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1.
NH3-SCR performances were explored to the relationship between structure morphology and physio-chemical properties over low-dimensional ternary Mn-based catalysts prepared by one-step synthesis method.Due to its strong oxidation performance,Sn-MnOx was prone to side reactions between NO,NH3 and O2,resulting in the generation of more NO2 and N2 O,here most of N2 O was driven from the non-selective oxidation of NH3,while ...  相似文献   

2.
A series of single-phase T-structured NdSrCu1??xCoxO4?? with oxygen vacancies and T0-structured Sm1:8Ce0:2Cu1??xCoxO4?? (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu1??xCoxO4?? catalysts were of oxygen vacancies whereas the Sm1:8Ce0:2Cu1??xCoxO4?? ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu1??xCoxO4?? decreased while the over-stoichiometric oxygen amount of Sm1:8Ce0:2Cu1??xCoxO4?? increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO3:702 catalyst showing the best e ciency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr??1, and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO3:702 > NdSrCu0:8Co0:2O3:736 > NdSrCu0:6Co0:4O3:789 > Sm1:8Ce0:2Cu0:6Co0:4O4:187 > Sm1:8Ce0:2Cu0:8Co0:2O4:104 > Sm1:8Ce0:2CuO4:045, in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu3+/Cu2+ redox ability of NdSrCu1??xCoxO4?? account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.  相似文献   

3.
The present article studies the effect of CeO2 and Al2O3 on the activity of Pd/Co3O4/cordierite catalyst in conversion of NO, CO, CnHm. The catalysts were characterized by temperature programmed reduction with hydrogen, X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy. It is shown that the effect of CeO2 on the properties of Pd/Co3O4/cordierite catalyst depends on preparation method. The catalyst obtained by co-deposition of cerium and cobalt oxides has higher activity in CO oxidation (CO + O2 and CO + NO) and total hexane oxidation (C6H14 + O2). Such phenomenon is probably caused by more than stoichiometric amount of formed oxygen vacancies, an increase in both mobility of surface oxygen and dispersity of components in the catalytic composition. It is demonstrated that CeO2 addition promotes the SO2 resistance of Pd/Co3O4/cordierite. The second support decreases the activity of Pd/Co3O4/cordierite catalyst in the reactions of CO and C6H14 with oxygen because of CoAl2O4 formation.  相似文献   

4.
氮氧化物(NOx)是造成细颗粒物、近地面臭氧等大气污染问题的重要前体物.随着大气污染治理行动的深入,对工业锅炉/窑炉烟气排放的NOx进行控制十分重要.采用不同方法制备了一系列Co_3O_4催化剂,考察了不同制备方法对CO选择性催化还原NO(CO-SCR)反应活性的影响,通过BET、XRD、Raman、HR-TEM和SEM等技术对该系列催化剂进行了表征.活性测试表明,以硫酸钴为前驱体用固态研磨法制备的Co_3O_4-S催化剂具有更优异的CO-SCR反应活性,且表现出较好的抗水蒸气性能,以醋酸钴为前驱体用固态研磨法制备的Co_3O_4-C催化剂显示出较好的抗水性能. NO氧化结果显示,催化剂的NO氧化效果越好,CO-SCR活性也越好. Raman表征结果显示,Co_3O_4-S表面可能含有更多的Co2+离子,从而有利于形成氧空位. H2-TPR结果表明,Co_3O_4-S催化剂的氧化还原性较好. HR-TEM表征发现Co_3O_4-S和Co_3O_4-O主要暴露(111)和(220)晶面,而更多(220)晶面的暴露可能更有利于反应的进行.  相似文献   

5.
垄作覆膜条件下田间氨挥发及影响因素   总被引:12,自引:4,他引:8  
通过大田试验,采用密闭法研究了垄沟覆膜栽培条件下冬小麦生育期内土壤氨挥发动态过程及相关土壤理化性质.结果表明,生育期内垄沟覆膜处理氨挥发累积量(以N计)为(1.66±0.3)~(3.28±0.51)kg.hm-2,常规栽培为(4.68±0.35)kg.hm-2,垄作栽培比常规栽培减少了29.8%~63.8%,氮肥损失率从常规栽培的1.9%下降到了0.3%~0.8%.小麦生育期内土壤氨挥发速率先升后降,冬前高、冬后低.常规栽培土壤氨挥发主要发生在越冬前,其挥发量占总挥发量的82%;而垄作栽培的越冬前挥发量只占挥发总量的49%~61%.越冬前常规栽培土壤氨挥发速率受土壤铵态氮浓度和土壤含水量的共同影响;而垄作条件下土壤氨挥发主要受土壤铵态氮浓度影响,地表温度和土壤含水量通过土壤铵态氮间接影响氨挥发.返青后2种栽培模式下的氨挥发主要受土壤铵态氮浓度的影响.常规栽培和垄沟覆膜高施氮量条件下土壤氨挥发累积量动态过程符合对数函数;而不施肥和垄沟覆膜低施氮量条件下的动态过程可以用线性函数表示.垄沟覆膜栽培在一定程度上改变了土壤氨挥发机制和过程,显著降低土壤氨挥发和氮肥损失.  相似文献   

6.
A series of cobalt doped TiO_2(Co-TiO_2) and Co Oxloaded TiO_2(Co/TiO_2) catalysts prepared by sol–gel and impregnation methods respectively were investigated on selective catalytic reduction with NH_3(NH_3-SCR) of NO. It was found that Co-TiO_2 catalyst showed more preferable catalytic activity at low temperature range. From characterization results of XRD,TEM, Raman and FT-IR, Co species were proved to be doped into TiO_2 lattice by replaced Ti atoms. After being characterized and analyzed by NH_3-TPD, PL, XPS, EPR and DRIFTS, it was found that the better NH_3-SCR activities of Co-TiO_2 catalysts, compared with Co/TiO_2 catalyst, were ascribed to the formation of more oxygen vacancies which further promoted the production of more superoxide ions(O-2). The superoxide ions were crucial for the formation of low temperature SCR reaction intermediates(NO-3) by reacting with adsorbed NO molecule. Therefore, these aspects were responsible for the higher low temperature NH_3-SCR activity of Co-TiO_2 catalysts.  相似文献   

7.
Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.  相似文献   

8.
CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.  相似文献   

9.
Co3O4-SnO2 hybrid oxides were prepared by the coprecipitation method and were used to oxidate methane (CH4) in presence of oxygen. The Co3O4-SnO2 with a molar ratio of Co/(Co + Sn) at 0.75 exhibited the highest catalytic activity among all the Co3O4-SnO2 hybrid oxides. Experimental results showed that the catalysts were considerably stable in the CH4 combustion reaction, and were verified by X-ray photoelectron spectra (XPS). It was found that Co3O4 was the active species, and SnO2 acted as a support or a promoting component in the Co3O4-SnO2 hybrid oxides. The surface area was not a major factor that affected catalytic activity. The hydrogen temperatureprogrammed reduction (H2-TPR) results demonstrated that the interaction between cobalt and tin oxides accelerated the mobility of oxygen species of Co3O4-SnO2, leading to higher catalytic activity.  相似文献   

10.
Series of Fe/Cu-SSZ-13 catalysts with different Fe loading content were synthesized by simple one-pot strategy. The obtained catalysts were subjected to selective catalytic reduction (SCR) of NOx with NH3 and were characterized by various techniques. The results show that Fe0.63/Cu1.50-SSZ-13 catalyst with proper Fe content exhibits excellent catalytic activity with widest operation temperature window from 160 to 580°C, excellent hydrothermal stability as well as good resistance to sulfur poisoning when compared with Cu-SSZ-13, signifying its great potential for practical applications. Further characterizations reveal that the synthesized Fe/Cu-SSZ-13 catalysts present typical chabazite (CHA) structure with good crystallinity, while isolated Cu2+ and monomeric Fe3+ are revealed as the predominant copper and iron species. At low temperatures, isolated Cu2+ species act as primary active sites for SCR reaction, while monomeric Fe3+ species provide sufficient active sites for sustain the SCR activity at high temperature. Moreover, Fe over doping would lead to the damage of zeolite structure, destruction of isolated Cu2+ site, as well as the formation of highly oxidizing Fe2O3, thus causing deterioration of catalytic performances.  相似文献   

11.
用氧吸收速率(OUR)表征活性污泥硝化活性的研究   总被引:52,自引:7,他引:52  
研究了用氧吸收速率(OxygenUptakeRate,简称OUR)表征活性污泥硝化活性的方法.利用生物抑制剂丙烯基硫脲(alylthiourea,简称ATU)和氯酸钠(NaClO3)可以选择性地抑制亚硝酸细菌和硝酸细菌的活性.通过测量不同时间的OUR,可以分别计算出污泥的亚硝化活性和硝化活性.结果表明:该方法的测量结果与实际反应器中的硝化反应情况相当一致.该方法简单易行,快速方便,适用于硝化系统中硝化活性的测量.  相似文献   

12.
斯林林  周静杰  吴良欢  胡兆平 《环境科学》2018,39(12):5383-5390
在太湖流域,通过田间试验研究了控释肥(CRF)、生物炭配施控释肥(BC+CRF)、生物炭配施稳定性肥(BC+SF)、生物炭配施控释肥和稳定性肥(BC+CRF+SF)4种施肥处理对稻田田面水p H、氮素动态变化、氮素径流流失的影响.结果表明,田面水平均p H介于5.64~8.15,生物炭配施控释肥和稳定性肥田面水p H降低3.16%~4.48%.田面水平均全氮(TN)质量浓度介于19.05~25.23 mg·L~(-1),生物炭配施控释肥和稳定性肥田面水TN质量浓度显著降低4.75%~6.58%.田面水无机氮素以铵态氮(NH_4~+-N)为主,NH_4~+-N和硝态氮(NO_3~--N)平均质量浓度分别介于0.01~17.26 mg·L~(-1)和0.24~3.11mg·L~(-1).与单施控释肥相比,各处理田面水NH_4~+-N和NO_3~--N质量浓度分别显著降低35.89%~48.78%和20.54%~37.01%.生物炭配施稳定性肥显著降低了田面水NH_4~+-N和NO_3~--N质量浓度,有效减少无机氮素径流流失风险.TN、NH_4~+-N、NO_3~--N径流流失量分别介于16.24~18.09、1.76~2.22、0.76~1.38 kg·hm~(-2).与单施控释肥相比,各处理TN、NH_4~+-N、NO_3~--N径流流失均有不同程度削减.生物炭配施控释肥和稳定性肥显著削减了氮素径流流失,有效降低区域稻田氮素面源污染风险.  相似文献   

13.
不同SAPO分子筛负载MnOx催化剂的低温NH3-SCR性能研究   总被引:1,自引:1,他引:0  
以磷酸硅铝分子筛SAPO-5、SAPO~(-1)1和SAPO-34为载体,采用乙醇分散法制备了用于低温氨选择性还原(NH_3-SCR)NO_x的分子筛负载MnO_x催化剂.活性测试结果显示,3种分子筛催化剂均展现出优良的NH_3-SCR活性,但三者在低温区间的SCR活性存在较明显差异,其SCR活性顺序如下:MnO_x/SAPO-34MnO_x/SAPO-5MnO_x/SAPO~(-1)1.借助XRD、N2吸附-脱附、XPS、H2-TPR、NH_3-TPD、NH_3FT-IR等技术对催化剂的表面活性物种及表面酸性等进行表征分析,结果表明,MnO_x主要以无定型状态分散于载体上,负载后载体的比表面积和孔体积均有所下降.XPS和H2-TPR分析证实,不同分子筛载体上MnO_x的表面浓度与氧化态明显不同.NH_3-TPD和NH_3FT-IR分析揭示了催化剂表面均存在Bronsted酸位和Lewis酸位,其中,Lewis酸性位对低温SCR反应起着关键作用.研究表明,催化剂的催化性能会因载体不同而存在差异,高Mn4+表面浓度和丰富的Lewis酸性位对催化剂在低温区间实现优良的催化活性尤为重要.  相似文献   

14.
Catalytic ozonation is progressively becoming an attractive technique for quick water purification but efficient and stable catalysts remains elusive. Here we solvothermally synthesized highly-dispersed Co3O4 nanocrystals over microscale nitrogen-doping graphene (NG) nanosheets and tested it as a synthetic catalyst in the ozonation of phenol in aqueous solutions. Transmission electron microscopy, powder X-ray diffraction, Fourier transform infrared spectra and X-ray photoelectron spectroscopy were used to determine its morphology, crystallinity, elemental composition and molecular bonds, respectively. The comparative experiments confirmed the highest catalytic activity and oxidation degree (AOSC) of Co3O4/NG among four nanocomposites (G, NG, Co3O4/G, and Co3O4/NG). Co3O4/NG also has exhibited the highest degradation rate: complete conversion of a near-saturated concentration of phenol (941.1 mg/L) was achieved within 30 min under ambient conditions with only a small dosage of Co3O4/NG (50 mg/L) and ozone (4 mg/L, flow rate: 0.5 L/min). It also resulted in 34.6% chemical oxygen demand (CODCr) and 24.2% total organic carbon (TOC) reduction. In this work, graphene nanosheets not only functioned as a support for Co3O4 nanocrystals but also functioned as a co-catalyst for the enhancement in phenol removal efficiency. The surface nitridation and Co3O4 modification treatment further improved the removal rate of the phenol pollutants and brought in the higher oxidation degree. Our finding may open new perspectives for pursuing exceptional activity for catalytic ozonation reaction.  相似文献   

15.
OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using MnSO4 (OMS-2-SO4) and Mn(CH3COO)2 (OMS-2-AC) as precursors. SO42 −-doped OMS-2-AC catalysts with different SO42 − concentrations were prepared next by adding (NH4)2SO4 solution into OMS-2-AC samples to investigate the effect of the anion SO42 − on the OMS-2-AC catalyst. All catalysts were then tested for the catalytic oxidation of ethanol. The OMS-2-SO4 catalyst synthesized demonstrated much better activity than OMS-2-AC. The SO42 − doping greatly influenced the activity of the OMS-2-AC catalyst, with a dramatic promotion of activity for suitable concentration of SO42 − (SO4/catalyst = 0.5% W/W). The samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma optical emission spectroscopy (ICP-OES), NH3-TPD and H2-TPR techniques. The results showed that the presence of a suitable amount of SO42 − species in the OMS-2-AC catalyst could decrease the Mn–O bond strength and also enhance the lattice oxygen and acid site concentrations, which then effectively promoted the catalytic activity of OMS-2-AC toward ethanol oxidation. Thus it was confirmed that the better catalytic performance of OMS-2-SO4 compared to OMS-2-AC is due to the presence of some residual SO42 − species in OMS-2-SO4 samples.  相似文献   

16.
The plant can be a source or a sink of ammonia (NH3) depending on its nitrogen (N) supply, metabolism and on the background atmospheric concentrations. Thus plants play a major role in regulating atmospheric NH3 concentrations. For a better understanding of the factors influencing the NH3 stomatal compensation point, it is important to analyse the dynamics of leaf NH3 fluxes. The relationship between the leaf NH3 fluxes and the leaf apoplast ammonium and nitrate concentrations, N nutrition and the light and dark periods was studied here.We designed an experiment to quantitatively assess leaf-atmosphere NH3 exchange and the stomatal compensation point and to identify the main factors affecting the variation of NH3 fluxes in oilseed rape. We tested day and night dynamics as well as the effect of five different N treatments. Two experimental methods were used: a dynamic open flux chamber and extraction of the apoplastic solution.Chamber measurements showed that there was a good correlation between plant NH3 fluxes and water fluxes. Compensation points were calculated by two different methods and ranged between 0.8 and 12.2 μg m−3 NH3 (at 20 °C) for the different N treatments. Apoplastic solution measurements showed that there was no significant differences in the apoplastic NH4+ concentrations ([NH4+]apo) extracted in dark and light periods for the same N treatment. Statistical analysis also showed that [NH4+]apo was correlated with [NH4+] in the nutrient solution and weakly correlated with [NO3]. Apoplast NH4+ concentrations ranged between 0.1 and 2.1 mM, bulk tissue NH4+ concentrations between 3.9 and 6.6 mM and xylem concentrations between 2.4 and 6.1 mM depending on the N supply.Calculated NH3 emission potential from the extraction measurements were over-estimated when compared with the value calculated from chamber measurements. Errors related to chamber measurements included separation of the cuticular and stomatal fluxes and the calculation of total resistance to NH3 exchange. Errors related to the extraction measurements included assessing the amount of cytoplasmic contamination. We do not have another method to assess the NH3 stomatal compensation point and the choice between these two measurement techniques should depend on the scales to which the measurements apply and the processes to be studied.  相似文献   

17.
Energy-saving and efficient monolithic catalysts are hotspots of catalytic purification of industrial gaseous pollutants. Here, we have developed an electrothermal catalytic mode, in which the ignition temperature required for the reaction is provided by Joule heat generated when the current flows through the catalyst. In this paper, Mn/NiAl/NF, Mn/NiFe/NF and Mn/NF metal-based monolithic catalysts were prepared using nickel foam (NF) as the carrier for thermal and electrothermal catalysis of n-heptane. The results indicated that Mn-based monolithic catalysts exhibit high activity in thermal and electrothermal catalysis. Mn/NiFe/NF achieve conversion of n-heptane more than 99% in electrothermal catalysis under a direct-current (DC) power of 6 W, and energy-saving is 54% compared with thermal catalysis. In addition, the results indicated that the introduction of NiAl (or NiFe) greatly enhanced the catalytic activity of Mn/NF, which attributed to the higher specific surface area, Mn3+/Mn4+, Ni3+/Ni2+, adsorbed oxygen species (Oads)/lattice oxygen species (Olatt), redox performance of the catalyst. Electrothermal catalytic activity was significantly higher than thermal catalytic activity before complete conversion, which may be related to electronic effects. Besides, Mn/NiFe/NF has good cyclic and long-term stability in electrothermal catalysis. This paper provided a theoretical basis for applying electrothermal catalysis in the field of VOCs elimination.  相似文献   

18.
Elevated atmospheric NH3 levels near intensive livestock operations can add significant N to local agroecosystems. In this study, the potential atmospheric NH3 sorbed by soil and water was assessed over a 2-year period starting October 2000 in an intensive livestock production area in southern Alberta, Canada. Fifty-two uneven grid sampling sites were selected in the 53,905 ha study area. The sorption rate of atmospheric NH3 was estimated weekly by exposing distilled water and air-dried soil samples to the atmosphere at the sampling sites. The increases in NH4–N content in the samples after 1-week exposure was regarded as an index of the atmospheric NH3 sorbed for that week. The NH3 sorption rates were highly variable across the 52 sites, with water ranging from 4 to 125 kg ha−1 year−1 with a mean of 22 kg N ha−1 year−1 and soil from 5 to 84 kg N ha−1 year−1 with a mean of 20 kg N ha−1 year−1. Considerable variation in NH3–N sorption across the study area reflects the effects of size, direction (upwind or downwind) and proximity of nearby livestock operations or other NH3 sources and operators’ activities around the sampling sites. The NH3 sorption rate at each site also varied considerably in response to weather conditions. The high rate of NH3 input poses a direct risk of surface water eutrophication in intensive livestock operation areas. If fertilizer recommendations are not reduced to account for NH3 sorption by soil, excess N may also contribute to eutrophication through runoff and leaching.  相似文献   

19.
环流曝气塔中生物脱氮过程的研究   总被引:3,自引:0,他引:3  
利用环流曝气塔进行同时硝化/反硝化(sND)脱氮实验.实验中,分别采用不同降解性能的碳源以及采用不同的碳源投加方式,研究反应器内的脱氮过程,监测处理过程中NOx--N浓度和溶解氧DO的变化.实验显示,在COD 800mg/L+800mg/L的分批加料方式下,NH4+-N的降解得到加强,出水中NH4+-N浓度低于3mg/L;利用较难降解物质作为碳源时,利于反应器内低溶解氧条件的出现,促进了反硝化的进行,实验在采用醇类碳源时脱氮效果好于葡萄糖的情况.  相似文献   

20.
Atmospheric dry deposition to branches of Pinus contorta and P. albicaulis was measured during summer 1987 in a sub-alpine zone at Eastern Brook Lake Watershed (EBLW), eastern Sierra Nevada, California. Results are presented as deposition fluxes of NO3, SO42−, PO43−, Cl, F, NH4+, Ca2+, Mg2+, Na+, K+, Zn2+, Fe3+, Mn2+, Pb2+ and H+, and compared with other locations in California and elsewhere. Deposition fluxes of anions and cations to the pine branches were low, several times lower than the values determined near the Emerald Lake Watershed (ELW), another sub-alpine location in the western Sierra Nevada. The sums of deposition fluxes of the measured cations and anions to pine surfaces were similar, in contrast to the ELW location where the sums of cation fluxes were much higher than the sums of anion fluxes. A strong positive correlation between depositions of NO3 and NH4+, as well as SO42− and Ca2+, suggested that large portions of these ions might have originated from particulate NH4NO3 and CaSO4 deposited on pine surfaces. An estimated total N dry deposition (surface deposition of NO3 and NH4+ and internal uptake of NO2 and HNO3) to the forested area of the EBLW was 29.54 eq ha−1 yr (about 414 g H ha−1 yr−1).  相似文献   

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