Characteristics of the sub-micron ash aerosol generated during oxy-coal combustion at atmospheric and elevated pressures

This paper is concerned with the effect of pressure on the particle size distribution and the size-segregated composition of the sub-micron ash aerosol created during oxy-coal combustion under near practical self-sustaining combustion conditions. The problem is important because pressurized oxy-coal combustion has been proposed as one promising technology to minimize CO₂ emissions. Sub-micron ash plays a major role in ash deposition mechanisms, which, in turn, can control boiler performance. In this work, the same bituminous coal was burned at pressures of 1, 8 and 15 bar in O₂/CO₂ environments. Tests employed a 100 kW (rated) oxy-fuel combustor (OFC) operated at atmospheric pressure (1 bar) and a 300 kW (rated) entrained-flow pressurized reactor (EFPR) at elevated pressures (8 and 15 bar). Although these tests were conducted under near practical combustion conditions, confounding effects of peak flame temperature variations were minimized for the 1 bar and 15 bar tests, allowing the role of elevated pressure to be isolated. For the EFPR tests, a specially designed sampling system was used to sample sub-micron ash aerosols from the pressurized combustor and is described in detail. Results showed that at the same peak temperature but higher pressure, the fractions of ash aerosol partitioned into the PM_0.6 and PM₁ size fractions were greatly diminished. Moreover, elevated pressures caused significant changes in the composition of the (size-segregated) sub-micron aerosol, especially in its alkali content, which increased significantly. Examination of fractions of each element that ended up in the sub-micron fume suggested that, at constant temperature, the effect of pressure on vaporization of semi-volatile metals was very different from that on the release into the gas phase of non-volatile metals and could not be explained by equilibrium.     

Pressurized oxy-fuel combustion of a char particle in the fluidized bed combustor

Pressurized oxy-fuel combustion of coal in fluidized bed (FB) holds the potential to realize low-cost CO₂ capture. However, the fundamental study in this manner is still rare due to the difficult access to the pressurized oxy-FB combustion tests. In this work, the experimental study of single char combustion was firstly conducted in a visualized pressurized FB combustor under various operating conditions. Then an experimentally verified particle-scale char combustion model was developed to reveal the dependence of char combustion on parameters. Results showed that the char conversion was accelerated with the increase of pressure, mainly due to the high oxygen diffusion and char gasification. The gasification played a non-negligible role in pressurized oxy-fuel combustion, especially under high oxygen concentration and bed temperature. Increasing oxygen concentration and bed temperature not only promotes the char oxidation rate and particle temperature, but also increases the gasification rate and the share of char conversion via gasification, resulting in shortening the burnout time of char. In addition, a higher fluidization number lowered both the burnout time and peak temperature of char particle, due to the simultaneous improvement of mass and heat transfer. The influences of char size and fluidization number on char gasification conversion ratio are very weak. In addition, the quantitative analysis of the influence of different operating parameters on the combustion process was obtained by model sensitivity analysis.     

Modeling of the submicron particles formation and initial layer ash deposition during high temperature oxy-coal combustion

The future use of coal as a fuel for power generation in the US depends on the availability of financially viable technologies for capture and storage of CO₂ emissions from power plants. Key second-generation candidates for CO₂ capture include high temperature and pressurized oxy-firing of coal, which has the potential to increase efficiency, lower capital costs, avoid air ingress and reduce oxygen requirements. However, unquantified challenges, such as flame behavior, heat transfer, ash transformation, ash deposition and char oxidation, still exist for those technologies. This study specifically focuses on the formation of submicron particles and initial layer ash deposition during high temperature oxy-coal combustion. Previous work has shown that the initial layer deposits are mainly formed of submicron size ash aerosols transported by thermophoresis. Unfortunately, the importance of submicron particle deposition has not received much attention, probably due to the insignificant deposit mass and difficulty in prediction of the submicron particles formation. In this work, models including mineral matter vaporization model, scavenging model and deposition model are developed and applied into a three-dimensional CFD framework to predict the submicron particles formation and subsequent initial layer deposits formation. The model results are comparable to experimental data. The merits of this work are that it has led to the development of a novel approach to predict both submicron particle formation and initial layer ash deposition during oxy-coal combustion.     

Influence of combustion temperature and coal types on alumina crystal phase formation of high-alumina coal ash

The alumina content (more than 40%) of high-alumina coal ash is comparative to the middle content bauxite ores in China. So far, in order to meet the high demand of alumina and the rise of circular economy industrial chain, extracting alumina from coal ash has become a way to comprehensively utilize high-alumina coal ash. However, this process has high requirements on the crystal phase and stability of alumina. Different from most studies, this paper focuses on how to produce coal ash more beneficial to the later refining of aluminum. Therefore, the effects of combustion temperature and coal types by classifying high-alumina coal into dull coal and bright coal on alumina crystal phase formation were studied. Through proximate analysis, ultimate analysis, calorific value analysis, X-ray fluorescence spectroscopy, X-ray diffraction (XRD) and scanning electron microscope (SEM) and other methods, it is found that γ-Al₂O₃ in high-alumina coal ash translated into more stable θ-Al₂O₃ and finally α-Al₂O₃ when combustion temperature is higher than 1000°C. Thus compared with pulverized coal boilers, circulating fluidized bed (CFB) boilers with lower combustion temperature can produce higher quality coal ash. Moreover, at the same combustion temperature, alumina crystal phase in dull coal ash is relatively less stable than that in bright coal ash, which is more suitable to the later refining and electrolysis of aluminum.     

Experimental study on co-firing characteristics of ammonia with pulverized coal in a staged combustion drop tube furnace

Utilizing ammonia as a co-firing fuel to replace amounts of fossil fuel seems a feasible solution to reduce carbon emissions in existing pulverized coal-fired power plants. However, there are some problems needed to be considered when treating ammonia as a fuel, such as low flame stability, low combustion efficiency, and high NO_x emission. In this study, the co-firing characteristics of ammonia with pulverized coal are studied in a drop tube furnace with staged combustion strategy. Results showed that staged combustion would play a key role in reducing NO_x emissions by reducing the production of char-NO_x and fuel(NH₃)-NO_x simultaneously. Furthermore, the effects of different ammonia co-firing methods on the flue gas properties and unburned carbon contents were compared to achieve both efficient combustion and low NO_x emission. It was found that when ammonia was injected into 300 mm downstream under the condition of 20% co-firing, lower NO_x emission and unburnt carbon content than those of pure coal combustion can be achieved. This is probably caused by a combined effect of a high local equivalence ratio of NH₃/air and the prominent denitration effect of NH₃ in the vicinity of the NH₃ downstream injection location. In addition, NO_x emissions can be kept at approximately the same level as coal combustion when the co-firing ratio is below 30%. And the influence of reaction temperature on NO_x emissions is closely associated with the denitration efficiency of the NH₃. Almost no ammonia slip has been detected for any injection methods and co-firing ratio in the studied conditions. Thus, it can be confirmed that ammonia can be used as an alternative fuel to realize CO₂ reduction without extensive retrofitting works. And the NO_x emission can be reduced by producing a locally NH₃ flame zone with a high equivalence ratio as well as ensuring adequate residence time.     

Measurements and modelling of oxy-fuel coal combustion

Oxy-fuel combustion is one of the most promising technologies to isolate efficiently and economically CO₂ emissions in coal combustion for the ready carbon sequestration. The high proportions of both H₂O and CO₂ in the furnace have complex impacts on flame characteristics (ignition, burnout, and heat transfer), pollutant emissions (NO_x, SO_x, and particulate matter), and operational concerns (ash deposition, fouling/slagging). In contrast to the existing literature, this review focuses on fundamental studies on both diagnostics and modelling aspects of bench- or lab-scale oxy-fuel combustion and, particularly, gives attention to the correlations among combustion characteristics, pollutant formation, and operational ash concerns. First, the influences of temperature and species concentrations (e.g., O₂, H₂O) on coal ignition, volatile combustion and char burning processes, for air- and oxy-firing, are comparatively evaluated and modelled, on the basis of data from optically-accessible set-ups including flat-flame burner, drop-tube furnace, and down-fired furnace. Then, the correlations of combustion-generated particulate/NO_x emissions with changes of combustion characteristics in both air and oxy-fuel firing modes are summarized. Additionally, ash deposition propensity, as well as its relation to the formation of fine particulates (i.e. PM_0.2, PM₁ and PM₁₀), for both modes are overviewed. Finally, future research topics are discussed. Fundamental oxy-fuel combustion research may provide an ideal alternative for validating CFD simulations toward industrial applications.     

循环流化床煤燃烧中氮氧化物排放的研究

循环流化床煤燃烧中氮氧化物排放的研究冯波，袁建伟，刘皓，卢建欣，林志杰，刘德昌（华中理工大学动力系武汉４３００７４）关键词循环流化床，氮氧化物１前言近年来，ＮＺＯ由于对臭氧层的破坏作用和一定的温室效应而引起了较大的关注。特别地，在流化床煤燃烧中（包括...     

钙基载氧体煤化学链燃烧脱硫试验研究

在钙基载氧体燃煤化学链燃烧技术过程中由于煤气化产物与载氧体之间的副反应导致反应过程中产生大量的SO₂气体。本文选择MAC铁矿石,CaO和石灰石作为脱硫剂,在小型加压固定床上研究不同温度、压力、Ca/S比条件下SO₂气体的脱除问题。结果表明,单独采用CaSO₄载氧体时,随温度升高SO₂气体浓度逐渐增加。添加铁矿石后,SO₂排放浓度降低,主要与Fe₂O₃能够催化抑制CaSO₄分解有关。添加CaO和石灰石脱硫剂后,随温度、压力以及Ca/S比增加,两种脱硫剂的脱硫效率均增加,且在相同的实验条件下得到的CaO的脱硫效果更佳。     

In-situ gasification chemical looping combustion of plastic waste in a semi-continuously operated fluidized bed reactor

Conventional air incineration of plastic waste has been considered as one of important sources of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) through de novo synthesis and precursor conversion. Chemical looping combustion (CLC) is an attractive technology for the conversion of plastic wastes to energy with the potential to drastically suppress the formation of PCDD/Fs. In this paper, the iG-CLC (in-situ gasification CLC) experiments of plastic waste were implemented in a semi-continuously operated fluidized bed reactor, which actually simulates the fuel reactor of a continuously-operated interconnected fluidized bed reactor. A kind of low-cost material, natural iron ore without/with 5 wt% CaO adsorbent through the ultrasonic impregnation method, was used as oxygen carrier (OC). Firstly, some key performances of the reactor system, such as the relevance of the bed inventory to the flow rate of fluidizing agent as well as the relationship between the feeding rate and overflow rate of OC, were calibrated. Then, 90 min of single experiment was conducted for each experimental case and an accumulative operation of more than 10 h was attained. Typically, the combustion efficiency can reach at about 98%, and both the carbon conversion and CO₂ yield can approach to 95% at 900 °C and input thermal power of 150 W with a mixture of 5 vol% H₂O and 95 vol% N₂ as the fluidizing agent (U_FR/U_mf = 3). Moreover, the results obtained in the semi-continuously operated fluidized bed reactor demonstrated that CaO decoration to iron ore is conductive to suppressing the formation of chlorobenzene (as a toxic matter and precursor/intermediate of PCDD/Fs) and does not obviously deteriorate the OC performance.     

从软、硬球模型探讨颗粒自转对流化状态的影响

发展流化床燃煤锅炉在国内外均受到广泛重视并被许多国家列为洁净煤燃烧技术之一．然而,一些涉及流化床基础理论的问题至今尚需进一步研究。针对流化床内颗粒自转是否对流化状态产生影响这一众多研究者所关心的问题,本文采用数值模拟的方法,分别用软、硬球模型对该问题进行了研究探讨,得到了与之相关的结论。     

流化床燃烧超低浓度煤层气的轴向气体分布

超低浓度煤层气由于甲烷含量低、浓度变化大而较难加以利用。采用实验和数值模拟的方法,研究了超低浓度煤层气在流化床中燃烧特性,得到燃烧产物的轴向分布规律,分析了进气浓度、床层温度、流化风速等因素对甲烷浓度轴向分布的影响。研究结果表明:随着床层高度的增加,无量纲甲烷浓度逐渐减小,在床层表面达到最小值,然后突然增加,随后达到稳定。实验范围内,CO浓度均小于20mL/m~3减小进气浓度、增加床层温度、降低流化风速部会使相同床层高度处的无量纲甲烷浓度减小。燃烧反应主要发生在密相区,随着进气浓度的减小、床层温度的增加、流化风速的降低,反应区域逐渐向床层下部移动。     

中试规模的第二代增压流化床联合循环发电技术研究与开发

第二代增压流化床联合循环发电技术(2G PFBC-CC)是当前具有应用前景的洁净煤发电技术之一。东南大学热能工程研究所构建了2 MWt加压喷动流化床部分气化炉,对原有1 MWt增压流化床燃烧炉进行了改造,形成了较完整的2G PFBC-CC系统．经过二年多的调试和试验研究,验证了2G PFBC-CC工艺可行性和先进性,部分气化炉产生的煤气热值在4．2 MJ／Nm3以上,满足燃气透平的要求,排出的半焦可在PFB燃烧炉内稳定燃烧,飞灰含碳量在2％以下,系统碳利用效率在99％以上。     

Behavior of coal-chlorine in chemical looping combustion

This work focuses on two aspects: (i) the behavior of coal-derived chlorine in chemical looping combustion (CLC); (ii) the potential adverse impacts of primary gaseous chlorine (i.e., HCl) on Cu-based oxygen carrier (OC). The inactivation mechanism of the sol-gel-derived CuO/Al₂O₃ OC is investigated. Systematic experiments are conducted in a batch fluidized reactor. First, in CLC of coal, chlorine distribution including HCl, Cl₂, Cl adsorbed in the outlet tube and Cl in solid phase is studied under various bed inventories, temperatures and gas atmospheres. The main gaseous Cl from coal is HCl, which shows a high reactivity towards CuO and is partially physically adsorbed by Al₂O₃. Unconverted HCl is 15.63 ± 0.20%, which could result in corrosion of the CO₂ transportation line and compression equipment. What's more, the coal ash exhibits a dechlorination function by forming KCl and CaCl₂. The CO₂ atmosphere and high temperature in fuel reactor show a promotion on the conversion of coal-Cl to HCl. Then, the corrosion of various OC components is evaluated by a mixture gas with 400 ppm HCl, i.e., Cu-Al (whole OC), CuO (active phase) and Al₂O₃ (inert support phase). It is found that a part of HCl is converted to Cl₂ via the Deacon reaction (4HCl + O₂ = 2H₂O + 2Cl₂) and oxidized by CuO (2CuO + 4HCl = 2CuCl + Cl₂ + 2H₂O). At the high concentration of HCl (400 ppm) atmosphere, CuO is partially lost from the OC, producing the gaseous copper chlorides, i.e., CuCl and (CuCl)₃, which are found to be condensed in the outlet tube. Besides, the solid-phase copper chlorides also degrade the oxygen donation capacity of the OC. Finally, the migration path of coal-chlorine during CLC is summarized. This work will contribute to the development of Cl-resistance OCs and control approaches for Cl emission.     

Combustion processes for carbon capture

A review of the technologies for coal-based power generation closest to commercial application involving carbon capture is presented. Carbon capture and storage (CCS) developments are primarily adaptations of conventional combustion systems, with additional unit operations such as bulk oxygen supply, CO₂ capture by sorbents, CO₂ compression, and storage. They use pulverized coal combustion in entrained flow—the dominant current technology for coal-based power, or gasification in entrained flow, although similar concepts apply to other solid-gas contacting systems such as fluidized beds. Currently, the technologies have similar generation efficiencies and are associated with efficiency penalties and electricity cost increases due to operations required for carbon capture. The R&D challenges identified for the combustion scientist and engineer, with current understanding being detailed, are those of design, optimisation and operational aspects of new combustion and gasification plant, controlling the gas quality required by CCS related units and associated emission compliance, and gas separations. Fundamental research needs include fuel reactions at pressure, and in O₂/CO₂ atmospheres, as few studies have been made in this area. Laboratory results interpreted and then included in CFD models of combustion operations are necessary. Also identified, but not detailed, are combustion issues in gas turbines for IGCC and IGCC-CCS. Fundamental studies should be a component of pilot-plant and demonstrations at practical scale being planned. Concepts for new designs of combustion equipment are also necessary for the next generation of technologies. The challenges involved with the design and operation of these integrated systems, while supplying electricity on demand, are considerable.     

Ignition and volatile combustion behaviors of a single lignite particle in a fluidized bed under O2/H2O condition

O₂/H₂O combustion, as a new evolution of oxy-fuel combustion, has gradually gained more attention recently for carbon capture in a coal-fired power plant. The physical and chemical properties of steam e.g. reactivity, thermal capacity, diffusivity, can affect the coal combustion process. In this work, the ignition and volatile combustion characteristics of a single lignite particle were first investigated in a fluidized bed combustor under O₂/H₂O atmosphere. The flame and particle temperatures were measured by a calibrated two-color pyrometry and pre-buried thermocouple, respectively. Results indicated that the volatile flame became smaller and brighter as the oxygen concentration increased. The ignition delay time of particle in dense phase was shorter than that in dilute phase due to its higher heat transfer coefficient. Also, the volatile flame was completely separated from particles (defined as off-flame) in dense phase while the flame lay on the particle surface (defined as on-flame) in dilute phase. The self-heating of fuel particles by on-flame in dilute phase was more obvious than that in dense phase, leading to earlier char combustion. At low oxygen concentration, the flame in the H₂O atmosphere was darker than that in the N₂ atmosphere because the heat capacity of H₂O is higher than that of N₂. With the increase of oxygen concentration, the flame temperature in the O₂/H₂O atmosphere was dramatically enhanced rather than that in the O₂/N₂ atmosphere, where the diffusion rate of oxygen in O₂/N₂ atmosphere became the dominant factor.     

城市下水污泥和煤/LPG在循环流化床上的混烧试验研究

在高6000 mm、直径300mm的循环流化床上进行了含水率为79％的湿污泥与煤／石油液化气(LPG)的混烧试验。试验结果表明:无论用煤还是LPG作为辅助燃料,试验都能在设定的工况条件下稳定运行;向炉内加入石灰石的量达到钙硫摩尔比为3．4∶1时,二氧化硫和氯化氢的排放达标,脱硫效率和脱氯效率分别为75％和94％;在试验中, 烟气中NOx排放、烟气中汞含量和二恶英类排放都不超标;试验产生的飞灰含碳量低,飞灰中痕量元素的浸出毒性不超标;计算表明,如果利用余热干燥污泥和预热空气可有效地减少辅助燃料的消耗量。     

煤燃烧过程中铜对多环芳烃生成的影响

研究了两种燃烧方式煤燃烧过程中金属铜的添加对多环芳烃生成的影响。结果表明:随着铜煤质量比的增加,管式炉煤燃烧多环芳烃生成浓度是减少的;流化床煤燃烧多环芳烃生成浓度是增加的,但要小于管式炉条件下两个数量级。多环芳烃生成毒性分布类似于多环芳烃生成浓度分布。而单个多环芳烃生成有着较大区别,同燃烧方式、存在状态、铜的含量等有较大关系。在燃烧温度下,铜的添加主要对高环物质的催化作用较为明显。     

Additional criteria for MILD coal combustion

We proposed a theoretical basis for Moderate or Intense Low-oxygen Dilution (MILD) coal combustion based on the turbulent scalar energy spectra. This is motivated by the hypothesis that smallest scalar mixing length scales should be on the order of the particle size or smaller to ensure that mixing can occur to prevent formation of diffusion flames. Our proposed criterion is evaluated using several experimental datasets from the literature for coal combustion in both MILD and traditional combustion regimes. The experimental results confirm that the smallest mixing length scales should be of the order of or smaller than the particle diameter, η_mix?d_p, to breakup the heat and mass transfer boundary layers around particles in MILD coal combustion. Results indicate that poor mixing of species with small Schmidt numbers around small particles leads to the high luminous intensity in the reactor. The effects of inlet velocity and jet diameter on the mixing length scales are analyzed. Higher inlet velocity and smaller jet diameter are expected to reach MILD regime. The proposed criterion can be used to guide experimental design to achieve MILD conditions for coal combustion.     

Optical characterization of methanol compression-ignition combustion in a heavy-duty engine

In the search for renewable fuels, there are very few candidates as compelling as methanol. It can be derived from refuse material and industrial waste, while the infrastructure exists worldwide to support broad and fast adoption, potentially even as a “drop-in” fuel for existing vehicles with only minor modifications. The most efficient engines currently available are compression-ignition engines, however they often come with high emissions or compromises like the soot-NO_x trade-off. Methanol however, is a low sooting fuel that can potentially be used in such engines despite its high resistance to auto-ignition and reduce emissions while maintaining high engine efficiency. Due to the auto-ignition resistance, few studies of methanol compression-ignition exist and even fewer are conducted in an optically accessible engine. Here, two cases of premixed combustion and two of spray-driven combustion of methanol are studied in a Heavy-Duty optically accessible engine. Ignition and combustion propagation are characterized with a combination of time-resolved natural flame luminosity measurements and single-shot, acetone fuel-tracer, laser induced fluorescence. Additionally, Mie-scattering is used to identify the interaction between liquid spray and ignition sites in spray-driven methanol combustion. Results show that methanol combusts drastically different compared to conventional fuels, especially in spray-driven combustion. The evaporative cooling effect of methanol appears to play a major role in the auto-ignition characteristics of the delivered fuel. Ignition sites appear right at the end of injection when the evaporative cooling effect is withdrawn or at liquid length oscillations where, again the effect is momentarily retracted. To the authors’ knowledge, this has not been documented before.     

Influence of wall heat loss on the emission characteristics of premixed ammonia-air swirling flames interacting with the combustor wall

The influence of wall heat loss on the emission characteristics of ammonia-air swirling flames has been investigated employing Planar Laser-Induced Fluorescence imaging of OH radicals and Fourier Transform Infrared spectrometry of the exhaust gases in combustors with insulated and uninsulated walls over a range of equivalence ratios, ?, and pressures up to 0.5 MPa. Strong influence of wall heat loss on the flames led to quenching of the flame front near the combustor wall at 0.1 MPa, resulting in large unburned NH₃ emissions, and inhibited the stabilization of flames in the outer recirculating zone (ORZ). A decrease in heat loss effects with an increase in pressure promoted extension of the fuel-rich stabilization limit owing to increased recirculation of H₂ from NH₃ decomposition in the ORZ. The influence of wall heat loss resulted in emission trends that contradict already reported trends in literature. NO emissions were found to be substantially low while unburned NH₃ and N₂O emissions were high at fuel-lean conditions during single-stage combustion, with values such as 55 ppmv of NO, 580 ppmv of N₂O and 4457 ppmv of NH₃ at ? = 0.8. In addition, the response of the flame to wall heat loss as pressure increased was more important than the effects of pressure on fuel-NO emission, thereby leading to an increase in NO emission with pressure. It was found that a reduction in wall heat loss or a sufficiently long fluid residence time in the primary combustion zone is necessary for efficient control of NH₃ and N₂O emissions in two-stage rich-lean ammonia combustors, the latter being more effective for N₂O in addition to NO control. This study demonstrates that the influence of wall heat loss should not be ignored in emissions measurements in NH₃-air combustion, and also advances the understanding of previous studies on ammonia micro gas turbines.