技术领域technical field
本发明涉及煤燃烧技术领域，具体涉及一种便于煤基化学链燃烧的方法和装置，实现煤等含碳固体燃料的高效利用及充分转化。The invention relates to the technical field of coal combustion, in particular to a method and device for facilitating coal-based chemical chain combustion, so as to realize efficient utilization and full conversion of carbon-containing solid fuels such as coal.
背景技术Background technique
直接以煤为燃料的化学链燃烧技术，作为一种新型的氧燃烧方式，直接以氧载体代替空气，实现煤的非混合无焰燃烧，具有显著的优点，不仅能在损失较小能量的情况下、实现煤燃烧过程中CO2的有效分离；而且避免了煤直接与空气燃烧过程中的不可逆损失，实现了系统内部热量的梯级利用，具有较高的燃烧效率；同时，还能有效的抑制煤燃烧过程中NOx的生成。The chemical looping combustion technology directly using coal as fuel, as a new type of oxygen combustion method, directly replaces air with oxygen carrier to realize the non-mixed flameless combustion of coal, which has significant advantages, not only can reduce the loss of energy Next, realize the effective separation of CO2 in the process of coal combustion; and avoid the irreversible loss in the process of direct coal combustion with air, realize the cascade utilization of heat inside the system, and have high combustion efficiency; at the same time, it can also effectively inhibit Formation ofNOx during coal combustion.
但是，直接以煤为燃料的化学链燃烧过程中，存在如下两个重大的限制环节，具体如下：However, in the chemical looping combustion process directly using coal as fuel, there are two major limitations as follows, specifically as follows:
首先，燃烧过程中，主要发生的仍旧是煤气化产物与氧载体之间的气固氧化反应，而不是煤粉颗粒直接与氧载体之间的固固反应；同时，由于煤气化速率远低于煤气化产物与氧载体之间的反应速率，是直接以煤为燃料的化学链燃烧的限制环节，导致化学链燃烧过程中，煤粉难以完全气化、充分利用，煤燃烧尾气中包含一定的可燃不凝结气体，主要为CO、H2、CH4。First of all, in the combustion process, the gas-solid oxidation reaction between the coal gasification product and the oxygen carrier mainly occurs, rather than the solid-solid reaction between the coal powder particles and the oxygen carrier directly; at the same time, because the coal gasification rate is much lower than The reaction rate between the coal gasification product and the oxygen carrier is the limiting link of the chemical looping combustion directly using coal as fuel, which makes it difficult to completely gasify and fully utilize the pulverized coal during the chemical looping combustion process, and the tail gas of coal combustion contains certain Flammable non-condensable gas, mainly CO, H2 , CH4 .
其次，直接以煤为燃料的化学链燃烧过程中，煤与氧载体的反应主要在燃料反应器中进行，燃料反应器的结构形式以鼓泡床反应器为主。鉴于煤与氧载体的二元床料中，煤的密度比氧载体的密度小得多，二者之间存在较大的密度差，易于发生床料偏析，导致煤与氧载体难于有效接触、充分流态化。而当煤粉颗粒运动到氧载体颗粒上端热解、气化时，所产生的不凝结可燃气体（主要包括CO、H2、CH4），因无法与氧载体接触，也难于被氧化。Secondly, in the chemical looping combustion process directly using coal as fuel, the reaction between coal and oxygen carrier is mainly carried out in the fuel reactor, and the structural form of the fuel reactor is mainly the bubble bed reactor. In view of the fact that in the binary bed material of coal and oxygen carrier, the density of coal is much smaller than that of oxygen carrier, there is a large density difference between the two, and bed material segregation is prone to occur, making it difficult to effectively contact coal and oxygen carrier. Fully fluidized. When the pulverized coal particles move to the upper end of the oxygen carrier particles for pyrolysis and gasification, the non-condensable combustible gases (mainly including CO, H2 , CH4 ) produced are difficult to be oxidized because they cannot contact the oxygen carrier.
正是基于上述原因，导致了直接以煤为燃料的化学链燃烧过程，煤粉难以有效气化、充分利用，煤燃烧尾气中所掺杂的不凝气体，主要包括CO、H2、CH4，不仅会导致CO2分离困难，耗能增加；而且导致煤粉难于充分燃烧，很不经济。It is based on the above reasons that the chemical looping combustion process directly using coal as fuel is difficult to effectively gasify and fully utilize pulverized coal. The non-condensable gases doped in the tail gas of coal combustion mainly include CO, H2 , CH4 , not only will lead to difficulties in CO2 separation and increased energy consumption; it will also make it difficult to fully burn pulverized coal, which is very uneconomical.
因此，采取有效措施，促进尾气中不凝结气体的燃烧转化，对于煤的高效转化及煤化学链燃烧的推广应用，都具有重要的意义。Therefore, it is of great significance to take effective measures to promote the combustion conversion of non-condensable gases in tail gas for the efficient conversion of coal and the popularization and application of coal chemical looping combustion.
发明内容Contents of the invention
本发明的目的在于提供一种具有自热制氧功能的煤粉燃烧方法，将煤的纯氧燃烧技术与化学链燃烧技术有机结合，既克服纯氧燃烧中纯O2制备的高成本、高耗能的限制，又促进煤的有效转化、高效利用，消除煤燃烧尾气中不凝结气体，获得高浓度的CO2，便于后续存贮处理。The purpose of the present invention is to provide a kind of pulverized coal combustion method with self-heating oxygen production function, the pure oxygen combustion technology of coal is combined with the chemical looping combustion technology organically, not only overcomes the high cost of pureO in pure oxygen combustion , the high cost of preparation The limitation of energy consumption also promotes the effective conversion and efficient utilization of coal, eliminates non-condensable gases in the tail gas of coal combustion, and obtains high-concentration CO2 , which is convenient for subsequent storage and treatment.
本发明的目的还在于提供实现上述方法的装置，将煤的纯氧燃烧技术与化学链燃烧技术有机结合，既克服纯氧燃烧中纯O2制备的高成本、高耗能的限制，又促进煤的有效转化、高效利用，消除煤燃烧尾气中不凝结气体，获得高浓度的CO2，便于后续存贮处理。The object of the present invention is also to provide a device for realizing the above method, organically combining the pure oxygen combustion technology of coal with the chemical looping combustion technology, which not only overcomes the limitation of high cost and high energy consumption of pureO2 preparation in pure oxygen combustion, but also promotes Effective conversion and efficient utilization of coal, elimination of non-condensable gases in coal combustion tail gas, and high concentration of CO2 , which is convenient for subsequent storage and treatment.
一种具有自热制氧功能的煤粉燃烧方法，具体为：A pulverized coal combustion method with self-heating oxygen production function, specifically:
（1）利用钨基氧化物作为复合氧载体，与含碳燃料发生还原反应，生成Cu、W、CO2和不凝结气体；(1) Use tungsten-based oxides as composite oxygen carriers to undergo reduction reactions with carbon-containing fuels to generate Cu, W, CO2 and non-condensable gases;
（2）步骤（1）还原反应生成的W和Cu，在空气气氛下发生氧化反应，重新生成CuWO4；(2) The W and Cu generated by the reduction reaction in step (1) undergo an oxidation reaction in an air atmosphere to regenerate CuWO4 ;
（3）步骤（2）氧化反应生成的CuWO4，借助氧化反应产生的热量，在水蒸气气氛下分解，产生O2、Cu2O和WO2，产生的O2与步骤（1）生成的不凝结气体反应生成CO2和水蒸气；(3) The CuWO4 generated by the oxidation reaction in step (2) is decomposed in the water vapor atmosphere with the help of the heat generated by the oxidation reaction to produce O2 , Cu2 O and WO2 , and the O2 generated in step (1) is the same as Non-condensable gases react to formCO2 and water vapor;
（4）步骤（3）分解产生的Cu2O和WO2，再在空气气氛下发生氧化反应，重新形成CuWO4，返回步骤（1）继续下一次循环反应，本步骤反应释放的热量作为步骤（1）还原反应的热源。(4) Decompose Cu2 O and WO2 produced in step (3), and then undergo an oxidation reaction in an air atmosphere to re-form CuWO4 , return to step (1) to continue the next cycle reaction, and the heat released in this step is used as the step (1) The heat source for the reduction reaction.
一种具有自热制氧功能的煤粉燃烧装置，包括依次管道连接形成回路的还原反应器的第一输出端、第一氧化反应器的输入端、第一氧化反应器的输出端、第一分离器的输入端、第一分离器的输出端、分解反应器的输入端、分解反应器的输出端、第二分离器的输入端、第二分离器的第一输出端、第二氧化反应器的输入端、第二氧化反应器的输出端、第三分离器的输入端、第三分离器的输出端和还原反应器的第一输入端；第二分离器的第二输出端通过冷凝器7管道连接还原反应器1的第二输入端。A pulverized coal combustion device with self-heating oxygen production function, comprising the first output end of the reduction reactor, the input end of the first oxidation reactor, the output end of the first oxidation reactor, the first input of separator, output of first separator, input of decomposition reactor, output of decomposition reactor, input of second separator, first output of second separator, second oxidation reaction The input end of the device, the output end of the second oxidation reactor, the input end of the third separator, the output end of the third separator and the first input end of the reduction reactor; the second output end of the second separator is condensed The device 7 is piped to the second input end of the reduction reactor 1.
本发明的技术效果体现在：Technical effect of the present invention is embodied in:
（1）本发明采用钨基氧化物作为复合氧载体，具有较高的反应协同性及释氧容量，因此具有较大的实用潜力。(1) The present invention uses tungsten-based oxide as the composite oxygen carrier, which has high reaction synergy and oxygen release capacity, so it has great practical potential.
（2）钨基氧化物分解释放O2为吸热反应，而钨基氧化物与煤反应的还原产物再与空气氧化再生又是放热反应，所释放出的热量完全满足钨基氧化物分解释放O2时所需要的热量，从而通过钨基氧化物还原产物的氧化再生及钨基氧化物的分解不仅实现了O2的制备，在无需外部热源的情况下，实现了热量的平衡。(2) The decomposition of tungsten-based oxides to releaseO2 is an endothermic reaction, while the reduction product of tungsten-based oxides reacted with coal and then oxidized and regenerated with air is an exothermic reaction, and the released heat fully meets the decomposition of tungsten-based oxides The heat required for the release ofO2 , so that the oxidative regeneration of tungsten-based oxide reduction products and the decomposition of tungsten-based oxides not only realize the preparation ofO2 , but also achieve heat balance without external heat sources.
（3）CuWO4分解产生的Cu2O和WO2在空气气氛下发生氧化反应，重新形成CuWO4，并释放热量，该热量可提供给钨基氧化物与煤的还原反应，促进煤的有效转化、高效利用，无须额外提供能量，降低耗能。(3) The Cu2 O and WO2 generated by the decomposition of CuWO4 undergo oxidation reaction in the air atmosphere, re-form CuWO4 , and release heat, which can be provided for the reduction reaction of tungsten-based oxides and coal, and promote the effective conversion of coal. Transformation, efficient utilization, no need to provide additional energy, and reduce energy consumption.
（4）制备得到的O2与钨基氧化物和煤还原反应产生的不凝结气体反应，生成CO2和水蒸气，有效消除了煤燃烧尾气中不凝结气体。(4) The preparedO2 reacts with the non-condensable gas produced by the reduction reaction of tungsten-based oxides and coal to generateCO2 and water vapor, which effectively eliminates the non-condensable gas in the coal combustion tail gas.
（5）燃料适应性广，除了不同反应性的煤外，其它固体含碳燃料，比如污泥、石油焦、生物质等，也适用。(5) The fuel has wide adaptability. In addition to coal with different reactivity, other solid carbon-containing fuels, such as sludge, petroleum coke, biomass, etc., are also applicable.
（6）制氧系统中，第一空气反应器与分解反应器采用嵌套式结构，能够有效的完成钨基氧化物与煤反应后的还原产物（Cu、W）的氧化再生，及再生氧化物的分解制氧，简化了系统流程。(6) In the oxygen production system, the first air reactor and the decomposition reactor adopt a nested structure, which can effectively complete the oxidation regeneration of the reduction products (Cu, W) after the reaction of tungsten-based oxides and coal, and the regeneration oxidation Decomposition of substances to produce oxygen simplifies the system flow.
（7）整个系统可以连续运行，而且通过运行条件优化，实现系统能量的自平衡，节能经济。(7) The whole system can operate continuously, and through the optimization of operating conditions, the self-balancing of system energy can be realized, which is energy-saving and economical.
附图说明Description of drawings
图1为本发明方法流程图；Fig. 1 is a flow chart of the method of the present invention;
图2为本发明装置结构图；Fig. 2 is a structural diagram of the device of the present invention;
图3为纯O2射流管的第一种布置图（对角布置）；Figure 3 is the first arrangement of pureO2 jet tubes (diagonal arrangement);
图4为纯O2射流管的第二种布置图（对冲布置）；Figure 4 is the second layout of the pureO2 jet tube (hedging layout);
图5为CuWO4分解释O2图。Fig. 5 is the CuWO4 min interpretation O2 diagram.
具体实施方式Detailed ways
下面结合附图对本发明做进一步详细的说明。The present invention will be described in further detail below in conjunction with the accompanying drawings.
图1给出本发明方法流程图，一种具有自热制氧功能的煤粉燃烧方法，具体为：Fig. 1 provides the method flowchart of the present invention, a kind of pulverized coal combustion method with self-heating oxygen production function, specifically:
（1）利用钨基氧化物作为复合氧载体，与含碳燃料发生还原反应，生成Cu、W、CO2和不凝结气体；(1) Use tungsten-based oxides as composite oxygen carriers to undergo reduction reactions with carbon-containing fuels to generate Cu, W, CO2 and non-condensable gases;
（2）步骤（1）还原反应生成的W和Cu，在空气气氛下发生氧化反应，重新生成CuWO4，并释放热量；(2) The W and Cu generated by the reduction reaction in step (1) undergo an oxidation reaction in an air atmosphere to regenerate CuWO4 and release heat;
（3）步骤（2）重新生成的CuWO4，借助氧化反应产生的热量分解产生O2、Cu2O和WO2，产生的O2与步骤（1）生成的不凝结气体反应生成CO2和水蒸气；(3) The regenerated CuWO4 in step (2) is decomposed by the heat generated by the oxidation reaction to produce O2 , Cu2 O and WO2 , and the produced O2 reacts with the non-condensable gas generated in step (1) to generate CO2 and water vapor;
（4）步骤（3）分解产生的Cu2O和WO2，在空气气氛下发生氧化反应，重新形成CuWO4，并释放热量，返回步骤（1）继续下一次循环反应，本步骤释放的热量作为步骤（1）还原反应的热源。(4) The Cu2 O and WO2 generated by the decomposition in step (3) undergo oxidation reaction in the air atmosphere to re-form CuWO4 and release heat, and return to step (1) to continue the next cycle reaction. The heat released in this step As a heat source for the reduction reaction in step (1).
本发明所提出的实现具有自热制氧功能的煤粉燃烧装置的一种较佳实现方式，如图2所示，包括燃料反应器系统、纯O2制备系统和空气反应器系统三部分。具体的，由还原反应器1、分离器10及飞灰捕集器11连接组成燃料反应器系统；由密封阀2、氧化反应器3、分解反应器4、分离器5，6及冷凝器7依次连接组成纯O2制备系统；由氧化反应器8及分离器9组成空气反应器系统。A preferred implementation of the pulverized coal combustion device with self-heating oxygen production function proposed by the present invention, as shown in Figure 2, includes three parts: a fuel reactor system, a pureO2 preparation system and an air reactor system. Specifically, the reduction reactor 1, the separator 10 and the fly ash trap 11 are connected to form a fuel reactor system; the sealing valve 2, the oxidation reactor 3, the decomposition reactor 4, the separators 5, 6 and the condenser 7 Connected in sequence to form a pureO2 preparation system; an air reactor system is composed of an oxidation reactor 8 and a separator 9.
鼓泡流化床设计为长方体（也可为圆柱体），所制备的纯O2通过射流管引入燃料反应器1中，射流管的布置方式或为四角布置（参见图3），射流管轴心与鼓泡流化床相邻两侧壁的夹角均为45°，所喷射的O2与不凝结气体以切圆方式燃烧；或者射流管放置在鼓泡流化床的侧壁中间，为对冲布置方式（参见图4）。这样加强了纯O2与不凝结气体的湍流混合，有利于不凝结气体的充分燃烧。The bubbling fluidized bed is designed as a cuboid (or a cylinder), and the prepared pure O2 is introduced into the fuel reactor 1 through the jet tube. The included angle between the center and the adjacent side walls of the bubbling fluidized bed is 45°, and the injectedO2 and non-condensable gas burn in a tangential circle; or the jet tube is placed in the middle of the side wall of the bubbling fluidized bed, For the hedging arrangement (see Figure 4). This strengthens the turbulent mixing of pureO2 and non-condensable gas, which is conducive to the complete combustion of non-condensable gas.
还原反应器1可采用鼓泡流化床、喷动床和二段式反应器等，氧化反应器3和8可采用快速流化床反应器、移动床等，分解反应器4可采用快速流化床反应器、移动床等。Reduction reactor 1 can adopt bubbling fluidized bed, spouted bed and two-stage reactor, etc., oxidation reactor 3 and 8 can adopt fast fluidized bed reactor, moving bed, etc., and decomposition reactor 4 can adopt fast fluidized bed reactor. Bed reactors, moving beds, etc.
本发明实例中，还原反应器1采用鼓泡流化床，氧化反应器3和8采用快速流化床反应器，分解反应器4采用快速流化床反应器。下面以煤等含碳固体为燃料，以CuWO4作为复合氧载体为例，进行一系列的反应过程，便于煤的充分转化，而所生成高纯的CO2，则便于后续存贮处理，具体实施流程如下：In the example of the present invention, the reduction reactor 1 adopts a bubbling fluidized bed, the oxidation reactors 3 and 8 adopt a fast fluidized bed reactor, and the decomposition reactor 4 adopts a fast fluidized bed reactor. In the following, coal and other carbon-containing solids are used as fuel, and CuWO4 is used as a composite oxygen carrier as an example. A series of reaction processes are carried out to facilitate the full conversion of coal, and the high-purity CO2 produced is convenient for subsequent storage and processing. Specifically The implementation process is as follows:
（1）首先，在鼓泡流化床1中，在CO2流态化介质作用下，引入定量的煤与CuWO4反应，生成CO2、水蒸气、少量不凝结气体CO、CH4和H2及钨基还原固相产物Cu、W；(1) First, in the bubbling fluidized bed 1, under the action of CO2 fluidized medium, a certain amount of coal is introduced to react with CuWO4 to generate CO2 , water vapor, a small amount of non-condensable gas CO, CH4 and H2 and tungsten-based reduction solid phase products Cu, W;
（2）步骤（1）得到的气相产物（包括CO2和水蒸气及携带的飞灰）通过分离器10，分离出的飞灰进入捕集器11进行捕获，而气相CO2和水蒸汽通过分离器10排出，冷凝分离后就可以得到高浓度的CO2，便于后续处理；(2) The gas phase products (including CO2 and water vapor and carried fly ash) obtained in step (1) pass through the separator 10, and the separated fly ash enters the trap 11 for capture, while the gas phase CO2 and water vapor pass through After being discharged from the separator 10, high-concentration CO2 can be obtained after condensation and separation, which is convenient for subsequent treatment;
（3）步骤（1）得到的固相产物W及Cu，通过密封阀2进入快速流化床反应器3中，在600-900℃和空气气氛下，进行氧化再生，重新生成CuWO4，而反应后的残余空气由分离器5的排气口排出；(3) The solid-phase product W and Cu obtained in step (1) enter the fast fluidized bed reactor 3 through the sealing valve 2, and undergo oxidation regeneration at 600-900°C in an air atmosphere to regenerate CuWO4 , while Residual air after the reaction is discharged by the exhaust port of separator 5;
（4）步骤（3）所再生形成的CuWO4，通过分离器5与残余空气分离，并由分离器5的料腿引入快速流化床反应器4，借助步骤（3）氧化反应产生的热量，在水蒸气气氛下，分解产生O2及固相产物Cu2O、WO2，并在分离器6中予以分离，O2及残余水蒸气通过冷凝器7进行冷凝分离，制得纯净的O2（参见图5）；步骤（1）所产生不凝结气体在反应器1中向上流动，不凝结气体与纯O2接触反应，充分转化，形成CO2和水蒸气；(4) The CuWO4 regenerated in step (3) is separated from the residual air through the separator 5, and introduced into the fast fluidized bed reactor 4 through the dipleg of the separator 5, and the heat generated by the oxidation reaction in step (3) is used to , in a water vapor atmosphere, decompose to produce O2 and solid phase products Cu2 O and WO2 , which are separated in separator 6, and O2 and residual water vapor are condensed and separated through condenser 7 to obtain pure O2 (see Figure 5); the non-condensable gas produced in step (1) flows upward in the reactor 1, and the non-condensable gas contacts and reacts with pure O2 and is fully converted to form CO2 and water vapor;
（5）而步骤（4）所分解形成的Cu2O和WO2固相产物则引入快速流化床反应器8中，在600-900℃和空气气氛下，氧化再生，重新形成CuWO4，并在分离器9中与残余空气分离；本步骤反应释放的热量作为步骤（1）还原反应的热源。(5) The Cu2 O and WO2 solid-phase products formed by decomposition in step (4) are introduced into the fast fluidized bed reactor 8, and oxidized and regenerated at 600-900°C in an air atmosphere to re-form CuWO4 , And it is separated from residual air in the separator 9; the heat released by the reaction in this step is used as the heat source for the reduction reaction in step (1).
（6）步骤（5）所再生制备得的CuWO4通过分离器9引入燃料反应器1中，与煤在反应器1下部进行还原反应，产生Cu、W等固相还原产物，并重新通过密封阀2引入反应器3，进行下一次循环反应。(6) The CuWO4 regenerated and prepared in step (5) is introduced into the fuel reactor 1 through the separator 9, and undergoes a reduction reaction with coal in the lower part of the reactor 1 to produce solid-phase reduction products such as Cu and W, which are re-passed through the sealed Valve 2 is introduced into reactor 3 for the next cycle reaction.
除了所述实例中的CuWO4以外，还可采用MnWO4、NiWO4及CoWO4等钨基氧化物作为复合氧载体。In addition to CuWO4 in the above examples, tungsten-based oxides such as MnWO4 , NiWO4 and CoWO4 can also be used as composite oxygen carriers.
本领域的技术人员容易理解，以上所述仅为本发明的较佳实施例而已，并不用以限制本发明，凡在本发明的精神和原则之内所作的任何修改、等同替换和改进等，均应包含在本发明的保护范围之内。It is easy for those skilled in the art to understand that the above descriptions are only preferred embodiments of the present invention, and are not intended to limit the present invention. Any modifications, equivalent replacements and improvements made within the spirit and principles of the present invention, All should be included within the protection scope of the present invention.
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