger pump, second high pressure plunger pump, the 3rd high pressure plunger pump, the 4th high pressure plunger pump, first mass flowmeter, second mass flowmeter, the 3rd mass flowmeter, the 4th mass flowmeter, water tank, a plurality of valves and temperature, System Controlled by Measuring Pressure; It is characterized in that:
First feeder, second feeder, second high pressure plunger pump, the 3rd high pressure plunger pump and storage tank are interconnected by pipeline and valve, form charging system;
Reactor is communicated with outlet, first feeder, the outlet of second feeder of preheater respectively; Interchanger is communicated with inlet, the water cooler inlet of reactor outlet, the first high-pressure plunger pump discharge, preheater respectively; Cooler outlet is communicated with the inlet of first back pressure valve; High-pressure separator is connected with first back pressure valve, second back pressure valve, the 3rd back pressure valve, the 4th high pressure plunger pump, forms high pressure water absorbing carbon dioxide system;
The outlet of the 3rd back pressure valve is communicated with the light pressure separator inlet end; The exit end of light pressure separator, second back pressure valve is communicated with first wet test meter, second wet test meter respectively.
Described reactor is supercritical water fluid bed reactor, vertically place, reactor bottom is an air distribution plate, adopting quartz sand in the fluidized-bed is the bed material, the lens washer flange seal is adopted on the top of reactor, fluid temperature (F.T.) distributes and measures by K type armoured thermocouple in the reactor, and reactor heats by electric heater, also can realize self-heating by the oxidizing reaction heat release.The high temperature fluid of preheater outlet makes the quartz sand on the air distribution plate be in fluidized state from bottom to top by reactor.The normal temperature material enters the middle and lower part of reactor from first feeder or the second feeder exit end, mixes with high temperature fluid in the reactor and bed material and is rapidly heated.
Described high-pressure separator can realize separating of hydrogen and carbonic acid gas in the gaseous product.When the large percentage of gas and water in the reaction after product, by the water filling in high-pressure separator of the 4th high pressure plunger pump, thus effectively the separating of realization hydrogen and carbonic acid gas.
In the described interchanger, the normal temperature high voltage water of the first high pressure plunger pump exit end reclaims the energy of reaction back high temperature fluid and realizes heating up, and has also reduced reaction back fluidic temperature simultaneously, has improved the energy conversion efficiency of total system.
The present invention adopts biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen-producing method, it is characterized in that, in reactor, utilize the heat release of supercritical oxidation reaction, for biomass gasification reaction provides heat, realize the coupling of heat release and heat absorption, improved the vaporization rate of interior heat exchange efficiency of reactor and biomass waste; Utilize the carbonic acid gas in the high pressure water absorption reaction product in the system, realize the dual-use function that hydrogen is produced and purified; Biomass waste can be converted into high-quality hydrogen by present method, reduces environmental pollution simultaneously, realizes pollution treatment and hydrogen manufacturing dual purpose.
Specifically carry out in accordance with the following methods:
(1) biomass waste, Xylo-Mucine (CMC), liquid oxidizer (hydrogen peroxide) are mixed with homogeneous material and put into storage tank, then by having the N of certain pressure
2In mass transport to the first feeder, be forced into predetermined pressure by second high pressure plunger pump and the 3rd high pressure plunger pump, be transported to reactor then;
(2) water is forced into predetermined pressure by first high pressure plunger pump and reclaims reaction back high temperature fluid heat by interchanger then, is heated to high temperature by preheater then, enters reactor;
(3) material reacts in reactor, the product that generates is cooled to normal temperature by interchanger and water cooler, realize separating of hydrogen and carbonic acid gas by entering behind the first back pressure pressure regulating valve in the high-pressure separator then, the carbonic acid gas that high pressure water absorbs drops to normal temperature by the 3rd back pressure valve pressure, then in light pressure separator with water sepn, and separated hydrogen is reduced to normal temperature by the second back pressure valve pressure in the high-pressure separator.
Technical characterstic of the present invention is:
(1) the existing pipe flow reactor of difference at first adopts supercritical water fluid bed reactor, can prevent to design unreasonable and pipe flow reactor wall slagging scorification blockage problem that cause because reaction not exclusively, or is flowed and transmission, reaction conditions are not coupled.
(2) but be in heat and mass in the bed material enhanced reactor of fluidized state in the reactor, help the gasification of biomass waste.
(3) in reactor, the material of low discharge normal temperature mixes with big flow high temperature fluid and bed material, can realize the biomass waste required condition that is rapidly heated that is gasified totally.
(4) heat release that utilizes supercritical oxidation to react in reactor for biomass gasification reaction provides heat, realizes the coupling of heat release and heat absorption, has improved the vaporization rate of interior heat exchange efficiency of reactor and biomass waste.
(5) utilize carbonic acid gas in the high pressure water absorption reaction product in the system, realize the dual-use function that hydrogen is produced and purified.Help focusing on and recycling of carbonic acid gas simultaneously.
(6) biomass waste can be converted into high-quality hydrogen by present method, reduces environmental pollution simultaneously, realizes pollution treatment and hydrogen manufacturing dual purpose.
Description of drawings
Fig. 1 is a supercritical water fluid bed partial oxidation gasification hydrogen production plant schema of the present invention.
Fig. 2 is a fluidized-bed reactor synoptic diagram of the present invention.
Fig. 3 is a high-pressure separator synoptic diagram of the present invention;
The present invention is described in further detail below in conjunction with specific embodiment that accompanying drawing and contriver provide.
Embodiment
Adopting gasified raw material among the present invention can be that biomass model compound (glucose, Mierocrystalline cellulose, xylogen etc.), protobiont matter waste (agricultural crop straw, various wastes etc.) also can be coals.Below be that example describes with agro-ecology matter stalk.
With reference to accompanying drawing 1, first, second feeder (2,3), second, third high pressure plunger pump (16,17), storage tank 1 are interconnected by pipeline and valve in the device of the present invention, form charging system; Reactor 4 is communicated with the outlet of preheater 6, first, second feeder (2,3) outlet respectively; Interchanger 5 is communicated with reactor 4 outlets, 15 outlets of first high pressure plunger pump, the inlet of preheater 6, water cooler 7 inlets respectively; Water cooler 7 outlets are communicated with the inlet of first back pressure valve 8; High-pressure separator 11 connects with first, second, third back pressure valve (8,9,10), the 4th high pressure plunger pump 18 respectively; The outlet of the 3rd back pressure valve 10 is communicated with light pressure separator 12 inlet ends; The exit end of light pressure separator 12, second back pressure valve 9 is communicated with first wet test meter 13, second wet test meter 14 respectively.
Its concrete working process is as follows: open first high pressure plunger pump 15, regulate first, second, third back pressure valve (8,9,10) and make system reach setting pressure, the mass rate of first high pressure plunger pump 15 is adjusted to set(ting)value (this flow is several times of mass flow usually).Open the heating unit of preheater 6 and reactor 4, make reactor inner fluid temperature reach set(ting)value.Meanwhile pulverize biomass and make its particle, then biomass and a small amount of Xylo-Mucine (CMC), hydrogen peroxide and pure water are mixedly configured into the uniform slurry of desired concn less than 40 orders.The biomass material that is disposed is added sealing storage tank 1, feed the N of certain pressure
2, with material from be delivered to first feeder 2 and second feeder 3.Open second, third high pressure plunger pump (16,17), make first feeder 2 and second feeder, 3 pressure be increased to system pressure.Open feeder exit end valve, material is added into reaction in the reactor 4, regulates mass flow simultaneously to set(ting)value.By after the cooling of interchanger 5 recovered energies, drop to room temperature by water cooler 7 temperature then after material reacts in reactor 4, be adjusted to separating pressure by the 3rd back pressure valve 10 pressure and enter high-pressure separator 11.Hydrogen and carbon dioxide separation in high-pressure separator 11, high concentration hydrogen is reduced to normal pressure by second back pressure valve, 9 pressure, and volumetric flow rate is by 13 meterings of first wet test meter.And carbonic acid gas separates in light pressure separator 12 by 10 step-downs of second back pressure valve after being absorbed by water.Gas composition analysis adopts the HP6890 gas-chromatography, and the carbon content of product liquid is by Elementar High II analyser analytical test.
The switch of the valve by first feeder 2, second feeder, 3 entrance ends and second high pressure plunger pump 16, the 3rd high pressure plunger pump 17, can realize a feeder in charging, thereby another feeder is adding the operation of material implement device long-time continuous stable.
With reference to accompanying drawing 2, fluidized-bed reactor 205 bottoms are provided with air distribution plate 206, and the lens washer flange seal is adopted on top, are about the quartzy casting bed material of 100-150 μ m for average particulate diameter on its air distribution plate 206.5 the K types that distributing in the reactor are driven dress thermopair 203 and are used to measure the reactor temperature distribution, and the reactor wall surface temperature is measured by wall thermopair 208.Reactor is by electric heater heating 202, fill insulant material 204 around the while.Material inlet 207 is above air distribution plate, the high-temperature water that preheater comes out enters reactor from the air distribution plate below, flow through to make in the process of reactor and be in fluidized state in the reactor, heat and mass in the enhanced reactor, help the gasification of biomass waste, prevent the slagging scorification of reactor wall simultaneously.Reactor outlet adopts the sealing means of flange lens washer 201, and reactor is dismantled easily, is convenient to the interpolation of bed material.
With reference to accompanying drawing 3, high-pressure separator 11 has two inlets and two outlets, and inlet 301 is cooled product gas-liquid mixture inlet, and inlet 302 is a high-pressure water inlet, and outlet 303 is the high concentration hydrogen outlet, and outlet 304 is the outlet of carbonic acid gas and water.For high pressure water is communicated with shower nozzle 305 by inlet 302, high pressure water spray flow from top to bottom fully absorbs the carbonic acid gas in the mobile gaseous product from bottom to top through multi-layer porous plate 306.The water of absorbing carbon dioxide flows out from exporting 304.High-pressure separator is utilized the pressure of supercritical gasification system self, utilizes the character of high pressure water absorbing carbon dioxide, has realized the separation of product, helps the concentrated discharging and the recycling of carbonic acid gas simultaneously.
The inventor provides following specific embodiment, referring to table 1-4.Table 1 is the gasification result of the glucose of different concns; Table 2 is corn cob gasification results of different concns; Table 3 is that oxygenant adds back glucose gasification result; Table 4 is that oxygenant adds back corn cob gasification result.
Experimental result shown in the table 1 shows at pressure 25MPa, and during 600 ℃ of temperature of reactor, concentration range is that the glucose of 5-30wt% can the continous-stable gasification.
Experimental result shown in the table 2 shows that concentration range is the corn cob energy continous-stable gasification of 5-18wt%, and reactor slagging scorification does not take place stops up.
Experimental result shown in the table 3 shows with oxidant concentration to be increased, and the content of hydrogen descends in the gaseous product, but the vaporization rate of glucose increases sharply, and there is maximum value in the absolute yield of hydrogen.Hydrogen peroxide is convenient to high-pressure delivery as oxygenant,
Experimental result shown in the table 4 shows that oxygenant adds, and density of hydrogen descends in the product, and the vaporization rate of biomass and gas yield increase.
Claims (3)
1. a biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen production plant comprises storage tank (1), first feeder (2) and second feeder (3), reactor (4), interchanger (5), preheater (6), water cooler (7), first back pressure valve (8), second back pressure valve (9), the 3rd back pressure valve (10), high-pressure separator (11), light pressure separator (12), first wet test meter (13), second wet test meter (14), first high pressure plunger pump (15), second high pressure plunger pump (16), the 3rd high pressure plunger pump (17), the 4th high pressure plunger pump (18), first mass flowmeter (19), second mass flowmeter (20), the 3rd mass flowmeter (21), the 4th mass flowmeter (22), water tank (23), a plurality of valves and temperature, System Controlled by Measuring Pressure; It is characterized in that:
Described first feeder (2) and second feeder (3) interconnect by pipeline, they respectively have two inlet ends, one of them inlet end is communicated with the exit end of second high pressure plunger pump (16) and the 3rd high pressure plunger pump (17) by second mass flowmeter (20) and the 3rd mass flowmeter (21), another inlet end is communicated with storage tank (1) exit end, and described storage tank (1) is provided with a gas inlet end and a material inlet end; The bottom of reactor (4) is communicated with the exit end of preheater (6), and the exit end of first feeder (2) and second feeder (3) all is communicated with reactor (4) middle and lower part inlet end; Described interchanger (5) has two inlet ends and two exit end, (5) inlet ends of reactor (4) exit end and interchanger are communicated with, reactor (4) is supercritical water fluid bed reactor, vertically place, reactor (4) bottom is an air distribution plate, adopting quartz sand in the fluidized-bed is the bed material, the lens washer flange seal is adopted on the top of reactor (4), fluid temperature (F.T.) distributes and measures by K type armoured thermocouple in the reactor (4), reactor (4) heats by electric heater, perhaps realize self-heating by the oxidizing reaction heat release, the high temperature fluid of preheater (6) outlet is from bottom to top by reactor (4), make the quartz sand on the air distribution plate be in fluidized state, the normal temperature material enters the middle and lower part of reactor (4) from first feeder or the second feeder exit end, expect to mix and be rapidly heated with interior high temperature fluid of reactor (4) and bed, another inlet end of interchanger (5) is communicated with first high pressure plunger pump (15) exit end; An exit end of interchanger (5) is communicated with the inlet end of preheater (6), and another exit end of interchanger (5) is communicated with water cooler (7) inlet end; Water cooler (7) exit end is communicated with the inlet end of first back pressure valve (8); Described high-pressure separator (11) has two inlet ends and two exit end, the exit end of first back pressure valve (8) is communicated with an inlet end of high-pressure separator (11), and the exit end of the 4th high pressure plunger pump (18) is communicated with another inlet end of high-pressure separator (11) by the 4th under meter (22); An exit end of high-pressure separator (11) is communicated with the inlet end of the 3rd back pressure valve (10), and the exit end of the 3rd back pressure valve (10) is communicated with light pressure separator (12) inlet end; Another exit end of high-pressure separator (11) is communicated with the inlet end of second back pressure valve (9); The exit end of light pressure separator (12), second back pressure valve (9) is communicated with first wet test meter (13), second wet test meter (14) respectively.
2. biomass castoff supercritical water fluid bed partial oxidation gasification hydrogen production plant as claimed in claim 1, it is characterized in that, described high-pressure separator (11) has two inlets and two outlets, one is cooled product gas-liquid mixture inlet (301), another is high-pressure water inlet (302), one is high concentration hydrogen outlet (303), and another is the outlet (304) of carbonic acid gas and water; High pressure water is communicated with shower nozzle (305) by inlet (302), and high pressure water spray flow from top to bottom fully absorbs the carbonic acid gas in the mobile gaseous product from bottom to top through multi-layer porous plate (306), and the water of absorbing carbon dioxide is from exporting (304) outflow.
3. hydrogen production process that uses the described biomass castoff supercritical water fluid bed partial oxidation hydrogen-preparation device of claim 1, it is characterized in that, this method is utilized the heat release of supercritical oxidation reaction, for biomass gasification reaction provides heat, in reactor, realize the coupling of heat release and heat absorption, with the vaporization rate of heat exchange efficiency and biomass waste in the raising reactor; Utilize the carbonic acid gas in the high pressure water absorption reaction product in the system, realize the dual-use function that hydrogen is produced and purified; Specifically carry out according to following steps:
(1) biomass waste is mixedly configured into the uniform slurry of desired concn with a small amount of Xylo-Mucine CMC, hydrogen peroxide and pure water and puts into storage tank, N2 by having certain pressure is forced into predetermined pressure with in mass transport to the first feeder by second high pressure plunger pump and the 3rd high pressure plunger pump then;
(2) pure water is forced into predetermined pressure by first high pressure plunger pump and reclaims reaction back high temperature fluid heat by interchanger then, is heated to high temperature by preheater then, enters reactor;
(3) material reacts the gaseous product that generates and is cooled to normal temperature by interchanger and water cooler in reactor, realize separating of hydrogen and carbonic acid gas by entering behind the first back pressure pressure regulating valve in the high-pressure separator then, the carbonic acid gas that high pressure water absorbs drops to normal temperature by the 3rd back pressure valve pressure, then in light pressure separator with water sepn, and separated hydrogen is reduced to normal temperature by the second back pressure valve pressure in the high-pressure separator.
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