Simultaneous easy CO2 recovery and drastic reduction of SOx and NOx in O2/CO2 coal combustion with heat recirculation

Coal combustion with O₂/CO₂ is promising because of its easy CO₂ recovery, extremely low NO_x emission and high desulfurization efficiency. Based on our own fundamental experimental data combined with a sophisticated data analysis, its characteristics were investigated. It was revealed that the conversion ratio from fuel-N to exhausted NO in O₂/CO₂ pulverized coal combustion was only about one fourth of conventional pulverized coal combustion. To decrease exhausted NO further and realize simultaneous easy CO₂ recovery and drastic reduction of SO_x and NO_x, a new scheme, i.e. O₂/CO₂ coal combustion with heat recirculation, was proposed. It was clarified that in O₂/CO₂ coal combustion, with about 40% of heat recirculation, the same coal combustion intensity as that of coal combustion in air could be realized even at an O₂ concentration of as low as 15%. Thus exhausted NO could be decreased further into only one seventh of conventional coal combustion. Simultaneous easy CO₂ recovery and drastic reduction of SO_x and NO_x could be realized with this new scheme.     

CO2 capture using oxygen enhanced combustion strategies for natural gas power plants

This paper describes a series of experiments conducted with natural gas in air and in mixtures of oxygen and recycled flue gas, termed O₂/CO₂ recycle combustion. The objective is to enrich the flue gas with CO₂ to facilitate its capture and sequestration. Detailed measurements of gas composition, flame temperature and heat flux profiles were taken inside CANMET's 0.3 MWth down-fired vertical combustor fitted with a proprietary pilot scale burner. Flue gas composition was continuously monitored. The effects of burner operation, including swirling of secondary stream and air staging, on flame characteristics and NO_x emissions were also studied. The results of this work indicate that oxy-gas combustion techniques based on O₂/CO₂ combustion with flue gas recycle offer excellent potential for retrofit to conventional boilers for CO₂ emission abatement. Other benefits of the technology include considerable reduction and even elimination of NO_x emissions, improved plant efficiency due to lower gas volume and better operational flexibility.     

Experimental investigation of NOx emissions in oxycoal combustion

This work presents the results of an experimental investigation on NO_x emissions from coal combustion in a pilot scale test facility. Three oxidiser atmospheres have been compared, namely air, CO₂/O₂, and O₂ enriched recirculated flue gas. NO_x emissions from two different combustion modes have been studied, swirl flame and flameless combustion. The influence of the burner oxygen ratio and the oxidiser O₂ concentration on NO_x formation and reduction have been analysed. With increasing burner oxygen ratio, an increase of NO_x emissions has been obtained for air and CO₂/O₂ in both, swirl flame and flameless combustion. In case of the swirl flame, flue gas recirculation leads to a reduction of NO_x emissions up to 50%, whereas in case of flameless combustion this reduction is around 40% compared to CO₂/O₂. No significant impact of the oxidiser O₂ concentration in the CO₂/O₂ mixture on NO_x emissions is observed in the range between 18 and 27 vol.% in swirl flames. An analysis of NO_x formation and reduction mechanisms showed, that the observed reduction of NO_x emissions by flue gas recirculation cannot be attributed to the reduction of recirculated NO_x alone, but also to a reduced conversion of fuel-N to NO.     

Comparisons of pulverized coal combustion in air and in mixtures of O2/CO2

Pulverized coal combustion in air and the mixtures of O₂/CO₂ has been experimentally investigated in a 20 kW down-fired combustor (190 mm id×3 m). Detailed comparisons of gas temperature profiles, gas composition profiles, char burnouts, conversions of coal–N to NO_x and coal–S to SO₂ and CO emissions have been made between coal combustion in air and coal combustion in various O₂/CO₂ mixtures. The effectiveness of air/oxidant staging on reducing NO_x emissions has also been investigated for coal combustion in air and O₂/CO₂ mixtures. The results show that simply replacing the N₂ in the combustion air with CO₂ will result in a significant decrease of combustion gas temperatures. However, coal combustion in 30% O₂/70% CO₂ can produce matching gas temperature profiles to those of coal combustion in air while having a lower coal–N to NO_x conversion, a better char burnout and a lower CO emission. The results also confirm that air/oxidant staging is very effective in reducing NO_x emissions for coal combustion in both air and a 30% O₂/70% CO₂ mixture. SO₂ emissions are proved to be almost independent of the combustion media investigated.     

The effect of O2 enrichment on NOx formation in biomass co-fired pulverised coal combustion

Oxygen enrichment of the combustion air in pulverised coal combustion for power plant is seen as a possible retrofit measure to improve CO₂ scrubbing and capture. This technique produces a reduced volume of flue gas with higher CO₂ concentration than normal air combustion that will contributes to the enhancement of amine scrubbing plant efficiencies. We report in this article the results of a study at the small pilot scale into the effect of these combustion modifications on the formation of NO_x and associated carbon burnout changes. Experiments were performed using a Russian coal, typical of that used in some UK power stations with shea meal and Pakistani cotton stalk as biomass fuels co-fired at a fraction of 15%th. The down-fired pulverised coal combustor was operated at 20 kWth under air-staged conditions for NO_x control and the secondary and over-fire air flows were both enriched by up to 79% (100% O₂) for a range of splits giving a 35% overall O₂ concentration for full enrichment. When the same enrichment process was applied to biomass/coal combustion different behaviour was observed with respect to NO_x formation. We have shown that oxygen enrichment can achieve benefits of improved carbon burnout with a positive impact on NO_x emissions over and above the primary aim of increasing CO₂ concentration in the flue gas for enhanced capture efficiencies. With all other conditions of overall stoichiometry, OFA levels and O₂ enrichment levels remaining the same, NO_x levels at 22% OFA initially increased over the range of secondary air enrichment, particularly for shea meal/coal co-firing. At 31% OFA the trends were to lower NO_x at high enrichment levels. However, co-firing with shea meal initially showed an increase in NO_x emission at lower levels of enrichment (up to 40% O₂) followed by overall lower NOx emissions at 100% O₂ in the secondary air. The results show that NO_x emissions can either increase or decrease depending on the operating conditions. The differences in behaviour are attributed, not only to the effects of enrichment on the stoichiometry of the near-burner zone, but also on the flame dynamics and intensity of combustion related to the associated reductions in gas velocity and swirl intensity by the transition from air to pure O₂ in the secondary oxidant stream.     

Numerical analysis of pulverized coal combustion characteristics using advanced low-NOx burner

A three-dimensional numerical simulation is applied to a pulverized coal combustion field in a test furnace equipped with an advanced low-NO_x burner called CI-α burner, and the detailed combustion characteristics are investigated. In addition, the validities of the existing NO_x formation and reduction models are examined. The results show that a recirculation flow is formed in the high-gas-temperature region near the CI-α burner outlet, and this lengthens the residence time of coal particles in this high-temperature region, promotes the evolution of volatile matter and the progress of char reaction, and produces an extremely low-O₂ region for effective NO reduction. It is also found that, by lessening the effect of NO reduction in Levy et al.'s model and taking the NO formation from char N into account, the accuracy of the NO prediction is improved. The efficiency factor of the conversion of char N to NO affects the total NO concentration downstream after the injection of staged combustion air.     

Impact of air staging along furnace height on NOx emissions from pulverized coal combustion

Experiments were carried out on an electrically heated multi-path air inlet one-dimensional furnace to assess NO_x emission characteristics of an overall air-staged (also termed air staging along furnace height) combustion of bituminous coal. The impact of main parameters of overall air-staged combustion technology, including burnout air position, air stoichiometric ratio, levels of burnout air (the number of burnout air arranged at different heights of the furnace), and the ratios of the burnout air flow rates and pulverized coal fineness of industrial interest, on NO_x emission were simulated to study in the experimental furnace, as well as the impact of air staging on the carbon content of the fly ash produced. These results suggest that air-staged combustion affects a pronounced reduction in NO_x emissions from the combustion of bituminous coal. The more deeply the air is staged, the further the NO_x emission is reduced. Two-level air staging yields a greater reduction in NO_x emission than single-level air staging. For pulverized coal of differing fineness, the best ratio between the burnout air rates in the two-level staging ranges from 0.6 to 0.3. In middle air-staged degree combustion with f_M = 0.75, pulverized coal fineness, R₉₀ (%), has a greater influence on NO_x emission, whereas R₉₀ has little influence on NO_x emission for deep air-staged degree with f_M = 0.61. Air-staged combustion with proper burnout air position has little effect on the burnout. For overall air-staged combustion, proper burnout air position and air-staged rate should be considered together in order to achieve high combustion efficiency.     

Theoretical and experimental study on the emission characteristics of waste plastics incineration by modified O2/RFG combustion technology

For mitigating the emission of greenhouse gas CO₂ from general air combustion systems, a clean combustion technology O₂/RFG is in development. The O₂/RFG combustion technology can significantly enhance the CO₂ concentration in the flue gas; however, using almost pure oxygen or pure CO₂ as feed gas is uneconomic and impractical. As a result, this study proposes a modified O₂/RFG combustion technology in which the minimum pure oxygen is mixed with the recycled flue gas and air to serve as the feed gas. The effects of different feed gas compositions and ratios of recycled flue gas on the emission characteristics of CO₂, CO and NO_x during the plastics incineration are investigated by theoretical and experimental approaches.Theoretical calculations were carried out by a thermodynamic equilibrium program and the results indicated that the emissions of CO₂ were increased with the O₂ concentrations in the feed gas and the ratios of recycled flue gas increased. Experimental results did not have the same trends with theoretical calculations. The best feed gas composition of the modified O₂/RFG combustion was 40% O₂ + 60% N₂ and the best ratio of recycled flue gas was 15%. As the O₂ concentration in feed gas and the ratio of recycled flue gas increased, the total flow rates and pressures of feed gas reduced. The mixing of solid waste and feed gas was incomplete and the formation of CO₂ decreased. Moreover, the emission of CO was decreased as the O₂ concentration in feed gas and the ratio of recycled flue gas increased. The emission of NO_x gradually increased with rising the ratio of recycled flue gas at lower O₂ concentration (<40%) but decreased at higher O₂ concentration (>60%).     

Calcination and sintering characteristics of limestone under O2/CO2 combustion atmosphere

The O₂/CO₂ coal combustion technology is an innovative combustion technology that can control CO₂, SO₂ and NO_x emissions simultaneously. Calcination and sintering characteristics of limestone under O₂/CO₂ atmosphere were investigated in this paper. The pore size, the specific pore volume and the specific surface area of CaO calcined were measured by N₂ adsorption method. The grain size of CaO calcined was determined by XRD analysis. The specific pore volume and the specific surface area of CaO calcined in O₂/CO₂ atmosphere are less than that of CaO calcined in air at the same temperature. And the pore diameter of CaO calcined in O₂/CO₂ atmosphere is larger than that in air. The specific pore volume and the specific surface area of CaO calcined in O₂/CO₂ atmosphere increase initially with temperature, and then decline as temperature exceeds 1000 °C. The peaks of the specific pore volume and the specific surface area appear at 1000 °C. The specific surface area decreases with increase in the grain size of CaO calcined. The correlations of the grain size with the specific surface area and the specific pore volume can be expressed as L = 744.67 + 464.64 lg(1 / S) and L = − 608.5 + 1342.42 lg(1 / ε), respectively. Sintering has influence on the pore structure of CaO calcined by means of influencing the grain size of CaO.     

CoAl2O4 spinel catalyst for soot combustion with NOx/O2

Mesoporous and nanosized cobalt aluminate spinel with high specific surface area was prepared using microwave assisted glycothermal method and used as soot combustion catalyst in a NO_x + O₂ stream. For comparison, zinc aluminate spinel and alumina supported platinum catalysts were prepared and tested. All samples were characterised using XRD, (HR)TEM, N₂ adsorption–desorption measurements. The CoAl₂O₄ spinel was able to oxidise soot as fast as the reference Pt/Al₂O₃ catalyst. Its catalytic activity can be attributed to a high NO_x chemisorption on the surface of this spinel, which leads to the fast oxidation of NO to NO₂.     

The application of FLOX/COSTAIR technologies to reduce NOx emissions from coal/biomass fired power plant: A technical assessment based on computational simulation

Nitrogen oxides (NO_x) is one of the harmful emissions from power plants. Efforts are made to reduce NO_x emissions by researchers and engineers all the times. NO_x emissions are from three resources during the combustion: prompt NO, fuel NO and thermal NO. The last one - thermal NO, which is described by ‘Zeldovich-mechanism’, is the main source for NO_x emissions. The thermal NO emission mainly results from the high combustion temperature in the combustion process. In order to control the NO formation, the control of peak combustion temperature is the key factor, as well as the oxygen concentration in the combustion areas. Flameless oxidation (FLOX) and continuous staged air combustion (COSTAIR) are two relatively new technologies to control the combustion temperature and the reaction rate and consequently to control the NO_x emissions.In this study both FLOX and COSTAIR technologies are assessed based on a 12 MW_e, coal-fired, circulating fluidised bed combustion (CFBC) power plant by using ECLIPSE simulation software, together with a circulating fluidised bed gasification (CFBG) plus normal burner plant. Two different fuels - coal and biomass (straw) are used for the simulation. The technical results from the study show that the application of FLOX technology to the plant may reduce NO_x emissions by 90% and the application of COSTAIR technology can reduce NO_x emissions by 80-85% from the power plant. The emissions from the straw-fuelled plants are all lower than that of coal-fuelled ones although with less plant efficiencies.     

Modeling of oxy-fuel combustion for a western Canadian sub-bituminous coal

The motivation of this research is to develop practical oxy-coal combustion techniques in order to facilitate the conversion of coal-fired utility power plants so as to recover a CO₂ rich flue gas stream for use and/or sequestration. The objective of this study is to ascertain the applicability and accuracy of a modeling tool to assist with future pilot scale oxy-fuel combustion experiments and burner scale-up studies. Two modes of oxy-coal combustion, O₂ enriched air (OEA) and recycled flue gas (RFG), were experimentally tested in a 0.3 MW_th pilot-scale combustor using a western Canadian sub-bituminous coal. The computational fluid dynamic tool was utilized to model the combustion, heat transfer and pollutant formation characteristics of these test cases and to examine the impact due to changes in the combustion medium, burner swirl and burner configuration. The model provided insights for the observed variation in NO_x production among the test cases: the dramatic increase in the OEA mode, the drop at higher burner swirl settings and the surprisingly small reduction in the RFG mode. Overall the model results compared well with measured data in all test cases and established confidence in using the model to explore new design concepts for oxy-coal combustion.     

Properties of char particles obtained under O2/N2 and O2/CO2 combustion environments

Pulverized coal combustion in O₂/N₂ and O₂/CO₂ environments was investigated with a drop tube furnace. Results present that the reaction rate and burn-out degree of O₂/CO₂ chars (obtained in O₂/CO₂ environments) are lower than that of O₂/N₂ chars (obtained in O₂/N₂ environments) under the same experimental condition. It indicates that a higher O₂ concentration in O₂/CO₂ environment is needed to achieve the similar combustion characteristic to that in O₂/N₂ environment. The main differences between O₂/N₂ and O₂/CO₂ chars rely on the pore structure determined by N₂ adsorption and chemical structure measured by FT-IR. For O₂/CO₂ char, the surface is thick and the pores are compact which contribute to the fragmentation reduction of particles burning in O₂/CO₂ environment. The organic functional group elimination rate from the surface of O₂/CO₂ chars is slower or delayed. The present research results might have important implications for further understanding the intrinsic kinetics of pulverized coal combustion in O₂/CO₂ environment.     

NOx and SOx emissions of a high sulfur self-retention coal during air-staged combustion

NO_x and SO_x emissions of air-staged combustion were investigated in a 1 MW tangentially-fired furnace combusting a high sulfur self-retention coal. Two variables including the air stoichiometric ratio of primary combustion zone and the relative location of over-fire air (OFA) injection ports were studied. These results suggest that NO_x reduction efficiency monotonically increases with increasing the relative location of OFA injection ports, and the lowest NO_x emissions are achieved when the air stoichiometric ratio of primary combustion zone is 0.85. In the meantime, SO_x emissions can be effectively reduced when the air stoichiometric ratio of primary combustion zone is 0.85 or 0.95, and SO_x emissions monotonically decrease with increasing the relative location of OFA injection ports.     

Modeling of NOx conversion during combustion under high CO2 concentration using detailed chemical kinetics

Combustion of fuels under enhanced oxygen atmospheres has been well investigated over the past decades in various types of combustors, varying from diesel engines to coal-fired boilers. Most studies have found significantly lower NO_x emissions during Oxy-coal combustion. In this paper, NO_x combustion chemistry under O₂/CO₂ atmosphere as well as air atmosphere was studied using detailed kinetic model. A suitable reaction mechanism was chosen based on the comparison between the calculation result and the experimental data. The influence of various parameters (temperature, CO₂ concentration) on NO_x conversion was investigated. The chemical effects of high CO₂ concentration on NO formation and destruction process was studied. On the basis of investigations through elementary chemical reactions, it can be concluded that high CO₂ concentration play a pronounced role on NO_x conversion process. Moreover, the dominant reaction steps contribution to production and destruction of NO as well as the most important reactions for NO reduction under different atmospheres were discussed.     

Influence of the adjustable vane position on the flow and combustion characteristics of a down-fired pulverized-coal 300 MWe utility boiler

Experiments with a small-scale cyclone burner used for burner enrichment in a down-fired pulverized-coal 300 MW_e utility have been conducted on an air/particle test facility. Particle separating efficiency was obtained with different positions of an adjustable vane. Industrial experiments were performed on a full-scale boiler. The gas temperature distribution along the primary air and coal mixture flow, gas temperature distribution of the furnace, and gas components such as O₂, CO, CO₂ and NO_X in the near-wall region were measured for the first time. The influence of the adjustable vane position on coal combustion in the furnace was determined. With the adjustable vanes at the nozzle, ignition of the primary air and pulverized-coal mixture was delayed and the gas temperature peak was above the burner arch, with high NO_X emission. Raising the vanes can bring forward the ignition point but results in the fuel-rich flow being up ahead of time, leading to a rise in carbon content in fly ash and NO_X emission.     

Experimental study of ash formation during pulverized coal combustion in O2/CO2 mixtures

The present paper was addressed to mineral transformations and ash formation during O₂/CO₂ combustion of pulverized coal. Four Chinese thermal coals were burned in a drop tube furnace to generate ashes under various combustion conditions. The ash samples were characterized with XRD analysis and ⁵⁷Fe Mössbauer spectroscopy. The impacts of O₂/CO₂ combustion on mineral transformation and ash formation were explored through comparisons between O₂/CO₂ combustion and O₂/N₂ combustion. It was found that, O₂/CO₂ combustion did not significantly change the mineral phases formed in the residue ashes, but did affect the relative amounts of the mineral phases. The differences observed in the ashes formed in two atmospheres were attributed to the impact of the gas atmosphere on the combustion temperatures of coal char particles, which consequently influenced the ash formation behaviors of included minerals.     

Study on coal chars combustion under O2/CO2 atmosphere with fractal random pore model

When predicting the variation of pore structure during O₂/CO₂ combustion of coal chars using the random pore model (RPM), it is impossible to calculate exactly the structure parameter ψ from the pore characteristics. The values of structure parameter ψ, which were calculated based on its fractal feature at various carbon conversions, should be almost constant. However, this investigation exhibited a drastic increase of ψ at the end of combustion reaction. In this work, structure parameter ψ of the RPM was modified according to the experimental analysis and a new model, fractal random pore model (FRPM), was constructed. Compared with other models such as RPM, discrete random pore model (DRPM), the Struis model (Model I) and the Liu model (Model II), it was found that fractal random pore model was more accurate to describe coal chars combustion, especially at higher conversions. Using the FRPM, O₂/CO₂ isotherm combustion of coal chars were analyzed at different temperatures.     

Experimental measurements of the NOx and CO concentrations operating in oscillatory and non-oscillatory burning conditions

The effects of combustion driven acoustic oscillations in carbon monoxide and nitrogen oxides emission rates of a combustor operated with liquefied petroleum gas (LPG) were investigated. Because the fuel does not contain nitrogen, tests were also conducted with ammonia injected in the fuel, in order to study the formation of fuel NO_x. The main conclusions were: (a) the pulsating combustion process is more efficient than the non-pulsating one and (b) the pulsating combustion process generates higher rates of NO_x, with and without ammonia injection, as shown by CO and NO concentrations as function of the O₂ concentration. An increase in the LPG flow rate, keeping constant the air to fuel ratio, increased the acoustic pressure amplitude and the frequency of oscillation. The injection of ammonia had no influence on either pressure amplitude or frequency.     

O2/CO2气氛下煤燃烧SO2/NO析出特性

在水平管式炉上研究了O₂浓度、CO₂浓度、温度及石灰石添加等各参数对O₂/CO₂气氛下徐州烟煤和龙岩无烟煤燃烧过程中SO₂/NO排放特性的影响。结果发现,O₂/CO₂气氛下,烟煤和无烟煤燃烧SO₂/NO的析出规律与空气气氛下不同,同等O₂浓度下析出量比空气气氛下小。O₂/CO₂气氛下,随着O₂浓度的提高,烟煤和无烟煤SO₂/NO排放量均增大;随着CO₂浓度的升高, SO₂/NO排放量均减小。O₂/CO₂气氛下,石灰石添加对SO₂排放的抑制作用低于空气气氛下;石灰石添加对NO的排放有一定减排作用。对煤灰的元素分析显示O₂/CO₂燃烧对SO₂的抑制主要是由于煤灰的自固硫能力增强,而对NO的减排作用则是促进燃料N向其他含N气体的转换。