Combustion and pollutant emission characteristics of coal in a pressurized fluidized bed under O_2/ CO_2 atmosphere

The pressurized combustion experiments of bituminous coal and lignite under air and O2/CO2 atmospheres were conducted to study the influences of pressure and atmosphere on combustion and the CO, NO, SO2 release process. Two indices, the maximum concentration and the total emission, were applied to quantitatively evaluate the influence of several different operating parameters such as pressure, atmosphere and temperature on the formation of NO and SO2 during coal combustion in the fluidized bed. The experimental results show that the releasing profiles of CO, NO and SO2 during coal combustion under a pressurized oxy- fuel atmosphere are similar to those under a pressurized air atmosphere, and the curves of measured gas components are all unimodal. Under the oxy-fuel condition, pressure increasing from 0.1 to 0.7 MPa can cause the inhibition of NO and SO2 emission. The elevation of temperature can lead to an increase in the maximum concentration and the total production of NO and SO2, and the increase under atmospheric pressure is higher than that under high pressure.

Simulation of gas-solid flow characteristics of the circulating fluidized bed boiler under pure-oxygen combustion conditions

Under the pressure of carbon neutrality,many carbon capture,utilization and storage technologies have witnessed rapid development in the recent years,including oxy-fuel combustion(OFC)technology.However,the conventional OFC technology usually depends on the flue gas recirculation system,which faces significant investment,high energy consumption,and potential low-temperature corrosion problem.Considering these deficiencies,the direct utilization of pure oxygen to achieve particle fluidization and fuel combustion may reduce the overall energy consumption and CO_(2)-capture costs.In this paper,the fundamental structure of a self-designed 130 t·h^(-1) pure-oxygen combustion circulating fluidized bed(CFB)boiler was provided,and the computational particle fluid dynamics method was used to analyze the gas-solid flow characteristics of this new-concept boiler under different working conditions.The results indicate that through the careful selection of design or operational parameters,such as average bed-material size and fluidization velocity,the pure-oxygen combustion CFB system can maintain the ideal fluidization state,namely significant internal and external particle circulation.Besides,the contraction section of the boiler leads to the particle backflow in the lower furnace,resulting in the particle suspension concentration near the wall region being higher than that in the center region.Conversely,the upper furnace still retains the classic core-annulus flow structure.In addition to increasing solid circulation rate by reducing the average bed-material size,altering primary gas ratio and bed inventory can also exert varying degrees of influence on the gas-solid flow characteristics of the pure-oxygen combustion CFB boiler.

Study on the emission characteristics of nitrogen oxides with coal combustion in pressurized fluidized bed

Nitrogen oxides are one of the most significant pollution sources during coal combustion. This experimental study was conducted in a 15 kWth lab-scale pressurized fluidized bed (inner diameter = 81-100 mm, H = 2100 mm) firing with bituminous coals. The effects of operating parameters, including bed temperature (800℃-900℃), operating pressure (0.1-0.4 MPa), excess air level (16%-30%) and flow pattern on NOX and N2O emissions were systematically studied during the tests. During each test the interaction effects of all the operating parameters were properly controlled. The results show that most operating parameters have an opposite effect on NOX and N2O emissions, and the N2O emissions mainly depend on the bed temperature. Increasing the operating pressure can significantly suppress the fuel-N conversion to NOX but enhance its conversion to N2O. With the rise of the excess air level and fluidization number, NOX emissions grow distinctly while N2O emissions remain almost unchanged. Total nitrogen oxide emissions increase with the bed temperature while decrease with the operating pressure.

Comparative study on SO_2 release and removal under air and oxy-fuel combustion in a fluidized bed combustor

SO2 release and removal were studied under both the air and oxy-fuel combustion conditions using an anthracite coal from the Jincheng mine in China on a bench-scale fluidized bed combustor （FBC）. Special attention was paid to the effects of the combustion atmosphere, 02 concentration, bed temperature, and limestone addition. The released amount of SO2 was clearly higher under 30% 02/70% CO2 than that of the air atmosphere. As the O2 concentration in O2/CO2 mixture increased from 21% to 40%, the released amount of SO2 increased significantly, but then it decreased when the 02 concentration increased up to 50%. The bed temperature from 860 to 920 ℃ has no obvious influence on the the SO2 release but shows a strong influence on the desulfurization with limestone in both oxy-fuel and air conditions. The maximum SO2 removal efficiency appears to be at 880 to 900 ℃ for both the air and oxy-fuel combustion conditions.

Emissions of SO_2, NO and N_2O in a circulating fluidized bed combustor during co-firing coal and biomass

This paper presents the experimental investigations of the emissions of SO2, NO and N20 in a bench scale circulating fluidized bed combustor for coal combustion and co-firing coal and biomass. The thermal capacity of the combustor is 30 kW. The setup is electrically heated during startup. The infuence of the excess air, the degree of the air staging, the biomass share and the feeding position of the fuels on the emissions of SO2, NO and N2O were studied. The results showed that an increase in the biomass shares resulted in an increase of the CO concentration in the flue gas, probably due to the high volatile content of the biomass. In co-firing, the emission of SO2 increased with increasing biomass share slightly, however, non-linear increase relationship between SO2 emission and fuel sulfur content was observed. Air staging significantly decreased the NO emission without raising the SO2 level. Although the change of the fuel feeding position from riser to downer resulted in a decrease in the NO emission level, no obvious change was observed for the SO2 level. Taking the coal feeding position R as a reference, the relative NO emission could significantly decrease during co-firing coal and biomass when feeding fuel at position D and keeping the first stage stoichiometry greater than 0.95. The possible mechanisms of the sulfur and nitrogen chemistry at these conditions were discussed and the ways of simultaneous reduction of SO2, NO and N2O were proposed.

Temperature dependence on reaction of CaCO_3 and SO_2 in O_2/CO_2 coal combustion

The temperature dependence on the reaction of desulfurization reagent CaCO3 and SO2 in O2/CO2 coal combustion was investigated by thcrmogravimetric analysis, X-ray diffraction measurement and pore structure analysis. The results show that the conversion of the reaction of CaCO3 and SO2 in air is higher at 500-1 100 ℃ and lower at 1 200 ℃ compared with that in O2/CO2 atmosphere. The conversion can be increased by increasing the concentration of SO2, which causes the inhibition of CaSO4 decomposition and shifting of the reaction equilibrium toward the products. XRD analysis of the product shows that the reaction mechanism of CaCO3 and SO2 differs with temperature in O2/CO2 atmosphere, i.e. CaCO3 directly reacts with SO2 at 500 ℃ and CaO from CaCO3 decomposition reacts with SO2 at 1 000 ℃. The pore analysis of the products indicates that the maximum specific surface area of the products accounts for the highest conversion at 1 100 ℃ in O2/CO2 atmosphere. The results reveal that the effect of the atmosphere on the conversion is temperature dependence.

Chemical-looping gasification of biomass in a 10 kW_(th) interconnected fluidized bed reactor using Fe_2O_3/Al_2O_3 oxygen carrier

Abstract:The aim of this research is to design and operate a 10 kW hot chemical-looping gasification(CLG)unit using Fe2O3/Al2O3as an oxygen carrier and saw dust as a fuel.The effect of the operation temperature on gas composition in the air reactor and the fuel reactor,and the carbon conversion of biomass to CO2and CO in the fuel reactor have been experimentally studied.A total60 h run has been obtained with the same batch of oxygen carrier of iron oxide supported with alumina.The results show that CO and H2concentrations are increased with increasing temperature in the fuel reactor.It is also found that with increasing fuel reactor temperature,both the amount of residual char in the fuel reactor and CO2concentration of the exit gas from the air reactor are degreased.Carbon conversion rate and gasification efficiency are increased by increasing temperature and H2production at 870℃reaches the highest rate.Scanning electron microscopy(SEM),X-ray diffraction(XRD)and BET-surface area tests have been used to characterize fresh and reacted oxygen carrier particles.The results display that the oxygen carrier activity is not declined and the specific surface area of the oxygen carrier particles is not decreased significantly.

Conversion of Fuel-N to N2O and NOx during Coal Combustion in Combustors of Different Scale

With focus on investigating the effect of combustor scale on the conversion of fuel-N to NOx and N20, experiments are carried out in three combustors, including single coal particle combustion test rig, laboratory scale circulating fluidized-bed boiler （CFB） and full scale CFB in this work. For single coal particle combustion, the majority of f-uel-N （65%-82%） is released as NOx, while only a little （less than 8%） fuel-N yields N20. But in labora- tory scale CFB, the conversion of fuel-N to N20 is increases, but the conversion of fuel-N to NOx is quite less than that of single coal particle combustion. This is because much char in CFB can promote the NOx reduction by in- creasing N20 formation. In full scale CFB, both of the conversion of fuel-N to NOx and the conversion of fuel-N to N20 are smaller than laboratory scale CFB.

Hydrothermal synthesis of zeolitic material from circulating fluidized bed combustion fly ash for the highly efficient removal of lead from aqueous solution

The utilization of coal fly ash derived from circulating fluidized bed combustion(CFBFA)still faces great challenges because of its unique characteristics.In this study,a zeolitic material with Na-P1 zeolite as the main phase was successfully synthesized via a hydrothermal method by using CFBFA as the raw material.The effects of hydrothermal temperature,time,and added CTAB amount on the characterizations of synthesized materials were investigated by XRD,SEM,and XPS.The properties of the optimal zeolitic material and its adsorption performance for Pb^(2+)in aqueous solution were evaluated.The influences of pH,initial concentration,dosage,and temperature on Pb^(2+)adsorption were also examined.Results revealed the following optimal parameters for the synthesis of zeolitic material:NaOH concentration of 2 mol·L^(-1),solid-to-liquid ratio of 1:10 g·ml^(-1),hydrothermal temperature of 110℃,hydrothermal time of 9 h,and CTAB amount of 1 g(per 100 ml solution).The adsorption capacities of the zeolitic material reached 329.67,424.69,and 542.22 mg·g^(-1) when the pH values of aqueous solution were 5,6,and 7,respectively.The Pb^(2+)removal efficiency can reach more than 99%in aqueous solution with the initial concentrations of 100-300 mg·L^(-1) under pH 6 and suitable adsorbent dosage.The adsorption and kinetics of Pb^(2+)on the zeolitic material can be described by Langmuir isotherm and pseudo-second-order kinetic models,respectively.The ion exchange between Pb^(2+)and Na^(+)and chemisorption are the main adsorption mechanism.All these findings imply that the synthesis of low-cost adsorbent for Pb^(2+)removal from weak acid and neutral aqueous solution provides a highly effective method to utilize CFBFA.

Role of iron-based catalysts in reducing NO_(x) emissions from coal combustion

Nitrogen oxide(NO_(x))pollutants emitted from coal combustion are attracting growing public concern.While the traditional technologies of reducing NO_(x) were mainly focused on terminal treatment,and the research on source treatment is limited.This paper proposes a new coal combustion strategy that significantly reduces NO_(x) emissions during coal combustion.This strategy has two important advantages in reducing NO_(x) emissions.First,by introducing iron-based catalyst at the source,which will catalyze the conversion of coke nitrogen to volatile nitrogen during the pyrolysis process,thereby greatly reducing the coke nitrogen content.The second is de-NO_(x) process by a redox reaction between NO_(x) and reducing agents(coke,HCN,NH_(3),etc.)that occurred during coke combustion.Compared to direct combustion of coal,coke prepared by adding iron-based catalyst has 46.1% reduction in NO_(x) emissions.To determine the effect of iron-based additives on de-NO_(x) performance,demineralized coal(de-coal)was prepared to eliminate the effect of iron-based minerals in coal ash.The effects of iron compounds,additive dosages,and combustion temperatures on de-NO_(x) efficiency are systematically studied.The results revealed that the NO_(x) emission of the coke generated by pyrolysis of de-coal loaded with 3%(mass)Fe_(2)O_(3) decreases to 27.3% at combustion temperature of 900℃.Two main reasons for lower NO_(x) emissions were deduced:(1)During the catalytic coal pyrolysis stage,the nitrogen content in the coke decreases with the release of volatile nitrogen.(2)Part of the NO_(x) emitted during the coke combustion was converted into N_(2) for the catalytic effect of the Fe-based catalysts.It is of great practical value and scientific significance to the comprehensive treatment and the clean utilization process of coal.

A pilot scale study on co-capture of SO_2 and NOx in O_2/CO_2 recycled coal combustion and techno-economic evaluation

This paper presents the study on co-capture of SO2 and NOx in O2/CO2 recycled coal combustion in a pilot scale facility with the heat input of 0.3 MW by using high-sulphur lean coal.Detailed comparison of SO2 and NOx emission indexes and desulphurization and denitration rates have been made among three working conditions of O2/CO2,O2/CO2 with limestone injection(O2/CO2+Ca) and O2/RFG(recycled flue gas) with limestone injection(O2/RFG+Ca).Combustion in air was performed as a base case.Results showed that in the O2/RFG with limestone injection,desulphurization and denitration rates could reach up to 96% and 89%,respectively.Limestone injection under the high-CO2 atmosphere caused a significant reduction on SO2 emission and NOx emission as well.This indicated O2/CO2 recycled coal combustion could reduce the investment on the flue gas purification.The techno-economic evaluation indicated that Oxy-combustion technique is not only feasible for CO2 emission control based on existing power plants but is also cost-effective.

Circulating Fluidized Bed Gasification of Low Rank Coal：Influence of O2/C Molar Ratio on Gasification Performance and Sulphur Transformation

To promote the utilization efficiency of coal resources,and to assist with the control of sulphur during gasification and/or downstream processes,it is essential to gain basic knowledge of sulphur transformation associated with gasification performance.In this research we investigated the influence of O_2/C molar ratio both on gasification performance and sulphur transformation of a low rank coal,and the sulphur transformation mechanism was also discussed.Experiments were performed in a circulating fluidized bed gasifier with O_2/C molar ratio ranging from 0.39 to 0.78 mol/mol.The results showed that increasing the O_2/C molar ratio from 0.39 to 0.78 mol/mol can increase carbon conversion from 57.65%to 91.92%,and increase sulphur release ratio from 29.66%to63.11%.The increase of O_2/C molar ratio favors the formation of H_2S,and also favors the retained sulphur transforming to more stable forms.Due to the reducing conditions of coal gasification,H_2S is the main form of the released sulphur,which could be formed by decomposition of pyrite and by secondary reactions.Bottom char shows lower sulphur content than fly ash,and mainly exist as sulphates.X-ray photoelectron spectroscopy(XPS)measurements also show that the intensity of pyrite declines and the intensity of sulphates increases for fly ash and bottom char,and the change is more obvious for bottom char.During CFB gasification process,bigger char particles circulate in the system and have longer residence time for further reaction,which favors the release of sulphur species and can enhance the retained sulphur transforming to more stable forms.

Chemical looping combustion of coal in interconnected fluidized beds

Chemical looping combustion is the indirect combustion by use of oxygen carrier. It can be used for CO2 capture in power generating processes. In this paper, chemical looping combustion of coal in interconnected fluidized beds with inherent separation of CO2 is proposed. It consists of a high velocity fluidized bed as an air reactor in which oxygen carrier is oxidized, a cyclone, and a bubbling fluidized bed as a fuel reactor in which oxygen carrier is reduced by direct and indirect reactions with coal. The air reactor is connected to the fuel reactor through the cyclone. To raise the high carbon conversion efficiency and separate oxygen carrier particle from ash, coal slurry instead of coal particle is introduced into the bottom of the bubbling fluidized bed. Coal gasification and the reduction of oxygen carrier with the water gas take place simultaneously in the fuel reactor. The flue gas from the fuel reactor is CO2 and water. Almost pure CO2 could be obtained after the condensation of water. The reduced oxygen carrier is then returned back to the air reactor, where it is oxidized with air. Thermodynamics analysis indicates that NiO/Ni oxygen carrier is the optimal one for chemical looping combustion of coal. Simulation of the processes for chemical looping combustion of coal, including coal gasification and reduction of oxygen carrier, is carried out with Aspen Plus software. The effects of air reactor temperature, fuel reactor temperature, and ratio of water to coal on the composition of fuel gas, recirculation of oxygen carrier particles, etc., are discussed. Some useful results are achieved. The suitable temperature of air reactor should be between 1050–1150°C and the optimal temperature of the fuel reactor be between 900–950°C.

CO_(2)和H_(2)O气化反应对富氧气氛煤热解和焦炭燃烧影响进展

富氧燃烧技术作为一种具有广阔前景的燃煤电站CO_(2)减排技术,对实现可持续发展的能源目标具有重要意义。由于CO_(2)和H_(2)O物理性质和气化反应的影响,煤在富氧气氛中的转化过程可能明显异于空气气氛。通过分析已有文献发现,CO_(2)对煤热解过程中挥发分的析出率和焦炭的物理结构和化学性质有一定影响,但较少学者关注CO_(2)和H_(2)O混合气体物性的作用。在煤或焦炭燃烧过程中,CO_(2)的高比热和低氧扩散速率对燃烧反应有明显抑制作用,但可能是由于H_(2)O浓度差异的原因,目前对CO_(2)和H_(2)O混合气体物性在燃烧过程中的影响机制还有争议,尤其是缺少加压下的数据。对于气化反应的影响,目前研究表明,CO_(2)单气化和CO_(2)/H_(2)O共气化提高了煤热解时挥发分轻质气体的产率,但焦炭产率却有所降低,而压力增加强化了这一影响。此外,气化作用下的煤焦可能由于表面积增加而提高了反应活性,其表面官能团结构也因气化而发生改变。关于煤或焦炭燃烧反应,目前普遍认为CO_(2)气化在温度较高和氧气浓度较低时可促进燃料碳消耗,H_(2)O的加入则进一步加速了这一过程。随着环境压力的升高,CO_(2)气化反应在燃料碳消耗中占比逐渐增大,但对于加压下CO_(2)/H_(2)O共气化的影响鲜有涉及。本研究总结了富氧气氛中CO_(2)和H_(2)O气化作用下的煤热解和焦炭燃烧行为,为今后富氧燃烧技术的发展提供了理论参考。

循环流化床NOx和SO_(2)协同脱除技术试验研究

结合循环流化床后燃技术(简称“后燃技术”)和炉内喷钙脱硫技术,在0.1 MW循环流化床试验台上研究了循环流化床NOx和SO_(2)协同脱除潜力,主要研究了后燃室脱硫剂添加量对NOx和SO_(2)排放影响以及炉内添加脱硫剂时燃烧温度对NOx和SO_(2)排放的影响。结果表明:通过后燃室注入脱硫剂可以降低SO_(2)排放,能够达到一定的脱硫效果。当燃烧温度较高时,后燃技术下炉内添加脱硫剂,脱硫效果很差。通过适当降低燃烧温度可以实现NOx和SO_(2)的协同脱除。当温度为845℃时,后燃技术下炉内脱硫时可直接实现超低NOx排放,而SO_(2)排放可以降至92.09 mg/m^(3)。后燃技术下炉内低温脱硫时,如果后燃室添加适量脱硫剂,则SO_(2)排放可进一步降低,有望实现NOx和SO_(2)双超低排放,进一步降低循环流化床污染物脱除成本。

燃煤在O_2/CO_2方式下SO_2生成特性的研究

研究了合山煤在O2 /CO2 方式下SO2 的生成特性 .结果表明在O2 /CO2 方式下 ,由于燃煤的燃烧特性和钙基吸收剂的煅烧分解特性不同于传统燃烧方式 ,SO2 的生成速度加快 ,生成量较空气气氛下大为减少 ,钙基吸收剂的脱硫率随温度升高而增加 ,表明O2 /CO2

流化床O_2/CO_2气氛木屑与煤混燃的数值模拟研究

针对6kW流化床燃烧室,建立炉内燃烧计算综合模型,对O_2/CO_2气氛流化床内煤燃烧和煤与生物质混燃过程进行数值模拟,对比研究燃料由煤变为煤与生物质混合燃料对炉内流场、温度场和燃烧特性的影响,同时对数值模拟结果进行实验验证。结果表明:在O_2/CO_2气氛下两种燃料燃烧时炉内速度、温度和组分浓度的总体分布趋势一致;生物质混燃较煤燃烧时速度、温度水平整体降低;炉内O_2和H_2O的质量分数增大而CO_2的质量分数减小;数值模拟值与实验值吻合较好。

Preheating Characteristics of Datong Coal in O2/CO2 and Air Atmospheres

Experimental studies were carried out to find the difference of preheating characteristics of Datong coal in O_2/CO_2 and air atmospheres by a circulating fluidized bed. It is found that pulverized coal could be both steadily preheated to above 800°C in the two different atmospheres, but the temperature distribution was more uniform along the riser in O_2/CO_2 atmosphere. During the preheating, the content of CO in the flue gas can reach 12.32% under the O_2/CO_2 atmosphere, far higher than that in air(5.94%). Simultaneously, the conversion rate of fixed carbon was higher in O_2/CO_2 atmosphere compared with that in air. It can be inferred the higher oxygen concentration and higher partial pressure of CO_2 have greatly accelerated the gasification reaction. The BET analysis indicated a number of large pores were transformed into micropores during the preheating progress, and the major contributors for overall pore volume of chars and specific surface area are the micro-pores and the mesopores with diameter ranging from 2 nm to 10 nm. The inner pore structure was more developed in O_2/CO_2 atmosphere.

五彩湾煤在O_2/CO_2燃烧条件下的积灰特性

锅炉燃用准东煤极易发生严重的受热面积灰结渣等问题,制约了新疆准东地区煤炭资源的大规模利用。在一维沉降炉燃烧与积灰试验系统上,研究了准东五彩湾煤的积灰特性,分析了稀释气体种类、O_2/CO_2燃烧中氧浓度对飞灰沉积的影响。结果表明:在21%氧浓度下,与稀释气体为N_2相比,稀释气体为CO_2时得到的沉积灰颗粒之间黏连现象不明显,积灰倾向较弱; O_2/CO_2燃烧条件下,随着氧浓度提高,五彩湾煤的积灰倾向加重,细散灰颗粒减少,球形灰颗粒比例增加,灰颗粒的黏连现象加重。SEM-EDS分析结果表明:O_2/CO_2燃烧中随氧浓度的提高,沉积灰中的块状灰颗粒表面缩孔及凹坑增多,且灰颗粒表面黏附了白色细散絮状灰,Na和Cl的富集加重,这是造成高氧浓度燃烧受热面积灰加剧的重要原因;稀释气体种类对五彩湾煤积灰倾向的影响研究中,稀释气体为N_2(空气燃烧)时,Na和Cl含量明显高于稀释气体为CO_2(O_2/CO_2燃烧)时的含量。此外,燃烧稀释气体为N_2的沉积灰中还出现了Ca和S元素的富集,高温下CaO与硅铝酸盐发生反应生成低温共熔体,这也是空气燃烧时积灰较O_2/CO_2燃烧严重的重要原因。XRD分析结果在一定程度上佐证了EDS的分析结论,灰分中CaSO_4、NaCl等低熔点物质的富集导致了空气燃烧工况和O_2/CO_2高氧浓度燃烧工况积灰的加剧。燃烧的颗粒温度差异是导致O_2/CO_2燃烧和空气燃烧积灰特性不同的主要原因,也是造成不同氧浓度下O_2/CO_2燃烧积灰特性差异的主要原因。煤燃烧的颗粒温度较高时,煤粉着火、燃烧性能得到改善,更高的颗粒温度会导致烟气中出现更多的熔融灰,灰颗粒表面出现熔融相进而增强了灰表面的黏性,加剧积灰现象。

CFB中基于赤泥催化的N_(2)O/NO_(x)/SO_(2)协同降低技术路线

随着污染物排放标准越发严格,为进一步发挥循环流化床污染物控制成本低的优势,需要明晰各个运行参数和因素对N_(2)O/NO_(x)/SO_(2)排放的影响规律,挖掘N_(2)O/NO_(x)/SO_(2)协同超低排放的可能性。基于“十四五”规划的要求和N_(2)O/NO_(x)/SO_(2)的研究现状,初步形成了一条或实现N_(2)O/NO_(x)/SO_(2)协同降低的技术路线:在保证燃烧效率的前提下,选择合适的床料(如赤泥)在炉内通过催化或反应脱除N_(2)O,通过平衡赤泥中的铝铁比例,实现N_(2)O和NO_(x)的双低排放,同时由于赤泥良好的吸附能力和较强的碱性,可进一步实现SO_(2)的脱除。如必要,通过流态重构或超细石灰石等将剩余的NO_(x)和SO_(2)降至合理水平,或通过SNCR和脱硫塔分别处理剩余的NO_(x)和SO_(2),使其达到排放标准,从而实现N_(2)O/NO_(x)/SO_(2)的协同超低排放。