WO2022166174A1 - 利用双燃料rcci发动机合成碳纳米管的装置和方法 - Google Patents

利用双燃料rcci发动机合成碳纳米管的装置和方法 Download PDF

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WO2022166174A1
WO2022166174A1 PCT/CN2021/114562 CN2021114562W WO2022166174A1 WO 2022166174 A1 WO2022166174 A1 WO 2022166174A1 CN 2021114562 W CN2021114562 W CN 2021114562W WO 2022166174 A1 WO2022166174 A1 WO 2022166174A1
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engine
fuel
carbon nanotubes
solenoid valve
dual
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French (fr)
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毛功平
徐志建
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Jiangsu University
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02D—CONTROLLING COMBUSTION ENGINES
    • F02D19/00—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures
    • F02D19/06—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures peculiar to engines working with pluralities of fuels, e.g. alternatively with light and heavy fuel oil, other than engines indifferent to the fuel consumed
    • F02D19/08—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures peculiar to engines working with pluralities of fuels, e.g. alternatively with light and heavy fuel oil, other than engines indifferent to the fuel consumed simultaneously using pluralities of fuels
    • F02D19/082—Premixed fuels, i.e. emulsions or blends
    • F02D19/084—Blends of gasoline and alcohols, e.g. E85
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
    • F01N3/022—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters characterised by specially adapted filtering structure, e.g. honeycomb, mesh or fibrous
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion
    • F01N3/206—Adding periodically or continuously substances to exhaust gases for promoting purification, e.g. catalytic material in liquid form, NOx reducing agents
    • F01N3/2066—Selective catalytic reduction [SCR]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02D—CONTROLLING COMBUSTION ENGINES
    • F02D45/00—Electrical control not provided for in groups F02D41/00 - F02D43/00
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M26/00—Engine-pertinent apparatus for adding exhaust gases to combustion-air, main fuel or fuel-air mixture, e.g. by exhaust gas recirculation [EGR] systems
    • F02M26/52—Systems for actuating EGR valves
    • F02M26/53—Systems for actuating EGR valves using electric actuators, e.g. solenoids

Definitions

  • the invention belongs to the fields of new energy development and waste gas reuse, and in particular relates to a device and method for synthesizing carbon nanotubes by utilizing dual-fuel reactivity to control the combustion flame in the cylinder of a compression ignition engine.
  • Carbon nanotubes have many excellent properties, such as high electrical and thermal conductivity, and strong mechanical properties. Since the nineteenth century, the research on carbon has been continuously relied on, and carbon nanoparticles such as carbon fibers and carbon nanotubes have been continuously synthesized and used. At present, the preparation methods of carbon nanotubes mainly include graphite arc method, laser evaporation method, chemical vapor deposition method, flame method and so on. Carbon nanotubes are divided into single-walled carbon nanotubes and multi-walled carbon nanotubes.
  • nanotubes can be used as The research and development of effective nano-carriers for transporting anti-cancer drugs and biological agents into cells can also be used to produce a series of bio-detectors for bio-diagnosis and preparation detection.
  • a series of electromechanical devices such as carbon nanotube-based molecular gears, nano-frequency resonators, and nano-actuators have been fabricated.
  • the flame method uses catalysts, such as Ni, Fe, etc., to catalyze the growth of carbon nanoparticles into carbon nanotubes in the process of catalyzing flame combustion.
  • the nanocarbon particles are most suitable for the growth of carbon nanotubes.
  • the engine produces a large amount of CO as a carbon source in RCCI combustion, while producing less other pollutants.
  • the production of carbon nanotubes by the traditional flame method does not have the conditions for continuous and mass production.
  • the use of flame has potential safety hazards, and the exhaust gas is difficult to handle and easily pollutes the atmosphere. If it is simply not economical to prepare carbon nanotubes, it has a large defect in industrial production.
  • the present invention provides a device and method for synthesizing carbon nanotubes by utilizing dual-fuel reactivity to control the combustion flame in a compression ignition engine cylinder, which can not only improve the economy of the engine, but also improve the combustion characteristics of the engine. It can reduce the generation of emission pollutants, and can greatly reduce the comprehensive operating cost of the engine through the production of high value-added carbon nanomaterials.
  • the present invention achieves the above technical purpose through the following technical means.
  • a device for synthesizing carbon nanotubes using a dual-fuel RCCI engine including:
  • Control system including ECU and coolant temperature sensor, pressure sensor and crankshaft position sensor connected with ECU signal;
  • the reaction system includes an engine, a fuel tank A and a fuel tank B, the engine is in communication with the fuel tank A and the fuel tank B, respectively, the fuel tank A is filled with highly reactive fuel, and the fuel tank B is filled with ethanol and nitric acid A mixture of iron powders;
  • After-treatment system including nanotube trap, air compressor and metal filter screen, pressure sensor and nanotube trap are sequentially placed in the exhaust pipe of the engine along the exhaust direction.
  • An exhaust branch pipe is arranged between the valve A and the nanotube trap, and a solenoid valve B is arranged at the inlet of the exhaust branch pipe, and a metal filter screen is arranged at the end of the exhaust branch pipe;
  • the rear end of the nanotube trap is also provided with a solenoid valve C, an air compressor is arranged between the electromagnetic valve C and the nanotube trap;
  • a pipe connected to the engine intake pipe is arranged at the rear end of the electromagnetic valve C, and an EGR valve is arranged on the pipe.
  • an air filter and a compressor are sequentially arranged in the intake duct of the engine along the intake direction.
  • a fuel nozzle A is installed in the intake pipe at the rear of the compressor, and the fuel nozzle A is connected to the fuel tank B through a pipe.
  • a fuel nozzle B is installed on the cylinder of the engine, and the fuel nozzle B is connected with the fuel tank A through a pipeline.
  • the highly reactive fuel is diesel or biodiesel.
  • an exhaust gas turbine is provided at the end of the exhaust pipe of the engine.
  • a method for synthesizing carbon nanotubes using a dual-fuel RCCI engine specifically:
  • Ethanol is first injected into the cylinder of the engine to form a mixture with air, and high reactive fuel is injected in the final stage of compression. After the reaction, the carbon nanotubes entering the exhaust pipe of the engine are captured by the nanotube trap;
  • the temperature in the cylinder of the engine is maintained at 800-1000°C, and the rotational speed of the engine is 500-1200 r/min.
  • the diesel fuel injection advance angle is decreased or the EGR rate is decreased or the consumption ratio of ethanol to high reactivity fuel is increased.
  • the range of the fuel injection advance angle is -40--25°, and the range of the EGR rate is 10-20%.
  • the ECU controls the solenoid valve A and the solenoid valve C to close, the solenoid valve B and the air machine to open, and uses the air machine and the nano filter to collect carbon nanotubes.
  • the invention utilizes a dual-fuel RCCI engine, injects volatile and low-reactivity fuel ethanol into the intake port, injects high-reactivity fuel (such as diesel and biodiesel) in the cylinder, and controls the injection timing of two different reactivity fuels (injection time). oil advance angle), injection amount (equivalent ratio), realize low-temperature premixed combustion, and form the concentration field, temperature field, reaction duration and other conditions of the precursor material most conducive to the growth of carbon nanotubes, and promote carbon nanotubes in the cylinder. continuous growth within.
  • high-reactivity fuel such as diesel and biodiesel
  • the present invention also selects ferric nitrate powder as the precursor material of the catalyst, which is dissolved in ethanol; the mixture of ethanol and air injected in the intake port enters the cylinder, and in the final stage of compression, a certain amount of highly reactive fuel is injected to realize RCCI combustion; in the combustion process, ferric nitrate is decomposed into Fe 2 O 3 at high temperature, which acts as a catalyst for the growth of carbon nanotubes, and the in-cylinder sulfide is a promoter. A large amount of CO generated during the combustion process is used as a carbon source, and the heat released by the combustion is used as a heat source.
  • carbon nanotubes are formed; the formed carbon nanotubes are discharged from the engine with the exhaust gas, and are in the pipeline by the nanotubes. It is captured by the trap; the remaining exhaust gas is discharged into the air after being treated by SCR, so as to realize clean emission; the captured carbon nanotubes can be recovered and purified after being backflushed by the nanotube trap for commercial use.
  • the invention realizes the batch preparation of carbon nanotubes through optimal combustion control, which can not only improve the economy of the engine, improve the combustion characteristics of the engine, and reduce the generation of emission pollutants, but also through the production of high value-added carbon nanomaterials, greatly improving the reduce the overall operating cost of the engine.
  • FIG. 1 is a schematic structural diagram of a device for synthesizing carbon nanotubes by utilizing dual-fuel reactivity to control the combustion flame in a compression ignition engine cylinder according to the present invention
  • the growth conditions for the commercial production of carbon nanotubes are extremely harsh, requiring a stable carbon source within a certain temperature range, as well as catalysts and promoters to accelerate the development of carbon nanotubes.
  • 600-1200°C is very beneficial to the growth of carbon nanotubes
  • the maximum combustion temperature of RCCI (Reactivity Controlled Compression Ignition) of the engine is about 1000°C.
  • the combustion temperature range is controlled within 800-1000° C., which is beneficial to the growth of carbon nanotubes, and can especially generate high-purity single-walled carbon nanotubes; the present invention ECU3 controls the engine to generate a large amount of CO and reduce the generation of HC and NOx with the help of the characteristics of the RCCI engine under a certain speed, load, equivalence ratio and fuel injection timing.
  • a large amount of CO is accumulated in the cylinder, while CO is also the main carbon source for the growth of carbon nanotubes, and a carbon monoxide-rich environment is formed in the cylinder, which can fully meet the needs of carbon nanotube growth.
  • the growth process of CO into carbon nanotubes is slow at a suitable temperature, so the growth process needs to be accelerated under the dual action of catalysts and promoters; iron, cobalt, nickel, and their metal salts, metal oxides, etc. are CO growth It is an effective catalyst for carbon nanotube formation, so 5000ppm of ferric nitrate powder 4 can be dissolved in ethanol 18. Compared with other metals and their salts and oxides, ferric nitrate has low toxicity and is easy to collect waste gas; Fe2O3 particles , which act as catalysts for CO growth. At a suitable temperature, CO gradually dissolves around these nanoparticles and grows into carbon nanotubes.
  • the grown carbon nanotubes are mixed with iron particles of Fe 2 O 3 and enter the exhaust pipe to be collected by the nanotube trap 5 , and the rest of the exhaust gas is treated by SCR6 and then discharged into the atmosphere.
  • a solenoid valve A15 and a solenoid valve C23 are respectively installed before and after the nanotube trap 5
  • an exhaust branch pipe is installed between the solenoid valve A15 and the nanotube trap 5
  • a solenoid valve is installed at the inlet of the exhaust branch pipe B22.
  • a high temperature resistant metal filter screen 16 is arranged in the exhaust branch pipe, and a pressure sensor 9 is arranged at the front end of the solenoid valve A15.
  • the ECU 3 controls the engine 1 to shut down, and closes the solenoid valve A15 and the solenoid valve C23 of the nanotube trap 5 after a period of time, and opens the solenoid valve B22 at the inlet of the exhaust branch pipe.
  • An air compressor 17 is installed between the DPF5 and the solenoid valve C23, the carbon nanotubes in the recoil nanotube trap 5 enter the exhaust branch pipe, and are collected after passing through the high temperature resistant nano filter screen 16 at the tail end of the exhaust branch pipe; The whole stage from the generation of the tube to the collection can realize the batch collection, green production and low emission of carbon nanotubes.
  • the device for synthesizing carbon nanotubes by using dual-fuel reactivity to control the combustion flame in a compression ignition engine cylinder includes a control system, a reaction system, an aftertreatment system and an EGR system.
  • the EGR system includes an EGR valve 8, a compressor 11, Exhaust gas turbine 12 and air cleaner 13 .
  • the control system includes an ECU3, a coolant temperature sensor 10, a pressure sensor 9 and a crankshaft position sensor 2.
  • the coolant temperature sensor 10 is provided in the cylinder coolant to obtain the temperature of the coolant in the cylinder, and the pressure sensor 9 is mounted on the exhaust pipe.
  • the crankshaft position sensor 2 is installed at the crankshaft of the engine to obtain the position of the piston and the speed of the engine; from the speed of the engine, the temperature of the coolant and the load signal (sent from the ECU3 to the engine 1) to obtain the in-cylinder temperature, the coolant
  • the temperature sensor 10 , the pressure sensor 9 and the crankshaft position sensor 2 are all connected to the ECU 3 for signal connection.
  • the reaction system includes an engine 1, a fuel nozzle A7, a fuel tank A14, ferric nitrate powder 4, ethanol 18, a highly reactive fuel 19 (such as diesel, biodiesel), a fuel nozzle B21 and a fuel tank B20, and the fuel nozzle B21 is installed in the engine 1
  • the fuel nozzle B21 is connected to the fuel tank A14 through a pipeline, and the fuel tank A14 is equipped with a highly reactive fuel 19;
  • the intake pipeline of the engine 1 is sequentially provided with an air filter 13 and a compressor along the intake direction. 11, and a fuel nozzle A7 is installed in the intake duct at the rear of the compressor 11.
  • the fuel nozzle A7 is connected to a fuel tank B20 through a pipeline, and the fuel tank B20 contains a mixture of ethanol 18 and ferric nitrate powder 4.
  • the aftertreatment system includes a nanotube trap 5, SCR6 (selective catalytic reduction system), an air compressor 17 and a high temperature resistant metal filter 16.
  • the exhaust pipe of the engine 1 is provided with pressure sensors 9, Nanotube trap 5, SCR6 and exhaust gas turbine 12, a solenoid valve A15 is provided at the pressure sensor 9, an exhaust branch pipe is provided between the solenoid valve A15 and the nanotube trap 5, and an electromagnetic valve is provided at the inlet of the exhaust branch pipe Valve B22, the end of the exhaust branch pipe is provided with a high temperature resistant metal filter screen 16; a solenoid valve C23 is provided between the nanotube trap 5 and the SCR6, and an air compressor 17 is provided between the solenoid valve C23 and the DPF5; the solenoid valve C23 and the A pipe communicating with the intake pipe of the engine 1 is provided between the SCR6, and an EGR valve 8 is provided on the pipe.
  • the working principle of the device for synthesizing carbon nanotubes by controlling the combustion flame in the cylinder of a compression ignition engine with dual fuel reactivity is as follows:
  • Ethanol 18 is injected into the cylinder in advance to form a mixture with air, and then diesel (high reactivity fuel 19) is injected at the end of the compression stage to cause the diesel to spontaneously ignite under high pressure; this process is a special RCCI combustion, resulting in the formation of More CO and HC and lower combustion temperature also form the necessary conditions for the formation of carbon nanotubes - carbon source and temperature; a certain amount of iron nitrate powder 4 is added to ethanol 18, and the combustion in cylinder 1 of the engine is extremely high.
  • the introduction of EGR technology realizes that part of the sulfide re-enters the cylinder, increases the sulfide concentration in the cylinder, and avoids the increase of emissions caused by the addition of additional sulfide.
  • the introduction of EGR will also reduce the in-cylinder temperature and NOx emissions. Not only can the in-cylinder temperature be adjusted between 800 and 1000°C through the EGR rate, but also NOx emissions can be reduced.
  • controlling the fuel injection advance angle, ethanol-diesel equivalence ratio, ethanol purity, engine speed, and engine load can increase CO emissions and reduce HC and NOx emissions, establishing excellent conditions for the carbon source of carbon nanotubes, which can greatly Reduce the emission of other pollutants in the RCCI process.
  • the generated carbon nanotubes will wrap the Fe 2 O 3 nanoparticles from the exhaust manifold into the exhaust pipe and take them out of the cylinder to avoid abnormal engine combustion caused by the retention of Fe 2 O 3 .
  • the carbon nanotubes entering the exhaust pipe are captured by the nanotube trap 5. When the nanotube trap 5 is fully collected, the value collected by the pressure sensor 9 installed in the pipeline increases, and the signal is transmitted to the ECU 3.
  • the ECU3 closes the solenoid valve A15 and the solenoid valve C23 in operation according to the signal value, and simultaneously opens the solenoid valve B22 and the air machine 17 of the exhaust branch pipe, and uses high-pressure air to recoil the carbon nanotube particles in the nanotube trap 5 to a high temperature resistance.
  • the collection is completed at the nano filter screen 16; the remaining exhaust gas is discharged into the air after the NOx is processed by the SCR6 and the exhaust gas turbine 12.
  • the diesel oil used in this example is the standard National V diesel oil, and the ethanol is anhydrous ethanol with a content greater than or equal to 99.7%, and its purity is self-configured in the later stage.
  • the emission of carbon source CO and HC in the cylinder is measured by the exhaust gas analyzer, and the concentration of NOx is detected by the NOx detection analyzer; content, EGR rate and engine speed), detect three main gas concentrations, and collect soot particles under different variables, observe their morphology characteristics under TEM scanning, focus on the purity and morphology of carbon nanotubes, and try to generate a single Morphology of carbon nanotubes.
  • Carbon nanotubes are discharged from the cylinder after being formed. After being processed by the nanotube trap 5, the carbon nanotubes can be collected well, and the post-processing system can also well capture the Fe 2 discharged from the cylinder. O 3 .

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Abstract

一种利用双燃料RCCI发动机合成碳纳米管的装置，包括反应系统、后处理系统和控制系统；反应系统包括发动机(1)、燃料箱A(14)和燃料箱B(20)，两燃料箱分别用于向发动机(1)供应混有硝酸铁的乙醇、高反应性燃料，在发动机气缸反应后的气体经后处理系统，实现碳纳米管的捕集；还公开了利用双燃料RCCI发动机合成碳纳米管的装置的合成方法；实现碳纳米管制备的同时，能提高发动机的经济性、改善发动机的燃烧特性、减少排放污染物的生成。

Description

利用双燃料RCCI发动机合成碳纳米管的装置和方法 技术领域
本发明属于新能源开发及废气再利用领域，具体涉及一种利用双燃料反应性控制压燃发动机缸内燃烧火焰合成碳纳米管的装置和方法。
背景技术
汽车作为一种逐渐普及的交通工具，其尾气排放的有害物质越来越受到人们的重视。柴油机作为汽车发动机的一种，在使用过程中存在噪声大、碳烟颗粒多等缺点，尤其碳烟颗粒的降低一直是研究重点。在添加纳米燃油添加剂后，虽然可以使一部分碳颗粒细化成纳米颗粒，但是纳米颗粒能够轻易穿过普通口罩，对人体造成极大的伤害。利用碳纳米管制备技术能够充分利用汽车所排放的尾气中的纳米碳颗粒，是解决我国现阶段环境问题的一个有效途径。
碳纳米管有着许多优异的性能，如较高的导电和导热能力，以及力学性能极强。自十九世纪对碳的研究不断深入依赖，碳纤维、碳纳米管等碳类纳米颗粒被不断合成、运用。目前，碳纳米管的制备方法主要有石墨电弧法、激光蒸发法、化学气相沉积法、火焰法等。碳纳米管分为单壁碳纳米管和多壁碳纳米管，在能源领域可以制备具有高灵敏度的气体探测器，也能是较为理想的储氢材料；在生物医药领域，碳纳米管能作为很好地抗癌药物、生物成剂等运输至细胞内的有效纳米载体的制备研发，也可制作一系列生物诊断、制剂检测的生物探测器；在纳米机电领域，凭借着高力学性能，能制作出一系列碳纳米管基分子齿轮、纳米高频谐振器以及纳米驱动器等机电器件。火焰法是利用催化剂，如Ni、Fe等，催化火焰燃烧过程中的碳纳米颗粒生长为碳纳米管，当温度为700℃左右时，纳米碳颗粒最适合向碳纳米管生长。发动机在RCCI燃烧中产生大量的CO可作为碳源，同时生成的其他污染物较少。传统火焰法制造碳纳米管不具备连续、批量生产的条件，火焰的使用具有安全隐患，其排放气体难以处理容易污染大气。如果作为单纯制备碳纳米管缺乏经济性，因此在工业生产上有较大的缺陷。
发明内容
针对现有技术中存在不足，本发明提供了一种利用双燃料反应性控制压燃发动机缸内燃烧火焰合成碳纳米管的装置和方法，不仅能提高发动机的经济性，改善发动机的燃烧特性，减少排放污染物的生成，还能通过高附加值碳纳米材料的生产，极大的降低发动机的综合运行成本。
本发明是通过以下技术手段实现上述技术目的的。
利用双燃料RCCI发动机合成碳纳米管的装置，包括：
控制系统，包括ECU以及与ECU信号连接的冷却液温度传感器、压力传感器和曲轴位置传感器；
反应系统，包括发动机、燃料箱A和燃料箱B，发动机分别与燃料箱A和燃料箱B连通，所述燃料箱A中装有高反应性燃料，所述燃料箱B中装有乙醇和硝酸铁粉末的混合物；
后处理系统，包括纳米管捕集器、空压机和金属滤网，压力传感器和纳米管捕集器沿排气方向依次在发动机的排气管道中，压力传感器处设有电磁阀A，电磁阀A和纳米管捕集器之间设有排气支管，且排气支管入口处设有电磁阀B，排气支管末端设有金属滤网；纳米管捕集器后端还设有电磁阀C，电磁阀C与纳米管捕集器之间设有空压机；电磁阀C后端设有与发动机进气管道连通的管道，且管道上设有EGR阀。
上述技术方案中，所述发动机的进气管道中沿进气方向依次设有空气滤清器和压气机。
上述技术方案中，所述压气机后部的进气管道中安装有燃料喷嘴A，燃料喷嘴A通过管道与燃料箱B连接。
上述技术方案中，所述发动机的气缸上安装有燃料喷嘴B，燃料喷嘴B与燃料箱A通过管道连接。
上述技术方案中，所述高反应性燃料为柴油或生物柴油。
上述技术方案中，所述发动机的排气管道末端设有废气涡轮。
一种利用双燃料RCCI发动机合成碳纳米管的方法，具体为：
乙醇先喷入到发动机的气缸内，与空气形成混合气，在压缩终了阶段喷入高反应性燃料，反应后，进入到发动机排气管道中的碳纳米管被纳米管捕集器捕集；
所述乙醇中加入5000ppm的硝酸铁粉末；所述乙醇与高反应性燃料的消耗量比值为0.4-0.67；
反应过程中，发动机气缸内的温度保持在800～1000℃，发动机的转速为500～1200r/min。
进一步，当温度低于800℃，减小柴油喷油提前角或者减小EGR率或者增大乙醇与高反应性燃料的消耗量比值。
进一步，所述喷油提前角的范围是-40～-25°，所述EGR率的范围是10～20％。
进一步，当压力传感器采集的数值变大时，ECU控制电磁阀A和电磁阀C关闭、电磁阀B和空气机打开，利用空气机和纳米滤网收集碳纳米管。
本发明的有益效果为：
本发明利用双燃料RCCI发动机，进气道喷射易挥发、低反应性的燃料乙醇，缸内喷射 高反应性燃料(如柴油、生物柴油)，通过控制两种不同反应性燃料的喷射时刻(喷油提前角)、喷射量(当量比)，实现低温预混合燃烧，并形成最有利于碳纳米管生长的前驱体物质的浓度场、温度场、反应持续时间等条件，促进碳纳米管在缸内持续生长。本发明还选取硝酸铁粉末作为催化剂的前驱体物质，溶解于乙醇中；在进气道喷射的乙醇与空气的混合物进入气缸内，在压缩终了阶段，喷入一定量的高反应性燃料，实现RCCI燃烧；燃烧过程中，硝酸铁在高温下分解成Fe 2O 3，作为碳纳米管生长的催化剂，缸内硫化物为促进剂。燃烧过程中产生的大量CO作为碳源，燃烧放出的热量作为热源，在催化剂Fe 2O 3的作用下，形成碳纳米管；成形的碳纳米管随废气排出发动机，并在管道中被纳米管捕集器捕获；剩余排气经SCR处理后排入空气中，从而实现清洁排放；被捕获的碳纳米管可经纳米管捕集器反冲后回收、提纯，实现商业利用。本发明通过燃烧优化控制，实现碳纳米管的批量制备，不仅能提高发动机的经济性，改善发动机的燃烧特性，减少排放污染物的生成，还能通过高附加值碳纳米材料的生产，极大的降低发动机的综合运行成本。
附图说明
图1为本发明所述利用双燃料反应性控制压燃发动机缸内燃烧火焰合成碳纳米管的装置结构示意图；
图中：1.发动机、2.曲轴位置传感器、3.ECU、4.硝酸铁粉末、5.纳米管捕集器、6.SCR、7.燃料喷嘴A、8.EGR阀、9.压力传感器、10.冷却液温度传感器、11.压气机、12.废气涡轮、13.空气滤清器、14.燃料箱A、15.电磁阀A、16.耐高温金属滤网、17.空压机、18.乙醇、19.高反应性燃料、20.燃料箱B、21.燃料喷嘴B、22.电磁阀B、23.电磁阀C。
具体实施方式
下面结合附图以及具体实施例对本发明作进一步的说明，但本发明的保护范围并不限于此。
碳纳米管的商业化生产的生长条件极为苛刻，需要在一定的温度范围内，有着稳定的碳源，并有催化剂与促进剂加快碳纳米管发展。对于碳纳米管的生长温度而言，600-1200℃极有利于碳纳米管的生长，而发动机的RCCI(Reactivity Controlled Compression Ignition，反应性控制压燃)燃烧最高温度在1000℃左右，本发明在经过对EGR率、喷油时刻、乙醇柴油当量比控制后，燃烧温度区间控制在800-1000℃内，有利于碳纳米管的生长，尤其是能够生成高纯度的单壁碳纳米管；本发明中，ECU3控制发动机在一定的转速、负荷、当量比、喷油时刻下，借助RCCI发动机的特点生成大量CO，并减少HC和NOx的生成，该过程中，在缸内聚集大量的CO，而CO也是碳纳米管生长的主要碳源，在气缸内形成富一氧化碳的环境，完全能满足碳纳米管生长的需要。CO在适宜的温度下生长为碳纳米管的过程是缓慢的， 因此需要催化剂和促进剂的双重作用下加速生长过程；铁、钴、镍，及其金属盐、金属氧化物等正是CO生长成碳纳米管的有效催化剂，因此在乙醇18内溶解5000ppm的硝酸铁粉末4，硝酸铁相对其他金属及其盐、氧化物毒性低、废气易收集；硝酸铁在高温下极易分解，分解成Fe 2O 3颗粒，可作为CO生长的催化剂。在适宜的温度下，CO在这些纳米颗粒周围逐渐溶解、生长为碳纳米管，同时铁纳米颗粒会被包裹在碳纳米管中央，并随着排气一起排出气缸，并不会对缸内燃烧产生额外的影响。经过研究发现，硫化物与金属颗粒的组合更容易促进碳纳米管的生长，而柴油相对其他燃料本身就含有很高的硫化物(促进剂)，在EGR的作用下部分排出气缸的硫化物会在EGR的作用下返回缸内，使得缸内硫化物含量增加，因此无需额外添加硫化物，这也无形中减少了碳纳米管火焰制备法过程中硫化物的排放。生长出的碳纳米管夹杂着Fe 2O 3的铁颗粒，进入到排气管中被纳米管捕集器5收集，其余排气经SCR6处理后排入大气中。排气管道中纳米管捕集器5前后分别安装有电磁阀A15和电磁阀C23，电磁阀A15与纳米管捕集器5之间安装有排气支管，且排气支管入口处安装有电磁阀B22、排气支管中设有耐高温金属过滤网16，电磁阀A15前端设有压力传感器9。当压力传感器9采集的压力信号过高，ECU3控制发动机1关闭，并在一段时间后关闭纳米管捕集器5电磁阀A15和电磁阀C23，打开排气支管入口处的电磁阀B22。DPF5与电磁阀C23之间装有空压机17，反冲纳米管捕集器5中碳纳米管进入排气支管，经排气支管尾端耐高温纳米滤网16后被收集；完成碳纳米管的生成到收集的全阶段，实现碳纳米管的批量收集、绿色生产、低排放。
如图1所示，利用双燃料反应性控制压燃发动机缸内燃烧火焰合成碳纳米管的装置包括控制系统、反应系统、后处理系统和EGR系统，EGR系统包括EGR阀8、压气机11、废气涡轮12和空气滤清器13。
控制系统包括ECU3、冷却液温度传感器10、压力传感器9和曲轴位置传感器2，冷却液温度传感器10设置在气缸冷却液中，用于获取气缸中冷却液的温度，压力传感器9安装在排气管道中，曲轴位置传感器2安装在发动机曲轴处，用于获取活塞的位置和发动机的转速；由发动机的转速、冷却液的温度和负荷信号(由ECU3发送给发动机1)获取缸内温度，冷却液温度传感器10、压力传感器9和曲轴位置传感器2均与ECU3进行信号连接。
反应系统包括发动机1、燃料喷嘴A7、燃料箱A14、硝酸铁粉末4、乙醇18、高反应性燃料19(如柴油、生物柴油)、燃料喷嘴B21和燃料箱B20，燃料喷嘴B21安装在发动机1的气缸上，燃料喷嘴B21与燃料箱A14通过管道连接，且燃料箱A14中装有高反应性燃料19；发动机1的进气管道中沿进气方向依次设有空气滤清器13和压气机11，且压气机11后部的进气管道中安装有燃料喷嘴A7，燃料喷嘴A7通过管道与燃料箱B20连接，且燃料箱B20中装有乙醇18和硝酸铁粉末4的混合物。
后处理系统包括纳米管捕集器5、SCR6(选择性催化还原系统)、空压机17和耐高温金属滤网16，发动机1的排气管道中沿排气方向依次设有压力传感器9、纳米管捕集器5、SCR6和废气涡轮12，压力传感器9处设有电磁阀A15，电磁阀A15和纳米管捕集器5之间设有排气支管，且排气支管入口处设有电磁阀B22，排气支管末端设有耐高温金属滤网16；纳米管捕集器5和SCR6之间设有电磁阀C23，电磁阀C23与DPF5之间设有空压机17；电磁阀C23与SCR6之间设有与发动机1进气管道连通的管道，且管道上设有EGR阀8。
本发明用双燃料反应性控制压燃发动机缸内燃烧火焰合成碳纳米管的装置工作原理如下：
乙醇18提前喷入到气缸内，与空气形成混合气，随后在压缩终了阶段喷入柴油(高反应性燃料19)，在高压下使柴油自燃；该过程是特殊的RCCI燃烧，导致气缸内生成更多的CO和HC，同时燃烧温度较低，也形成了碳纳米管的生成必要条件-碳源和温度；在乙醇18中加入一定量的硝酸铁粉末4，在发动机1缸内燃烧中极易分解形成Fe 2O 3，即作为碳纳米管的催化剂；同时柴油中含有较高量的硫化物，与催化剂的共同使用可以加快碳纳米管的生长。反应过程中，电磁阀A15、电磁阀C23均打开，电磁阀B22和空气机17均关闭；且冷却液温度传感器10、压力传感器9和曲轴位置传感器2实时采集数据。为了减少发动机硫化物排放，引入EGR技术实现部分硫化物重新进入气缸，增加气缸内硫化物浓度，避免额外加入硫化物而导致排放物的增加。而引入的EGR也会降低缸内温度和NOx的排放，不仅可以通过EGR率调节缸内温度在800～1000℃，更能减少NOx的排放。同时，控制喷油提前角、乙醇柴油当量比、乙醇纯度、发动机转速、发动机负荷皆可提升CO的排放和降低HC和NOx的排放，为碳纳米管的碳源建立优良条件，这也能大大降低RCCI过程中其他污染物的排放。而生成的碳纳米管会包裹Fe 2O 3纳米颗粒从排气歧管进入到排气管道中，带离出气缸，避免Fe 2O 3的滞留而导致的发动机燃烧异常。进入到排气管道中的碳纳米管被纳米管捕集器5捕捉，当纳米管捕集器5收集满时安装在管道内的压力传感器9采集数值升高，并将信号传递给ECU3。ECU3根据信号值关闭工作中的电磁阀A15、电磁阀C23，同时打开排气支管的电磁阀B22、空气机17，利用高压空气将纳米管捕集器5中碳纳米管颗粒反冲至耐高温纳米滤网16处完成收集；其余排气经过SCR6和废气涡轮12处理NOx后排入空气中。
实施例
(1)选择某款柴油机机作为原机，在进气管道处加装燃油喷射嘴B21，实现进气道喷射和缸内直喷的双燃料RCCI发动机。
(2)本实例中所使用的柴油为标准国五柴油，乙醇为含量大等于99.7％的无水乙醇，其纯度由后期自行配置。
(3)为保障在运行过程中，形成碳纳米管生长的适宜环境，对于发动机的部分运行条件 展开先期试验，其中对发动机运行过程中重要的几项参数展开试验，实验值主要如下：乙醇与柴油的消耗量(Kg/h)比值(当量比)：0～1.0，乙醇纯度：20～100％，喷油提前角：-40～0°，硝酸铁含量：0～7000ppm，EGR率：0～20％，发动机转速：0～1500r/min；试验时，利用燃烧分析仪确定发动机缸内温度，通过对比试验发现，缸内温度在600-1200℃时碳纳米管的生长较好，但是由于低温燃烧导致碳烟颗粒物数量、表面积增加，碳纳米管纯度低，因此提高缸内生产温度；由于RCCI发动机燃烧温度总体较低，因此温度保持在800～1000℃较为适宜；当温度低于800℃，减小柴油喷油提前角(延迟点燃时燃料喷嘴B21的喷油时间)或者减小EGR率(减小EGR阀8的开度)或者增大乙醇与柴油的消耗量比值(通过燃料喷嘴A7和燃料喷嘴B21，增加喷油量)。
(4)缸内碳源CO、HC的排放使用废气分析仪测量其浓度，NOx使用NOx检测分析仪检测其浓度；通过调节不同变量(喷油提前角、乙醇柴油当量比、乙醇纯度、硝酸铁含量、EGR率和发动机转速)，检测三种主要气体浓度，并采集不同变量下的碳烟颗粒，在投射电镜扫描下观察其形貌特征，重点观察碳纳米管纯度、形貌，尽量生成单一形态的碳纳米管。对不同变量取样五次，以减少测量误差，并依据碳纳米管的纯度和形貌的结果，确定不同变量的取值；经过实验对比发现：乙醇与柴油的消耗量(Kg/h)比值：0.4-0.67，乙醇纯度：60～70％，喷油提前角：-40～-25°，硝酸铁含量：5000ppm，EGR率：10～20％，发动机转速：500～1200r/min。当变量处于这些范围时，碳纳米管具有一定纯度、单一形貌、产出量。
(5)碳纳米管生成后从气缸中排出，经过纳米管捕集器5处理后，碳纳米管能够很好地被收集，同时后处理系统也能很好地捕捉从气缸内排出的Fe 2O 3。
所述实施例为本发明的优选的实施方式，但本发明并不限于上述实施方式，在不背离本发明的实质内容的情况下，本领域技术人员能够做出的任何显而易见的改进、替换或变型均属于本发明的保护范围。

Claims (10)

  1. 利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，包括：
    控制系统，包括ECU(3)以及与ECU(3)信号连接的冷却液温度传感器(10)、压力传感器(9)和曲轴位置传感器(2)；
    反应系统，包括发动机(1)、燃料箱A(14)和燃料箱B(20)，发动机(1)分别与燃料箱A(14)和燃料箱B(20)连通，所述燃料箱A(14)中装有高反应性燃料(19)，所述燃料箱B(20)中装有乙醇(18)和硝酸铁粉末(4)的混合物；
    后处理系统，包括纳米管捕集器(5)、空压机(17)和金属滤网(16)，压力传感器(9)和纳米管捕集器(5)沿排气方向依次在发动机(1)的排气管道中，压力传感器(9)处设有电磁阀A(15)，电磁阀A(15)和纳米管捕集器(5)之间设有排气支管，且排气支管入口处设有电磁阀B(22)，排气支管末端设有金属滤网(16)；纳米管捕集器(5)后端还设有电磁阀C(23)，电磁阀C(23)与纳米管捕集器(5)之间设有空压机(17)；电磁阀C(23)后端设有与发动机(1)进气管道连通的管道，且管道上设有EGR阀(8)。
  2. 根据权利要求1所述的利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，所述发动机(1)的进气管道中沿进气方向依次设有空气滤清器(13)和压气机(11)。
  3. 根据权利要求2所述的利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，所述压气机(11)后部的进气管道中安装有燃料喷嘴A(7)，燃料喷嘴A(7)通过管道与燃料箱B(20)连接。
  4. 根据权利要求1所述的利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，所述发动机(1)的气缸上安装有燃料喷嘴B(21)，燃料喷嘴B(21)与燃料箱A(14)通过管道连接。
  5. 根据权利要求1所述的利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，所述高反应性燃料(19)为柴油或生物柴油。
  6. 根据权利要求1所述的利用双燃料RCCI发动机合成碳纳米管的装置，其特征在于，所述发动机(1)的排气管道末端设有废气涡轮(12)。
  7. 一种根据权利要求1-6任一项所述的利用双燃料RCCI发动机合成碳纳米管的装置的合成方法，其特征在于：
    乙醇(18)先喷入到发动机(1)的气缸内，与空气形成混合气，在压缩终了阶段喷入高反应性燃料(19)，反应后，进入到发动机(1)排气管道中的碳纳米管被纳米管捕集器(5)捕集；
    所述乙醇(18)中加入5000ppm的硝酸铁粉末(4)；所述乙醇(18)与高反应性燃料(19)的消耗量比值为0.4-0.67；
    反应过程中，发动机(1)气缸内的温度保持在800～1000℃，发动机(1)的转速为500～1200r/min。
  8. 根据权利要求7所述的合成方法，其特征在于，当温度低于800℃，减小柴油喷油提前角或者减小EGR率或者增大乙醇(18)与高反应性燃料(19)的消耗量比值。
  9. 根据权利要求8所述的合成方法，其特征在于，所述喷油提前角的范围是-40～-25°，所述EGR率的范围是10～20％。
  10. 根据权利要求8所述的合成方法，其特征在于，当压力传感器(9)采集的数值变大时，ECU(3)控制电磁阀A(15)和电磁阀C(23)关闭、电磁阀B(22)和空气机(17)打开，利用空气机(17)和纳米滤网(16)收集碳纳米管。
PCT/CN2021/114562 2021-02-04 2021-08-25 利用双燃料rcci发动机合成碳纳米管的装置和方法 Ceased WO2022166174A1 (zh)

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