微波处理对模型焦脱除NO特性的影响

运用自制的微波电加热反应系统,进行了不同微波功率、温度和试验方式对模型焦脱除NO反应性能的影响研究。结果表明:一定程度的微波改性可以促进模型焦吸收NO;NO还原率随微波功率的增大先增大后减小;常温下改性时间为90s时,存在最佳改性功率480 W,该功率改性的模型焦NO还原率最高;常温下改性模型焦的NO还原率普遍高于同功率下的800℃改性模型焦的NO还原率.对部分模型焦进行压汞分析和XPS分析,结果表明,微波处理改变了模型焦的孔隙结构和表面官能团,比表面积和孔容积的增大以及表面含氧官能团的减少有利于NO的吸收。微波热效应和非热效应共同作用影响模型焦还原NO过程。恒温800℃下间歇施加微波方式的NO还原提高率远低于程序升温式。     

利用甲醇氧化烟气中NO的实验研究

对利用甲醇氧化烟气中NO的反应开展了系统的实验研究。研究了反应时间、反应温度、甲醇用量比例、烟气中O2、SO2及夹带的固体颗粒对NO氧化率的影响。结果表明,在一定的条件下,甲醇能够氧化烟气中的NO;NO氧化率受反应时间和反应温度的综合影响,随着反应时间的增加,有效反应温度区域向低温方向移动,最大NO氧化率降低;随着甲醇用量比例的增加, NO氧化率增加;O2浓度增加可促进NO氧化;烟气中的SO2对反应有催化作用,可显著提高NO氧化率;烟气中固体颗粒的存在阻碍了自由基反应的进行,显著降低了NO的氧化率。     

PEM燃料电池内水分布和温度分布的数值模拟

本文建立了一个两相流、非等温、三维模型来研究PEM燃料电池内的传递过程,讨论了其内部水分布和温度分布特性。模拟结果表明水分布和温度分布都不均匀。沿着流动方向阳极侧水浓度逐渐降低,而阴极侧水浓度却不断升高,导致阴极容易形成液态水;在垂直流动方向上,脊下水的浓度和液态水饱和度都高于流道下;不同放电电压下阴极GDL中液态水分布趋势不同。沿流动方向温度逐渐降低,反应气体不足时降低梯度更大;脊下膜电极中温度低于流道下;垂直膜电极方向上最高温度在阴极催化层,放电电压越低,温度梯度越大;相同放电电压下质子交换膜越厚,各处的温度越低,温度梯度也越小。     

太赫兹辐射场下的石墨烯光生载流子和光子发射

通过半经典的玻尔兹曼平衡方程理论研究了太赫兹辐射场下的石墨烯光生载流子和光子发射.研究得到了太赫兹辐射场下石墨烯的光生载流子浓度和光子发生率的解析公式.研究发现,掺杂电子浓度越小,或者温度越低,光生载流子浓度越大;掺杂电子浓度越大,或者温度越低,石墨烯的光子发射率越大.通过改变门电压或温度,可以有效地调控石墨烯光生载流子浓度和光子发射概率.理论研究结果和解析表达式对发展以石墨烯为基础的新型太赫兹光电器件具有重要的参考价值.     

化学脱灰对低灰煤粉性质的影响

本文研究了HCl-HF-HCl方法脱灰对低灰煤粉性质的的影响.研究发现,酸处理不仅使煤的灰分脱除,也使其挥发分降低,煤变质程度越低,挥发分降低幅度越大;通过对脱灰滤液的检测,发现脱落的有机质主要是短链烷烃及其同系物,也有少量的含氧物质;酸处理后煤粉中金属离子也将全部脱除;燃烧特性研究发现,煤粉脱灰后高变质程度煤反应活性提高,低变质程度煤反应活性下降,取决于有机质和金属离子脱除与比表面积增加之间的平衡.因此,化学脱灰不能证明矿物对煤粉燃烧的影响.     

CFB富氧燃烧中CO_2对煤焦与NO还原作用的影响

为了考察高浓度CO_2对煤焦与NO还原所带来的影响,本文在悬浮床反应器上开展了。N_2和CO_2气氛下煤焦与NO的还原实验。结果表明:在无煤焦或矿物组分催化下CO不与NO发生反应;900℃N_2气氛下,在煤焦与NO反应初期NO还原率保持不变,而在整个反应过程中碳比反应率和CO_2生成比例则持续增大;N_2气氛下,煤焦与NO反应的含碳产物在700℃时以CO_2为主,而随着温度升高CO的生成比例增大,900℃时CO的生成占主导地位;高浓度的CO_2对煤焦-NO还原反应有明显的抑制作用,且温度越高抑制作用越显著,这可能是因CO_2气化抢占碳活性位所致。     

第一壁泄漏杂质的分布计算

以数值计算法计算了第一壁冷却剂泄漏氦杂质在等离子体中的分布,氦分布的峰值在SOL(Scrape-ofLayer)区。当要求等离子体中心的氦浓度小于5%时,允许的最大泄漏率N_max约为0.35×10^-3Mol/s,允许的最大裂纹尺寸长约为3.1mm,宽约为0.63mm。影响杂质分布和浓度的主要因素有壁温、等离子体边缘温度、密度和SOL区的温度密度长度。壁温越低、等离子体边缘温度越低、密度越高、温度和密度长度越大,则中心杂质浓度越小,且杂质分布峰值越接近第一壁。     

CaO表面CO对NO还原作用的实验与模型研究

循环流化床炉内石灰石脱硫对NOx排放产生影响,包括对挥发分氮氧化的催化作用以及对CO-NO还原的催化作用。利用固定床反应器对不同条件下CaO颗粒表面NO+CO的催化反应特性进行了探究。实验表明,无氧条件下,CaO能够显著催化CO还原NO,NO转化率与反应温度和CO浓度正相关,与NO浓度负相关.基于Langmuir-Hinshelwood机理建立了CaO催化NO+CO反应动力学模型,模型考虑了颗粒内、外扩散的影响.该模型适用于氧气浓度很低、CO浓度较高条件下。而在有氧气氛中,该反应受到明显抑制,且O2浓度越高,抑制作用越明显;当CaO周围氧气浓度远大于CO时,可忽略CaO对NO的催化还原作用。     

利用链式反应同步氧化烟气中NO和SO2的研究

燃煤烟气中NO和SO2的氧化对于提高其脱除效率和改良脱除产物有重要意义。基于大气化学的研究成果,本文提出了利用链式反应同步氧化烟气中NO和SO2的设想。阐述了该方法的反应机理,数值实验研究了在烟气条件下该链式反应发生的可能性以及反应温度对NO和SO2氧化率的影响,提出了利用低成本的添加剂引发链式反应的方法,并分析了选择添加剂的原则。     

低起始温度的线性升温热处理对直拉硅中氧沉淀的影响

研究了直拉硅片从不同的温度线性升温(Ramping)到750℃，然后在750℃退火64 h过程中的氧沉淀行为. 结果表明，Ramping对硅片中氧沉淀的形成有明显的促进作用，且起始温度越低促进作用越强. 这是因为在Ramping处理中，低温(450—650℃)热处理阶段氧的扩散速率显著增强，促进了氧沉淀核心的形成，且较低的Ramping升温速率有利于氧沉淀核心的稳定和继续长大. 进一步的实验结果还表明，低起始温度的Ramping处理可应用于硅片的内吸杂工艺，能促进氧沉淀的生成提高硅片的内吸杂能力，减少热预     

煤和煤焦还原NO的实验研究

本文报告了在 ＮＯ初始浓度为 １０００ × １０－６、不同的反应区温度和化学当量比的条件下,不同煤粉及其煤焦对ＮＯ还原的实验结果．实验结果表明,ＮＯ的还原率不仅取决于反应区的化学当量比和反应温度,而且更重要的是取决于再燃燃料的性质、以及再燃燃料中金属氧化物的含量。煤粉作为再燃燃料还原ＮＯ时,煤焦的异相机理起主要作用。     

Soot and NO formation in counterflow ethylene/oxygen/nitrogen diffusion flames

Formation of soot and NO in counterflow ethylene/oxygen/nitrogen diffusion flames was numerically investigated. Detailed chemistry and complex thermal and transport properties were used. A simplified two-equation soot model was adopted. The results indicate that NO emission has negligible influence on soot formation. However, soot formation affects the emission of NO through the radiation induced thermal effect and the reaction induced chemical effect. When the oxygen index of the oxidant stream is lower, the relative influence of chemical reaction caused by soot on NO emission is more important, while the relative influence of the radiation induced thermal effect becomes more important for the flame with a higher oxygen index in the oxidant stream.     

Soot and NO emissions control in a natural gas/diesel fuelled RCCI engine by φ-T map analysis

Soot and NO emissions are considered as major pollutants to the atmosphere from compression ignition engines. Researchers have been dedicated to the reduction of soot and NO emissions. Thus, an advance combustion regime, i.e. reactivity controlled compression ignition (RCCI), was proposed to mitigate the formation of these emissions. In this study, the dynamic ?-T (equivalence ratio vs. temperature) map analysis was applied to visualise the combustion processes associated with the in-cylinder temperature and equivalence ratio in an RCCI engine. Therefore, the soot and NO emissions can be efficiently reduced by controlling the combustion process out of the emissions islands on the ?-T map. This analysis method employs KIVA4-CHEMKIN and SENKIN code to construct ?-T maps under various conditions. To find out the significant parameters of controlling combustion process and emissions formation, four parameters were taken into consideration in a natural gas (NG) and diesel fuelled RCCI engine: NG percentage, the first start of injection (SOI) timing, split fraction of diesel and exhaust gas recirculation (EGR) rate. Each parameter was varied at three levels. Finally, the ?-T maps and final soot and NO emissions were compared among varied conditions for each parameter. It is found that the increased NG percentage can significantly reduce soot because of the absence of C-C bond in NG and the reduced diesel fuel impingement on the surface of the piston or cylinder wall. Increasing EGR can decrease the peak combustion temperature due to the dilution effect and thermal effect, consequently maintaining RCCI at low temperature combustion region. This study also indicates that dynamic ?-T map analysis is efficient at manipulating the combustion process to mitigate the soot and NO emissions formation.     

Catalytic soot oxidation in microscale experiments: Simulation of interactions between co-deposited graphitic nanoparticle agglomerates and platinum nanoparticles

Continuously regenerating catalytic soot traps are under development to reduce particulate emissions from diesel exhaust. A good understanding of the processes that take place during soot oxidation is needed to optimize diesel soot trap performance. To gain insight into these processes from the perspective of nanoparticle technology, the effects of catalyst particle size and the interparticle distance between soot and catalyst particles were measured. A model catalyst was prepared by depositing Pt nanoparticles on a SiO/SiO₂-coated transmission electron microscope (TEM) grid. A soot surrogate composed of graphitic nanoparticle agglomerates generated by laser ablation was deposited on the same surface. This system simulates, morphologically, catalytic soot traps used in practice. The reaction was carried out in a tubular flow reactor in which the gas phase simulated diesel exhaust gas, composed of a mixture of 10% O₂ and 1000 ppm NO with the remainder N₂. The progress of the carbon nanoparticle oxidation was monitored off-line by analysis of electron microscopy images of the agglomerates before and after reaction. This experimental method permitted the correlation of reaction rate with particle sizes and separation distances as well as catalyst surface area in the direct environs of the soot particles. The experimental results revealed no effect of Pt catalyst particle size in the range 7–31 nm on the rate of reaction. Also observed were a decrease in the rate of reaction with increasing distance between carbon agglomerates and catalyst particles and a linear dependence of the reaction rate on the fractional catalyst surface area coverage.     

Effect of pressure on soot formation in the pyrolysis of <Emphasis Type="Italic">n</Emphasis>-hexane and the oxidation of fuel-rich mixtures of <Emphasis Type="Italic">n</Emphasis>-heptane behind reflected shock waves

The results of detailed kinetic simulations of the formation of soot particles in the pyrolysis of n-hexane–argon mixtures and in the oxidation of fuel-rich (φ = 5) n-heptane–oxygen–argon mixtures behind reflected shock waves at pressures of 20–100 bar and a constant concentration of carbon atoms or a constant fraction of argon in the initial mixture within the framework of a modified reaction mechanism are reported. The choice of n-hexane and n-heptane for examining the effect of pressure on the process of soot formation was motivated by the availability for these hydrocarbons of experimental measurements in reflected shock waves at high pressures (up to ~100 bar). The temperature dependences of the yield of soot particles formed in the pyrolysis of n-hexane are found to be very weakly dependent on pressure and slightly shifting to lower temperatures with increasing pressure. In general, pressure produces a very weak effect on the soot formation in the pyrolysis of n-hexane. The effect of pressure and concentration of carbon atoms in the initial mixture on the process of soot formation during the oxidation of fuel-rich n-heptane mixtures behind reflected shock waves is studied. The results of our kinetic simulations show that, for both the pyrolysis of n-hexane and the oxidation of fuel-rich n-heptane–oxygen mixtures, the influence of pressure on the process of soot formation is negligible. By contrast, the concentration of carbon atoms in the initial reaction mixture produces a much more pronounced effect.     

Acoustically assisted removal of nitrogen oxide from high temperature flue gas

The present study focuses on a possibility for improving NO removal efficiency from flue gas by application of powerful sound waves. The sound waves (frequency 6.9-17.2kHz, intensity 144-160dB) are propagated from Hartmann sound generators to a preheated graphite disk inside a vertical reaction tube (height 1.8m, I.D. 105mm). An Ar-NO synthetic mixture (NO 911-934ppm) is blown onto the disk surface to perform reactions in the system C-NO. It is found that the NO reduction rate can be significantly enhanced by the sound waves but the enhancement effect is dependent on the sound frequency, intensity and temperature of disk surface. The better effects are obtained at a temperature of 973K and sound frequencies between 9.6 and 12.4kHz. Under these conditions, the sound application results in 3-5-fold enhancement of NO reduction rate. The obtained effects are explained in terms of gas-phase mass transfer controlling mechanism and of near surface turbulent diffusivity.     

Prediction of soot formation characteristics in a pulverized-coal combustion field by large eddy simulations with the TDP model

In this study, the soot formation characteristics in a pulverized-coal combustion field formed by a 4 kW Central Research Institute of Electric Power Industry (CRIEPI) jet burner were predicted by large eddy simulation (LES) employing a tabulated-devolatilization-process model (TDP model) [N. Hashimoto et al., Combust. Flame 159 (2012) 353–366]. This model enables to take into account the effect of coal particle heating rate on coal pyrolysis. The coal-derived soot formation model proposed by Brown and Fletcher [A. L. Brown and T. H. Fletcher, Energy Fuels 12 (1998) 745–757] was employed in the LES. A comparison between the data predicted by LES and the soot volume fraction distribution data measured by laser induced incandescence confirmed that the soot formation characteristics in the coal combustion field of the CRIEPI burner can be accurately predicted by LES. A detailed analysis of the data predicted by LES showed that the soot particle distribution in this burner is narrow because the net soot formation rate is negative on both sides of the base of the soot volume fraction. At these positions, soot particles diffused from the peak position of soot volume fraction are oxidized due to a relatively high oxygen concentration. Finally, the effect of soot radiation on the predicted gas temperature distribution was examined by comparing the simulation results obtained with and without soot radiation. This comparison showed that the maximum gas temperature predicted by the simulation performed with soot radiation was over 100 K lower than that predicted by the simulation performed without soot radiation. From result strongly suggests the importance of considering a soot formation model for performing numerical simulations of a pulverized-coal combustion filed.     

Kinetics of nitrous acid formation in nitric acid solutions under the effect of power ultrasound

Sonochemical nitrous acid formation was investigated in 0.1-4.0 mol dm(-3) aqueous nitric acid solutions under the effect of power ultrasound with 20 kHz frequency. HNO2 steady-state concentration was obtained under long-time sonication; the excess HNO2 formed is decomposed and evoluted from the solution as NO and NO2 gases. The HNO2 steady-state concentration and the HNO2 initial formation rate depend linearly on the HNO3 concentration and acoustic intensity (1.8-3.5 W cm(-2)) and decrease with rising temperature in the range 21-50 degrees C. The HNO2 formation rate depends on the type of saturating gas as follows: Ar > N2 > He > air. NO and O2 are the major gaseous products of HNO3 sonication. The NO2 accumulation of in the gas phase is observed only when the decomposition of HNO2 formed becomes noticeable. The gaseous products formation rates depend on the HNO3 concentration, acoustic intensity and the type of saturating gas. The mechanism of HNO2 sonochemical formation is assumed to be the thermal decomposition of HNO3 in the gaseous vicinity of collapsing bubbles or in the overheated liquid reaction zone surrounding the cavitational bubbles.     

Oxygen exchange between NO gas and adsorbed atomic oxygen on Pt(335)

We have used temperature-programmed desorption with isotopically labeled gases to study O exchange between gas phase NO and adsorbed atomic O on Pt(335). We find two distinct types of adsorbed O, one of which exchanges at least 40 times faster than the other, at room temperature. Based on their relative concentrations, we tentatively identify the more active species as O at the step edge and the less active one as O at terrace sites. The temperature dependence of the faster exchange rate implies two parallel reaction pathways. Above 240 K, the exchange rate increases with temperature with an apparent activation energy of 3.8 kcal mol⁻¹. At lower temperatures the exchange rate is nearly temperature-independent, with an apparent activation energy near zero but a very low pre-exponential factor. These results are interpreted in terms of a competition between oxygen exchange and NO desorption. The low-temperature process probably requires special sites or adsorbate configurations. The room temperature exchange rates of O₂ gas with preadsorbed atomic O, and with NO at edge sites, are more than 100 times slower than for NO gas and adsorbed O.