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Recent Patents on Mechanical Engineering 2009, 2, 228-239

Towards Improvements in Thermal Efficiency and Reduced Harmful Emissions of Combustion Processes by Using Recirculation of Heat and Mass: A Review
Wojciech M. Budzianowski 1,* and Ryszard Miller2
Division of Chemical and Biochemical Processes, Department of Chemistry, Wroclaw University of Technology, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw, Poland; 2Institute of Power Engineering and Fluid Mechanics, Department of Mechanical and Power Engineering, Wroclaw University of Technology, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw, Poland
Received: May 25, 2009; Accepted: July 10, 2009; Revised: July 21, 2009
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Abstract: Combustion processes are main constituents of several energy technologies. A key issue in combustion researches is the improvement in reduction of harmful emissions. Besides, the achievement of high-energy-efficiency processes through advanced heat recovery systems is desirable. When recirculated systems are utilized those two aspects can be achieved simultaneously. Therefore, the current review describes recent patented developments in heat and massrecirculating systems over the last 10 years (2000-2009). In relation to heat-recirculating systems recuperative, regenerative and porous media combustion are covered. The most significant inventions are discussed and their improvements and possible applications are emphasized. Further, flue gas recirculating systems' novel configurations and solutions are described. Their practical power engineering applications in the field of e.g. boilers, internal combustion engines, gas turbines and radiant tube burners are emphasized. For each group of patents the principles of improvements in thermal efficiency and in reducing harmful emissions are expounded.

Keywords: Heat and mass recirculation, combustion, energy efficiency & harmful emissions. 1. INTRODUCTION The paper reviews recent advances in the development of thermally efficient and having low harmful emissions power generation systems. The focus is on heat-recirculating and mass-recirculating combustion systems. Such recirculation has a substantial impact on both the improved thermal efficiency of combustion systems and on the reduction of emissions of harmful substances. Heat and mass recirculation loops are common in the most of novel natural gas-based energy technologies currently being under constant development [1]. Therefore, the current review emphasizes the significance of novel inventions, methods, techniques and designs disclosed in the patents associated with heat and/or mass recirculation in combustion systems. We study heat-recirculating combustion systems utilizing the recuperative and regenerative modes of heat exchange. We show that the thermal efficiency of such heat recirculating systems can be much increased and lead to superadiabatic conditions. Further, the heat and massrecirculating systems, i.e. flue gas recirculation systems (FGR) also known as exhaust gas recirculation systems (EGR) are approached. Abd-Alla has reviewed such systems in view of internal combustion (IC) engines [2]. Paul and Datta [3] comprehensively describe three main mechanisms of NOX formation in combustion, i.e. thermal (Zeldovich)
*Address Correspondence to this author at the Division of Chemical and Biochemical Processes, Department of Chemistry, Wroclaw University of Technology, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw, Poland; Tel: +48 71 3203814; Fax: +48 71 3203814; E-mail: wojciech.budzianowski@pwr.wroc.pl

nitrogen oxidation, prompt NOX, and fuel NOX and show that the rate of NO X formation in combustion of typical fuels is usually dominated by the thermal mechanism. Conequently, the FGR systems offer the substantial reduction of thermal NOX emissions in combustion. It is attributed to e.g. the reduction in N2 and O2 contents which are replaced by CO2 and H2O, shorter residence times of reactants due to preheating and dilution, and also to reduced local peak temperatures due to improved intermixing [3, 4]. The flue gas recirculation is also utilized in fuel oxyforming processes. For instance, Tsolakis et al. [5] have investigated the effect of exhaust-assisted fuel reforming on reaction profiles in diesel engines. Scribano et al. [4] have utilized the FGR for industrial radiant tube burners. Cavaliere and de Joannon [6] have given some light on the classification of recirculating combustion systems. The authors classify combustion processes in terms of inlet reactor temperature Tin and temperature increase during combustion T. According to the proposed nomenclature processes that have both Tin and T higher than a self ignition temperature of the mixture Tsi are called HiCOT High Temperature Combustion Technology (some authors term it HiTAC - High Temperature Air Combustion). Further, processes with Tin < Tsi and T > Tsi are called feedback combustion and processes with Tin > Tsi and T < Tsi are named mild combustion. In heat and massrecirculating systems both those temperatures are affected by a system configuration and applied heat and/or mass recirculation techniques, which can lead to e.g. a superadiabatic effect, O2 deficiency and/or CO2 enrichment etc.. Hence, recirculating systems can operate under different combustion regimes including highly diluted flameless fuel
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oxidation, which are characterized by different oxidation mechanisms. Therefore, we investigate the patented developments on heat and mass recirculating systems in relation to a standard combustion power engineering equipment including gas turbines, internal combustion (IC) engines, boilers, furnaces, radiant tube burners etc. We look at specific ways in which heat and/or mass recirculation is applied to those different combustion power generation systems. We analyze how relevant modifications can improve its thermal efficiency and reduce harmful emissions. The principles of such improvements are discussed. All searches are also directed at seeking for novelty aspects in combustion related power generation technologies that use heat and/or mass recirculation. 2. METHODOLOGY The patent database ESPACENET (http://ep.espacenet. com) provided by the European Patent Office is used for patent publication searches. The relevant patent publication numbers are retrieved by using the European Classification system (ECLA) mostly using the category F23C9, i.e. combustion apparatus with arrangements for recycling or recirculating combustion products or flue gases. Additional patents are retrieved by using specific keywords searches, e.g. combustion, recirculation, heat recovery, thermal efficiency, flue (or exhaust) gas recirculation etc. 3. HEAT AND MASS RECIRCULATING SYSTEMS AND ITS EFFECT ON COMBUSTION Recirculation of heat and mass is defined, for the purpose of the present review, as the recirculation of released combustion heat and combustion products back to incoming reactants. The combustion heat can be recirculated by the use of a recuperator or a regenerator. Combustion products are usually recycled back to the substrates by using an external piping. However, in porous media combustion the combustion heat can be recycled back by itself without the need for any other equipment. Accordingly, technologies such as chemical looping combustion in which metals are recirculated to transfer oxygen from an air reactor to a fuel reactor do not fall into such defined heat and massrecirculating systems. Also numerous patents related to phenomena like the formation of local internal circulation zones of reactants in combustion chambers [e.g. 7], although their physical nature is in fact similar to the recirculation of combustion products (both heat and mass) back to incoming reactants, are not reviewed here. 3.1. Recirculation of Combustion Heat Heat-recirculating systems are very practical since they can improve the thermal efficiency of combustion processes. The combustion literature reports several kinds of heatrecirculating burners, e.g. a spiral Swiss roll or countercurrent combustors. The spiral Swiss roll heat-recirculating devices have found application in micro-combustors [8-10]. At small scales heat and friction losses become more significant thus the utilization of devices based on existing macro-scale systems such as internal combustion engines

which have moving parts and produce hot exhaust gases may be impractical. Therefore, other approaches to electricity generation including those based on ther-moelectric, piezoelectric, pyroelectric and thermophotovol-taic phenomena can be used in conjunction with heat-recirculating microcombustors. Kim et al. [11] have reported the utilization of a small heat-recirculating spiral Swiss-roll burner as a heater. The recirculation of heat is also an important aspect in combustion of lean gaseous fuels. Such processes include energy recovery from landfill gases, combustion of biomass derived syngas, reburn of exhaust gases from existing combustion systems or industrial processes, and mitigation of fugitive methane emissions such as coal mine ventilation gases. The advantages of burning low-calorific value fuels can include an increase in energy efficiency of existing energy generation systems, a decrease in the consumption of conventional fossil fuels, and a reduction in greenhouse gas emissions. Porous burners for lean-burn applications have been recently reviewed by Wood and Harris [12]. The heat-recirculating systems usually operate in a recuperative mode or in a regenerative mode of heat exchange. The regenerators can include porous media which can also participate in heat recirculation. The patented developments in those modes of combustors' operation are discussed below. 3.1.1. Recuperative Heat Exchange In heat-recirculating systems with recuperative heat exchange thermal energy is transferred from hot combustion products to cold substrates without mass transfer and thus without any dilution of reactants. As a consequence, the total reactant enthalpy (sum of thermal and chemical enthalpy) is higher than that of incoming cold reactants enabling sustained combustion under conditions (lean mixtures, small heating value fuels, large heat losses) that would extinguish without recirculation. Such processes are often self-sustained or auto-thermal and are sometimes referred to as superadiabatic or excess enthalpy combustion [13]. Budzianowski and Miller [14, 15] have reported some qualitative description on superadiabatic recuperative combustors. Those authors investigate a recuperative annular catalytic converter Fig. (1), for auto-thermal combustion of lean gaseous fuels. It is shown that recirculation of heat by using a recuperator coupled to a combustor leads to bifurcation behavior. The papers report some bifurcation diagrams with inlet tempeature, inlet concentration, mass flow rate, gas velocity and pressure as the bifurcation parameters. The recirculation of heat in a recuperative mode is often utilized in gas turbine technologies. Namely, Belokon and Touchton [16] provide a single shaft recuperated gas turbine engine and a method employing catalytic combustion, Fig. (2). According to the disclosure, the combustor (20) inlet temperature can be controlled to remain above the minimum required catalyst operating temperature at a wide range of operating conditions from full-load to part-load and from hot-day to cold-day conditions. The fuel (56) is passed through the compressor (14) along with the air and the portion of exhaust gases from the turbine (16). The mixture

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Kim and Hwang [17] have found that at part load turbine operation, a higher turbine exit temperature and consequently a recuperator inlet temperature, which increases turbine efficiency, can be higher in a two-shaft turbine configuration. Budzianowski and Miller have recently reviewed catalytic devices and techniques used in the conjunction with such gas turbine combustors [18]. The heat recirculation via recuperation is also used in more sophisticated systems that include thermophotovoltaic (TPV) generators and solid-oxide fuel cells (SOFC). In the TPV generators, the combustion energy heats surfaces which then emit infrared radiation. An array of photovoltaic (PV) cells surrounds this emitter, receives its infrared radiant energy, and converts it to electricity. Fraas and Avery [19] propose such a TPV generator equipped with a recuperator to recycle heat from the combustion exhaust stream back into the combustion air. Preheating the combustion air in the recuperator allows for flameless fuel oxidation. A folded back coaxial emitter support tube provides a long path length limiting thermal conduction along its cylindrical wall from the very hot emitter section to the cooled seal flange. The limited axial conduction enables to achieve higher heat recirculation ratios. According to the patent, these cylindrical TPV generators can potentially be used to generate heat and power in domestic applications with 90% fuel utilization efficiency. Further, especially small SOFC systems (< 1 kW) require close thermal integration to attain high operating temperatures above 700C in a fuel reformer. Also, a recuperator can be applied for preheating the fresh air prior to entering the cathode chamber [20]. A recuperative fuel cell hybrid power plant is disclosed by Balan and Deangelis [21]. A fuel cell can not play a role of a simple combustor but it has to be integrated with a gas turbine arrangement in a specific way. In accordance with the invention, a reformer is configured to reform air and fuel which is passed to a fuel cell anode. Compressed air is supplied to a recuperator heated by turbine exhaust, and heated compressed air is mixed with the recirculated exhaust from the fuel cell prior to entering a fuel cell cathode. A tail gas burner, which is required for all SOFCs, combusts a mixture of cathode exhaust and reformed residual fuel, and the resulting combustion gases are directed to the turbine. The thermodynamic expansion of the gases produces work and exerts motive forces to drive the turbine, which, in turn, drives the compressor and generates electricity in a generator. Electricity from the generator and fuel cell stack are converted to an appropriate form and used in a distribution power supply network. Finally, heat from turbine exhaust is transferred to a fresh fuel in a de-sulferizer before being exhausted from plant. Thus, the invention offers an efficient heat-recirculating system having low temperature of exhausted gases. 3.1.2. Regenerative Heat Exchange Another concept in heat-recirculating systems, in the recent patented literature, is a regenerative heat exchange. The regenerative systems are usually directed at VOCs combustion or to thermally efficient low NOX burner designs associated with High Temperature Combustion Technology (HiCOT) [22-24]. The thermal and chemical behavior of

Fig. (1). The scheme of the recuperative catalytic converter.

Fig. (2). The scheme of the recuperated gas turbine engine and the method employing catalytic combustion (adapted from [16]).

is heated in a gas-to-gas heat exchanger (22). Additionally, the exhaust gas is recirculated (42) and its flow rate is controlled (50) to control the inlet temperature to the catalytic combustor (20). Thus, the invention combines catalytic combustion, thermal control, recuperation and flue gas recycle. It offers, especially at part load conditions, a substantial increase of turbine electrical efficiency and combustor inlet temperature.

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high temperature air combustion flames is significantly different than that of normal air flames. The main differences include increased thermal uniformity in the combustion zone. Further, HiCOT technology offers the significant reduction of NOX emissions. It is achieved by decreased oxygen content which reduces the rate of nitrogen oxidation. Further, as the inflowing gas is preheated the combustion can be completed at decreased residence times which reduce the amount NOX formed. Furthermore, the higher gas throughputs allow for the improved intermixing of fuel and air which enables to avoid peak temperature regions in which nitrogen oxides are formed by the thermal mechanism. Regenerators can have different geometries. Some of them can use porous media combustion. The porous media in the combustion zone not only regenerates the combustion heat, but also put the combustion heat to the upstream preheating the fuel gases by conduction and radiation. The utilization of regenerative VOCs oxidizers seems to be thermally fairly attractive. There are two groups of such systems, i.e. thermal and catalytic VOCs oxidizers. Baker and Ginger [25] provide a natural gas injection system for a regenerative thermal oxidizer (RTO), Fig. (3). According to the invention, a lean fuel is combusted and regeneratively heats two inert beds (20). Natural gas injection enables to control the temperature level in the RTO. The cleansed gas after leaving the regenerative heat exchanger is in part recycled and mixed with the incoming gas to the RTO. The natural gas injection ensures thermal stability of the RTO. The proposed method may include generating a flameless oxidation of the contaminated air and the natural gas, thereby releasing heat within the heat exchanger (20) without generating thermal NO X emissions. Other configurations of RTO systems are disclosed in [26-29]. A similar idea is associated with the invention of Sankaranarayanan et al. [30] who propose a controlled combustion for regenerative reactors with mixer/flow distributor.

Regenerative heat recovery is utilized in several standard power engineering devices, e.g. gas turbines and IC engines. Bolotin [31] discloses a power plant concept having the regenerative heat recovery. According to the disclosure, a regenerative heat exchanger is installed downstream of an exhaust device. The inlet of the regenerative heat exchanger is connected via water pump to water reservoir. The plant comprises turbine cooling system that consists of the following serially connected components - fuel-steam and fuel-air heat exchangers. The outlet from the regenerative heat exchanger is connected to a water reservoir via the fuelsteam heat exchanger and the steam turbine located on a free turbine shaft. Further, Wait [32] proposes a power plant concept with IC engines and regenerative heat recovery, Fig. (4). The thermal transfer IC engine (12) with an air transfer cylinder (54) is located between a pair of power cylinders (14, 16). The transfer cylinder has an intake valve (60) and two transfer valves (66, 68) alternately feeding the two power cylinders (14, 16). The power cylinders each contain a mono valve (30, 32) used for both intake and exhaust. Counter-flow manifolds (18, 20) connect the mono valves (30, 32) of the power cylinders to the transfer valves of the transfer cylinder. A regenerator (22, 24) with catalytic converter properties is located in the each counter-flow manifold (18, 20). The regenerator (22, 24) is heated by exhaust gases exiting the power cylinders, prior to exiting the engine through exhaust dump valves (26, 28). Uncompressed intake air is pushed from the transfer cylinder through the regenerator where it is heated and delivered to the power cylinder for conventional processing. The heat recovery system provides high compression temperatures at low compression ratios, reducing engine fuel consumption. Further, the regenerative heat recovery technique is applied to the construction of furnaces or industrial burners. Accordingly, Jiuju et al. [33] provide a regenerativerecuperative combined heating furnace. Suzukawa and Mori [34] disclose a regenerative burner and its combustion method that splits a fuel into a primary and a secondary fuels thus a fuel-air ratio and combustor temperature can be controlled in order to reduce NO X emissions. Kraft et al. [35] propose a tri-sector regenerative oxidant preheater for oxyfired pulverized coal combustion. Deng [36] discloses a porous media combustion superadiabatic burner with reciprocating flow having a hot water circulation system for the removal of excess heat which can be further utilized for e.g. human existence purposes in remote locations. 3.2. Recirculation of Flue Gases Recirculation of flue gases offers simultaneous recycling of heat and mass. Such systems can further intensify combustion processes in terms of its thermal efficiency and reduction of unwanted emissions. Recycled flue gases are either mixed with fresh substrates or injected directly into a combustor. The flue gas recirculation (FGR) systems substantially reduce NOX emissions since the combustion air is diluted with the recirculated burned gas. The dilution decreases an oxygen content in the combustion mixture which decreases temperature fluctuations in the flame as well as the mean temperature. Further, the dilution and preheating enable to reduce residence times, and hence, low thermal NOX emissions can be attained. Further, such

Fig. (3). The scheme of the natural gas injection system for a regenerative thermal oxidizer (RTO) (adapted from [25]).

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Fig. (4). The scheme of the power plant concept with IC engines and regenerative heat recovery (adapted from [32]).

recycling beneficially cumulates combustion products in combustion process streams. However, when using high flue gas recirculation ratios inert constituents of air, i.e. N2 and Ar also cumulate in the combustor. To avoid this problem O2 - enriched combustion can be utilized. In this case, which is discussed later in the text, the inflow of nitrogen is low and consequently higher mass recirculation ratios can be attained. In IC engines community the FGR technology is commonly called EGR but in order to keep a uniform nomenclature throughout the text we use the same acronym (FGR) for all analyzed systems including IC engines. 3.2.1. Combustion of Fuel-Air Mixtures Utilization of O2 - enriched combustion requires a high purity O2 source e.g. an air separation unit (ASU) which is usually relatively costly. Therefore, fuel-air combustion is often preferred and also the most of existing power generation plants utilize fuel-air combustors. When using a FGR approach it is usually necessary to cool the exhaust gas before it is put back into the power cycle in order to maintain a sufficiently low temperature since for a given gas turbine a power output is inversely proportional to a compressor inlet temperature [37]. Such necessity of cooling usually decreases overall thermal efficiency of power plants. In fuelair combustion the recirculation of flue gases is possible without any major modification of a combined cycle plant equipment. Gas turbine combustors can consume fossil fuels and air for power generation. The use of FGR heats the reacting mixture above the auto-ignition temperature and provides its dilution by increasing the content of inerts. A stable flame attained at fairly high flue gas recirculation ratios becomes non-visible and non-audible. It is attributed to even concentration and temperature profiles. This alternate combustion mode arises as a result of a very high level of dilution of the reacting mixture. Further, in conventional gas turbine systems a lean premix flame must be aerodynamically stabilized via e.g. a swirl device to prohibit extinction instabilities. In contrast, the flames in a gas turbine combustor with a highly preheated mixture comprising recycled reaction products do not require such aerodynamic stabilization.

Carrea and Jansohn [38] propose a method for combustion of fuels in a gas turbine combustor utilizing FGR. According to the invention, a recirculated flue gas dilutes and heats a combustible fluid. The heating causes a spontaneous ignition temperature to be exceeded, and a lowpollutant volumetric flame is formed in a highly dilute atmosphere. The invisible volumetric flame is distributed approximately uniformly through a combustion volume. The recirculation of sufficient quantities of the flue gas is attained on account of a jet pump effect. Gas turbines are typically operated with a very lean flame (the relative air to fuel ratio  > 2) at around 20 bar with the oxidant preheated to 720 K by compression and with a flame temperature of around 1750 K. Further, high FGR-induced dilution slows down the kinetics of the combustion process, which thus affects both ignition delay times and the overall combustion reaction times. Therefore, the application of the FGR approach to gas turbines requires taking into account the associated operating conditions and constraints. Carrea et al. [39] disclose such a gas turbine system adapted to operate with FGR, Fig. (5). The system comprises a compressor (2) adapted to compress oxidant (5), a combustion chamber (3) adapted to accept the compressed oxidant (7) and provide an exit means for flue gas (9), a turbine (4), and flue gas recirculation means (12,13) adapted to recirculate the flue gas (9) from the combustion chamber (3) and mix the said flue gas with the compressed oxidant (7) from the compressor (2) in order to provide a highly diluted mode of combustion with a flue gas recirculation ratio from 1 to 2, preferably from 1 to 1.5. A portion of flue gas (13) is recirculated via a combination of paths upstream (18) and downstream (19) of a catalytic preburner (17) in order to attain an appropriate temperature level and dilution at the entrance to the combustion chamber (3). A part of the compressed oxidant (8) (typically below 25%) can bypass the combustor (3) and can be used as a cooling agent upstream the turbine (4). In order to achieve necessary autoignition of the diluted fuel/oxidant mixture and the characteristic combustion conditions the oxidant must be preheated. The proposed FGR gas turbine can operate without the need for an additional separate preheater of the

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Fig. (5). The scheme of the gas turbine having exhaust gas recirculation (adapted from [39]).

oxidant since it can be sufficiently preheated by compression work in the compressor. Besides, the highly diluted combustion does not require flame aerodynamic stabilization devices. However, the requirements of combustion the invention offers relatively low FGR ratios (from 1 to 1.5). Also, Brautsch et al. [40] cover a gas turbine system having FGR. The invention relates to a method for safe, low NOx emission operation of a gas turbine system having fuel gas that is rich in hydrogen, and a gas turbine system having a device for flue gas recirculation into the compressor inlet and for fuel gas dilution. For this purpose, the oxygen content in the combustion air is reduced by means of recirculation of recooled exhaust gas, and the fuel gas is diluted using compressed exhaust gas. The oxygen reduction in the combustion air results in minimum residual oxygen in the exhaust gas, thus making it usable for fuel gas dilution. Furthermore, the water content in the combustion air is also increased via the return of the water created as a combustion product by means of the exhaust gas recirculation. The oxygen reduction in fuel gas, the increased water content in fuel gases, and the fuel gas dilution leads to a reduction of the flame velocity of fuel gases rich in hydrogen, thus enabling a robust, safe, and low-emission combustion with regard to flashback. A combined cycle power plant with FGR that utilizes a blend of fuels containing hydrogen, to provide improved thermal efficiency and improved flame stability at high flue gas recirculation rates is covered in [41]. Hydrogen gas is known for its high reactivity thus it stabilizes combustion at high flue gas recirculation ratios. The addition of hydrogen (or hydrogen/CO) to natural gas with FGR has the benefits of increasing flame speed, extending the limit of flammability, lowering ignition energy, enhancing flame stability, and reducing unwanted emissions. Another FGR gas turbine system is disclosed by Evulet et al. [42]. The disclosure proposes a retrofittable flue gas recirculation system. Relatively hot flue gases from an expander are directed to a heat recovery steam generator (HRSG). The HRSG allows for cooling the recycled flue gases which are further supplied to the compressor and consequently the overall gas turbine efficiency can be higher. In one of the proposed embodiments a portion of recirculated flue gases after passing the HRSG unit is directed to a CO2 capture unit. The operation of most of CO2 capture units in

such a FGR systems are enhanced due to the increased concentration of CO2, here up to 10 % by volume. Further, Varatharajan et al. [43] disclose a system for reducing NO X emissions from a gas turbine engine by reforming hydrocarbon fuels and doping natural gas-based combustion with H2-enriched gas. It is claimed that in H2doped natural gas combustion a greater operability window for generating power and simultaneously maintaining low NOX emissions is created which is attributed to the higher reactivity of H2-enriched blends of fuels. The system includes a reformer configured to receive a fuel and produce a hydrogen-enriched stream, a combustion system configured to burn the hydrogen enriched-stream and produce electricity and an exhaust stream, and a recuperator configured to recover heat from the exhaust stream, wherein the recovered heat is recycled back to the reformer. The reformer converts e.g. methane to syngas, i.e. mainly to H2 and CO which is much more reactive than original methane. Consequently, the temperatures in the combustor can be reduced (methane typically requires above 1300C). Optionally, an auxiliary CO2-enriched stream can be supplied to the combustor. The optional injection of CO2 can dilute the system further reducing NO X emissions and also it can affect the reforming process by the inclusion of dry methane reforming reactions. Steam generating cogeneration boilers used to recover heat from combustion engines that produce electrical energy e.g. gas turbines can also use FGR. Labasque and Segret [44] disclose such a heat recovery boiler which in its own combustion system utilizes FGR. According with the invention the boiler is operated by feeding its combustion system with air and with a stream of flue gases recycled to a level typically between 50 and 65%, so as to allow the efficiency of the boiler to be increased and to decouple it, at least temporarily, from the combustion engine driving a generator, the exhaust gases from which are burnt in a postcombustion mode in the boiler in a cogeneration mode. It is found that with a more then 80% degree of recirculation the efficiency of the boiler exceeds 92%. Another type of a boiler design having a FGR is released by Kayahara et al. [45]. Accordingly, the system uses gaseous or liquid fuels that are burned with the recirculated flue gas. Downstream, in the combustion chamber, a plurality of water tubes is arranged and farther at the outlet of this zone a part of flue

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gases is recirculated by means of external piping. This watertube boiler achieves reduction in NOX and CO at the same time by reducing the oxygen content and having even temperature distribution. A similar construction and governing principles for emissions reductions to water-tube boilers are met in the petrochemical industry in hydrocarbon evaporation and cracking in tubular natural gas fired equipments [46]. Further, Gilli [47] provides another improvement for heat recovery boilers. Accordingly, the contaminated flue gases leaving the combustor of a steam generator are fed to a separate heat exchanger for recovery of heat which is transferred to already cleaned flue gases which are then fed back to the combustor. The disclosure allows for increased FGR ratios, high thermal efficiency of the boiler and separation of particulate matter and other contaminants from recirculated gases. The heat exchanger can also be used to preheat an oxygen stream. Numerous patents have recently been disclosed for IC engines having a FGR with most of them relating to the automotive industry. Solutions are aimed at the reduced consumption of a fuel and harmful emissions from engines. Chauvel et al. [48] propose a system in which the recirculated gas is supplied to the engine by means of two manifolds, Fig. (6). The engine (10) has a FGR system (38) with a heat exchanger (42), e.g. condenser, for recovering a part of exhaust gas from the engine and for injecting the recovered gas in a combustion chamber of a set of cylinders (12-18). Gas intake manifolds (28, 30) supply the recirculated exhaust gas and fresh air mixture to the cylinders, such that each of the two adjacent cylinders is supplied by one of the manifolds. An intake conduit has two branches to emerge in the manifolds and to be located in an equal distance from the cylinders. Two manifolds enable to recirculate flue gases in a partly independent way of engine operation. Grunditz et al. [49] provide another IC engine having FGR. A FGR arrangement is adapted to lead a first flow of exhaust gas, the FGR flow, from an outlet side of the engine to an inlet side of the engine, an exhaust gas conduit adapted to lead away a second flow of exhaust gas, the exhaust flow, from the outlet side of the engine, and an energy recovering unit, such as a turbo, associated with the exhaust gas conduit.

The unit is adapted to recover exhaust gas energy from the exhaust flow. The system includes a heat exchanger adapted to allow heat exchange between at least a part of the FGR flow and at least a part of the exhaust flow, the heat exchanger being associated with the exhaust gas conduit at a position downstream the energy recovering unit. An advantage of the invention is related to increasing, if it is necessary for exhaust aftertreatment processes, the temperature of the exhaust gases by heat exchange between the exhaust and recycled gases. The next large group of patents is related to radiant tube burners. Kim and Park [50] provide a radiant tube burner having a FGR system, Fig. (7). It is aimed at reducing NOx emissions by using recirculation (6) of a large amount of flue gas when the heat load of a burner is high and by recirculating a small amount of flue gas when the load is low to prevent the decrease of thermal efficiency of a burner. With FGR highly O2- and N2-diluted atmosphere and simultaneously preheated combustion mixture allows for the reduction of thermal NOX, i.e. the rate of formation is thermally reduced so as the concentration of substrates (i.e. O2 and N2) while the thermal efficiency of the burner remains unchanged due to recycled heat. The main idea associated with FGR operation is similar in some other disclosures, i.e. in [51-54]. Furthermore, furnaces and industrial burners also utilize FGR. In a disclosure by Atreya [55] it has been estimated that various combustion processes employed in e.g. steel, glass or aluminum industries use only 40% of the chemical energy of fuel while 60% is lost. Therefore, a method of waste heat recovery from high temperature furnace (12) flue gases is provided, Fig. (8). The invention propose a new approach for FGR, i.e. a high velocity stream (16) is injected into an entrainment zone to form a high velocity jet which entrains a part of the heated effluent stream (14). The momentum of the system is conserved and a mixed stream is pressurized and recirculated to a burning zone of a combustion source. The injected gas may comprise substantially pure oxygen. At the top of the system the recuperator is provided to recirculate heat from that part of flue that are not recycled. The invention decreases oxygen and fuel require-

Fig. (6). The scheme of the internal combustion engine having FGR (adapted from [48]).

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Fig. (7). The scheme of the radiant tube burner having a FGR system (adapted from [50]).

Fig. (8). The scheme of the waste heat recovery from high temperature furnace exhaust gases (adapted from [55]).

ments, is relatively easy to implement and require low capital expenditures. Further, Wood and Agrawal [56] propose another, selfoperated FGR system associated with a burner, Fig. (9). Accordingly, a flue gas intake is localized in a flue gas duct which aerodynamically captures a portion of a flue gas stream without detrimental impedance of the gas flow. A similar idea of self-sustained FGR but realized by using two completely different methods is disclosed in [57, 58]. According to those two disclosures, suitable passages are foreseen to connect the combustor outlet to the inlet channel of air. The passages are designed to communicate and then mix flue gas and air flows (having opposite directions) thus recirculation a part of flue gases back to the combustion chamber.

Atreya [59] proposes a furnace design that utilizes flame radiation. According to this invention, flame radiation heats metal surfaces and then hot flue gases flows in the opposite direction to the flow direction of fuel-air mixture exchanging heat. The furnace design combines the benefits of oxygen enriched combustion, intensive flame radiation, highly preheated combustion air, flue gas recirculation (FGR), buoyancy driven flows and NOx reburn chemistry in a single unit to significantly reduce energy consumption and pollutant formation. A novel aspect of intensive radiation enables to achieve even temperature profiles in a combustion chamber, and hence it avoids peak temperatures and reduces NOX formation.

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chlorides are burnt. However, in the presence of excess sulfur dioxide the chlorides are converted to sulfates. The preferred embodiment comprises electrostatic collector, chlorides washer and sulfate removal washer. Dust-free, hydrogen chloride reduced gas is tapped off prior to the sulfate washer, warmed in heat exchanger and mixed with secondary air. The amount of gas added is then arranged to be such that the sulfur dioxide to hydrogen chloride ratio in the combustion zone is greater than 1. Benson et al. [67] proposes an apparatus for heating a furnace in which recirculated gases are well dispersed which results in lower peak flame temperatures and therefore minimizes the formation of the pollutants, such as nitrogen oxides. Some other burner configurations having FGR are disclosed in [68-70]. Barry [71] discloses a method and apparatus for controlling combustion in a furnace in which the flue gas generated by the burning in the combustion zone is fed back to the combustion zone through a recirculation path to cool the combustion zone so that the temperature is below the melting or softening point of the residual ash in the solid materials. Water is heated and vaporized by the flue gas so as to cool the flue gas. Generated water vapor is also introduced to the combustion zone to increase the burning rate. The disclosures [72] provide a FGR systems of a burner having a filtering system to remove the larger particulate materials and pollutants, and then return the gas back to the combustion chamber. 3.3. Oxy-Fuel Combustion Conventional combustion of fuels uses air as an oxidant in which the N2 is an inert gas. In systems that include FGR nitrogen also cumulates in the system. Consequently, only modest FGR ratios can be utilized. Besides, the nitrogen from ambient air has to be heated up to the appropriately high combustion temperature. Further, there exist species that can not be oxidized in fuel-air fired systems at temperatures conventionally available to combustors. In such a case O2 - enriched combustion can help to reduce the require-ed combustion temperature for complete species conversion. Furthermore, oxy-fuel combustion offers to achieve much higher flue gas recirculation ratios than in air-combustion as much less inerts are present in the system. In oxy-fuel combustion FGR is usually inevitable for the dilution of combustion mixtures with inert gases in order to avoid too high flame temperatures. Therefore, the combustion process is realized in a CO2-rich atmosphere. The patented literature discloses boilers as a main area of implementation of oxy-fuel combustion. Gilli et al. [73] propose a burning fossil fuels (6) in a steam generating boiler (1) using an oxy-fuel process, by using flue gas (8) to preheat oxygen (7) used in combustion, Fig. (10). In accordance with the invention the oxygen stream (7) is preheated by being used to cool the waste gas (8) in a gastight heat exchanger, e.g. a plate- or pipe-based heat exchanger (9). Further, the invention offers to recirculate flue gases (11). The idea can be used also for coal-fired boilers. By using recirculation of flue gases which contain no nitrogen and have high content of CO2 the concentration of

Fig. (9). The scheme of the simple method for a self-operated FGR system associated with a burner (adapted from [56]).

Further, Crowther and Holmes [60] disclose an improved industrial burner having a FGR where internally recirculated waste gases are extracted directly from the chamber atmosphere and mixed with incoming oxidant. It enables to design a more compact device and thus it reduces heat losses to the surroundings. For the extraction of flue gases directly from a combustion chamber Schindler et al. [61] propose a venturi tube. The system is arranged to recirculate a stream of flue gas from a location within a combustion chamber adjacent to the combustion zone by induction into the venturi tube at a low pressure location adjacent to the throat of the venturi tube so that the recirculated stream of internal flue gas is inducted into and intermixed with the flow of air at the throat of the venturi tube. Kubota [62] propose to arrange a fan in order to forcibly recirculate flue gases. Kayahara and Takubo [63] provide another combustion method and apparatus having FGR. Accordingly, the combustion method for NOx reduction controls the temperature of combustion gas derived from a burner by using heat absorbers, FGR and water injection. Hu et al. [64] propose a hydrogen blended combustion system with FGR. The system offers improved thermal efficiency and improved flame stability at high flue gas recirculation ratios being of special interest. Kalina [65] provides another combustion system with FGR that oxidizes a fuel in a combustion chamber with an oxidizing stream including an air stream and a first recycled flue gas stream and mixing a produced hot flue gas stream with a second recycled flue gas stream to form reduced temperature flue gas stream which can be used directly in a power generator or to heat a reactor. The method and apparatus allow the flow rates of the streams to be adjusted so that temperatures in the combustion chamber and in the heat transfer units of the power generator or reactor can be kept below temperature that would thermally damage the combustion chamber, heat transfer units or reactors. An interesting invention is disclosed by Millard [66]. It proposes a method related to prohibiting burner's corrosion by combustion gases in a burner having a FGR. Corrosion is normally caused by the formation of free chlorine as alkali

Improvement of Combustion Processes by Recirculation

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Fig. (10). The scheme of the method for burning fossil fuels in a steam generator using oxy-fuel process (adapted from [73]).

CO2 is increased in the system which enables its easier capture by using cryogenic fractionation or chemical absorption [74]. Consequently, such a system can be thermally efficient due to recirculation of heat and mass and advantageously offers some process improvements for CO2 capture technologies. Marin and Charon [75] also disclose a method for operating a boiler using oxygen-enriched oxidants. Their method includes introducing oxygen-enriched air, or oxygen and air. Fuel and O2-enriched air are introduced into the combustion chamber of the steam-generating boiler and are combusted to generate thermal energy. At least a portion of the flue gases are collected and recirculated through the boiler. In the steam-generating boiler, the oxygen-enriched oxidant is introduced at one or more locations within the radiation zone and the convection zone of the boiler. Additionally, flue gas is collected and recirculated into one or more locations within the radiation zone and/or the convection zone of the boiler. According to the invention, the amount of oxygen enrichment and the total gas flow through the boiler is controlled so as to maintain the heat transfer patterns within the boiler at the originally - designed specification for operation by air combustion. Devault and McDonald [76] propose a cyclone furnace for oxygen fired boilers with FGR. The cyclone furnace and method uses a cyclone burner having a cyclone barrel with a re-entrant throat connected to a main furnace for passing combustion products including flue gas that is rich in carbon dioxide. Crushed coal and oxygen are supplied to the cyclone burner and at least some of the flue gas from the main furnace is recirculated to the cyclone barrel. CO2 enriched combustion enables to reduce NO X emissions and thus the cyclone furnace with FGR becomes more suitable for coal combustion. An invention by Hu and Pranda [77] relate to an FGR system which maintains a desired oxygen concentration for

stable combustion at increased recirculation rates. It provides an oxygen-enriched air assisting system for improving the efficiency of cogeneration system with FGR in which at least a desired oxygen concentration is maintained for stable combustion at increased recirculation rates. Oxygen-enriched gas is injected into the recirculated exhaust gas to achieve the desired effective oxygen concentration. 4. CURRENT & FUTURE DEVELOPMENTS Heat and mass recirculating systems offer substantial improvements in combustion processes. It was shown that recuperative heat exchange increased life expectancy of various combustion equipment, while reducing operating and maintenance costs for economic recovery of enthalpy from heated process streams. Regenerative heat recovery was utilized in e.g. turbines and IC engines. It enabled strong preheating of combustion mixture leading to the considerably decreased formation of NO X. However, the main field of application was still VOCs oxidation. The FGR systems were applied in numerous energy technologies. The main improvements related to thermal efficiency and reduction of harmful emissions primarily by means of the reduction of oxygen content, even temperature fields and decreased gas residence times. The recirculated combustion systems had more compact designs which allowed for the reduction of both fuel consumption and harmful emissions. At high FGR ratios combustion mixtures became highly diluted while reactants were highly preheated. It offered flameless fuel oxidation which generated reduced NO X emissions and the overall thermal efficiency of combustion was also increased. The oxygen-enriched combustion offers increased FGR ratios which are somehow limited in air combustion due to the cumulation of nitrogen. However, the current state of the art does not offer enough fuel flexible power generation at satisfactory thermal-to-electricity efficiency and the level of harmful emis-

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sions still can be reduced. In the most of energy technologies the level of 40% for thermal-to-electricity efficiency is considered to be satisfactory. Fuel requirements are still very high which do not favors the inclusion into the energy sector some novel fuels, e.g. renewable low-calorific fuels. Therefore, further developments are needed in heat and mass recirculating systems. In the recuperative heat-recirculating systems we expect that the novel types of efficient, radially miniaturized, tight, compact and high-temperature-pressure-resistant recuperators will develop [78]. The heat and mass recirculation technology will be applied to the larger number of energy technologies including those currently not implemented while being under constant development [e.g. 20]. It is expected that practical systems that apply much higher FGR ratios than currently available will soon develop. It may include oxy-fuel combustion systems. Further, the theory of complicated heat and/or mass recirculating systems for power generation will be improved which will enable more reliable theoretical comparisons of not-yet-implemented attractive novel energy technologies. This will include porous media combustion [24] and radiation effects [46]. The theoretical developments will also refer to high-pressure systems [15] and to highly diluted flameless fuel oxidation. Such combustion techniques will be more extensively applied to lean biomass or coal derived gases from e.g. gasification units [79]. It is also expected that the described approaches of mass and heat recirculation will be gradually integrated into more hybrid systems for its application to specific power generators. Furthermore, it is expected that the current market requirements for fuel flexible power generators will direct future researches at thermally efficient and fuel flexible clean power generation systems that will extensively use heat and mass recirculation. Besides, the FGR technique will create an alternative that will allow for the enrichment of process streams in CO2 which will be applied to air combustion, oxygen-enriched combustion, and to fuel reforming reactions. Carbon dioxide can enhance fuel reforming process, i.e. by means dry reforming. Also CO2 enrichment can decrease the costs of CO2 capture. ACKNOWLEDGEMENTS Wojciech Budzianowski gratefully acknowledges the financial support from Wroclaw University of Technology under the grant no. 332116/2008. CONFLICT OF INTEREST The authors declare no conflict of interest. ACRONYMS EGR FGR GT = = = Exhaust gas recirculation Flue gas recirculation Gas turbine High temperature combustion technology High temperature air combustion Heat recovery steam generator Internal combustion

IR PV RTO TPV SOFC VOC

= = = = = =

Infrared Photovoltaic Regenerative thermal oxidizer Thermophotovoltaic Solid-oxide fuel cell Volatile organic compound

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