Plasma-catalytic Selective Reduction of NO with C_(2)H_(4)in the Presence of Excess Oxygen

This paper reports observations of significant synergistic effects between dielectric barrier discharge (DBD) plasmas and Cu-ZSM-5 catalysts for C2H4 selective reduction of NOx at 250 °C in the presence of excess oxygen by using a one-stage plasma-over-catalyst (POC) reactor. With the reactant gas mixture of 530 ppm NO, 650 ppm C2H4, 5.8% O2 in N2 and GHSV = 12000 h-1, the pure catalytic, pure plasma-induced (discharges over fused silica pellets) and plasma- catalytic (in the POC reactor) NOx conversion are 39%, 1.5% and 79%, respectively. The in-situ optical emission spectra of the reactive systems imply some short-lived active species formed from plasma-induced and plasma-catalytic processes may be responsible to the observed synergistic effects in this one-stage POC system.

Catalytic Performance of MnO_x-WO_3/TiO_2 Catalyst for Selective Catalytic Reduction of NO_x with NH_3 and Its Tolerance Towards SO_2

The performance of Mn-W/TiO2 for selective catalytic reduction（SCR） of NOx with NH3 and its resistance to different concentrations of SO2 at various temperatures were investigated. The results show that WO3 increased the active sites and enhanced the strength of acid, so it was an effective promoter of MnOJTiO2. The NOx conversion on Mn-W/TiO2 ranges from 80.3% to 99.6% between 100 ℃to 350℃ at GHSV=18900 h 1, while N2 product selectivity changes from 100% to 98.7%. In the presence of 0.01% SO2 and 6% H20, NOx conversion maintained 98.5% at 120℃. The influence of more than 0.01% SO2 on the activity of MnOx-WO3/TiO2 will disappear if the temperature rises above 250℃. By means of heating and sweeping with He, the activity of the catalysts can be recovered. At 300℃, NOx conversion yielded 99% with 0.07% SO2 and reached the level of commercial V-W/TiO2 catalysts. The Mn-W/TiO2 catalyst showed excellent performance for SCR of NOx with NH3 in a wider range of temperature with strong tolerance to SO2.

Research progress in the SO2 resistance of the catalysts for selective catalytic reduction of NOx

The selective catalytic reduction （SCR） of NOx with NH3 has been proven to be an efficient technology for NOx conversion to N2. However, the catalysts used for SCR usually suffer from the problem of sulfur poisoning which seriously limits their practical application. This review summarized sulfur poisoning mechanisms of various SCR deNG catalysts and strategies to reduce deactivation caused by SO2 such as doping metals, controlling the structures and morphologies of the catalysts, and selecting appropriate supports. The methods and procedures of catalysts preparation and the reaction conditions also have effect on SO2-resistance of the catalysts. Several novel catalyst systems that exhibited good SO2 resistance are also introduced. This paper could provide guidance for the development of highly efficient sulfur-tolerant deNOx catalysts.

Cerium-tungsten oxides supported on activated red mud for the selective catalytic reduction of NO_(x)

Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.

Selective catalytic NO_x reduction on Antimony promoted V_2O_5-Sb/TiO_2 catalyst

Quantum chemical calculation was carried out to choose a promoter which can reduce the poisoning of V2O5/TiO2 catalysts by SO2. Several atoms were chosen as candidates and new catalysts were synthesized by impregnation method. The NOx conversion rate was measured at temperatures between 100 and 400 ℃ and poisoning effect was investigated. The most promising candidate promoter, Se, was excluded because of its high vapor pressure. On the other hand, Sb shows best promoting properties. Sb promoted catalyst reaches the maximum NOx conversion rate at 250 ℃. It also shows considerably enhanced resistance to poisoning of V2O5/TiO2 catalysts by SO2.

(La0.8A0.2)MnO3(A=Sr,K) perovskite catalysts for NO and C10H22 oxidation and selective reduction of NO by C(10)H(22)

In this work, we studied the catalytic activity of LaMnO3 and(La0.8A0.2)MnO3(A = Sr, K) perovskite catalysts for oxidation of NO and C10H22 and selective reduction of NO by C10H22. The catalytic per‐formances of these perovskites were compared with that of a 2 wt% Pt/SiO2 catalyst. The La site substitution increased the catalytic properties for NO or C10H22 oxidation compared with the non‐substituted LaMnO3 sample. For the most efficient perovskite catalyst,(La0.8Sr0.2)MnO3, the results showed the presence of two temperature domains for NO adsorption:(1) a domain corre‐sponding to weakly adsorbed NO, desorbing at temperatures lower than 270 °C and(2) a second domain corresponding to NO adsorbed on the surface as nitrate species, desorbing at temperatures higher than 330 °C. For the Sr‐substituted perovskite, the maximum NO2 yield of 80% was observed in the intermediate temperature domain (around 285 °C). In the reactant mixture of NO/C10H22/O2/H2O/He,(La0.8Sr0.2)MnO3 perovskite showed better performance than the 2 wt% Pt/SiO2 catalyst: NO2 yields reaching 50% and 36% at 290 and 370 °C, respectively. This activity improvement was found to be because of atomic scale interactions between the A and B active sites, Sr2+ cation and Mn4+/Mn3+ redox couple. Thus,(La0.8Sr0.2)MnO3 perovskite could be an alternative free noble metal catalyst for exhaust gas after treatment.

Enhancement of Activity of SnO_(2)-doped In_(2)O_(3)/Al_(2)O_(3) Catalyst for NO Reduction with Propene in the Presence of H_(2)O and SO_(2)

The novel bimetallic Sn-Im/Al2O3 catalysts prepared by three methods for NO reduction by propene were investigated. The results showed that the catalytic activity was enhanced significantly in the presence of H2O on sol-gel catalyst, and the maximum NO conversion increased from 46% to 92%, even in the presence of 100 ppm SO2, NO conversion was still 80%.

Effect of TiO_2 surface properties on the SCR activity of NOx emission abatement catalyst

NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and so on, and the effect of TiO\-2 surface properties on the SCR(selective catalytic reduction) activity of V\-2O\-5/TiO\-2 catalysts was studied. It was found that the TiO\-2 surface properties had strong affect on the SCR activity of V\-2O\-5/TiO\-2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.

Effect of Preparation Method on Cu Active Sites and the Reaction Pathway in NO Reduction by NH3 over Cu–SSZ-13

To study the infl uence of the preparation method on Cu active sites and the reaction pathway in NO reduction by NH 3 over Cu-SSZ-13, three kinds of catalysts (Cu ion-exchanged SSZ-13 1 , one-pot synthesis Cu-SSZ-13 2 , and Ce 0.017 -Fe 0.017 /Cu- SSZ-13 [Ce and Fe ion exchange on the basis of Cu-SSZ-13 2 ]) were prepared. In situ diff use refl ectance infrared Fourier transform spectroscopy and H 2 temperature program reduction were used to study the diff erences in the reaction pathways and Cu active sites over the three kinds of catalysts. Density functional theory was employed to study the eff ect of active sites on the reaction pathway. In situ DRIFTS showed that the reaction pathway on Cu-SSZ-13 1 during NO oxidation was diff erent from that on Cu-SSZ-13 2 and Ce 0.017 -Fe 0.017 /Cu-SSZ-13. The diff erence was that intermediate NO 2 was involved in the selective catalytic reduction reaction on Cu-SSZ-13 1 , whereas NO 2 was not found during the reaction process on Cu-SSZ-13 2 and Ce 0.017 -Fe 0.017 /Cu-SSZ-13. H 2 -TPR studies revealed that the three catalysts had diff erent Cu active sites, which were located in the six-membered ring, eight-membered ring, and CHA cage. On the basis of DFT studies, NO and O 2 were more conducive to form nitrate when the Cu species was on the six- and eight-membered rings;by contrast, NO and O 2 were more conducive to form NO 2 in the cage. These results showed that diff erent preparation methods led to various Cu active sites, and varying Cu active sites could lead to diff erent NO oxidation processes.

Control of an Industrial SCR Catalyst Using Ceramic NOx Sensors

Selective Catalytic Reduction (SCR) catalysts respond slowly to transient inputs, which is troublesome when designing ammonia feed controllers. An experimental SCR test apparatus installed on a slipstream of a Coo-per-Bessemer GMV-4, 2-stroke cycle natural gas engine is utilized. Ammonia (NH3) feed rate control algo-rithm development is carried out. Two control algorithms are evaluated: a feed forward control algorithm, using a pre ammonia injection ceramic NOx sensor and a feed forward plus feedback control algorithm, us-ing a pre ammonia injection ceramic NOx sensor and post catalyst ceramic NOx sensor to generate feedback signals. The feed forward algorithm controls to constant user input NH3/NOx molar ratio. The data show the lack of pressure compensation on the ceramic NOx sensors cause errors in feed forward NOx readings, re-sulting in sub optimal ammonia feed. The feedback system minimizes the post catalyst ceramic NOx sensor signal by adjusting the NH3/NOx molar ratio. The NOx sensors respond to ammonia + NOx;therefore, the feed forward plus feedback algorithm minimizes the sum of NOx emissions and ammonia slip. Successful application of the feedback control minimization technique is demonstrated with feedback periods of 15 and 5 minutes with molar ratio step sizes of 5 and 2.5%, respectively.

Characterization of polycyclic aromatic hydrocarbon emissions from diesel engine retrofitted with selective catalytic reduction and continuously regenerating trap

Two after treatment units, selective catalytic reduction （SCR） and continuously regenerating trap （CRT）, were independently retrofitted to a diesel engine, with the objective to investigate their impact on the conversion/reduction （CR） of polycyclic aromatic hydrocarbons （PAHs）. The experiments were conducted under the European steady state cycle （ESC） first without any retrofits to get baseline emissions, and then with SCR and CRT respectively, on the same engine. The particulate matter （PM）-phase PAHs were trapped in fiberglass filters, whereas gas-phase PAHs were collected in cartridges, and then analyzed using a gas chromatograph-mass spectrometer （GC-MS）. Both PM-phase and gas-phase PAHs were greatly reduced with CRT showing respective CR of 90.7% and above 80%, whereas only gas-phase PAHs were abated in the case of SCR, with CR of above 75%. Lower molecular weight （LMW） PAHs were in abundance, while naphthalene exhibited a maximum relative contribution （RC） to LMW-PAHs for all three cases. Further, the CR of naphthalene and anthracene were increased with increasing catalyst temperature of SCR, most likely due to their conversion to solid particles. Moreover, the Benzo[a]Pyrene equivalent （BaPeq） of PAHs was greatly reduced with CRT, owing to substantial reduction of total PAHs.

MOF衍生Co-C/FeOx复合材料的制备及其催化CO_(2)还原性能探究

以MOFs为模板,通过水热合成､高温煅烧制备得到Co-C/FeO_(x)复合材料,在300℃､0.2 MPa条件下探究了其对CO_(2)的催化还原性能。通过调控Co-C和FeO_(x)的质量比探究CO_(2)还原产物的分布,结果表明,当Co-C和FeO_(x)质量比为1∶4时,CO_(2)转化率为28.8%,C2H6和C_(3)H_(8)的选择性提高至28.6%。FeO_(x)的引入促进了中间体CO的生成,Co-C和FeO_(x)两者的结合使CO_(2)还原兼顾了CO_(2)转化率与C^(2+)产物的选择性。该研究不仅为CO_(2)选择性还原为多碳产物提供了一种有效策略,还展示了以MOFs为前驱体合成的碳负载金属/金属氧化物复合材料在催化中的应用潜力。

High Activity SnO_2/Al_2O_3 Catalyst for NO Reduction in the Presence of Oxygen

The novel sol-gel SnO2/Al2O3 catalysts for selective catalytic reduction NO by propene under lean burn condition were investigated. The results showed thatthe maximum NO conversion was 82% on the SnO2/Al2O3 (5%Sn) catalyst, and the presence of H2O and SO2 improved the catalytic activity at low temperature. The catalytic activity of NO2 reduction by propene is much higher than that of NO at the entire temperature range, and the maximum NO2 conversion reached nearly 100% around the temperature 425℃.

高原环境下柴油机NOX排放控制试验研究

柴油机是当前工业及经济发展中不可或缺的动力机械,同时也是NOX排放的主要贡献者。要助力经济高质量发展,内燃机行业新质生产力加速形成,使柴油机更高效绿色,提升SCR转化效率,减少NOX排放是关键。文章利用台架及大气模拟装置,在80kPa、90kPa、100kPa大气压力下进行试验,研究不同海拔下NO与NO2排放特性,以及NO2与NOX的比值对SCR转化效率的影响。研究结果表明:随着转速的升高,NO及NO2排放均下降,海拔越高二者排放越少。NO与NO2排放呈此消彼长的关系,当NO2与NOX的比值增大时,SCR转化效率逐步提高,但当比值大于50%时,SCR转化效率会有明显下降。

Kinetic Study of Co-β-Zeolite for Selective Catalytic Reduction of NO_x with Propane

The effects of grain size,space velocity,temperature and reactant concentration on the kinetics of NOx reduction with propane over Co-β-zeolite catalyst were investigated.The external mass transfer phenomenon was examined by varying the space velocity.The results show that the transfer can be negligible when the space velocity is greater than 60000 h-1 in low temperature range.However,the transfer exists at high temperatures even when the space velocity reaches a high level.Variation of the catalyst grain size from 0.05 to 0.125 mm does not change the conversion rate of NOx.The concentrations of components,NOx,C3H8 and O2,were also investigated to have a better understanding of mechanism.Based on the experimental data,the selectivity formula was proposed.The results shows that lower temperature is helpful to get higher selectivity as the activation energy of hydrocarbon oxidation,Ea,2,is greater than that of NOx reduction,Ea,1,(Ea,2>Ea,1).High NOx concentration and low C3H8 concentration are beneficial to high selectivity.However in order to maintain high activity simultaneously,the temperature and C3H8 concentration should be high enough to promote NOx reduction.10%(Φ) H2O and 75×10-6(Φ) SO2 were introduced into the reaction system,and Co-β-zeolite shows strong resistance to water and SO2.

富氧条件下Co／ZSM-5催化剂对C3H8选择还原NOx的性能

采用多种物理化学手段研究了在模拟的轻型柴油车尾气中不同Co担载量及Cu掺杂的Co/ZSM-5催化剂的Co组分分散状态、可还原性、NO吸附脱附性质对C3H8选择性催化还原NOx性能的影响。结果表明,浸渍法制备的Co/ZSM-5催化剂上既有外表面上的Co3+和Co2+物种,也有孔内的Co2+离子。富氧条件下Co/ZSM-5催化剂上C3H8选择性催化还原NOx的活性主要与ZSM-5载体孔外表面分散的CoOx物种中的钴离子可还原能力和NO吸附脱附性能密切相关。Co/ZSM-5催化剂上适宜的Co担载量约为4.0wt%,低担载量时随Co担载量增加,表面CoOx物种中钴离子可还原能力增强,C3H8选择性催化还原NOx的低温转化活性增加;高担载量时,随Co担载量增加,单位Co离子的NO吸附量的减少以及催化剂表面活性中心数的减少,导致了Co/ZSM-5催化剂NOx的转化率和催化剂比速率(k)的下降。孔外表面Co3O4晶体的存在使催化剂表面产生较强的NO吸附,并在高温时有利于C3H8的氧化燃烧,使C3H8选择性催化还原NOx的活性降低。

V_2O_5-MoO_3/TiO_2催化剂的NOx选择性催化还原及SO_2氧化活性

采用浸渍法以TiO2为载体制备V2O5-MoO3/TiO2选择性催化还原催化剂,研究V2O5和MoO3负载量对于催化剂选择性催化还原反应及SO2氧化活性的影响,并考察氧含量、氨氮物质的量比和反应空速对3%V2O5-6%MoO3/TiO2催化剂选择性催化还原脱硝活性的影响。结果表明,随着催化剂中V2O5负载质量分数增加,V2O5-MoO3/TiO2催化剂的选择性催化还原活性和SO2氧化活性均呈上升趋势。MoO3的负载对催化剂的SO2氧化活性有明显抑制作用。MoO3负载质量分数超过9%,制备的催化剂既保持较高的低温选择性催化还原活性,又使选择性催化还原反应中的SO2转化率小于1%。

低温脱除NOx催化剂的开发

开发了一种以NH3为还原剂、选择性催化还原氮氧化物的负载铜低温催化剂。试验结果表明,活性组分和助催化剂的含量、催化剂的焙烧条件和反应空速对NO的转化率有显著的影响。催化剂具有高活性温域宽、氮氧化物去除率高和压碎强度好等特点。应用试验表明,在废气中NOx为21562mg/m3、NOx+空气为870m3/h,空速为4100h-1、反应温度280℃的条件下,氮氧化物的脱除率达99 6%。

NOx选择催化还原的研究进展

NOx的控制是当今空气污染防治的热点、难点问题 ,而选择催化还原是脱氮的较为有效的方法。

新型碳质催化剂用于NH_3选择性催化还原NOx的研究

以城市污水处理厂剩余污泥为原料制备了一种新型碳质催化剂。通过试验考察了催化剂在NH3选择催化还原NO中的应用效果。结果表明,催化性能较好,最佳的制备和催化反应条件为:锌铁物质的量比1∶0.5,热解温度750℃,反应温度400℃,O2浓度15%。在此条件下,NOx的最大转化率达98.3%。通过考察证明催化剂自身具有一定的还原性能。对催化剂进行了FTIR、TG、SEM和BET分析,结果表明,催化剂具有很丰富的孔结构、活性粒子和表面官能团,比表面积较大,最大可达307 m2.g-1,分析结果显示具有良好的催化条件。