CN106675661A - Method for continuous pyrolysis and gasification of material - Google Patents
Method for continuous pyrolysis and gasification of material Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 63
- 238000002309 gasification Methods 0.000 title claims abstract description 62
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- 238000006243 chemical reaction Methods 0.000 claims abstract description 100
- 239000000047 product Substances 0.000 claims abstract description 29
- 239000003054 catalyst Substances 0.000 claims abstract description 27
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- 230000008676 import Effects 0.000 claims description 5
- 229910000000 metal hydroxide Inorganic materials 0.000 claims description 5
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- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 4
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 4
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 4
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- 235000007164 Oryza sativa Nutrition 0.000 claims description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 2
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- 235000016383 Zea mays subsp huehuetenangensis Nutrition 0.000 claims description 2
- 235000002017 Zea mays subsp mays Nutrition 0.000 claims description 2
- -1 biological Jiao Chemical compound 0.000 claims description 2
- 239000002802 bituminous coal Substances 0.000 claims description 2
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims description 2
- 239000000920 calcium hydroxide Substances 0.000 claims description 2
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims description 2
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- 239000003077 lignite Substances 0.000 claims description 2
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims description 2
- 239000000347 magnesium hydroxide Substances 0.000 claims description 2
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 2
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- JPJALAQPGMAKDF-UHFFFAOYSA-N selenium dioxide Chemical compound O=[Se]=O JPJALAQPGMAKDF-UHFFFAOYSA-N 0.000 claims description 2
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- 238000005336 cracking Methods 0.000 abstract description 13
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- FFBHFFJDDLITSX-UHFFFAOYSA-N benzyl N-[2-hydroxy-4-(3-oxomorpholin-4-yl)phenyl]carbamate Chemical compound OC1=C(NC(=O)OCC2=CC=CC=C2)C=CC(=C1)N1CCOCC1=O FFBHFFJDDLITSX-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention discloses a method for continuous pyrolysis and gasification of a material. The method comprises the following steps: 1, a raw material and a catalyst enter a microwave pyrolysis and gasification system, fall to a first-stage rotating disc of a microwave reaction chamber, and sequentially undergo drying, activating and pyrolysis treatment with rotating; 2, a pyrolysis treated material falls to a second-stage rotating disc of the microwave reaction chamber, and the pyrolysis treated material and a pyrolysis volatile compound undergo a gasification and reforming reaction under the action of water vapor; and 3, a solid product obtained in step 2 falls to a residue storage tank below the microwave reaction chamber from middle holes of the second-stage rotating disc through a second-stage pushing baffle plate, and is discharged from a reaction system under stirring and screw dual action, and a gas product enters a settlement chamber from an annular sieve plate at the bottom of the microwave reaction chamber, and undergoes settlement treatment to obtain the gasification product. The method has the advantages of fast cracking speed, high gasification efficiency, high quality of the gas product, meeting of liquid fuel synthesis requirements, and good application prospect.
Description
Technical field
The present invention relates to a kind of method of material continuous pyrolysis gasification.
Background technology
Traditional heating mode is from outward appearance to inner essence heated by radiation, convection current and conduction, and in order to avoid thermograde is excessive, firing rate is tended not to too soon, can not carry out selective heating to each component of material.Because microwave can be directed through entering inside material, compared with traditional heating mode, heating using microwave can realize the balanced heating of material inside and outside, have the advantages that heating rate is fast, energy utilization efficiency is high, and microwave can the component different to material intermediary electrical characteristics carry out selective heating.Therefore the particularity of heating using microwave makes its thermal decomposition product compared with traditional gasification technology with greater advantages, is a kind of very promising material mode of heating.
Although microwave technology with batch (-type) fixed bed as representative realizes a series of processes such as the microwave-heating gasification of material, but the serialization and scale-up problem of microwave heating process is can't resolve, and the microwave heating technique of serialization is then the only way for realizing microwave large-scale application.The continuous process of microwave current pyrolytic gasification mainly includes rotary kiln, steel band kiln, helical duct kiln, disk rotary rotary kiln etc..Wherein, it is big that rotary kiln has that kiln body sealing and gas carry amount of dust, steel band kiln can occur at high temperature the change of steel band micro-wave dielectric and cause deformation to cause potential safety hazard, the relatively low impact efficiency of heating surface of helical duct kiln material compactedness, and the common problem that above-mentioned several method is present is to be difficult in dimension amplify simultaneously, this is clearly inapplicable for the various lots of materials such as biomass, coal are processed.
Disk rotary rotary kiln is heated during circular motion on pallet using material; in theory disk often rotates a circle; complete a cracking process; can adjust rotating speed to control pyrolytic gasification process according to material properties simultaneously; its maximum feature is to avoid ensureing the problem that material is fully pyrolyzed by extending certain dimension; amplify while realizing reactor various dimensions within the specific limits, be conducive to the scale and industrialization of microwave reactor.CN201310263370.X discloses a kind of disc type microwave continuous cracker and its method for cracking waste old, cavity is cracked using disc type, and upper and lower cavity is divided into by nonmetallic sealing plate, wherein microwave generator is on the top of cavity, solid product derives conveying in bottom, this layout not only realizes the continuity of cracking process, and improves junked tire microwave cracking efficiency, and the ratio of products therefrom is about fuel gas 40%, liquid oil 10%, carbon black 50%.But microwave generator is arranged on reaction chamber top and there is volatiles pollution microwave guiding device and Microwave-Transparent Materials windowsill by the method, and then causes microwave energy to assemble damage microwave component herein.CN201180072503.4 proposes to introduce microwave from reaction chamber bottom, the volatiles of generation can be extracted from reaction chamber top, the problem of microwave generator pollution is avoided, at the same it is square into preferably microwave energy region on a rotary disc, be conducive to the fast flash pyrolysis cracking of microwave radiation technology formula.But the arrangement of microwave source is only limitted to the bottom of reaction chamber in the method, locus is limited, to realize fast flash pyrolysis cracking, needs to be equipped with high power magnetron to increase microwave field strength, and this can increase considerably cost.
The content of the invention
Not enough for prior art, the invention provides a kind of method of material continuous pyrolysis gasification, the method rate of cleavage is fast, gasification efficiency is high, obtains gas products quality height, the requirement of synthetic liquid fuel is disclosure satisfy that, with applications well prospect.
The method of the material continuous pyrolysis gasification of the present invention, including following content：
（1）Microwave-heating gasification system is entered by the raw material and catalyst of helical feed, the one-level rotating circular disk in microwave reaction chamber is dropped down onto under gravity and is dried as rotation is sequentially passed through, is activated and pyrolysis processing；
（2）Material after pyrolysis processing falls into two grades of rotating circular disks in microwave reaction chamber in the presence of one-level advances baffle plate and proceeds in the presence of vapor gasification and reforming reaction together with volatiles；
（3）Jing steps（2）The solid product for processing, including the slag ladle that catalyst, coke and ash content are fallen into below microwave reaction chamber by two grades of propulsion baffle plates from the central aperture of two grades of rotating circular disks, reaction system is discharged in the case where mixing worm double action is stirred, and gaseous product then enters expansion chamber by the annular sieve plate in microwave reaction bottom of chamber portion, Jing settlement treatments obtain gasification product.
In the inventive method, step（1）Described raw material is the material for referring to decompose under the high temperature conditions, including biomass, trade waste, coal, oil shale etc., wherein biomass include any biomass containing lignocellulosic such as maize straw, rice husk, straw, wooden unit, leaf or branch, trade waste includes the organic wastes such as waste plastic, waste rubber tire, municipal refuse, and coal includes brown coal, lower-grade metamorphic bituminous, mesometamorphism bituminous coal and the high deterioration coal of any low caking index.Raw material shape can be the material for including any shapes such as sheet material, circle, cylinder, taper, cuboid, and raw material maximum direction size is less than 50mm, preferably 5 ~ 10mm.
In the inventive method, step（1）Raw material and catalyst microwave reaction chamber and in Action of Gravity Field free-falling to one-level rotating circular disk, 300 ~ 600 DEG C for the treatment of temperature, power density 1 × 10 is entered by feeding screw5~6×105W/m31 ~ 10kg/h of feed rate, because one-level rotating circular disk is pyrolysis zone, higher temperature can make raw material be dehydrated successively, activate and pyrolytic process, according to the selection of feedstock property and catalyst, the process time of whole process 1 ~ 10 minute, can control specific process time by one-level rotating circular disk rotating speed.In microwave field, hydrone in raw material is conducive to improving heating rate, and dehydration can change material structure, play a part of activation, further improve pyrolysis or catalytic pyrolysis degree, the vapor for generating simultaneously may also participate in the reactions such as cracking, oxidation, reduction and the reformation in gasification reformer section, play the effect of similar gasification gas, the exogenous vapor consumption of reduction.Raw material changes into most of pyrolysis devolatilization product and a small amount of semicoke after catalytic pyrolysis process, and wherein semicoke accounts for 10% ~ 20%, and volatiles account for 80% ~ 90%, and volatiles include about 10% ~ 30% condensable property component.
In the inventive method, step（1）Described catalyst is made up of charcoal class microwave absorption, metal oxide and the part of hydroxide three, charcoal class microwave absorption is used as carrier, metal oxide and hydroxide are used as active component, wherein metal oxide accounts for the 1% ~ 10% of catalyst quality, hydroxide accounts for the 1% ~ 10% of catalyst quality, balance of carrier；Charcoal class microwave absorption includes activated carbon, biological Jiao, graphite etc., preferred biological burnt；Metal oxide is the metal oxide with both sexes, including the one or more combination in nickel oxide, titanium oxide, zirconium oxide, lanthana, selenium oxide, aluminum oxide etc., preferred nickel oxide；Hydroxide includes the one or more combination in potassium hydroxide, NaOH, lithium hydroxide, calcium hydroxide, magnesium hydroxide etc., preferred potassium hydroxide.Above-mentioned catalyst feeds intake mass ratio for 1 with biomass material:2~1:20.
The preparation method of the biomass pyrolytic catalyst of the present invention, including following content：The mixing of charcoal class microwave absorption, metal oxide and hydroxide is placed in ball mill, then ball-milling treatment under room temperature condition is added to the mixture that above-mentioned crushing is mixed in double screw extruder, and extruding pelletization obtains product.
100 ~ 150 revs/min of described rotational speed of ball-mill, process time is 2 ~ 8 hours；
Described extrusion condition is as follows：25 ~ 60 DEG C of extrusion temperature, extruded velocity is 0.05 ~ 0.15mm/s, and extruder head length is 6 ~ 20mm, extrudes a diameter of 0.5 ~ 2mm.
In the inventive method, step（2）The gasification and reforming reaction temperature are 600 ~ 800 DEG C, 1 ~ 10 minute reaction time, power density 6 × 105~10×105W/m3, import 1 ~ 10m of vapor flow3/ h, wherein entering the vapor flow of gasification reforming zone in 0.5 ~ 5m3/ h, remaining vapor can repeat back to use by hollow rotating shaft, and the temperature of vapor is 120 ~ 200 DEG C.In gasification reforming process, the semicoke formed from pyrolytic process can rapidly inhale ripple intensification, accelerate coke tar cracking into light oil even micro-molecular gas, and the volatile component in the presence of vapor in semicoke can not only be discharged further, and biological Jiao surface carbon deposit can be eliminated, while can also be catalyzed CxHyAnd CO2The conversion reaction of synthesis gas is carried out, solid-liquid content is further reduced, charcoal conversion ratio is improved.Gas after reformation of gasifying is processed accounts for 90 ~ 95%, tar content 0.01 ~ 0.1%, semicoke 5 ~ 10%.
In the inventive method, step（3）The catalyst, coke and ash content are dropped into and remain in that after slag ladle higher temperature, due to the body heat effect mechanism of microwave, coke temperature is enabled to reach 600 ~ 800 DEG C, so high temperature can heat the vapor of hollow rotating shaft, also can guarantee that gaseous product remains gaseous state when through sieve plate and settlement treatment, improve energy regenerating utilization ratio.
In the inventive method, step（3）Described sieve plate is convex sieve plate, and convex 1 ~ 10cm of length, hole diameter of sieve (perforated) plate Φ 1 ~ Φ 5mm, the downward-sloping angle of sieve plate is 10 ° ~ 60 °.It is such to be designed to reduce the particle carrying amount in gas, while and unsifted particle can be imported into slag ladle by sieve plate inclined-plane.
In the inventive method, step（3）Described settlement treatment adopts multilayer expansion chamber, extends the time of staying of gas, improves and carry in gas the settling efficiency of particle, while can also promote the vapor in gas to continue to be reacted with high-temperature particle charcoal, further reduces the solid carrying amount of gas.The gasification product H for finally giving2/ CO between 1.5 ~ 2.2,10 ~ 20mg/m of tar content3, the conversion efficiency of whole process biological carbon is 90 ~ 98%.
Present invention simultaneously provides a kind of material continuous microwave pyrolysis gasification system, including feeding screw, microwave reaction chamber, microwave generator, one-level rotating circular disk, two grades of rotating circular disks, hollow rotating shaft, sieve plate, expansion chamber, slag ladle and spiral slag-discharging devices；Feeding screw is located at microwave reaction chamber top；Microwave reaction chamber outside arranges microwave generator；One-level rotating circular disk and two grades of rotating circular disks are provided with inside microwave reaction chamber, two-stage rotating circular disk is fixed by hollow rotating shaft；One-level propulsion baffle plate is connected with hollow rotating shaft top, hollow rotating shaft bottom is connected with vapor reuse pipe；Two grades of rotating circular disk tops are provided with metal liner, and metal liner is connected with two grades of propulsion baffle plates；Microwave reaction bottom of chamber portion is annular shape, is made up of downward-sloping sieve plate, sieve plate（Annulus annular section）Lower section connection expansion chamber, expansion chamber arranges gas products outlet；The non-sieve plate part in microwave reaction bottom of chamber portion（Circular little circular portion）Communicate with lower section slag ladle, there is agitator in slag ladle, and communicate with spiral slag-discharging device.
Wherein, described microwave-heating reaction chamber exterior lateral sides are distributed a number of microwave quartz window, each window one microwave generator of correspondence, the power of single microwave generator is 500 ~ 2000W, specific number of windows is set according to situations such as the volume of reactor, it is general to arrange 4 ~ 50, it is ensured that the power density in reactor is 1 × 105~10×105W/m3。
Described microwave-heating gasification system adopts vertical moving-burden bed reactor, and according to rotating circular disk is arranged different reaction intervals, one-level rotating circular disk top are divided（Including one-level rotating circular disk）For pyrolysis zone, 300 ~ 600 DEG C of temperature；Between one-level rotating circular disk and two grades of rotating circular disks（Including two grades of rotating circular disks）For reforming zone of gasifying, 600 ~ 800 DEG C of temperature.The temperature in each area is controlled by corresponding microwave generator, in order to avoid because caused by temperature control biomass be heated uneven or even there is a problem of half-cooked, all microwave temperature control mechanisms are all adjusted to ensure that material is full-time and absorb microwave and heat using continuous power in the present invention.
Described microwave reaction chamber is provided with two-stage rotating circular disk, and wherein one-level rotating circular disk is the conical structure without bottom surface portions, and the 1/2 ~ 4/5 of a diameter of microwave reaction chamber internal diameter in circular cone bottom surface, circle element of a cone is 10 ~ 45 ° with the angle of horizontal direction；Two grades of rotating circular disks are the handstand frustum cone structure of supreme bottom surface part, the bottom surface of round platform（Two grades of rotating circular disks side upwards）The 1/100 ~ 1/10 of a diameter of microwave reaction chamber internal diameter, the 1/5 ~ 1/2 of a diameter of microwave reaction chamber internal diameter of the upper bottom surface of round platform, the bus of round platform and the angle of horizontal direction are 10 ~ 45 °.Firsts and seconds rotating circular disk is fixed on hollow rotating shaft by disk bottom metallic supports, and metallic supports are connected by bolt with rotating circular disk.
Two-stage rotating circular disk structure of the present invention can be processed making according to existing process technology, can be with one-shot forming, it is also possible to made according to following structure.
Wherein, the structure of described one-level rotating circular disk is as follows：By disk（Fig. 3）Support with metal（Fig. 4）Two parts are constituted, and disk is made up of the eccentric circular ring armor of four pieces of material same dimensions of the same race around identical central angle, and the central angle per block size is 90 °, and the minimum concentric circles internal diameter of one-level disk is equal or slightly larger than hollow rotating shaft external diameter；The material of disk be inorganic hybrid material, the one or more combination in silica, carborundum, silicon nitride, aluminum oxide, ferroso-ferric oxide, zirconium oxide, magnesia；Metal support by some metal donut 4-1,4-2,4-3 ... the circular cone " outer inclined-plane " constituted by welding manner and four groups of sheet materials（Per group includes a pair sheet materials in enantiomorphic relationship, such as 4a ' and 4a ", 4b ' and 4b ' ', 4c ' and 4c ' ', 4d ' and 4d ' '）" muscle " composition constituted on welding（Fig. 4）, wherein minimum metal donut 4-1 is directly welded in hollow rotating shaft 6 and is fixed, " outer inclined-plane " is 10 ~ 45 ° with the angle of horizontal direction, in four groups of described sheet materials, 4a ' and 4a ", 4b ' and 4b ' ' vertical weldings be in " outer inclined-plane "（Fig. 5）, 4c ' and 4c ' ', 4d ' and 4d ' ' paperbacked weldings are in " outer inclined-plane "（Fig. 6）, angle is 90 ° between two groups of sheet materials that are vertical or being laid in " outer inclined-plane ", and angle is 45 ° between per group of sheet material vertical and that " outer inclined-plane " is laid in per group.Four groups of sheet materials 4a ' and 4a ", 4b ' and 4b ' ', 4c ' and 4c ' ', 4d ' and 4d ' ' outer ends connect respectively inside curved metal catch 4-1a ' and 4-1a ' ', 4-1b ' and 4-1b ' ', 4-1c ' and 4-1c ' ', the 4-1d ' and 4-1d ' ' in the center of circle（Fig. 5 and Fig. 6）, metal catch is furnished with the fixation that bolt can be used for disk.
The structure of two grades of described rotating circular disks is as follows：Two grades of rotating circular disks are supported by disk and metal and constituted, disk is made up of the eccentric circular ring armor of four pieces of material same dimensions of the same race around identical central angle, central angle per block size is 90 °, and the minimum concentric circles internal diameter of two grades of disks is the 1/5 ~ 1/2 of microwave reaction chamber internal diameter；The material of disk be inorganic hybrid material, the one or more combination in silica, carborundum, silicon nitride, aluminum oxide, ferroso-ferric oxide, zirconium oxide, magnesia；The metal of two grades of rotating circular disks support by some metal donut 5-1,5-2,5-3 ... the handstand round platform " outer inclined-plane " constituted by welding manner and four groups of sheet materials（Per group includes a pair sheet materials in enantiomorphic relationship）" muscle " composition constituted on welding（Fig. 8）, wherein minimum metal donut 5-1 is connected by metal electrode with hollow rotating shaft 6, the angle of " outer inclined-plane " and horizontal direction is 10 ~ 45 °, in four groups of described sheet materials, 5a ' and 5a ", 5b ' and 5b ' ' is perpendicular to " outer inclined-plane "（Fig. 9）, 5c ' and 5c ' ', 5d ' and 5d ' ' are laid in " outer inclined-plane "（Figure 10）, angle is 90 ° between two groups of sheet materials that are vertical or being laid in " outer inclined-plane ", and angle is 45 ° between per group of sheet material vertical and that " outer inclined-plane " is laid in per group.Two ends all connect inside curved metal catch 5-1a ' and 5-1a ' ', 5-1b ' and 5-1b ' ', 5-1c ' and 5-1c ' ', the 5-1d ' and 5-1d ' ' in the center of circle inside and outside four groups of sheet materials 5a ' and 5a ", 5b ' and 5b ' ', 5c ' and 5c ' ', 5d ' and 5d ' '（Fig. 9 and Figure 10）, metal catch is furnished with the fixation that spiral can be used for disk.
Described one-level（Two grades）The connection and fixation that disk is supported with metal is perpendicular to " outward by two groups（It is interior）Inclined-plane " sheet material, two groups be laid in " outward（It is interior）What inclined-plane " sheet material and curved metal catch were realized jointly.Eccentric circular ring tray bottom is by being laid in " outward（It is interior）Inclined-plane " sheet material is supported, and two edge grains of fan-shaped the ring disk are by perpendicular to " outward（It is interior）Inclined-plane " sheet material is surrounded, and the outer ring surface of fan-shaped the ring disk or inside and outside anchor ring are further reinforced by metal catch and bolt.
Described two-stage rotating circular disk is fixed by hollow rotating shaft, and through whole microwave cavity and slag ladle, hollow rotating shaft is hollow structure to hollow rotating shaft, and inside can be passed through vapor isoreactivity gas；Rotary shaft is partly distributed some pores between one-level rotating circular disk and two grades of rotating circular disks；Rotary shaft is provided with outer tube on one-level rotating circular disk top, wherein outer tube welding one-level propulsion baffle plate, is shaped as parallelogram, and parallelogram acute angle and one-level rotating circular disk inclination angle right angle each other, one-level propulsion baffle plate presses close to as far as possible one-level rotating circular disk；In slag ladle part axle outer layer welding rabbling mechanism, rabbling mechanism refer to it is any can play agitation and push the device or mode of material, including leaf formula oar, anchor formula slurry, propeller mixer, turbine agitator, dasher, anchor agitator etc..
In the present invention, microwave reaction chamber is made up of the outer wall and ceramic liner of metal, including upper microwave reaction chamber and lower microwave reaction chamber, it is respectively provided with inner bag, upper microwave reaction chamber correspondence one-level rotating circular disk, two grades of rotating circular disks of lower microwave reaction chamber correspondence, and by flange connection and sealing.
It is not provided with microwave source at flange arrangement simultaneously, it is ensured that up and down interfering with each other for microwave reaction chamber microwave substantially reduces so that temperature is more prone to control.In order to prevent upper microwave reaction chamber inner bag from sliding, in upper microwave reaction chamber metal outer wall bottom（On flange arrangement）Upper welding internal diameter is supported less than the circular metal liner of corresponding ceramic liner external diameter.In the same manner, also on lower microwave reaction chamber metal outer wall top（Under flange arrangement）Circular metal liner of the welding internal diameter less than correspondence ceramic liner external diameter.One side metal inner lining is close to lower microwave reaction chamber inner bag, on metal liner welding propulsion baffle plate can close two grades of rotating circular disks to greatest extent, while can also meet the further pyrolysis of the biological material of two grades of rotating circular disks（Because inner bag is in microwave source generation area）.On the other hand, metal liner can also play the requirement of fixed ceramic liner and sealing reactor.
In the present invention, flange lower end between one-level rotating circular disk and two grades of rotating circular disks is connected with metal liner, two grades of propulsion baffle plates are welded on metal liner, two grades of propulsion baffle shapes are parallelogram, parallelogram acute angle and two grades of rotating circular disk inclinations angle right angle each other, two grades of propulsion baffle plates press close to as far as possible two grades of rotating circular disks.
The present invention is not limited to two-stage rotating circular disk, can arrange Multi-stage rotary disk and microwave reaction chamber according to specific needs, and the connection by multiple flanges and multistage propulsion baffle design realize the continuous microwave pyrolytic gasification of material；Multi-stage rotary disk is such as set, and from top to bottom the structure of the rotating circular disk of the first order to penultimate stage is identical, the level rotating circular disk structure last of bottom is identical with two grades of rotating circular disks in two-stage rotating circular disk of the present invention.
Described slag ladle is located at immediately below microwave reaction chamber, and the internal diameter of slag ladle is more than the round platform upper bottom surface diameter of two grades of rotating circular disks, is the 2/5 ~ 2/3 of microwave reaction chamber internal diameter；In slag ladle in addition to the rabbling mechanism in rotary shaft, helical slag removing machine structure is arranged at bottom, while guaranteeing that material fully reacts, can improve the treating capacity of whole system according to solid accumulation situation control stirring and deslagging speed in reaction system.
The present invention has compared with prior art advantages below：
1st, there is a problem of serialization for existing microwave-heating gasification technology and amplify difficult, designed and developed with Multi-stage rotary disk（At least two-stage）Serialization disk rotary rotary kiln, extend the time of staying of the material in microwave reaction chamber, promote fully carrying out for pyrolytic gasification, it is also beneficial to improve the treatment scale of unit simultaneously, overcomes traditional disc rotary kiln single-stage rotating disk to there is a problem of that pyrolysis is insufficient and needs high power magnetron just to can guarantee that higher position reason amount.In addition, the serialization disk rotary rotary kiln of this Multi-stage rotary disk is more increased in height, floor space is little, it is easier to which scale is amplified and industrial applications.
2nd, the serialization disk rotary rotary kiln of Multi-stage rotary disk realizes continuous pyrolysis gasification of the material in reactor by inclined rotating circular disk and propulsion baffle design.Simultaneously the middle control rotary shaft of rotating circular disk is passed through low temperature vapor can ensure the use temperature of vapor, while can also avoid middle control rotary shaft from deforming because temperature is too high, increase the service life.
3rd, the serialization disk rotary rotary kiln of Multi-stage rotary disk adopts the wall heating using microwave of reaction chamber side; traditional microwave source is avoided to be pyrolyzed volatile matter bonding or bottom by the hidden danger of biological burnt pollution on reaction chamber top; simultaneously side wall does not have feed inlet and outlet, air inlet/outlet etc. to arrange; with more spaces for putting microwave source, the handling process of amplification and the scale of microwave power is also beneficial to.
4th, the serialization disc rotary kiln gasification process of Multi-stage rotary disk improves pyrolytic gasification efficiency using cheap microwave adaptability catalyst, reduces the generation of the accessory substances such as tar and semicoke, and the conversion efficiency of carbon is significantly improved.Microwave adaptability catalyst adopts biological Jiaozhuo that pyrolytic process is produced for microwave absorption carrier, the metal oxide and hydroxide of microwave weak absorbing and strong catalytic pyrolysis are had concurrently as active component, both the catalysis activity of active component had been played, the constructive variations inactivation for avoiding active component long-time microwave action to cause again simultaneously, extends catalyst service life.
5th, the serialization disk rotary rotary kiln pyrolytic gasification technique of Multi-stage rotary disk will be pyrolyzed, gasification and reform etc. course of reaction carry out effective integration, improve the efficiency of energy utilization of whole system, reduce the production cost of gasification, the Combination Design of the spiral slag ladle, sieve plate and multilayer expansion chamber that adopt simultaneously can further reduce the solid particle carrying amount in gas, the efficiency of carbon con version of material is improved, is that internal carbon cycle technology is utilized there is provided effective way.
Description of the drawings
Fig. 1 material continuous pyrolysis gasification reactor apparatus（By taking two-stage rotating circular disk as an example）Structural representation；
Fig. 2 microwave reactions chamber internal structure schematic diagram；
The material splicing schematic diagram of Fig. 3 one-level rotating circular disks；
Fig. 4 one-level rotating circular disks metal supports general structure schematic diagram；
Fig. 5 one-level rotating circular disk vertical metal supporting construction schematic diagrames；
Fig. 6 one-levels rotating circular disk tiling metal support structure schematic diagram；
The material splicing schematic diagram of bis- grades of rotating circular disks of Fig. 7；
Bis- grades of rotating circular disk metals of Fig. 8 support general structure schematic diagram；
Bis- grades of rotating circular disk vertical metal supporting construction schematic diagrames of Fig. 9；
Bis- grades of rotating circular disks tiling metal support structure schematic diagrames of Figure 10.
Wherein，Feeding screw 1，Microwave reaction chamber 2，Microwave generator 3，One-level rotating circular disk 4，Two grades of rotating circular disks 5，Hollow rotating shaft 6，One-level advances baffle plate 7，Two grades of propulsion baffle plates 8，Welding rod 9，Metal liner 10，Sieve plate 11，Expansion chamber 12，Gas products outlet 13，Slag ladle 14，Agitator 15，Spiral slag-discharging device 16，Vapor reuse pipe 17，Metal jacket pipe 18，Vapor pore 19，Ceramic liner 20，Flange 21，One-level rotating circular disk material 4a、4b、4c、4d，Two grades of rotating circular disk material 5a、5b、5c、5d，One-level rotating circular disk vertical metal supports sheet material 4a ' and 4a "、4b ' and 4b ' '，One-level rotating circular disk tiling metal profile material 4c ' and 4c ' '、4d ' and 4d ' '，Two grades of rotating circular disk vertical metals support sheet material 5a ' and 5a ' '、5b ' and 5b ' '，Two grades of rotating circular disks tiling metal profile material 5c ' and 5c ' '、5d ' and 5d ' '，One-level rotating circular disk metal catch 4-1a ' and 4-1a ' '、4-1b ' and 4-1b ' '、4-1c ' and 4-1c ' '、4-1d ' and 4-1d ' '，Two grades of rotating circular disks metal catch 5-1a ' and 5-1a ' '、5-1b ' and 5-1b ' '、5-1c ' and 5-1c ' '、5-1d ' and 5-1d ' '.
Specific embodiment
Below in conjunction with the accompanying drawings explanation and embodiment are described in detail to the present invention program, but the present invention is not limited by following embodiments.
Material continuous pyrolysis gasification reactor apparatus as shown in Figure 1, including feeding screw 1, microwave reaction chamber 2, microwave generator 3, one-level rotating circular disk 4, two grades of rotating circular disks 5, sieve plate 11, expansion chamber 12, slag ladle 14 and spiral slag-discharging devices 15.Feeding screw 1 is located at the top of microwave reaction chamber 2；The outside of microwave reaction chamber 2 arranges microwave generator 3；One-level rotating circular disk 4 and two grades of rotating circular disks 5 are provided with inside microwave reaction chamber 2, two-stage rotating circular disk is all fixed by hollow rotating shaft 6, wherein two grades of rotating circular disks 5 are connected by welding rod 9 with hollow rotating shaft 6；One-level propulsion baffle plate 7 is connected with the top of hollow rotating shaft 6, and hollow rotating shaft bottom is connected with vapor reuse pipe 17；Two grades of tops of rotating circular disk 5 are provided with metal liner 10, and metal liner 10 is connected with two grades of propulsion baffle plates 8；
The bottom of microwave reaction chamber 2 is annular shape, is made up of downward-sloping sieve plate 11, sieve plate 11（Annulus annular section）Lower section connection expansion chamber 12, expansion chamber 12 arranges gas products outlet 13；The non-sieve plate part of the bottom of microwave reaction chamber 2（Circular little circular portion）Communicate with lower section slag ladle 14, have agitator 15 in slag ladle 14, and communicate with spiral slag-discharging device 16.
Microwave reaction chamber 2 as shown in Figure 2 includes upper and lower two parts, and by the connection and sealing of flange 21, flange 21 is located between one-level rotating circular disk 4 and two grades of rotating circular disks 5.One-level propulsion baffle plate 7 plate on flange 21 is fixed by the metal jacket pipe 18 of hollow rotating shaft 6, and hollow rotating shaft 6 is provided with some vapor pores 18 between one-level rotating circular disk 4 and two grades of rotating circular disks 5.The lower end of flange 21 is connected with metal liner 10, two grades of propulsion baffle plates 8 is welded on metal liner 10 and is close to two grades of rotating circular disks 5, and metal liner 10 is below and ceramic liner 20 carries out encapsulation process.
One-level rotating circular disk 4 such as Fig. 3 ~ 6 is made up of material 4a, 4b, 4c, 4d splicing, and by vertical metal sheet material 4a ' and 4a ", 4b ' and 4b ' ', tiling sheet metal 4c ' and 4c ' ', 4d ' and 4d ' ' are supported and are fixed with metal catch 4-1a ' and 4-1a ' ', 4-1b ' and 4-1b ' ', 4-1c ' and 4-1c ' ', 4-1d ' and 4-1d ' '.
Two grades of rotating circular disks 5 such as Fig. 7 ~ 10 are made up of material 5a, 5b, 5c, 5d splicing, and by vertical metal sheet material 5a ' and 5a ' ', 5b ' and 5b ' ', tiling sheet metal 5c ' and 5c ' ', 5d ' and 5d ' ' are supported and are fixed with metal catch 5-1a ' and 5-1a ' ', 5-1b ' and 5-1b ' ', 5-1c ' and 5-1c ' ', 5-1d ' and 5-1d ' '.
The material continuous pyrolysis gasification installation specific work process of the present invention is as follows：Material sends into microwave reaction chamber 2 by feeding screw 1, and fall under gravity into one-level rotating circular disk 4, when material is paved with substantially on one-level rotating circular disk 4, one-level rotating circular disk 4 and two grades of rotating circular disks 5 are rotated simultaneously, advanced in the presence of baffle plate 7 by the one-level of one-level rotating circular disk 4, material constantly falls into two grades of rotating circular disks 5 from one-level rotating circular disk 4, start microwave generator 3 when two grades of rotating circular disks 5 are paved with material substantially, the temperature precise control of pyrolysis zone and gasification reformer section is realized by continuously adjusting the power of each microwave generator.Material carries out pyrolytic reaction in one-level rotating circular disk 4, and the semicoke of generation is sent to two grades of rotating circular disks 5 by one-level propulsion baffle plate 7, and with gas-liquid volatiles in vapor（It is passed through from vapor pore 19）In the presence of gasify, fraction solids（Semicoke）There is cracking reaction, the C in gas in generation gasification reaction, part tarxHyAnd CO2Also reforming reaction is carried out under the synergy of coke/vapor, solid-liquid content is further reduced, efficiency of carbon con version is improved.Gas after gasification and reformation are processed enters sieve plate 11 and removes the fraction solids particulate matter in portion gas from two grades of center-aisles of rotating circular disk 5, then gas solid separation is continued in expansion chamber 12, discharge from gas products outlet 13, obtain the synthesis gas product of high-quality.The coke and ash content of residual advances baffle plate 8 to fall into slag ladle 14 from two grades of center-aisles of rotating circular disk 5 under acting at two grades, by the drive of agitator 15, progressively moves down, and finally removes reaction system by spiral slag-discharging device 16.
The effect of the present invention is further illustrated below by embodiment, percentage composition therein is weight/mass percentage composition.
The preparation of the catalyst used in embodiment
Using the method for dry ball milling, biology Jiao that nickel oxide, potassium hydroxide and pyrolytic process are generated is according to mass ratio 1:1:10 are mixed, and ball milling 2 hours under the conditions of 150 revs/min of rotating speed, obtain uniform powdered carbon catalyst, are then cold-pressed into strip particle, and size is φ 4mm × 6mm, and gained Catalyst Definitions are NiO1.0KOH1.0/C10, wherein NiO contents are that 8.33%, KOH contents are 8.33%.
Embodiment 1
Biomass material and microwave catalyst NiO1.0KOH1.0/C10According to 15:1 ratio sends into microwave reaction chamber 2 by feeding screw 1, and falls under gravity into one-level rotating circular disk 4（The 3/5 of a diameter of microwave reaction chamber internal diameter in circular cone bottom surface, element of cone is 15 ° with the angle of horizontal direction）, when material is paved with substantially on one-level rotating circular disk 4, while rotating one-level rotating circular disk 4 and two grades of rotating circular disks 5（The 19/20 of a diameter of microwave reaction chamber internal diameter of bottom surface of round platform, the 1/4 of a diameter of microwave reaction chamber internal diameter of the upper bottom surface of round platform, the bus of round platform and the angle of horizontal direction are 20 °）Advanced in the presence of baffle plate 7 by the one-level of one-level rotating circular disk 4, material constantly falls into two grades of rotating circular disks 5 from one-level rotating circular disk 4, start microwave generator 3 when two grades of rotating circular disks 5 are paved with material substantially, the temperature for arranging pyrolysis zone and gasification reformer section is respectively 600 DEG C and 800 DEG C, and corresponding microwave power is respectively 6 × 105
W/m3、10×105 W/m3.After microwave microwave reaction chamber 2 is to setting temperature, feed rate 10kg/h is adjusted, raw material first processes 10min in pyrolysis zone, and semicoke accounts for 20% in the gas-liquid-solid product of formation, and volatiles account for 80%, and volatiles include about 20% condensable property component.The semicoke of generation is sent to two grades of rotating circular disks 5 by one-level propulsion baffle plate 7, and with volatiles in vapor（It is passed through from vapor pore 19）In the presence of gasify, while control import vapor flow 10m3/ h, the temperature of vapor is 200 DEG C, wherein entering the vapor flow of gasification reforming zone in 5m3/ h, remaining vapor is recycled by vapor reuse pipe 17.Under vapor effect, fraction solids（Semicoke）There is cracking reaction, the C in gas in generation gasification reaction, part tarxHyAnd CO2Also reforming reaction is carried out under the synergy of coke/vapor, now pyrolysis devolatilization is divided into 92% in product, wherein condensable property component 0.05%, and semicoke 8%, the lasting 10min of gasification reforming process.Gas after gasification and reformation are processed enters sieve plate 11 from two grades of center-aisles of rotating circular disk 5（The downward-sloping angle of sieve plate is 30 °）And the fraction solids particulate matter in portion gas is removed, and then continue gas solid separation in expansion chamber 12, discharge from gas products outlet 13, obtain the synthesis gas product of high-quality, H2/ CO 1.95, tar content 0.0018%（About 18mg/m3）, the conversion efficiency of whole process biological carbon reaches 92%.The coke and ash content of residual advances baffle plate 8 to fall into slag ladle 14 from two grades of center-aisles of rotating circular disk 5 under acting at two grades, by the drive of agitator 15, progressively moves down, and finally removes reaction system by spiral slag-discharging device 16.
Embodiment 2
Biomass material and microwave catalyst NiO1.0KOH1.0/C10According to 2:1 ratio sends into microwave reaction chamber 2 by feeding screw 1, and falls under gravity into one-level rotating circular disk 4（The 1/2 of a diameter of microwave reaction chamber internal diameter in circular cone bottom surface, element of cone is 10 ° with the angle of horizontal direction）, when material is paved with substantially on one-level rotating circular disk 4, while rotating one-level rotating circular disk 4 and two grades of rotating circular disks 5（The 9/10 of a diameter of microwave reaction chamber internal diameter of bottom surface of round platform, the 1/5 of a diameter of microwave reaction chamber internal diameter of the upper bottom surface of round platform, the bus of round platform and the angle of horizontal direction are 45 °）Advanced in the presence of baffle plate 7 by the one-level of one-level rotating circular disk 4, material constantly falls into two grades of rotating circular disks 5 from one-level rotating circular disk 4, start microwave generator 3 when two grades of rotating circular disks 5 are paved with material substantially, the temperature for arranging pyrolysis zone and gasification reformer section is respectively 300 DEG C and 600 DEG C, and corresponding microwave power is respectively 1 × 105
W/m3、6×105 W/m3.After microwave microwave reaction chamber 2 is to setting temperature, feed rate 1kg/h is adjusted, raw material first processes 1min in pyrolysis zone, and semicoke accounts for 10% in the gas-liquid-solid product of formation, and volatiles account for 90%, and volatiles include about 10% condensable property component.The semicoke of generation is sent to two grades of rotating circular disks 5 by one-level propulsion baffle plate 7, and with volatiles in vapor（It is passed through from vapor pore 19）In the presence of gasify, while control import vapor flow 1m3/ h, the temperature of vapor is 120 DEG C, wherein entering the vapor flow of gasification reforming zone in 0.5m3/ h, remaining vapor is recycled by vapor reuse pipe 17.Under vapor effect, fraction solids（Semicoke）There is cracking reaction, the C in gas in generation gasification reaction, part tarxHyAnd CO2Also reforming reaction is carried out under the synergy of coke/vapor, now pyrolysis devolatilization is divided into 95% in product, wherein condensable property component 0.02%, and semicoke 5%, the lasting 1min of gasification reforming process.Gas after gasification and reformation are processed enters sieve plate 11 from two grades of center-aisles of rotating circular disk 5（The downward-sloping angle of sieve plate is 60 °）And the fraction solids particulate matter in portion gas is removed, and then continue gas solid separation in expansion chamber 12, discharge from gas products outlet 13, obtain the synthesis gas product of high-quality, H2/ CO 2.2, tar content 0.001%（About 10mg/m3）, the conversion efficiency of whole process biological carbon reaches 98%.The coke and ash content of residual advances baffle plate 8 to fall into slag ladle 14 from two grades of center-aisles of rotating circular disk 5 under acting at two grades, by the drive of agitator 15, progressively moves down, and finally removes reaction system by spiral slag-discharging device 16.
Embodiment 3
Biomass material and microwave catalyst NiO1.0KOH1.0/C10According to 20:1 ratio sends into microwave reaction chamber 2 by feeding screw 1, and falls under gravity into one-level rotating circular disk 4（The 4/5 of a diameter of microwave reaction chamber internal diameter in circular cone bottom surface, element of cone is 45 ° with the angle of horizontal direction）, when material is paved with substantially on one-level rotating circular disk 4, while rotating one-level rotating circular disk 4 and two grades of rotating circular disks 5（The 99/100 of a diameter of microwave reaction chamber internal diameter of bottom surface of round platform, the 1/2 of a diameter of microwave reaction chamber internal diameter of the upper bottom surface of round platform, the bus of round platform and the angle of horizontal direction are 10 °）Advanced in the presence of baffle plate 7 by the one-level of one-level rotating circular disk 4, material constantly falls into two grades of rotating circular disks 5 from one-level rotating circular disk 4, start microwave generator 3 when two grades of rotating circular disks 5 are paved with material substantially, the temperature for arranging pyrolysis zone and gasification reformer section is respectively 600 DEG C and 800 DEG C, and corresponding microwave power is respectively 6 × 105
W/m3、10×105 W/m3.After microwave microwave reaction chamber 2 is to setting temperature, feed rate 10kg/h is adjusted, raw material first processes 10min in pyrolysis zone, and semicoke accounts for 20% in the gas-liquid-solid product of formation, and volatiles account for 80%, and volatiles include about 30% condensable property component.The semicoke of generation is sent to two grades of rotating circular disks 5 by one-level propulsion baffle plate 7, and with volatiles in vapor（It is passed through from vapor pore 19）In the presence of gasify, while control import vapor flow 10m3/ h, the temperature of vapor is 200 DEG C, wherein entering the vapor flow of gasification reforming zone in 5m3/ h, remaining vapor is recycled by vapor reuse pipe 17.Under vapor effect, fraction solids（Semicoke）There is cracking reaction, the C in gas in generation gasification reaction, part tarxHyAnd CO2Also reforming reaction is carried out under the synergy of coke/vapor, now pyrolysis devolatilization is divided into 90% in product, wherein condensable property component 0.1%, and semicoke 10%, the lasting 10min of gasification reforming process.Gas after gasification and reformation are processed enters sieve plate 11 from two grades of center-aisles of rotating circular disk 5（The downward-sloping angle of sieve plate is 10 °）And the fraction solids particulate matter in portion gas is removed, and then continue gas solid separation in expansion chamber 12, discharge from gas products outlet 13, obtain the synthesis gas product of high-quality, H2/ CO 1.5, tar content 0.002%（About 20mg/m3）, the conversion efficiency of whole process biological carbon reaches 90%.The coke and ash content of residual advances baffle plate 8 to fall into slag ladle 14 from two grades of center-aisles of rotating circular disk 5 under acting at two grades, by the drive of agitator 15, progressively moves down, and finally removes reaction system by spiral slag-discharging device 16.
Claims (10)
1. a kind of method that material continuous pyrolysis gasify, it is characterised in that including following content：（1）Microwave-heating gasification system is entered by the raw material and catalyst of helical feed, the one-level rotating circular disk in microwave reaction chamber is dropped down onto under gravity and is dried as rotation is sequentially passed through, is activated and pyrolysis processing；（2）Material after pyrolysis processing falls into two grades of rotating circular disks in microwave reaction chamber in the presence of one-level advances baffle plate and proceeds in the presence of vapor gasification and reforming reaction together with volatiles；（3）Jing steps（2）The solid product for processing, including the slag ladle that catalyst, coke and ash content are fallen into below microwave reaction chamber by two grades of propulsion baffle plates from the central aperture of two grades of rotating circular disks, reaction system is discharged in the case where mixing worm double action is stirred, and gaseous product then enters expansion chamber by the annular sieve plate in microwave reaction bottom of chamber portion, Jing settlement treatments obtain gasification product.
2. in accordance with the method for claim 1, it is characterised in that：Step（1）Described raw material is biomass, trade waste, coal or oil shale；Wherein biomass are maize straw, rice husk, straw, wooden unit, leaf or branch, trade waste is the organic wastes such as waste plastic, waste rubber tire, municipal refuse, and coal is brown coal, lower-grade metamorphic bituminous, mesometamorphism bituminous coal and the high deterioration coal of any low caking index.
3. in accordance with the method for claim 2, it is characterised in that：Raw material maximum direction size is less than 50mm.
4. in accordance with the method for claim 1, it is characterised in that：Step（1）Raw material and catalyst microwave reaction chamber and in Action of Gravity Field free-falling to one-level rotating circular disk, 300 ~ 600 DEG C for the treatment of temperature, 1 × 105 ~ 6 × 105W/m of power density is entered by feeding screw3, 1 ~ 10kg/h of feed rate, process time 1 ~ 10 minute.
5. in accordance with the method for claim 1, it is characterised in that：Step（1）Described catalyst is made up of charcoal class microwave absorption, metal oxide and hydroxide, charcoal class microwave absorption is used as carrier, metal oxide and hydroxide are used as active component, wherein metal oxide accounts for the 1% ~ 10% of catalyst quality, hydroxide accounts for the 1% ~ 10% of catalyst quality, balance of carrier；Charcoal class microwave absorption includes activated carbon, biological Jiao, graphite etc., preferred biological burnt；Metal oxide is the one or more combination in the metal oxide with both sexes, including nickel oxide, titanium oxide, zirconium oxide, lanthana, selenium oxide or aluminum oxide, preferred nickel oxide；Hydroxide includes the one or more combination in potassium hydroxide, NaOH, lithium hydroxide, calcium hydroxide or magnesium hydroxide, preferred potassium hydroxide.
6. in accordance with the method for claim 1, it is characterised in that：Catalyst feeds intake mass ratio for 1 with biomass material:2~1:20.
7. in accordance with the method for claim 1, it is characterised in that：Step（2）The gasification and reforming reaction temperature are 600 ~ 800 DEG C, 1 ~ 10 minute reaction time, power density 6 × 105~10×105W/m3, import 1 ~ 10m of vapor flow3/ h, wherein entering the vapor flow of gasification reforming zone in 0.5 ~ 5m3/ h, remaining vapor repeats back to use by hollow rotating shaft, and the temperature of vapor is 120 ~ 200 DEG C.
8. in accordance with the method for claim 1, it is characterised in that：Step（3）Described sieve plate is convex sieve plate, and convex 1 ~ 10cm of length, hole diameter of sieve (perforated) plate Φ 1 ~ Φ 5mm, the downward-sloping angle of sieve plate is 10 ° ~ 60 °.
9. in accordance with the method for claim 1, it is characterised in that：Step（3）Described settlement treatment adopts multilayer expansion chamber.
10. in accordance with the method for claim 1, it is characterised in that：Step（3）The gasification product H for obtaining2/ CO between 1.5 ~ 2.2,10 ~ 20mg/m of tar content3, the conversion efficiency of whole process biological carbon is 90 ~ 98%.
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| CN201510740287.6A CN106675661B (en) | 2015-11-05 | 2015-11-05 | A kind of method of material continuous pyrolysis gasification |
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| CN201510740287.6A CN106675661B (en) | 2015-11-05 | 2015-11-05 | A kind of method of material continuous pyrolysis gasification |
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| CN111848398A (en) * | 2020-07-14 | 2020-10-30 | 重庆市万利来化工股份有限公司 | Dehydrogenation reaction device for synthesizing methyl formate and process thereof |
| CN111848398B (en) * | 2020-07-14 | 2022-11-15 | 重庆市万利来化工股份有限公司 | Dehydrogenation reaction device for synthesizing methyl formate and process thereof |
| CN114479952A (en) * | 2020-10-27 | 2022-05-13 | 中国石油化工股份有限公司 | Biomass hydrogen production heat carrier and preparation method and application thereof |
| CN113289630A (en) * | 2021-05-19 | 2021-08-24 | 哈尔滨工业大学（深圳） | Catalyst for diesel reforming reaction, preparation method thereof, hydrogen production reformer and system |
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