Effect of periodic operation over Pt catalysts in simulated oxidizing exhaust gas

The effect of periodic operation over Pt and Pt/Ba catalysts supported on γ-alumina under oxidizing conditions was investigated using simulated automotive exhaust gas from lean-burn combustion. The conversion of hydrocarbons and NO_x was measured in cycled feedstream and steady feedstream under oxidizing conditions. The activities of the catalysts were improved in the cycled feedstream between oxidizing and reducing atmospheres under average oxidizing conditions. In particular, the NO_x reduction on the Pt/Bt catalyst was higher than that on the Pt catalyst in the cycling operation. From the mass spectral analysis in streams of NOO₂C₃H₆ and NOO₂H₂ (balance He) gas, it was found that NO was oxidized and stored on the Pt/Ba catalyst under oxidizing conditions, and that the stored NO_x on the catalyst was subsequently reduced to N₂ under reducing conditions.     

低温等离子体诱导低碳烃选择性催化还原NOx研究进展

综述了近年来低温等离子体诱导低碳烃选择性催化还原NOx的研究进展,详细介绍了难活化的甲烷及较易活化的非甲烷低碳烃气体如乙烯、丙烯及丙烷等的研究现状,探讨了低温等离子体诱导低碳烃选择性催化还原NOx的反应机理,并展望了低温等离子体诱导低碳烃选择性催化还原NOx今后研究方向。     

降低催化裂化装置再生烟气NO_x排放技术研究进展

综述了催化裂化装置再生烟气中氮氧化物主要减排途径的研究进展,再生器构造设计、再生器下游烟气处理工艺以及氮氧化物减排助剂是目前的主要研究方向,建议今后加大对催化裂化烟气中NO x排放的关注并研发工艺流程简单、技术可靠的脱氮工艺。     

The removal of NOx from a lean exhaust gas using storage and reduction on H3PW12O40·6H2O

NO_x sorption and reduction capacities of 12-tungstophosphoric acid hexahydrate (H₃PW₁₂O₄₀·6H₂O, HPW) were measured under representative alternating conditions of lean and rich exhaust-type gas mixture. Under lean conditions, the sorption of NO_x is large and is equivalent to 37 mg of NO_x/g_HPW. Although a part of these NO_x remains unreduced, HPW is able to reduce some of the NO_x to produce N₂ by a reaction between the sorbed NO₂ and hydrocarbon (HC), but this process is slow. The addition of 1% Pt affects strongly the chemical behaviour occurring during the course of a rich operation. The NO desorption observed at the beginning of the rich phase is strongly accelerated. The direct correlation between NO₂ consumption and CO₂ production shows that the principal pathway is the reaction CO+NO₂→CO₂+NO. In a mixture of reducing gas (CO, HC, H₂), the competition is strongly in favour of CO though in its absence the reaction observed was the hydrogenation of propene to propane.     

涂装废气焚烧炉烟气余热利用的改善

针对某汽车涂装车间使用废气焚烧炉的实际情况,制定了烟气余热利用的改进方案,从节能效益和减排效益两个方面论证了方案的可行性及优越性.     

Oxidation of methane over Pt and Pd supported on alumina in lean-burn natural-gas engine exhaust

Catalytic oxidation of hydrocarbons in lean-burn natural-gas engine exhaust has been studied for Pt and Pd supported on alumina. A Pt–Pd/alumina catalyst exhibited higher and longer-lasting hydrocarbon oxidation activity than Pt–Rh/alumina, Pt/alumina, and Pd/alumina catalysts. Increasing the palladium content in Pt–Pd/alumina catalyst increased the oxidation activity and had more durability. While increasing the platinum content a little bit also improved the activity, adding much more did not. Supporting the platinum on alumina retarded the sintering of Pd and PdO, thus lengthening the oxidation activity of the Pt–Pd/alumina catalyst.     

Selective reduction of nitrogen oxides with hydrocarbons over solid acid catalysts in oxygen-rich atmospheres

Highly selective reduction of nitrogen oxides to dinitrogen occurs to a high level in oxygen-rich atmospheres by using a small amount of propane as a reducing agent over alumina, silica-alumina, titania and zirconia catalyst. Judging from the data of activity and ammonia TPD measurement on a series of silica-alumina catalysts, acidity is suggested to be one of the main factors that determine catalytic activity.     

超重力氧化还原法用于天然气脱硫的探索性研究

报道了用氮气和硫化氢的混合气模拟含硫天然气,在超重机中应用配合铁氧化还原法进行脱硫实验,研究了原料气中硫化氢浓度、原料气中气体流量、脱硫液流量、超重机转子转速和脱硫液pH值对H2S脱除率和气相传质系数的影响,确定了配合铁体系在超重机中适宜的反应条件。结果表明,在本实验条件下H2S脱除率稳定在99.9%左右。实验设备体积小,硫化氢脱除率稳定且高效。     

Effect of Operating Conditions on NOx and CO Emissions in a Pilot‐Scale Vortexing Fluidized‐Bed Combustor with Flue Gas Recirculation

In order to study the effect of flue gas recirculation (FGR) by primary air mixed with FGR or nitrogen on NO_x emissions in a fixed total primary air flow rate, the bed temperature, stoichiometric oxygen ratio in the combustion chamber, and excess oxygen ratio were investigated in a pilot‐scale vortexing fluidized‐bed combustor (VFBC). As a result, the NO_x emissions could effectively be decreased with FGR in the VFBC. The lower NO_x emissions were attributed to the fact that the FGR allows NO_x to enter the reactor again with the chance of being reduced and that the FGR contains more CO₂ to suppress NO_x formation or promote NO_x reduction through its conversion to CO by reaction with char.     

Activity and stability of Ag–alumina for the selective catalytic reduction of NOx with methane in high-content SO2 gas streams

In this work, we investigated the activity and stability of Ag–alumina catalysts for the SCR of NO with methane in gas streams with a high concentration of SO₂, typical of coal-fired power plant flue gases. Ag–alumina catalysts were prepared by coprecipitation–gelation, and dilute nitric-acid solutions were used to remove weakly bound silver species from the surface of the as prepared catalysts after calcination. SO₂ has a severe inhibitory effect, essentially quenching the CH₄-SCR reaction on this type catalysts at temperatures <600 °C. SO₂ adsorbs strongly on the surface forming aluminum and silver sulfates that are not active for CH₄-SCR of NO_x. Above 600 °C, however, the reaction takes place without catalyst deactivation even in the presence of 1000 ppm SO₂. The reaction light-off coincides with the onset of silver sulfate decomposition, indicating the critical role of silver in the reaction mechanism. SO₂ is reversibly adsorbed on silver above 600 °C. While alumina sites remain sulfated, this does not hinder the reaction. Sulfation of alumina only decreases the extent of adsoption of NO_x, but adsorption of NO_x is not the limiting step. Methane activation is the limiting step, hence the presence of sulfur-free Ag–O–Al species is a requirement for the reaction. Strong adsorption of SO₂ on Ag–alumina decreases the rates of the reaction, and increases the activation energies of both the reduction of NO to N₂ and the oxidation of CH₄, the latter more than the former. Our results indicate partial contribution of gas phase reactions to the formation of N₂ above 600 °C. H₂O does not inhibit the reaction at 625 °C, and the effect of co-addition of H₂O and SO₂ is totally reversible.     

Effects of charge temperature and exhaust gas re-circulation on combustion and emission characteristics of an acetylene fuelled HCCI engine

In this work, experiments were conducted on a homogeneous charge compression ignition (HCCI) engine with acetylene as the sole fuel at different power outputs. Initially, the intake air was heated to different temperatures in order to determine the optimum level at every output. Charge temperatures needed were in the range of 40-110 °C from no load to a BMEP (Brake Mean Effective Pressure) of 4 bar. Subsequently, exhaust gas re-circulation (EGR) was done at the identified charge temperatures and brake thermal efficiency was found to improve. At high BMEPs, use of EGR led to knocking. Thus, fine control over charge temperature and EGR quantity is needed at these conditions. Nitric oxide and smoke levels were very low. However, HC levels were high at about 1700-2700 ppm. Brake thermal efficiencies were comparable to or even better than the compression ignition mode of operation.     

Effect of SO2 on the catalytic activity of Ga2O3–Al2O3 for the selective reduction of NO with propene in the presence of oxygen

The effect of coexisting SO₂ on the catalytic activity of Ga₂O₃–Al₂O₃ prepared by impregnation, coprecipitation and sol–gel method for NO reduction by propene in the presence of oxygen was studied. Although the activity of Al₂O₃ and Ga₂O₃–Al₂O₃ prepared by impregnation (Ga₂O₃/Al₂O₃(I)) and coprecipitation (Ga₂O₃–Al₂O₃(CP)) was depressed considerably by the presence of SO₂, NO conversion on Ga₂O₃–Al₂O₃ prepared by sol–gel method (Ga₂O₃–Al₂O₃(S)) was not decreased but increased slightly by SO₂ at temperatures below 723 K. From catalyst characterization, SO₂ treatment was found to cause two important effects on the surface properties: one is the creation of Brønsted acid sites on which propene activation is promoted (positive effect), and the other is the poisoning of NO_x adsorption sites on which NO reduction proceeds (negative effect). It was presumed that the influence of SO₂ treatment on the catalytic activity is strongly related to the balance between the negative and positive. The activity enhancement of Ga₂O₃–Al₂O₃(S) by SO₂ was accounted for by the following consideration: (1) increase of the propene activation ability by SO₂, (2) incomplete inhibition of NO_x adsorption sites by SO₂.