SHS方法制备的锰铁系NH3-SCR催化剂的性能研究和机理分析

为提高传统选择性催化还原(SCR)催化剂低温窗口的NO去除效率,运用自蔓延高温合成法(Self-Propagating High-temperature Synthesis)制备了一系列低温锰铁系催化剂.对其在SCR法去除NO中的反应性能进行评价,分析了活性组分和液相点燃温度的影响;利用X射线衍射仪(XRD)对催化剂晶...     

外部燃料重整掺氢对天然气发动机性能的影响

利用外部燃料重整系统对天然气燃料进行了重整反应,燃料重整率为12％,将反应后的重整气体通入进气管内与新鲜空气混合,再通入气缸内燃烧,以此来比较外部燃料重整掺氢燃烧对天然气发动机性能的影响.试验结果显示:结合外部燃料重整掺氢燃烧,发动机的循环变动明显改善,燃烧持续期缩短,相同工况下的燃料消耗率变化很小;THC排放量在各工况下明显减少,50％扭矩负荷率下相对减少量达到22％;NOx排放量也有所减少,特别是在低扭矩负荷率下,相对减少量达到15％;由于重整气体本身含有一定量的CO,再加上H2的还原作用,导致CO的排放量出现了不同程度的上升.     

Catalytic Combustion of Lean Methane Assisted by Electric Field over Pd/Co<Subscript>3</Subscript>O<Subscript>4</Subscript> Catalysts at Low Temperature

A series of Pd/Co₃O₄ catalysts were prepared by Self-Propagating High-Temperature Synthesis (SHS) method in this study, and electric field was applied for catalytic combustion of lean methane over Pd/Co₃O₄ catalysts at low temperature. When electric field was applied, the catalytic combustion performance of Pd/Co₃O₄ catalysts was greatly improved, and the application of electric field could reduce the load of active element Pd to some extent while maintaining the same efficiency. Based on experimental tests and the analysis results of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H₂-temperature-programmed reduction (H₂-TPR) and in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS), the mechanism of catalytic oxidation of CH₄ over Pd/Co₃O₄ catalysts in electric field was proposed. The catalytic combustion of CH₄ occurs only when the temperature is higher than 250 °C normally, but when electric field was applied, the whole process of CH₄ oxidation was promoted significantly and the reaction temperature was reduced. Electric field could promote the reduction of the support Co₃O₄ to release the lattice oxygen, resulting in the increase of PdO_x and the surface chemisorbed oxygen, which could provide more active sites for the low-temperature oxidation of CH₄. Furthermore, electric field could accelerate the dehydroxylation of CoOOH to further enhance the activity of the catalysts.     

掺混甲烷对乙烯层流预混火焰炭烟形貌的影响

针对掺混甲烷的乙烯层流火焰中的炭烟颗粒从形貌角度进行了研究,构建了具有相同当量比(2.07)、火焰温度、气体流速的层流预混乙烯火焰和掺混甲烷的乙烯火焰,并各自选取了3个高度进行热泳探针取样,采用TEM和AFM方法对各个工况的炭烟颗粒粒径分布、平均粒径、平均体积当量球径进行了对比。发现少量的甲烷掺混会令乙烯火焰中炭烟颗粒的尺寸变大,而当甲烷掺混量变多时该现象消失。而通过对颗粒的圆度、球度和分形维数计算和分析,发现即使是很小的颗粒也具有相似的不规则形状,这一现象广泛存在于各种火焰和各种大小的颗粒中,不受掺混比的影响,并且越大的颗粒结构越松散。     

自蔓延燃烧法制备Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy催化剂催化NO制NH3反应的性能研究

被动式氨SCR系统是一种应用在稀燃发动机,可减少NOx排放,生产SCR用氨的后处理方法,该系统使用NO与H2作为原料气在催化剂的作用下产生氨气用于后续SCR脱硝.通过试验研究,采用自蔓延燃烧合成(SHS)法合成了Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy(x=0,0.1,0.2,0.4)催化剂.用XRD、BET、Raman、H2-TPR、XPS、原位表征等方法研究了它们的催化活性.建立了Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy(x=0,0.1,0.2,0.4)催化剂的反应性与物种组成、酸性质和氧化还原性能的关系.结果表明,适量的铜掺杂可以形成更多的酸性位点,调节表面元素的价态分布,有助于产生更高的催化效率.其中,Pd0.01Cu0.1Ce0.45Zr0.45Ox的氨转化率最高,反应温度窗口较宽(225～375℃),NO向NH3转化率大于90％.这是由于高度分散的CuO增强了CuO与Ce0.5Zr0.5O2载体之间的相互作用,从而提高了催化活性.     

溶液燃烧法制备TiV_(0.1)Mn_(0.1)Er_(0.01)O_x催化剂催化还原NO_x的性能研究

为了拓宽选择性催化还原NO_x钒基催化剂的活性温度窗口,采用溶液燃烧合成法制备了TiV_(0.1)O_x催化剂,依次加入Mn元素与Er元素形成新的催化剂,分别对它们进行了SCR活性及选择性测试,发现负载Mn元素可以提高钒基催化剂的低温活性,同时也会降低钒基催化剂的高温活性,负载适量的Er元素可以提高钒基催化剂的高温活性和N_2选择性。利用N2吸附脱附法进行BET比表面积和孔容孔径分析,发现负载Er元素增大了比表面积,进而提升了催化剂活性。利用X射线衍射(XRD)图谱进行晶体结构分析,所有催化剂样品均没有发现VO_x,MnO_x或ErO_x的衍射峰,说明溶液燃烧法制备的催化剂活性组分在TiO2颗粒上呈无定型态分布,分散度高。最终优选出最佳Mn和Er比例的TiV_(0.1)Mn_(0.1)Er_(0.01)O_x催化剂,在160~470℃之间保持80%以上的NO_x去除率。     

Study on Oxidation Activity of CuCeZrO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> Doped with K for Diesel Engine Particles in NO/O<Subscript>2</Subscript>

CuCeZrO_x and KCuCeZrO_x catalysts were synthesized and coated on the blank diesel particulate filter (DPF) substrate and a particulate matter (PM) loading apparatus was used for soot loading. The catalytic performances of soot oxidation were evaluated by temperature programmed combustion (TPC) test and characterization tests were conducted to investigate the physicochemical properties of the catalysts. The reaction mechanism in the oxidation process was analyzed with diffuse reflectance infrared Fourier transform spectroscopy. The results demonstrated that CuCeZrO_x catalyst exhibited high activities of soot oxidation at low temperature and the best results have been attained with Cu_0.9Ce_0.05Zr_0.05O_x over which the maximum soot oxidation rate decreased to 410 °C. Characterization tests have shown that catalysts containing 90% Cu have uniformly distributed grains and small particle sizes, which provide excellent oxidation activity by providing more active sites and forming a good bond between the catalyst and the soot. The low-temperature oxidation activity of soot could be further optimized due to the excellent elevated NO’s conversion rate by partially substituting Cu with K. The maximum particle oxidation rate can be easily realized at such a low temperature as 347°C.     

NH_3—SCR法降低柴油机NO_x排放的研究进展

分析了降低柴油机NOx排放的NH3—SCR选择性催化还原技术的化学反应机理,阐述了该后处理技术结合优化缸内燃烧在提高柴油机燃油经济性的同时大幅度降低NOx和PM排放等方面的优势,并详细介绍了国内外车用柴油机NH3—SCR技术的机理研究进展及应用研究情况。     

一氧化氮在低温等离子体中的氧化试验研究

采用低温等离子体反应技术将部分NO预氧化成NO2,研究了放电电压、气体成分对等离子体氧化NO性能的影响。研究发现,O2和碳氢的存在能显著提高等离子体中NO的氧化效率,且NO2的生成量随加入的O2和碳氢浓度升高而增加。同时也发现,O2和碳氢对NO预氧化的促进作用存在一定的理想范围。     

SCR 反应物理化学过程模型及验证

针对柴油机选择性催化还原（SCR）脱硝技术,建立了零维 SCR 反应器数学模型,并利用 VC ＋＋编写了仿真计算软件。通过小样台架试验测试了钒基催化剂在不同温度、空速、含氧量、NO2与 NO x 的摩尔比以及氨氮比条件下的 NO x 转化率,并与计算结果进行对比。结果表明,模型计算值与试验结果具有很好的一致性,低温条件下,空速越低,NO2与 NO x 的摩尔比越大,NO x 的转化率越高。