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1.
The NO formation characteristics and reaction pathways of opposed-jet H2/CO syngas diffusion flames were analyzed with a revised OPPDIF program which coupled a narrowband radiation model with detailed chemical kinetics in this work. The effects of strain rates ranging from 0.1 to 1000 s?1 and diluents including CO2, H2O and N2 on NO production rates were investigated for three typical syngas compositions. The numerical results demonstrated that NO is produced primary through NNH-intermediate route and thermal route at high strain rates, where the reaction of NH + O = NO + H (R51) also become more active. Near the strain rate of 10 s?1, the flame temperature is the highest and thermal route is the dominant NO formation route, but NO would be consumed by reburn route where NO is converted to NH through HNO, especially for H2-rich syngas. At low strain rates, radiative heat loss results in a lower flame temperature and further reduce NO formation, while the reaction of N + CO2 = NO + CO (R140) become more important, especially for CO-rich syngas. With the diluents, NO production rates decreased with increasing dilution percentages. When the flame temperature is very high as the thermal route is dominant near strain rate of 10 s?1, CO2 dilution makes flame temperature and NO production rate the lowest. Toward both lower and higher strain rates, adding H2O is more effective in reducing NO because R140 and NNH-intermediate route are suppressed the most by H2O dilution respectively.  相似文献   

2.
The radiation effect on flame temperature and NO emission of H2-lean (0.2H2 + 0.8CO) and H2-rich (0.8H2 + 0.2CO) syngas/air counterflow diffusion flames was numerically investigated using OPPDIF code incorporated with the optical thin model, statistical narrow band model and adiabatic condition. Firstly, the coupled effect of strain rate and radiation was studied. Disparate tendencies of NO emission with an increasing strain rate between H2-lean and H2-rich syngas flames were found at very small strain rate, and the effect of radiation reabsorption on NO formation can be neglected when the strain rate was greater than 100 s?1 for both H2-lean and H2-rich syngas flames. Because the radiation effect is vital to flames with small strain rate, its impact on flame temperature and NO emission was investigated in detail at a strain rate of 10 s?1. The results indicated that NO formation is more sensitive to radiation reabsorption than flame temperature, especially for the H2-rich syngas flame. The underlying mechanism was discovered by using reaction pathway analysis. Furthermore, the radiation effect under CO2 dilution of the syngas fuel was examined. It was demonstrated that the radiation effect on flame temperature became more prominent with the increase of CO2 concentration for both H2-lean and H2-rich syngas. The radiation effect on NO emission increased first and then decreased with an increasing CO2 content for H2-lean syngas, whereas for H2-rich syngas the radiation effect is monotonic.  相似文献   

3.
This paper reported a numerical study on the NOx emission characteristics of opposed-jet syngas diffusion flames. A narrowband radiation model was coupled to the OPPDIF program, which used detailed chemical kinetics and thermal and transport properties to enable the study of 1-D counterflow syngas diffusion flames with flame radiation. The effects of syngas composition, pressure and dilution gases on the NOx emission of H2/CO synthetic mixture flames were examined. The analyses of detailed flame structures, chemical kinetics, and nitrogen reaction pathways indicate NOx are formed through Zeldovich (or thermal), NNH and N2O routes both in the hydrogen-lean and hydrogen-rich syngas flames at normal pressure. Zeldovich route is the main NO formation route. Therefore, the hydrogen-rich syngas flames produce more NO due to higher flame temperatures compared to that for hydrogen-lean syngas flames. Although NNH and N2O routes also are the primary NO formation paths, a large amount of N2 will be reformed from NNH and N2O species. For hydrogen-rich syngas flames, the NO formation from NNH and N2O routes are lesser, where NO can be dissipated through the reactions of NH + NO  N2 + OH and NH + NO  N2O + H more actively. At a rather low pressure (0.01 atm), NNH-intermediate route is the only formation path of NO. Increasing pressure then enhances NO formation reactions, especially through Zeldovich mechanisms. However, at higher pressures (5–10 atm), NO is then converted back to N2 through reversed N2O route for hydrogen-lean syngas flames, and through NNH as well for hydrogen-rich syngas flames. In addition, the dilution effects from CO2, H2O, and N2 on NO emissions for H2/CO syngas flames were studied. The hydrogen-lean syngas flames with H2O dilution have the lowest NO production rate among them, due to a reduced reaction rate of NNH + O  NH + NO. But for hydrogen-rich syngas flames with CO2 dilution, the flame temperatures decrease significantly, which leads to a reduction of NO formation from Zeldovich route.  相似文献   

4.
Syngas is a promising alternative fuel for stationary power generation due to cleaner combustion than convectional fossil fuels. During the gasification processes, the by-products of CO2, H2O, or N2 may be present in the syngas mixture to control the flame temperature and emissions. Several studies indicated that syngas with dilutions is capable of reducing pollutant emissions such as NOx emissions. This work applied a numerical model of opposed-jet diffusion fames to explore the dilution effects on NOx formation and differentiate the inert effect, thermal/diffusion effect, chemical effect, and radiation effect from CO2, H2O, or N2 dilutions. The numerical study was performed by a revised OPPDIF program coupling with narrowband radiation model and detail chemical mechanism. The dilution effects on NOx formation were analyzed by comparing the realistic and hypothetical cases. Regardless the diluent types, the inert effect is the main cause to reduce NO production, followed by chemical effect and radiation effect. The thermal/diffusion effect may promote NO formation because the preferential diffusion due to different diffusivities between diluents and syngas magnifies the reaction rate locally. CO2 dilution reduces NO by radiation effect at low strain rate, and contributes NO reduction by chemical effect at high strain rate. At the same dilution percentage, CO2 dilution reduces NO production the most, followed by H2O and N2. Besides the thermal/diffusion effect, the chemical effect of H2O enhances NO production through thermal route and reburn route.  相似文献   

5.
The NO mechanism under the moderate or intense low-oxygen dilution (MILD) combustion of syngas has not been systematically examined. This paper investigates the NO mechanism in the syngas MILD regime under the dilution of N2, CO2, and H2O through counterflow combustion simulation. The syngas reaction mechanism and the counterflow combustion simulation are comprehensively validated under different CO/H2 ratios and strain rates. The effects of oxygen volume fraction, CO/H2 ratio, pressure, strain rate, and dilution atmosphere are systematically investigated. For all the MILD cases, the contribution of the prompt and NO-reburning routes to the overall NO emission is less than 0.1% due to the lack of CH4 in fuel. At atmospheric pressure, the thermal route only accounts for less than 20% of the total NO emission because of the low reaction temperature. Moreover, at atmospheric pressure, the contribution of the NNH route to NO emission is always larger than 55% in the N2 atmosphere. The N2O-intermediate route is enhanced in CO2 and H2O atmospheres due to the increased third-body effects of CO2 and H2O through the reaction N2 + O (+M) ? N2O (+M). Especially in the H2O atmosphere, the N2O-intermediate route contributes to 60% NO at most. NO production is reduced with increasing CO/H2 ratio or pressure, mainly due to decreased NO formation from the NNH route. Importantly, a high reaction temperature and low NO emission are simultaneously achieved at high pressure. To minimize NO emission, the reactions should be operated at high values of CO/H2 ratios (i.e., >4) and pressures (e.g., P > 10 atm), low oxygen volume fractions (e.g., XO2 < 15%), and using H2O as a diluent. This study provides a new fundamental understanding of the NO mechanism of syngas MILD combustion in N2, CO2, and H2O atmospheres.  相似文献   

6.
The effect of CO2/N2/CH4 dilution on NO formation in laminar coflow H2/CO syngas diffusion flames was experimentally and numerically investigated. The results reveal that the NO emission index increases with H2/CO mole ratio. In all cases, CO2/N2/CH4 dilution can reduce the peak temperature of syngas flame and have the ability to reduce peak flame temperature is decreased in the following order: CO2>N2>CH4. CO2/N2 dilution reduces the NO formation in syngas flame while CH4 dilution promotes the NO formation. Besides, the dilution of CO2/N2/CH4 can reduce the peak mole fraction of OH and its variations with H2/CO mole ratio and dilution ratio show the same trend as the peak flame temperature variations. The height of the flame with CO2 and N2 dilution increases with dilution ratio. The flame with CH4 dilution becomes higher and wider with the increase of dilution ratio.  相似文献   

7.
A deep understanding of the ignition characteristics of syngas in O2/CO2 and O2/H2O atmospheres is essential for the application of oxy-syngas combustion. In the present work, ignition properties of a syngas with a typical H2-to-CO ratio (1:2) in O2/N2, O2/CO2 and O2/H2O atmospheres were investigated numerically. The ignition temperatures were determined by a 1-D model of a micro flow reactor with a controlled wall temperature profile, demonstrating that CO2 and H2O can lead to an increase in the ignition temperature compared to N2, and the increase is more pronounced for the O2/H2O atmosphere. The analysis manifests that CO2 and H2O can suppress OH production at the region with relatively lower wall temperature by promoting R10: H + O2(+M) = HO2+(M) to compete with R11: H + HO2 = 2OH for H radical. Moreover, the direct reaction effect (directly take part in reactions as reactants) and third-body effect of CO2 and H2O on ignition temperature were numerically isolated by adopting artificial species. The computation results reveal that the increase in ignition temperature mainly results from the enhanced reaction rate of R10 by the third-body effects of CO2 and H2O.  相似文献   

8.
This paper reports a numerical study on the combustion and extinction characteristics of opposed-jet syngas diffusion flames. A model of one-dimensional counterflow syngas diffusion flames was constructed with constant strain rate formulations, which used detailed chemical kinetics and thermal and transport properties with flame radiation calculated by statistic narrowband radiation model. Detailed flame structures, species production rates and net reaction rates of key chemical reaction steps were analyzed. The effects of syngas compositions, dilution gases and pressures on the flame structures and extinction limits of H2/CO synthetic mixture flames were discussed. Results indicate the flame structures and flame extinction are impacted by the compositions of syngas mixture significantly. From H2-enriched syngas to CO-enriched syngas fuels, the dominant chain reactions are shifting from OH + H2→H + H2O for H2O production to OH + CO→H + CO2 for CO2 production through the key chain-branching reaction of H + O2→O + OH. Flame temperature increases with increasing hydrogen content and pressure, but the flame thickness is decreased with pressure. Besides, the study of the dilution effects from CO2, N2, and H2O, showed the maximum flame temperature is decreased the most with CO2 as the dilution gas, while CO-enriched syngas flames with H2O dilution has highest maximum flame temperature when extinction occurs due to the competitions of chemical effect and radiation effect. Finally, extinction limits were obtained with minimum hydrogen percentage as the index at different pressures, which provides a fundamental understanding of syngas combustion and applications.  相似文献   

9.
In recent years, research efforts have been channeled to explore the use of environmentally-friendly clean fuel in lean-premixed combustion so that it is vital to understand fundamental knowledge of combustion and emissions characteristics for an advanced gas turbine combustor design. The current study investigates the extinction limits and emission formations of dry syngas (50% H2-50% CO), moist syngas (40% H2-40% CO-20% H2O), and impure syngas containing 5% CH4. A counterflow flame configuration was numerically investigated to understand extinction and emission characteristics at the lean-premixed combustion condition by varying dilution levels (N2, CO2 and H2O) at different pressures and syngas compositions. By increasing dilution and varying syngas composition and maintaining a constant strain rate in the flame, numerical simulation showed among diluents considered: CO2 diluted flame has the same extinction limit in moist syngas as in dry syngas but a higher extinction temperature; H2O presence in the fuel mixture decreases the extinction limit of N2 diluted flame but still increases the flame extinction temperature; impure syngas with CH4 extends the flame extinction limit but has no effect on flame temperature in CO2 diluted flame; for diluted moist syngas, extinction limit is increased at higher pressure with the larger extinction temperature; for different compositions of syngas, higher CO concentration leads to higher NO emission. This study enables to provide insight into reaction mechanisms involved in flame extinction and emission through the addition of diluents at ambient and high pressure.  相似文献   

10.
One-dimensional premixed freely-propagating flames for (CH4+CO2/H2O)/air(79%N2+21%O2) mixtures were modeled using ChemkinⅡ/Premix Code with the detailed mechanism GRI-Mech 3.0. The investigation of the effects of CO2 and steam addition on the H2 intermediate formation and NO emission was conducted at the initial conditions of 1 atm and 398 K. Both physical and chemical effects of CO2, H2O on laminar burning velocities and adiabatic flame temperatures were also analyzed. The calculations show that with the increase of αCO2 and αH2O, both physical and chemical effects of CO2 and H2O result in the reduction of laminar burning velocities (LBVs) and adiabatic flame temperatures (AFTs) in which the chemical effects of CO2 addition are more significantly than H2O. Especially, the chemical effects of steam promote the increase of AFTs and the influence in rich BG65 flames are larger than in methane. With a proper amount of H2O addition, the chemical effects of H2O on the peak concentration of H2 are more significantly than physical at Φ = 1.2. Moreover, CO2, steam and their mixture addition have significant reduction on the NO emission. The most sensitive reaction for the formation of H2 and NO emission were determined. The responsible reactions for H2 formation and NO emission are R84 OH + H2 <=> H + H2O and R240 CH + N2 <=> HCN + N (a prompt routine), respectively.  相似文献   

11.
Extensive computations were made to determine the flammability limits of opposed-jet H2/CO syngas diffusion flames from high stretched blowoff to low stretched quenching. Results from the U-shape extinction boundaries indicate the minimum hydrogen concentrations for H2/CO syngas to be combustible are larger towards both ends of high strain and low strain rates. The most flammable strain rate is near one s−1 where syngas diffusion flames exist with minimum 0.002% hydrogen content. The critical oxygen percentage (or limiting oxygen index) below which no diffusion flames could exist for any strain rate was found to be 4.7% for the equal-molar syngas fuels (H2/CO = 1), and the critical oxygen percentage is lower for syngas mixture with higher hydrogen content. The flammability maps were also constructed with strain rates and pressures or dilution gases percentages as the coordinates. By adding dilution gases such as CO2, H2O, and N2 to make the syngas non-flammable, besides the inert effect from the diluents, the chemical effect of H2O contributes to higher flame temperature, while the radiation effect of H2O and CO2 plays an important role in the flame extinction at low strain rates.  相似文献   

12.
The present study numerically investigated the effect of oxygen enrichment on the precise structure and NOx formation characteristics of turbulent syngas non-premixed flames. The turbulence-chemistry interactions were represented by a Lagrangian flamelet model. In context with the Lagrangian flamelet model, the NO concentration was obtained directly from the flamelet calculation based on full NOx chemistry, with radiative heat loss being accounted for through the flamelet energy equation. Computations were performed for three different syngas compositions with a designated nitrogen dilution level. Numerical results indicated that, for the CO-rich composition with the lowest LHV yielding the highest scalar dissipation rate and shortest flight time, the flame structure was dominantly influenced by turbulence-chemistry interactions. On the other hand, with regard to the H2-rich composition with the highest LHV yielding the lowest injection velocity and longest flight time, the flame structure was strongly influenced by radiative cooling. The peak NO level was remarkably elevated by increased oxygen level due to the elevated temperature of the oxygen-enriched flame. In the enhanced oxygen level (30%), the H2-rich case produced the highest NO level due to a higher temperature and longer residence time within the hot flame zone, while the CO-rich case yielded the lowest NO level due to a lower temperature and shorter residence time. It was also found that, by enhancing the oxygen level, contributions of NNH and N2O to total NO emission rapidly decreased while the contributions of the thermal NO path were progressively dominant for all cases.  相似文献   

13.
Flame characteristics of swirling non-premixed H2/CO syngas fuel mixtures have been simulated using large eddy simulation and detailed chemistry. The selected combustor configuration is the TECFLAM burner which has been used for extensive experimental investigations for natural gas combustion. The large eddy simulation (LES) solves the governing equations on a structured Cartesian grid using a finite volume method, with turbulence and combustion modelling based on the localised dynamic Smagorinsky model and the steady laminar flamelet model respectively. The predictions for H2-rich and CO-rich flames show considerable differences between them for velocity and scalar fields and this demonstrates the effects of fuel variability on the flame characteristics in swirling environment. In general, the higher diffusivity of hydrogen in H2-rich fuel is largely responsible for forming a much thicker flame with a larger vortex breakdown bubble (VBB) in a swirling flame compare to the H2-lean but CO-rich syngas flames.  相似文献   

14.
Hydrogen (H2) is considered as a carbon-free alternative fuel. The heat release characteristics of H2 flame as a key parameter in its combustion process are unclear. In this study, the combustion and heat release characteristics of H2/air diffusion flame on a micro-jet array burner were experimentally and numerically investigated. It is shown that the OH distribution and flame length based on Bilger mechanism are in good agreement with the experimental results. Furthermore, the intensity and distribution of OH and heat release rate can be adjusted by the thermal power and equivalence ratio. A uniform flame with intensive heat release rate can be achieved at a thermal power of 0.1 kW. R41: H + O2 = OH + O and R43: H + O2 + M = HO2 + M are the main reactions with oxidizer consumption to form reactive radicals. R40: OH + H2 = H2O + H and R47: OH + OH = O + H2O with OH consumption are the main heat release reactions at the upstream and downstream of the flame.  相似文献   

15.
Demand for the clean and sustainable energy encourages the research and development in the efficient production and utilisation of syngas for low-carbon power and heating/cooling applications. However, diversity in the chemical composition of syngas, resulting due to its flexible production process and feedstock, often poses a significant challenge for the design and operation of an effective combustion system. To address this, the research presented in this paper is particularly focused on an in-depth understanding of the heat generation and emission formation of syngas/producer gas flames with an effect of the fuel compositions. The heat generated by flame not only depends on the flame temperature but also on the chemistry heat release of fuel and flame dimension. The study reports that the syngas/producer gas with a low H2:CO maximises the heat generation, nevertheless the higher emission rate of CO2 is inevitable. The generated heat flux at H2:CO = 3:1, 1:1, and 1:3 is found to be 222, 432 and 538 W m-2 respectively. At the same amount of heat generated, H2 concentration in fuel dominates the emission of NOx. The addition of CH4 into the syngas/producer gas with H2:CO = 1:1 also increases the heat generation significantly (e.g. 614 W m-2 at 20%) while decreases the emission formation. In contrast, adding 20% CO2 and N2 to the syngas/producer gas composition reduces the heat generation from 432 W m-2 to 364 and 290 W m-2, respectively. The role of CO2 on this aspect, which is weaker than N2, thus suggests CO2 is preferable than N2. Along with the study, the significant role of CO2 on the radiation of heat and the reduction of emission are examined.  相似文献   

16.
Experimental investigations of H2 and H2-enriched syngas flame radiation properties have been conducted through spectroscopic and DFCD (Digital Flame Colour Discrimination) techniques. A spectrograph was employed to quantify the emission profile of H2-based flames in the UV–visible spectral domain. The OH* emission was found to be the strongest in reactants with highest amount of H2. Further addition of CO and/or CO2 resulted in the reduction of OH* intensity with the addition of CO2 causing greater radical intensity-loss than that of CO. The decrease in OH* intensity is accompanied by a corresponding increase in the CO–O* broadband continuum in the short-wavelength domain of the visible spectrum. Such reduction of OH* along with increase in CO–O* intensity can be related to the endothermic reaction mechanism of CO + OH => CO2 + H, which describes the role of CO/CO2 addition in H2-enriched syngas flames. Comparison with direct imaging results provided additional credence to the effect of temperature reduction as flames with CO and/or CO2 additions resembled colourations closer to typical bluish premixed hydrocarbon flame. The employment of DFCD processing effectively characterised different syngas combustion conditions by combining aspects of digital flame colour intensities with spatial combustion distributions. This colour signal quantification method was shown to yield useful characterisation of H2-based flames, similar to the use of OH* chemiluminescence intensity variation from spectrometry. Also, DCFD analysis was able to depict the variances between the burning of different syngas gaseous constituents. Thus, useful image-based parameters related to the H2-based combustion can be derived and potentially applied as a practical monitoring and characterisation mean for syngas combustion.  相似文献   

17.
Oxy-steam combustion is a potential new-generation option for CO2 capture and storage. The ignition and combustion characteristics of single coal and biomass particles were investigated in a flow tube reactor in O2/N2 and O2/H2O at various oxygen concentrations. The ignition and combustion processes were recorded using a CCD camera, and the two-color pyrometry was used to estimate the volatile flame temperature and char combustion temperature. In O2/N2 and O2/H2O, coal ignites heterogeneously at <O2> = 21–50%. In O2/N2, biomass ignites homogeneously at <O2> = 21–30%, while it ignites heterogeneously at <O2> = 40–50%. In O2/H2O, biomass ignites homogeneously at <O2> = 21–50%. With increasing oxygen concentration, the ignition delay time, volatile burnout time and char burnout time are decreased, and the volatile flame temperature and char combustion temperature are increased. At a certain oxygen concentration in both atmospheres, the ignition delay time, volatile burnout time and char burnout time of biomass are shorter than those of coal. Moreover, biomass has a higher volatile flame temperature but a lower char combustion temperature than coal. The ignition delay time, volatile burnout time and char burnout time in O2/H2O are lower than those in O2/N2 for coal and biomass. The presence of H2O can improve the combustion rates of coal and biomass. The volatile flame shows a lower temperature in O2/H2O than in O2/N2 at <O2> = 21–50%. The char combustion shows a lower temperature in O2/H2O than in O2/N2 at <O2> = 21–30%, while this behavior is switched at <O2> = 40–50%. The results contribute to the understanding of the ignition and combustion characteristics of coal and biomass in oxy-steam combustion.  相似文献   

18.
Fe-Ba/ZSM-5 catalysts were prepared for NO + O2 adsorption and NO reduction by CO at 250–400 °C. NO adsorption and reduction were investigated for different Fe contents, while the Ba content was fixed at 5 wt.%. The catalysts were characterized by BET, SEM, XRD, XPS, H2-TPD, and in situ DRIFTS. The NO + CO activity tests of Fe-Ba/ZSM-5 catalysts showed that the NO reduction efficiencies were strongly affected by temperature. The NOx adsorption capacity of Fe-Ba/ZSM-5 catalysts increased with increasing Fe loading. The results of catalyst characterization showed that the dispersion of Fe species is one of the most important factors affecting NO reduction and adsorption performance. High Fe loading increased the amount of adsorbed NOx, while the NO + CO reaction was favored by good dispersion of Fe species. However, the NOx adsorption capacity decreased for Fe loadings above 8.3% due to the aggregation of metal oxides.  相似文献   

19.
Laminar burning velocities of CO–H2–CO2–O2 flames were measured by using the outwardly spherical propagating flame method. The effect of large fraction of hydrogen and CO2 on flame radiation, chemical reaction, and intrinsic flame instability were investigated. Results show that the laminar burning velocities of CO–H2–CO2–O2 mixtures increase with the increase of hydrogen fraction and decrease with the increase of CO2 fraction. The effect of hydrogen fraction on laminar burning velocity is weakened with the increase of CO2 fraction. The Davis et al. syngas mechanism can be used to calculate the syngas oxyfuel combustion at low hydrogen and CO2 fraction but needs to be revised and validated by additional experimental data for the high hydrogen and CO2 fraction. The radiation of syngas oxyfuel flame is much stronger than that of syngas–air and hydrocarbons–air flame due to the existence of large amount of CO2 in the flame. The CO2 acts as an inhibitor in the reaction process of syngas oxyfuel combustion due to the competition of the reactions of H + O2 = O + OH, CO + OH = CO2 + H and H + O2(+M) = HO2(+M) on H radical. Flame cellular structure is promoted with the increase of hydrogen fraction and is suppressed with the increase of CO2 fraction due to the combination effect of hydrodynamic and thermal-diffusive instability.  相似文献   

20.
This study systematically investigates the detailed mechanism of nitrogen oxides (NOx) in CH4 and CH4/H2 jet flames with O2/CO2 hot coflow. After comprehensive validation of the modeling by experiments of Dally et al. [Proc. Combust. Inst. 29 (2002) 1147–1154]; the effects of CO2 replacement of N2, mass fraction of oxygen in the coflow (YO2), and mass fraction of hydrogen in the fuel jet (YH2) on NO formation and destruction are investigated in detail. For methane oxy-fuel combustion, the NNH route is found to control the NO formation at YO2 ≤ 3%, while both NNH and N2O-intermediate routes dominate the NO production at 3% < YO2 < 10%. When YO2 ≥ 10%, NO is obtained mainly from thermal mechanism. Moreover, in the oxy-combustion of methane and hydrogen fuel blends with YO2 = 3%, with hydrogen addition the contribution of the NNH and prompt routes increases, while that of the N2O-intermediate route decreases. Furthermore, the chemical effect of CO2 is significant in reducing NO in both oxy-combustion of methane with YO2 ≤ 3% and combustion of methane and hydrogen fuel blends with YH2 ≤ 10%.  相似文献   

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