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《环境科学学报(英文版)》2023,35(4):459-469
A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co3O4 phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O2-TPD), temperature-programmed reduction of hydrogen (H2-TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH3/CO2-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co2+, lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T50 and T90 (the temperature at which the CH4 conversion rate was 50% and 90%, respectively) were 318 and 367°C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites. 相似文献
13.
采用聚合羟基复合阳离子合成交联黏土A1-Ce-PILC,经SO4^2-改性后,以浸渍法制备了铜基交联黏土催化剂Cu/A1-Ce-PILC,并将其应用于C3H6选择性催化还原NO的反应,350℃时NO转化率达到最大值56%,700℃时下降至22%.为探究催化剂高温失活的原因,采用XPS、TPR、TGA、Py-IR和DSC对反应前后催化剂的物化性能进行了表征.结果表明,经过H2预处理活化后活性组分Cu物种以Cu^+形式存在,而高温反应后Cu物种除以Cu^+和Cu^2+ 2种形式存在外,还出现了少量CuO物种;高温反应过程中A1-Ce-PILC上结构羟基和SO4^2-流失导致催化剂表面酸性减弱;此外,还存在表面积炭覆盖了部分活性中心并堵塞了催化剂孔道的现象.这三者的共同影响促进了C3H6深度氧化,抑制了NO还原,从而导致催化剂的失活. 相似文献
14.
利用多年的环境监测数据,分析南昌市环境空气中主要污染物尘类、二氧化硫和氮氧化物产生的原因,并提出有效控制上述污染物的具体措施。 相似文献
15.
In this study, in order to research the synergistic inhibition effect of nitrogen and ultrafine water mist on gas explosion in a vented duct, a semi-confined transparent chamber was designed with the size of 120 × 120 × 840 mm, and the experiments were carried out with stoichiometric methane/air premixed mixture (fraction of methane: 9.5%), adding different fractions of nitrogen and ultrafine water mist. The experimental results showed the following: The combination of nitrogen and ultrafine water mist had a synergistic inhibiting effect on methane/air explosion, which was preferable to the single use of any kind. With the increase of spraying time of water mist and fraction of nitrogen, the initial shape of the explosion flame became snakelike, and at the same time the peak flame propagation speed and peak overpressure decreased significantly. When the nitrogen fraction was increased to 10% and the mist spraying time was increased to 2min, synergistic inhibiting effect on overpressure was high efficient. However, with the increase of spraying time of water mist and fraction of nitrogen going on, the amount of increase of explosion inhibition efficiency was gradually reduced. 相似文献
16.
Liang Lu Yuqi Jin Hongmei Liu Xiaojun Ma Kunio Yoshikawa 《Waste management (New York, N.Y.)》2014,34(1):79-85
Nitrogen evolution was studied during the co-combustion of hydrothermally treated municipal solid wastes (HT MSW) and coal in a bubbling fluidized bed (BFB). HT MSW blending ratios as 10%, 20% and 30% (wt.%) were selected and tested at 700, 800, 900 °C. Emissions of NO and N2O from blends were measured and compared with the results of mono-combustion trials. Moreover, concentrations of precursors like NH3 and HCN were also quantified. The results are summarized as follows: NO emissions were predominant in all the cases, which rose with increasing temperature. The blending of HT MSW contributed to the NO reduction. N2O emissions decreased with temperature rising and the blending of HT MSW also presented positive effects. At 30% HT MSW addition, both NO and N2O emissions showed the lowest values (391.85 ppm and 55.33 ppm, respectively at 900 °C). For the precursors, more HCN was detected than NH3 and both played important roles on the gas side nitrogen evolution. 相似文献
17.
Zhi-Long Ye Xiaoqing Xie Lanhua Dai Ziwen Wang Wenhua Wu Fuyi Zhao Xiaoming Xie Shiqing Huang Meiling Liu Shaohua Chen 《Waste management (New York, N.Y.)》2014,34(11):2305-2311
Fresh leachate, generated in municipal solid waste incineration (MSWI) plants, contains various pollutants with extremely high strength organics, which usually requires expensive and complex treatment processes. This study investigated the feasibility of blending treatment of MSWI leachate with municipal wastewater. Fresh MSWI leachate was pretreated by coagulation–flocculation with FeCl3 2 g/L and CaO 25 g/L, plate-and-frame filter press, followed by ammonia stripping at pH above 12. After that, blending treatment was carried out in a full-scale municipal wastewater treatment plant (WWTP) for approximately 3 months. Different operational modes consisting of different pretreated leachate and methanol addition levels were tested, and their performances were evaluated. Results showed that throughout the experimental period, monitored parameters in the WWTP effluent, including COD (<60 mg/L), BOD5 (<20 mg/L), ammonium (<8 mg/L), phosphorus (<1.5 mg/L) and heavy metals, generally complied with the Chinese sewage discharged standard. Under the experimental conditions, a certain amount of methanol was needed to fulfill TN removal. An estimation of the operation cost revealed that the expenditure of blending treatment was much lower than the total costs of respective treatment of MSWI leachate and municipal wastewater. The outcomes indicated that blending treatment could not only improve the treatability of the MSWI leachate, but also reduce the treatment cost of the two different wastewaters. 相似文献
18.
Gene E. Likens 《Ambio》2021,50(2):278
Early studies published in Ambio showed large-scale acidification of lakes in southern Sweden and Norway from acid rain. These studies were important for delimiting various scientific issues and thus for eventually contributing to legislation, which reduced emissions of sulfur dioxide and nitrogen oxides and helped to mitigate this major environmental problem. Long-term studies and monitoring in Sweden and Norway and at Hubbard Brook Experimental Forest in New Hampshire helped guide this legislation in Europe and in the USA. 相似文献
19.
Dense blooms of diazotrophic filamentous cyanobacteria are formed every summer in the Baltic Sea. We estimated their contribution to nitrogen fixation by combining two decades of cyanobacterial biovolume monitoring data with recently measured genera-specific nitrogen fixation rates. In the Bothnian Sea, estimated nitrogen fixation rates were 80 kt N year−1, which has doubled during recent decades and now exceeds external loading from rivers and atmospheric deposition of 69 kt year−1. The estimated contribution to the Baltic Proper was 399 kt N year−1, which agrees well with previous estimates using other approaches and is greater than the external input of 374 kt N year−1. Our approach can potentially be applied to continuously estimate nitrogen loads via nitrogen fixation. Those estimates are crucial for ecosystem adaptive management since internal nitrogen loading may counteract the positive effects of decreased external nutrient loading. 相似文献
20.
为揭示不同金属氧化物对湖泊沉积物DOM(溶解性有机质)影响机制,通过室内模拟试验,在沉积物表层分别覆盖Fe、Al、Mn氧化物及湖沙后培养1 a,并利用三维荧光和紫外光谱方法进行表征.结果表明:① 覆盖Al、Fe、Mn氧化物和湖沙主要降低了0~3 cm沉积物的w(DOC),降幅分别为8.61%、6.27%、22.38%和0.44%. ② 沉积物中DOM的类络氨酸峰(peak B1)和类色氨酸峰(peak T2)均产生较大变化.其中三种氧化物均显著降低了上层沉积物中DOM的peak T2,使底层DOM的peakT2显著增加. Mn氧化物使DOM的peak B1降低,Fe和Al氧化物使DOM的peak B1增加,湖沙则使两类峰均降低. ③ 覆盖金属氧化物改变了沉积物DOM结构特征,其中覆盖Fe氧化物增强了其芳香性,而覆盖Mn氧化物和Al氧化却降低其芳香性,但三者均使DOM腐质化程度及官能团数量增加,并使FI(Fluorescence Index,荧光指数)增大,表明DOM向生物源转化.研究显示,沉积物表层覆盖金属氧化物影响了沉积物中DOM迁移和转化,并促进了其降解,导致其分子量和腐殖化程度增加. 相似文献