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WO2019029599A1 - Procédé et système d'huile synthétique de micro-biomasse à base de plateforme mobile - Google Patents

Procédé et système d'huile synthétique de micro-biomasse à base de plateforme mobile Download PDF

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Publication number
WO2019029599A1
WO2019029599A1 PCT/CN2018/099536 CN2018099536W WO2019029599A1 WO 2019029599 A1 WO2019029599 A1 WO 2019029599A1 CN 2018099536 W CN2018099536 W CN 2018099536W WO 2019029599 A1 WO2019029599 A1 WO 2019029599A1
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Prior art keywords
biomass
tank
oil
gas
fischer
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English (en)
Chinese (zh)
Inventor
黄·J·R
童浩
郑申棵
朱晓玮
贺蓉
詹晓东
张岩丰
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Wuhan Harvest Yangtze Ecological Technology Research Institute Co Ltd
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Wuhan Harvest Yangtze Ecological Technology Research Institute Co Ltd
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/04—Purifying combustible gases containing carbon monoxide by cooling to condense non-gaseous materials
    • C10K1/046—Reducing the tar content
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
    • C10K3/04—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment reducing the carbon monoxide content, e.g. water-gas shift [WGS]
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0956—Air or oxygen enriched air
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0959—Oxygen
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel

Definitions

  • the invention relates to a biomass synthetic oil system, in particular to a method and system for miniaturizing biomass-based synthetic oil based on a mobile platform.
  • biomass can not only make important contributions to improving the world's primary energy structure and reducing the demand for fossil energy, but also reduce greenhouse gas emissions, ensure energy supply security, and improve trade. It plays a role in balancing, promoting rural development and improving urban waste disposal methods.
  • Biomass Synthetic Oil Technology is one of the most promising biomass energy conversion technologies. Biomass can be converted to liquid fuels through biomass pretreatment, biomass gasification, syngas purification conversion, Fischer-Tropsch synthesis, and optional wax oil processing.
  • the pretreatment process of biomass is to process the biomass raw materials through crushing, drying and molding, so that the water content and particle size of the raw materials reach the requirements of the feed of the gasifier.
  • the gasification process of biomass is a series of high-temperature pyrolysis, oxidation, reduction and reforming reactions of biomass under certain thermodynamic conditions with the aid of a suitable gasifying agent (oxygen or water vapor) to obtain CO and
  • a suitable gasifying agent oxygen or water vapor
  • the crude syngas is dominated by H 2 and is accompanied by CH 4 , CO 2 , tar and residue.
  • Biomass gasification can be divided into fixed bed gasification, moving bed gasification, fluidized bed gasification and entrained flow gasification.
  • the purification process of syngas is to remove impurities such as sulfur, nitrogen, oxygen, chlorine and the like in the raw syngas, and adjust the ratio of H 2 /CO in the syngas to meet the subsequent Fischer-Tropsch synthesis catalyst. And reactor requirements.
  • the Fischer-Tropsch synthesis process converts syngas into synthetic oil (crude naphtha, heavy oil) and crude wax product under certain conditions of temperature and pressure and catalyst.
  • Conventional Fischer-Tropsch reactors have fixed bed reactors, fluidized bed reactors and slurry bed reactors, the catalysts of which are mainly cobalt-based catalysts and iron-based catalysts.
  • the synthetic oil can be further refined through hydrocracking, hydrorefining and fractionation processes to obtain products such as gasoline, diesel, aviation kerosene, wax and lubricating oil.
  • Biomass raw materials have the characteristics of low energy density, complex composition, seasonality and regionality, which bring certain difficulties to the utilization of biomass resources.
  • the cost of collecting and transporting biomass resources is accelerating as the radius of collection increases. Therefore, large-scale bio-based synthetic oil plants have significant challenges and challenges in the collection, storage and supply of biomass materials.
  • biomass resources can be divided into large collection radius biomass resources, medium collection radius biomass resources and small collection radius biomass.
  • the collection radius is 30-80 km, and the annual output is 10,000-20,000 tons of synthetic oil.
  • the small collection radius biomass resources can be supplied to the 1,000-ton BTL plant with a collection radius of 3-10 km and an annual output of 0.6-2 kg. oil.
  • biomass resources are small collection radius biomass resources, which can meet the production needs of thousands of tons of BTL plants.
  • the object of the present invention is to provide a compact, efficient, flexible and convenient mobile platform-based miniaturized biomass synthetic oil method and system.
  • the mobile platform-based miniaturized biomass synthetic oil method is a biomass material gasification unit, a syngas purification conversion unit and a Fischer-Tropsch synthesis unit which are sequentially arranged and arranged on a mobile platform. After the mobile platform is flexibly transported to the biomass distribution site or the set treatment site as needed, the process of synthetic oil production is directly performed on the mobile platform.
  • the process specifically includes the following steps:
  • the biomass raw material having the particle size and the water content satisfying the feeding requirements is sent to the gasification furnace of the biomass raw material gasification unit, and the gas is reacted with air and/or oxygen as a gasifying agent to obtain a crude synthesis gas.
  • the tar in the crude syngas is catalytically cracked into a small molecule gaseous substance by the decoking catalyst in the decoking tank, and then cooled and filtered to obtain a preliminary purified syngas;
  • the preliminary purified synthesis gas is sent to the conversion tank of the synthesis gas purification conversion unit, and the conversion reaction is carried out under the catalysis of the water gas shift catalyst to increase the H 2 /CO ratio; and then sent to the purification tank of the synthesis gas purification conversion unit, By purifying different kinds of degreasers layered in the purification tank, the harmful gas impurities of various properties are removed, and the purified synthesis gas is obtained;
  • the purified synthesis synthesis gas is sent to the Fischer-Tropsch synthesis reactor of the Fischer-Tropsch synthesis unit, and the Fischer-Tropsch synthesis reaction is carried out under the catalysis of the Fischer-Tropsch catalyst, and the reaction product is separated to obtain gas oil, crude naphtha and light hydrocarbon tail gas.
  • the Fischer-Tropsch synthesis reactor adopts a microchannel reactor or a tubular fixed-bed reactor for enhancing heat and mass transfer; wherein the tubular fixed-bed reactor is preferably enhanced by internal members (such as inner fins) in the tube process. Heat transfer mass tubular fixed bed reactor.
  • the microchannel reactor has great advantages in enhancing heat and mass transfer.
  • the internal component is used to enhance heat and mass transfer, so that the reactor can appropriately increase the inner diameter of the reaction pipe and shorten the length of the reactor.
  • the above two Fischer-Tropsch synthesis reactors ensure that the reactor size is reduced and the reactor is miniaturized under a certain production intensity, so that it is more suitable for being arranged on mobile platforms such as vehicles and ships.
  • the gasification furnace has an operating temperature of 800 to 1300 ° C, an operating pressure of 0.08 to 3 MPa, and the gasifying agent is an oxygen-enriched air having an oxygen content of 25 to 50% by weight, and oxygen required.
  • the PSA oxygen generation mechanism is obtained;
  • the decoking catalyst is one or more of a nickel-based catalyst, charcoal, and dolomite,
  • the decoking tank has an operating temperature of 750-900 ° C, and the tar cracking efficiency is 90-99.
  • the heat transfer oil heat exchanger is used for heat exchange and temperature reduction; the temperature of the preliminary purified synthesis gas is 200-400 ° C, the tar content is below 5 mg/Nm 3 , and the particulate matter content is below 5 mg/Nm 3 .
  • the operating pressure of the shift tank is 1 to 3 MPa, the operating temperature is 200 to 400 ° C, and the water gas shift catalyst is a cobalt-molybdenum type water gas shift catalyst;
  • the volume ratio of H 2 /CO is 1.5 to 2.2, the volume content of oxygen is 5 ppm or less, and the volume content of sulfur and chlorine is 0.1 ppm or less.
  • the Co-Mo type shift catalyst is a wide temperature sulfur-tolerant shift catalyst, and the active temperature range is 180-500 ° C.
  • the catalyst has many advantages: 1) sulfur resistance, avoiding the cold and heat disease after the first desulfurization, and the crude synthesis of gasification
  • the amount of water vapor in the gas can meet the requirements of the conversion, without additional steam content; 2) with organic sulfur hydroconversion function, can effectively reduce the content of organic sulfur in the shift gas; 3) high CO conversion activity, especially low temperature activity It is much higher than Fe-Cr catalyst, which can reduce the catalyst loading and reduce the reactor volume.
  • It is suitable for the catalytic conversion of crude syngas with high sulfur content in raw materials, and has the minimum requirement for sulfur in crude syngas. The upper limit is required, so the subsequent purification process is simpler; 5) the catalyst exhibits higher strength.
  • the carrier of the cobalt-molybdenum wide temperature sulfur-tolerant shift catalyst is usually ⁇ -Al 2 O 3 , magnesium-aluminum composite oxide or fine-grained spinel, and thus exhibits high strength, and the strength of the catalyst after vulcanization treatment can be improved.
  • the Fischer-Tropsch synthesis reactor employs a cobalt-based or iron-based catalyst, or a bifunctional catalyst having both cracking effects; the Fischer-Tropsch synthesis reactor is operated at a temperature of 200 to 350 ° C, and is operated.
  • the pressure is 1-3 MPa, the heat transfer coefficient is 0.5-0.8 W/cm 2 /K;
  • the separation of the Fischer-Tropsch synthesis reaction product includes: I) the crude synthetic oil mixture, the waste water and the light hydrocarbon tail gas are separated by at least one-stage cooling, II
  • the crude synthetic oil mixture is further subjected to fractional distillation to obtain gas oil and crude naphtha.
  • the cobalt-based catalyst is a common Fischer-Tropsch synthesis catalyst, which has high Fischer-Tropsch activity and carbon chain growth ability, and has few oxygen compounds in the product, is stable during the reaction, is not easy to deposit carbon and poison, but The methane selectivity is obviously increased during the reaction at high temperature, so it can only work under low temperature conditions and is not sensitive to the water gas shift reaction.
  • the iron-based catalyst is also a common Fischer-Tropsch synthesis catalyst, and the reaction conditions are more adaptable.
  • the iron-based catalyst can synthesize low-carbon olefins, heavy hydrocarbons and oxygenates with high selectivity by adjusting the auxiliary component composition or reaction temperature.
  • the iron-based catalyst has a high activity for water gas shift, and the Fischer-Tropsch reaction can be carried out at a lower H 2 /CO.
  • the bifunctional catalyst having both cracking action is a catalyst which combines a molecular sieve or a noble metal-loaded molecular sieve with a Fischer-Tropsch synthesis catalyst.
  • the bifunctional catalysts with cracking mainly carry out two kinds of reactions, one is the traditional Fischer-Tropsch synthesis reaction for producing hydrocarbon products, and the other is the hydrogenation of hydrocarbon products formed by Fischer-Tropsch synthesis under acid catalysis. Pyrolysis, hydroisomerization and other reactions.
  • one is a physical mixed catalyst, that is, the Fischer-Tropsch synthesis catalyst is mechanically mixed with a solid acid or a solid acid catalyst supporting a noble metal in a certain ratio;
  • the second is a core-shell catalyst, which is at a fee.
  • the active component of the catalyst is deposited on the surface of the solid acid membrane;
  • the third is a supported catalyst, and the active component of the Fischer-Tropsch synthesis catalyst is directly loaded onto the solid acid.
  • molecular sieves are excellent carriers for one-step liquid fuel catalysts for syngas.
  • the separation of the Fischer-Tropsch synthesis reaction product is carried out by two-stage cooling separation, and the first-stage cooling separation is carried out in a thermal separation tank, the operating temperature is 120-180 ° C, the operating pressure is 1-3 MPa, and the separation is performed.
  • the heavy oil, waste water and light hydrocarbon components are discharged;
  • the second stage cooling separation is carried out in a cold separation tank, the operating temperature is 20-40 ° C, the operating pressure is 0.2-3 MPa, and the light hydrocarbon component of the first stage cooling separation is cold.
  • the separation tank is cooled to separate waste water, light oil and light hydrocarbon tail gas.
  • the mobile platform is further integrated with a wax oil processing unit connected to the Fischer-Tropsch synthesis unit; in the step 3), the separation of the reaction product further includes separation of the wax oil, and the separated wax oil is fed.
  • Hydrocracking is carried out in a hydrocracking tank of a wax oil processing unit, and the required hydrogen is supplied by a PSA hydrogen generator of a wax processing unit; the operating temperature of the hydrocracking tank is 300 to 400 ° C, and the operating pressure is 6 ⁇ 10MPa, hydrogen oil volume ratio is 800 ⁇ 1500 (hydrogen oil volume ratio refers to the ratio of working hydrogen in the standard state (1atm, 0 ° C) volume flow rate and feedstock oil volume flow rate), volumetric space velocity is 0.5 ⁇ 2.0h -1 ; The hydrocracked product is fractionated to obtain gas oil and crude naphtha.
  • the biomass pretreatment unit pair is disposed on the mobile platform and connected to the biomass feedstock gasification unit.
  • the biomass raw material is pretreated, that is, the particle diameter of the biomass raw material is controlled to be less than 5 cm by one or more methods of crushing, drying and molding, and the moisture content is controlled to be 25 wt% or less.
  • the removing agent comprises a deoxidizing agent, a dechlorinating agent, a desulfurizing agent, and the removal order is oxygen, chlorine, sulfur;
  • the deoxidizing agent is a copper-based catalyst (3093 deoxidizing agent) supported by activated carbon;
  • the dechlorination agent is a catalyst containing an alkali metal or an alkaline earth metal as an active component, or a transition metal (such as Cu, Zn, Ca, Fe, Mn, etc.) which is easily combined with chlorine as an active component;
  • the desulfurizing agent is Zinc oxide remover.
  • the oxygen content of the syngas must be strictly controlled below 5 ppm to meet the feed requirements of the Fischer-Tropsch reaction process.
  • Chlorine not only poisons the catalyst surface, but also penetrates into the inner layer of the catalyst.
  • chlorine reacts with the desulfurizer zinc oxide. Zinc chloride is formed, and the melting point of zinc chloride is low.
  • the desulfurizing agent is easily sintered to block the pores of the desulfurizing agent, which directly affects the desulfurization effect.
  • chlorine corrodes pipes and equipment, which seriously affects the normal operation of production equipment.
  • the sulfur-containing compound is an impurity gas which is very harmful in the synthesis gas, and easily reacts with the active metal in the Fischer-Tropsch synthesis catalyst to form a metal sulfide having no catalytic activity, causing catalyst poisoning to be deactivated.
  • the light hydrocarbon tail gas is partially or completely sent to a generator set integrated on the mobile platform for power generation for system power supply; if there is surplus, the remaining part of light hydrocarbon tail gas is recycled back to the fee.
  • the synthesis reactor continues to participate in the synthesis reaction, or recycles back to the gasifier to continue to participate in the gasification reaction, so that the light hydrocarbon tail gas is fully utilized, the utilization of biomass resources is improved, and the emission of organic pollutants is reduced.
  • the invention also provides a mobile platform-based miniaturized biomass-based synthetic oil system (Mobility Biomass To Liquid, MBTL for short), which is moved by a mobile platform and performs production activities thereon, and the mobile platform is integrally arranged a biomass feedstock gasification unit, a synthesis gas purification conversion unit, and a Fischer-Tropsch synthesis unit;
  • the biomass feedstock gasification unit includes a gasification furnace for biomass gasification, and a gas for inputting biomass raw materials to the gasification furnace Pulp furnace feeding device, PSA oxygen generator (PSA refers to pressure swing adsorption) which supplies gasification agent for gasification furnace, decoking tank for removing tar in gasification-generated crude syngas, used for heat exchange and cooling a heat transfer oil heat exchanger, a filter for filtering solid particulate matter, and a gas storage tank for buffering preliminary purification of the synthesis gas;
  • PSA oxygen generator refers to pressure swing adsorption
  • the gasification agent inlet of the gasification furnace is
  • the light hydrocarbon tail gas line is also connected to a gasification agent inlet of the gasification furnace and a synthesis gas inlet of a Fischer-Tropsch synthesis reactor, respectively.
  • the mobile platform is further integrated with a wax oil processing unit, and the wax oil processing unit comprises a wax separation tank for separating the crude wax in the Fischer-Tropsch synthesis product, and is used for hydrogenating the separated crude wax.
  • a cracking tank, and a PSA hydrogen producing machine (PSA refers to pressure swing adsorption) for supplying hydrogen to the hydrocracking process;
  • the wax separating tank is disposed between the oil and gas outlet of the Fischer-Tropsch synthesis reactor and the oil and gas inlet of the thermal separation tank
  • the crude wax outlet of the wax separation tank is connected to the crude wax inlet of the hydrocracking tank;
  • the light hydrocarbon tail gas inlet of the PSA hydrogen generator is connected to the light hydrocarbon tail gas line, and the hydrogen of the PSA hydrogen generator
  • the outlet is connected to a hydrogen inlet of the hydrocracking tank;
  • the cracking product outlet of the hydrocracking tank is connected to the crude synthetic oil inlet of the fractionating column.
  • the mobile platform is further integrated with a biomass pretreatment unit, the biomass pretreatment unit comprises a sequentially connected crusher, a dryer and a molding machine; the gasifier feeding device comprises a lock bucket And a screw conveyor, the biomass outlet of the lock bucket is connected to the biomass inlet of the gasifier, the biomass inlet of the lock bucket is connected to the biomass outlet of the screw conveyor; the life of the screw conveyor The material inlet is connected to the biomass outlet of the molding machine.
  • the biomass pretreatment unit comprises a sequentially connected crusher, a dryer and a molding machine
  • the gasifier feeding device comprises a lock bucket And a screw conveyor, the biomass outlet of the lock bucket is connected to the biomass inlet of the gasifier, the biomass inlet of the lock bucket is connected to the biomass outlet of the screw conveyor; the life of the screw conveyor
  • the material inlet is connected to the biomass outlet of the molding machine.
  • the large-scale commercial plant adopts an air separation device to obtain a large amount of oxygen.
  • the air separation device is bulky and complicated in process, and the oxygen is produced through the processes of air compression, purification, refrigeration and cryogenic rectification, and is not applicable to MBTL.
  • MBTL is preferably a PSA oxygen generator, and the smaller volume meets the oxygen supply requirements of a small gasifier, and is suitable for MBTL.
  • the hydrogen production unit selects the PSA hydrogen generator.
  • the purification tank uses physical adsorption to remove gaseous impurities.
  • the composite high-efficiency integrated purification tank can realize the high-efficiency removal of coarse syngas impurities by layering different degreasers in the purification tank with the same working conditions.
  • the purifying tank is small in volume and simple in operation, and is suitable for MBTL.
  • the large-scale commercial plant adopts a slurry bed reactor or a tubular fixed-bed reactor.
  • the volume of the reactor is huge.
  • the reactor volume of Shell's SMDS process is ⁇ 7m ⁇ 20m, the corresponding capacity is 5800bpd; the synthesis reactor adopts microchannel.
  • the reactor or the tubular fixed-bed reactor with enhanced mass transfer heat transfer enhances heat transfer and mass transfer through the change of the reactor configuration, and reduces the reactor volume under the premise of ensuring the yield, and is suitable for MBTL.
  • the invention aims at transforming and utilizing biomass resources in remote rural areas, and integrates biomass pretreatment, gasification, synthesis gas purification conversion, Fischer-Tropsch synthesis, etc. into mobile platforms (such as vehicles, ships, etc.) to form an MBTL system. Realize the processing and utilization of small collection radius biomass resources, while meeting the needs of local synthetic oil products.
  • the MBTL system is innovative and optimized from equipment selection, process parameters and routes, process links, etc. to meet mobility and economic requirements.
  • the advantages of the first MBTL system of the present invention are:
  • the equipment is compact and efficient. In the selection of equipment, such as PSA oxygen generator, decoking tank, heat transfer oil heat exchanger, purification integrated tank, synthetic reactor, etc., the size of the equipment is reduced while ensuring the production scale, making the MBTL process more efficient. .
  • the light hydrocarbon tail gas is used for power generation or partial circulation to participate in gasification or synthesis reaction, which reduces the emission of gaseous pollutants; the produced synthetic wastewater is stored in the waste water tank for unified treatment; the generated gasification waste residue is collected and used for soil fertilization.
  • the invention can process different types of biomass.
  • the mobile platform adopts a vehicle the vehicle can be driven on a road in a remote rural area, and self-powering can be realized during the operation of the system, so that the development of biomass resources in remote rural areas can be well applied. And use.
  • the investment risk is small.
  • the invention has small investment, short construction period, low operating cost and greatly reduced investment risk.
  • FIG. 1 is a schematic diagram of the overall structure of a miniaturized biomass-based synthetic oil system based on a mobile platform provided by the present invention, wherein the pre-processing unit and the wax oil processing unit are optional parts.
  • FIG. 2 and FIG. 3 are process flow diagrams of a miniaturized biomass-based synthetic oil system based on a mobile platform provided by the present invention.
  • FIG. 2 includes a wax oil processing unit
  • FIG. 3 does not include a wax oil processing unit.
  • Embodiment 4 is a three-dimensional perspective view of the apparatus arrangement of Embodiment 1, and the connections between the devices are reasonably set according to the process flow chart.
  • Figure 5 is a three-dimensional perspective view of the apparatus arrangement of Embodiment 4, and the connections between the devices are reasonably set according to the process flow chart.
  • Figure 6 is a schematic view showing the structure of the purification tank of Figure 2.
  • the mobile platform-based miniaturized biomass synthetic oil system uses a mobile platform such as a vehicle or a ship to carry and operate.
  • the vehicle includes a front 100 with a generator and an engine, a frame with a loading function, and at least one container 106 for arranging the installation of the MBTL system.
  • a pre-processing unit 101, a biomass feed gasification unit 102, a syngas purification conversion unit 103, a Fischer-Tropsch synthesis unit 104, an optional wax oil processing unit 105, and an optional generator set are integrally disposed within the container 106.
  • FIG. 3 is a process flow diagram of the MBTL system, wherein FIG. 2 includes a wax oil processing unit, FIG. 3 does not include a wax oil processing unit, and a dashed box indicates an optional device or device.
  • the shape, weight and transportation of transport vehicles are in compliance with the relevant laws and regulations of national road transport.
  • the generator in the front 100 can supply electrical energy for the start of the MBTL system.
  • the container 106 is a 40-foot high cabinet with a size of 11.8m ⁇ 2.13m ⁇ 2.72m and a gross weight of 22t and a volume of 68m 3 .
  • the three side cabinet doors of the container can be opened for easy operation before the production operation of the device.
  • the MBTL system covers an area of 12 to 100 m 2 and carries a height of 1 to 3 m and is transported by a loading vehicle or multiple loading vehicles. When multiple loading vehicles are used, the production operation of the system is achieved by splicing.
  • the biomass feedstock gasification unit 102 includes a gasification furnace 6 for biomass gasification, a gasifier feed device for inputting biomass feedstock to the gasification furnace 6, and a PSA for supplying a gasification agent to the gasification furnace 6.
  • a gas storage tank 11 for initially purifying the synthesis gas is buffered.
  • the gasification agent inlet of the gasification furnace 6 is connected to the gasification agent outlet of the PSA oxygen generator 7, and the synthesis gas outlet of the gasification furnace 6 is connected to the synthesis gas inlet of the decoking tank 8, and the synthesis gas outlet of the decoking tank 8 is
  • the synthesis gas inlet of the heat transfer oil heat exchanger 9 is connected, and the synthesis gas outlet of the heat transfer oil heat exchanger 9 is connected to the synthesis gas inlet of the filter 10, and the synthesis gas outlet of the filter 10 is connected to the synthesis gas inlet of the gas storage tank 11.
  • the gasifier feeding device comprises a lock bucket 5 and a screw conveyor 4, and the biomass outlet of the lock bucket 5 is connected with the biomass inlet of the gasifier 6, the biomass inlet of the lock bucket 5 and the biomass outlet of the screw conveyor 4. Connected.
  • the syngas purification conversion unit 103 includes a compressor 12 for increasing the pressure of the syngas, a shift tank 13 for increasing the H 2 /CO ratio, and a purge tank 14 for removing harmful impurities.
  • the syngas inlet of the compressor 12 is connected to the syngas outlet of the gas tank 11.
  • the syngas outlet of the compressor 12 is connected to the syngas inlet of the shift tank 13, and the syngas outlet of the shift tank 13 is connected to the syngas inlet of the purge tank 14.
  • the Fischer-Tropsch synthesis unit 104 includes a Fischer-Tropsch synthesis reactor 15, a thermal separation tank 16 for successively cooling and separating Fischer-Tropsch synthesis products, a cold separation tank 17, and a fractionation for fractionating the crude synthetic oil mixture obtained by cooling separation.
  • the syngas inlet of the Fischer-Tropsch synthesis reactor 15 is connected to the syngas outlet of the purification tank 14, and the oil and gas outlet of the Fischer-Tropsch synthesis reactor 15 is connected to the oil and gas inlet of the thermal separation tank 16.
  • the gas phase outlet of the hot separation tank 16 is connected to the gas phase inlet of the cold separation tank 17, and the heavy oil outlet of the hot separation tank 16 and the light oil outlet of the cold separation tank 17 are connected to the crude synthetic oil inlet of the fractionation column 18, respectively.
  • the naphtha distillation outlet of the fractionation column 18 is connected to the crude naphtha tank 20, and the diesel outlet of the fractionation column 18 is connected to the gas oil tank 21.
  • the decoking tank 8 is a dry decoking tank using catalytic cracking and decoking.
  • the heat transfer oil heat exchanger 9 is an indirect heat exchanger in which a heat transfer oil is used as a heat exchange medium.
  • the purification tank 14 is a composite high-efficiency integrated tank in which a deoxidizer layer 14.1, a dechlorination agent layer 14.2 and a desulfurizer layer 14.3 are sequentially disposed in the gas flow direction.
  • the Fischer-Tropsch synthesis reactor 15 is a microchannel reactor, or a tubular fixed bed reactor that enhances heat and mass transfer.
  • the biomass pretreatment unit 101 comprises a crusher 1, a dryer 2 and a forming machine 3 which are connected in series, and the biomass outlet of the molding machine 3 is connected to the biomass inlet of the screw conveyor 4. If the biomass feedstock itself meets the feed requirements, the biomass pretreatment unit 101 may not be provided.
  • the light hydrocarbon tail gas outlets of the cold separation tank 17 and the fractionation column 18 are connected to the gas inlet of the generator set through the light hydrocarbon tail gas line.
  • the light hydrocarbon tail gas line is also connected to the gasification agent inlet of the gasification furnace 6, and the synthesis gas inlet of the Fischer-Tropsch synthesis reactor 15, respectively.
  • the wax oil processing unit 105 includes a wax separation tank 22 for separating the crude wax in the Fischer-Tropsch synthesis product, a hydrocracking tank 23 for cracking the separated crude wax, and a hydrogenation of PSA for supplying hydrogen for the hydrocracking process.
  • Machine 24 The wax separation tank 22 is disposed between the oil and gas outlet of the Fischer-Tropsch synthesis reactor 15 and the oil and gas inlet of the thermal separation tank 16, and the crude wax outlet of the wax separation tank 22 is connected to the crude wax inlet of the hydrocracking tank 23.
  • the light hydrocarbon tail gas inlet of the PSA hydrogen generator 24 is connected to a light hydrocarbon tail gas line, and the hydrogen outlet of the PSA hydrogen generator 24 is connected to the hydrogen inlet of the hydrocracking tank 23.
  • the cracked product outlet of the hydrocracking tank 23 is connected to the crude synthetic oil inlet of the fractionation column. If the Fischer-Tropsch synthesis uses a bifunctional catalyst having both cracking action, the wax oil processing unit 105 may not be provided.
  • the collected biomass feedstock first enters the biomass pretreatment unit 101.
  • the biomass raw material is crushed by the crusher 1 to a particle size of 0 to 5 cm; and dried by a dryer 2 to have a moisture content of 0 to 25 wt%; finally, it is extruded through a molding machine 3 to make The particle size of the biomass reaches 0 to 5 cm.
  • the biomass pretreatment unit has a processing capacity of 5 to 150 tpd (tons per day) of biomass. After pretreatment by the biomass pretreatment unit 101, the biomass feedstock can meet the feed requirements of the biomass feedstock gasification unit 102.
  • the biomass pellet obtained by the pretreatment of the biomass material enters the lock bucket 5 through the screw conveyor 4, and the pressure of the lock bucket 5 can reach 0.2 to 3 MPa, and then enters the gasifier 6.
  • the gasification furnace 6 is a horizontal fixed bed gasification furnace or a vertical fixed bed gasification furnace, and the operating temperature is 800 to 1300 ° C, and the operating pressure is 0.08 to 3 MPa.
  • the gasifying agent is air, oxygen-enriched or oxygen. When oxygen or oxygen is used, the PSA oxygen generator 7 is used to supply oxygen to the gasifier.
  • the crude syngas from the gasifier is removed by the decoking tank 8 to remove potential tar, the catalytic decoking temperature is 750-900 ° C, the catalytic decoking efficiency is 90-99%, and then cooled by the heat transfer oil heat exchanger 9 (after heating The heat transfer oil is sent to the external air cooling device or the water cooling device for cooling), the temperature is lowered to 200-400 ° C, the solid impurities are removed through the filter 10, the tar content is 0-5 mg/Nm 3 , and the particulate matter content is 0-5 mg/Nm. 3 .
  • the resulting preliminary purified syngas enters the gas storage tank 11 for temporary storage.
  • the gasification furnace 6 has a gasification intensity of 300 to 1000 kg/m 2 /h, a treatment capacity of 5 to 150 tpd of biomass, and a gas generating capacity of 3,000 to 90,000 Nm 3 /d.
  • the gasification intensity can be controlled at 300 ⁇ 1000kg / m 2 / h, and in this gasification intensity range, the size of the gasifier can be in the vehicle.
  • the preliminary purified synthesis gas from the biomass feedstock gasification unit 102 enters the synthesis gas purification conversion unit 103.
  • the processing capacity of the synthesis gas purification conversion unit is 3000 to 90000 Nm 3 /d, which can increase the H 2 /CO volume ratio in the synthesis gas to 1.5 to 2.2, and the sulfur content and chlorine content are reduced to 0 to 0.1 ppm, including The amount of oxygen is reduced to 0 to 5 ppm.
  • the compressor 12 raises the pressure of the preliminary purification synthesis gas to 1 to 3 MPa and then enters the shift tank 13.
  • the shift tank 13 is a cobalt-molybdenum type water gas shift catalyst having an operating temperature of 200 to 400 ° C and an operating pressure of 1 to 3 MPa, which can increase the H 2 /CO volume ratio to 1.5 to 2.2.
  • the converted syngas enters the purification tank 14, and the operating temperature is 200 to 400 ° C, and the operating pressure is 1 to 3 MPa.
  • the purification tank 14 adopts a composite high-efficiency integrated purification tank, and the different degreasing agents, including a desulfurizing agent, a deoxidizing agent and a dechlorinating agent, are loaded in different tank layers, and the order of removal is oxygen, chlorine and sulfur, and the syngas can be used in the syngas.
  • the sulfur content and chlorine content are reduced to 0-0.1ppm, the oxygen content is reduced to 0-5ppm;
  • the deoxidizer is a copper-based catalyst supported by activated carbon;
  • the dechlorination agent is a catalyst containing an alkali metal or an alkaline earth metal as an active component. Or a transition metal which is easily combined with chlorine is a catalyst of an active ingredient;
  • the desulfurizing agent is a zinc oxide remover.
  • the purge-transformed synthesis gas from the purification conversion unit 103 enters the Fischer-Tropsch synthesis unit 104.
  • the Fischer-Tropsch synthesis reactor 15 has an operating temperature of 200 to 350 ° C and an operating pressure of 1 to 3 MPa.
  • the heat transfer coefficient of the Fischer-Tropsch synthesis reactor is controlled at 0.5-0.8 W/cm 2 /K. In the heat transfer coefficient range, the synthesis reactor can remove the heat generated by the Fischer-Tropsch synthesis reaction in time, and on the other hand, reduce the catalyst bed.
  • the temperature of the layer hot spot increases the service life of the catalyst, and on the other hand, the overall synergistic efficiency of the reactor and the catalyst is improved, and the production capacity is enhanced, so that the demand for the vehicle production can be better met.
  • the Fischer-Tropsch catalyst employs a conventional cobalt- or iron-based catalyst or a bifunctional catalyst having cracking action. If a bifunctional catalyst is used, the Fischer-Tropsch synthesized product exits the Fischer-Tropsch synthesis reactor 15 (Fig. 3) and directly enters the thermal separation tank 16 to obtain heavy oil (mainly diesel components), wastewater and light hydrocarbons, respectively. Component.
  • the thermal separation tank 16 has an operating temperature of 120 to 180 ° C and an operating pressure of 1 to 3 MPa.
  • the wastewater enters the waste water tank 19 from the bottom of the hot separation tank 16, the heavy oil enters the fractionation column 18 from the side line, and the light hydrocarbon component enters the cold separation tank 17.
  • the operating temperature of the cold separation tank 17 is 20 to 40 ° C, and the operating pressure is 0.2 to 3 MPa.
  • the waste water enters the waste water tank 19, and the light oil (mainly the naphtha component) from the side line enters the fractionation tower 18, and the light hydrocarbon tail gas is emitted from the top.
  • Crude naphtha and gas oil are separately obtained from the fractionation column 18, and enter the crude naphtha tank 20 and the gas oil tank 21, respectively.
  • At least a portion of the light hydrocarbon tail gas is sent to the generator set for power generation, and the remainder is recycled back to the Fischer-Tropsch synthesis reactor 15 to continue to participate in the synthesis reaction, or recycled back to the gasifier 6 to continue to participate in the gasification reaction.
  • the gasification waste produced by Fischer-Tropsch synthesis is collected for soil fertilization.
  • the Fischer-Tropsch synthesis product contains a crude wax, which is required to enter the optional wax oil processing unit 105 for wax processing (Fig. 2), specifically: first, the wax separation tank 22, The crude wax and other hydrocarbon components are separated and the other hydrocarbon components enter the thermal separation column 16.
  • the crude wax enters the hydrocracking tank 23 to undergo a hydrocracking reaction, cracks the long-chain hydrocarbon into a short-chain hydrocarbon, and the obtained product enters the fractionating column 18.
  • the operating temperature of the hydrocracking column is 300-400 ° C
  • the operating pressure is 6-10 MPa
  • the hydrogen-oil ratio is 800-1500
  • the volumetric space velocity is 0.5-2.0 h -1 .
  • the circulating hydrogen is supplied from the PSA hydrogen generator 24.
  • the raw material of the hydrogen generator may be derived from the crude syngas of the gas storage tank 11.
  • the biomass processing capacity of the MBTL system is 5 to 150 tpd (ton/day), and the raw materials are agricultural and forestry wastes mainly composed of straw, twigs, sapwood, wood chips, biomass-forming fuel, processed livestock manure, And one or more of the classified household wastes.
  • the synthetic oil has a capacity of 5 to 100 bpd (barrel/day) and the products are crude naphtha and gas oil.
  • the yield of crude naphtha is 15% to 30% (mass fraction)
  • the yield of gas oil is 30% to 75% (mass fraction)
  • the yield of tail gas is 5% to 30% (mass fraction)
  • the yield of a product refers to the mass fraction of each product in the total product.
  • the various unit devices involved above may not be limited to the biomass synthetic oil technology, and may be used alone or in combination with other processes: 1) the pretreatment unit may be separately used for biomass crushing treatment; 2) the biomass feed gasification unit may be applied. The gasification process for other applications of syngas; 3) the syngas purification conversion unit can be applied to other gas purification processes; 4) the Fischer-Tropsch synthesis unit can be applied to natural gas, flare gas, oil field gas, gas purge As a raw material Fischer-Tropsch synthesis process, the synthesis reactor can be used as a highly efficient heat exchanger without loading the catalyst; 5) The wax oil processing unit can also be used in other hydrocracking and hydrofinishing processes.
  • the straw is used as a biomass raw material
  • the treatment amount is 12 tpd
  • the production capacity is 10 bpd synthetic oil.
  • All equipment is installed in a container, and the installation is shown in Figure 4.
  • the Fischer-Tropsch synthesis reactor 15 employs a microchannel reactor, and the Fischer-Tropsch synthesis catalyst employs a bifunctional catalyst having a cracking action.
  • the Fischer-Tropsch synthesized oil contains no wax, so the wax oil processing unit 105 is not used.
  • Light hydrocarbon tail gas is all used to generate electricity to power the system.
  • Table 1 The specific process parameters are shown in Table 1.
  • the sapwood is a biomass material
  • the treatment amount is 18 tpd
  • the production capacity is 30 bpd synthetic oil.
  • the Fischer-Tropsch synthesis reactor 15 employs a microchannel reactor, and the Fischer-Tropsch synthesis catalyst employs a bifunctional catalyst having a cracking action.
  • the Fischer-Tropsch synthesized oil contains no wax, so the wax oil processing unit 105 is not used.
  • Light hydrocarbon tail gas is all used to generate electricity to power the system.
  • Table 1 The specific process parameters are shown in Table 1.
  • the straw-forming fuel is used as a biomass material
  • the treatment amount is 45 tpd
  • the production capacity is 50 bpd.
  • the Fischer-Tropsch synthesis reactor 15 employs a tubular fixed bed reactor, the catalyst uses an iron-based catalyst, and the Fischer-Tropsch synthesized oil contains wax oil, so a wax oil processing unit 105 is required.
  • the light hydrocarbon tail gas is recycled back to the Fischer-Tropsch synthesis reactor and the other half is used to generate electricity for the system.
  • the specific process parameters are shown in Table 1.
  • a mixture of chicken manure and sapwood (mass ratio 1:1) is used as a biomass material, the treatment amount is 63 tpd, and the production capacity is 70 bpd synthetic oil. All equipment is installed in three containers, and the installation is shown in Figure 5.
  • the Fischer-Tropsch synthesis reactor 15 uses a microchannel reactor, the Fischer-Tropsch synthesis catalyst uses a cobalt-based catalyst, and the Fischer-Tropsch synthesized oil contains a wax oil, so a wax oil processing unit 105 is required.
  • the light hydrocarbon tail gas is recycled halfway back to the Fischer-Tropsch synthesis reactor and the other half is used to power the system.
  • the specific process parameters are shown in Table 1.
  • a mixture of domestic garbage and sapwood (1:1) is used as a biomass material, and the treatment amount is 108 tpd, and the production capacity is 90 bpd synthetic oil.
  • the Fischer-Tropsch synthesis reactor 15 employs a microchannel reactor, and the catalyst employs a cobalt-based catalyst having a cracking action.
  • the Fischer-Tropsch synthesized oil does not contain wax, so the wax oil processing unit 105 is not used.
  • a quarter of the light hydrocarbon tail gas is recycled back to the synthesis reactor 15, one quarter of which is recycled back to the gasifier 6, and the remaining one is used to generate electricity to power the system.
  • the specific process parameters are shown in Table 1.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Abstract

L'invention concerne une procédé et un système d'huile synthétique de micro-biomasse à base de plateforme mobile, le procédé comprenant l'intégration sur une plateforme mobile d'une unité de gazéification de matière première de biomasse, d'une unité de conversion de purification de gaz synthétique, et une unité de synthèse de fischer-tropsch qui sont connectées en séquence et, après que la plateforme mobile soit transportée de manière flexible en fonction des exigences d'un site de distribution de biomasse ou d'un site de manipulation défini, la mise en œuvre directe d'un processus de production d'huile synthétique sur la plateforme mobile. Le système comprend une unité de gazéification de matière première de biomasse utilisée pour la gazéification de biomasse, une unité de conversion de purification de gaz synthétique utilisée pour la purification et la conversion de gaz synthétique brut, et une unité de synthèse de fischer-tropsch utilisée pour mettre en œuvre une synthèse de fischer-tropsch sur le gaz synthétique purifié et converti tous intégrés sur une plateforme mobile. Ce système peut être déplacé au moyen d'un montage sur une plateforme mobile, et une activité de production est mise en œuvre sur celle-ci, présentant les avantages d'être sur une micro-échelle, mobile, économiquement réalisable, flexible et pratique.
PCT/CN2018/099536 2017-08-11 2018-08-09 Procédé et système d'huile synthétique de micro-biomasse à base de plateforme mobile Ceased WO2019029599A1 (fr)

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CN110975883B (zh) * 2019-12-05 2023-03-24 东北石油大学 一种用于二氧化碳加氢制航空煤油的双功能核-壳催化剂的制备方法
CN112280584A (zh) * 2020-09-15 2021-01-29 四川仪陇益邦能源有限公司 一种利用生物质能制造环保溶剂和石蜡的方法及其设备
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