Highly catalytic activity of Mn/SBA-15 catalysts for toluene combustion improved by adjusting the morphology of supports

Rod-like, hexagonal and fiber-like SBA-15 mesoporous silicas were synthesized to support MnO_x for toluene oxidation. This study showed that the morphology of the supports greatly influenced the catalytic activity in toluene oxidation. MnO_x supported on rod-like SBA-15(R-SBA-15) displayed the best catalytic activity and the conversion at 230°C reached more than 90%, which was higher than the other two catalysts. MnO_x species consisted of coexisting MnO_2 and Mn_2O_3 on the three kinds of SBA-15 samples. Large amounts of Mn_2O_3 species were formed on the surface and high oxygen mobility was obtained on MnO_x supported on R-SBA-15, according to the H_2 temperature programmed reduction(H_2-TPR)and X-ray photoelectron spectroscopy(XPS) results. The Mn/R-SBA-15 catalyst with greater amounts of Mn_2O_3 species possessed a large amount of surface lattice oxygen, which accelerated the catalytic reaction rate. Therefore, the surface lattice oxygen and high oxygen mobility were critical factors on the catalytic activity of the Mn/R-SBA-15 catalyst.     

N-doped CoAl oxides from hydrotalcites with enhanced oxygen vacancies for excellent low-temperature propane oxidation

A series of nitrogen-doped CoAlO (N-CoAlO) were constructed by a hydrothermal route combined with a controllable NH₃ treatment strategy. The effects of NH₃ treatment on the physico-chemical properties and oxidation activities of N-CoAlO catalysts were investigated. In comparison to CoAlO, a smallest content decrease in surface Co³⁺ (serving as active sites) while a largest increased amount of surface Co²⁺ (contributing to oxygen species) are obtained over N-CoAlO/4h among the N-CoAlO catalysts. Meanwhile, a maximum N doping is found over N-CoAlO/4h. As a result, N-CoAlO/4h (under NH₃ treatment at 400°C for 4 hr) with rich oxygen vacancies shows optimal catalytic activity, with a T₉₀ (the temperature required to reach a 90% conversion of propane) at 266°C. The more oxygen vacancies are caused by the co-operative effects of N doping and suitable reduction of Co³⁺ for N-CoAlO/4h, leading to an enhanced oxygen mobility, which in turn promotes C₃H₈ total oxidation activity dominated by Langmuir-Hinshelwood mechanism. Moreover, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) analysis shows that N doping facilities the decomposition of intermediate species (propylene and formate) into CO₂ over the catalyst surface of N-CoAlO/4h more easily. Our reported design in this work will provide a promising way to develop abundant oxygen vacancies of Co-based catalysts derived from hydrotalcites by a simple NH₃ treatment.     

Study on catalysts for combustion of lean CH4

In this study, cerarnics honeycomb-supported ABO₃ perovskite type oxides were preparedby changing the composition of A and B site cations, and observed their activities for lean CH₄ oxidation. In the case of change in A site composition La_0.3Sr_0.2MnO₃ and La_0.6Sr_0.4MnO₃ is the mostactive catalysts for 1 v% CH₄ and 2 v% CH₄ respectively. But LaMn_0.5Co_0.5O₃ oxide is the best ac-tive catalyst for 1-2v% CH₄ among the oxides by changing B site compositions of LaBO₃ and su-perior to La_0.3Sr_0.2MnO₃ and La_0.6S_0.4MnO₃catalysts.Adding trace Pd improved the activity and characteristics of space velocity for LaMn_0.5CO_0.5O₃and La_0.3Sr_0.2MnO₃ Although LaMn_0.5Co_0.5O₃ +Pd (0.03 wt%) was less active than the Pd catalyst,the activity was more than Pt catalyst at a conversion level below 90%.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NOx) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition, NOx was suppressed with the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NOx suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Synergistic effects of non-thermal plasma-assisted catalyst and ultrasound on toluene removal

A wire-mesh catalyst coated by La_0.8Sr_0.2MnO₃ was combined with a dielectric barrier discharge (DBD) reactor for toluene removal at atmospheric pressure. It was found that toluene removal efficiency and carbon dioxide selectivity were enhanced in the catalytic packed-bed reactor. In addition, ozone and nitrogen monoxide from the gas effluent byproducts decreased. This is the first time that ultrasound combined with plasma has been used for toluene removal. A synergistic effect on toluene removal was observed in the plasma-assisted ultrasound system. At the same time, the system increased toluene conversion and reduced ozone emission.     

Torpor at high ambient temperature in a neotropical didelphid,the grey short-tailed opossum (Monodelphis domestica)

The grey short-tailed opossum, Monodelphis domestica, has been an established research animal for more than five decades, but relatively, little is known about its thermophysiology. Here we studied core body temperature (T _b) and metabolic rate (MR) of female adult M. domestica housed in the laboratory at an ambient temperature (T _a) of 26 °C. In expanding previous reports, the average recorded core T _b of M. domestica was 34.3 °C. The T _b of an individual M. domestica can drop below 30 °C (minimal T _b: 28.6 °C) accompanied by a reduction in MR of up to 52 % even while having ad libitum access to food. These findings demonstrate for the first time the presence of spontaneous torpor in M. domestica. Metabolic suppression at relatively high T _a and T _b furthermore broadens our perspective on the use of torpor as a metabolic strategy not just restricted to cold climates.     

Selective catalytic reduction of NOx from exhaust of lean-burn engine over Ag-Al2O3/cordierite catalyst

A highly effective Ag-Al₂O₃ catalyst was prepared using the in-situ sol-gel method, and characterized by surface area using nitrogen adsorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. The catalyst performance was tested on a real lean-burn gasoline engine. Only unburned hydrocarbons and carbon monoxide in the exhaust were directly used as reductant (without any external reductant), the maximum NO _x conversion could only reach 40% at 450°C. When an external reductant, ethanol was added, the average NO _x conversion was greater than 60%. At exhaust gas temperature range of 350–500°C, the maximum NO _x conversion reached about 90%. CO and HC could be efficiently oxidized with Pt-Al₂O₃ oxidation catalyst placed at the end of SCR converter. However, NO _x conversion drastically decreased because of the oxidation of some intermediates to NO _x again. The possible reaction mechanism was proposed as two typical processes, nitration, and reduction in HC-SCR over Ag-Al₂O₃.     

Synergistic effect of Pt nanoparticles and micro-mesoporous ZSM-5 in VOCs low-temperature removal

Micro-mesoporous ZSM-5 zeolites were obtained by the post-treatment of tetrahydroxy ammonium hydroxide (TPAOH) solution with different concentration. The hierarchical pore structure formed during the desilication process facilitates the dispersion of Pt nanoparticles and Pt/ZSM-5 catalysts exhibit rather high catalytic activity for the deep oxidation of various VOCs at low temperature. The catalyst treated with TPAOH of 0.1 mol/L (Pt/ZSM-5(0.1)) shows the lowest degradation temperature (T_90%) of 128 and 142°C, respectively for benzene and n-hexane. Compared with the untreated Pt/ZSM-5 catalyst, the abundant mesopores, small Pt particle size and finely dispersed Pt contribute to the superior catalytic activity and stability of the Pt/ZSM-5 catalysts for VOCs removal. More importantly, the existence of H₂O in the feed gases hardly affected the activity of Pt/ZSM-5(0.1) catalyst at the low reaction temperature of 128°C, which is very important for VOCs low-temperature removal in the future practical applications.     

Hot bats: extreme thermal tolerance in a desert heat wave

Climate change is predicted to increase temperature extremes and thus thermal stress on organisms. Animals living in hot deserts are already exposed to high ambient temperatures (T _a) making them especially vulnerable to further warming. However, little is known about the effect of extreme heat events on small desert mammals, especially tree-roosting microbats that are not strongly protected from environmental temperature fluctuations. During a heat wave with record T _as at Sturt National Park, we quantified the thermal physiology and behaviour of a single free-ranging little broad-nosed (Scotorepens greyii, henceforth Scotorepens) and two inland freetail bats (Mormopterus species 3, henceforth Mormopterus) using temperature telemetry over 3 days. On 11 and 13 January, maximum T _a was ～45.0 °C, and all monitored bats were thermoconforming. On 12 January 2013, when T _a exceeded 48.0 °C, Scotorepens abandoned its poorly insulated roost during the daytime, whereas both Mormopterus remained in their better insulated roosts and were mostly thermoconforming. Maximum skin temperatures (T _skin) ranged from 44.0 to 44.3 °C in Scotorepens and from 40.0 to 45.8 °C in Mormopterus, and these are the highest T _skin values reported for any free-ranging bat. Our study provides the first evidence of extensive heat tolerance in free-ranging desert microbats. It shows that these bats can tolerate the most extreme T _skin range known for mammals (3.3 to 45.8 °C) and delay regulation of T _skin by thermoconforming over a wide temperature range and thus decrease the risks of dehydration and consequently death.     

Survival of Coronaviruses in Water and Wastewater

The advent of severe acute respiratory syndrome and its potential environmental transmission indicates the need for more information on the survival of coronavirus in water and wastewater. The survival of representative coronaviruses, feline infectious peritonitis virus, and human coronavirus 229E was determined in filtered and unfiltered tap water (4 and 23°C) and wastewater (23°C). This was compared to poliovirus 1 under the same test conditions. Inactivation of coronaviruses in the test water was highly dependent on temperature, level of organic matter, and presence of antagonistic bacteria. The time required for the virus titer to decrease 99.9% (T_99.9) shows that in tap water, coronaviruses are inactivated faster in water at 23°C (10 days) than in water at 4°C (>100 days). Coronaviruses die off rapidly in wastewater, with T_99.9 values of between 2 and 4 days. Poliovirus survived longer than coronaviruses in all test waters, except the 4°C tap water.     

Improvement of the activity and SO2 tolerance of Sb-modified Mn/PG catalysts for NH3-SCR at a low temperature

A series of MnM/palygorskite (PG) (M = La, W, Mo, Sb, Mg) catalysts was prepared by the wetness co-impregnation method for low-temperature selective catalytic reduction (SCR) of NO with NH₃. Conversion efficiency followed the order Sb > Mo > La > W > Mg. A combination of various physico-chemical techniques was used to investigate the influence of Sb-modified Mn/PG catalysts. MnSb_0.156/PG catalyst showed highest NO conversion at low temperatures in the presence of SO₂ which reveals that addition of Sb oxides effectively enhances the SCR activity of catalysts. A SO₂ step-wise study showed that MnSb_0.156/PG catalyst displays higher durable resistance to SO₂ than Mn/PG catalyst, where the sulfating of active phase is greatly inhibited after Sb doping. Scanning electron microscopy and X-ray diffraction results showed that Sb loading enhances the dispersion of Mn oxides on the carrier surface. According to the results of characterization analyses, it is suggested that the main reason for the deactivation of Mn/PG is the formation of manganese sulfates which cause the permanent deactivation of Mn-based catalysts. For Sb-doped Mn/PG catalyst, SO_x ad-species formed were mainly combined with SbO_x rather than MnO_x. This preferential interaction between SbO_x and SO₂ effectively shields the MnO_x as active species from being sulfated by SO₂ resulting in the improvement of SO₂ tolerance on Sb-added catalyst. Multiple information support that, owing to the addition of Sb, original formed MnO_x crystallite has been completely transformed into highly dispersed amorphous phase accounting for higher SCR activity.     

复合型高锰酸钾缓释体的制备及其缓释性能研究

采用熔化成型法,以环境友好型材料石蜡和硅砂为复合材料制备复合型高锰酸钾缓释体,研究其在水中和TCE溶液中的缓释性能及缓释过程.研究结果表明:当固定高锰酸钾含量为6 9,蜡砂比在1:4 ～1:6之间时,复合型高锰酸钾缓释体成型度适中,高锰酸钾的缓释量随着时间的延长逐渐增大,13 d高锰酸钾累积释放百分数分别为28.3％和58.8％,可以作为缓释材料,实现高锰酸钾的持续可控释放当固定蜡砂比,释放速率随着高锰酸钾百分含量的增大而增大.SEM分析结果表明,复合型高锰酸钾缓释体在水中和TCE溶液中的释放机理:首先表层外露的高锰酸钾晶体遇水快速溶解留下一些孔洞和缝隙,然后水分子通过这些孔洞进入缓释体内部溶解高锰酸钾,最后由浓度梯度差将高锰酸钾扩散到水相中,与溶液中TCE发生氧化降鳃反应.蜡砂比为1:4和1:6的缓释体4h对TCE的去除率分别为90％和100％;实际的高锰酸钾释放量分别约为理论所需高锰酸钾总量的1.7倍和2.6倍,说明该法制备得复合型高锰酸钾缓释体可通过控制蜡砂比来持续释放高锰酸钾,用于氯代烃的去除.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NO_x) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition,NO_xwas suppressedwith the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NO_x suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Catalyst for NOx removal in nitric-acid plant gaseous effluents

The behaviour of a V₂O₅WO₃TiO₂ phosphorated catalyst, in the Selective Catalytic Reduction (SCR) of equimolar NO + NO₂ mixtures, is studied in order to analyse the possibility of its industrial utilization for the treatment of nitric-acid plant stack gases. With this new catalyst, an NO_x conversion higher than 90% molar can be achieved, the ammonia concentration at the exit gas being lower than that required to form ammonium salts, throughout the temperature range of commercial interest: 250–450°C, at a relatively high space velocity (GHSV ⩽ 40000 h⁻¹ NC). The effect of several operating variables such as oxygen concentration and NO₂/NO molar ratio in the feed is also discussed.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

城市生活垃圾滚筒筛分选特性研究

滚筒筛筛分是生活垃圾分选中常用的工艺,国内目前有关滚筒筛分选生活垃圾的研究尚不多见.因此,本实验通过自行设计的一台处理能力为150kg.h-1的滚筒筛,采用实际生活垃圾进行分选实验,确定最佳运行参数范围.结果表明,当滚筒筛孔径为120mm时,在V实测/V极限（V实测为滚筒转动时实时测定转速,V极限为物料与滚筒一起转动时...     

Integrated removal of NO and mercury from coal combustion flue gas using manganese oxides supported on TiO2

A catalyst composed of manganese oxides supported on titania(MnO_x/TiO_2) synthesized by a sol–gel method was selected to remove nitric oxide and mercury jointly at a relatively low temperature in simulated flue gas from coal-fired power plants. The physico-chemical characteristics of catalysts were investigated by X-ray fluorescence(XRF), X-ray diffraction(XRD), and X-ray photoelectron spectroscopy(XPS) analyses, etc. The effects of Mn loading,reaction temperature and individual flue gas components on denitration and Hg~0 removal were examined. The results indicated that the optimal Mn/Ti molar ratio was 0.8 and the best working temperature was 240°C for NO conversion. O_2 and a proper ratio of [NH_3]/[NO]are essential for the denitration reaction. Both NO conversion and Hg~0 removal efficiency could reach more than 80% when NO and Hg~0 were removed simultaneously using Mn0.8 Tiat 240°C.Hg~0 removal efficiency slightly declined as the Mn content increased in the catalysts. The reaction temperature had no significant effect on Hg~0 removal efficiency. O_2 and HCl had a promotional effect on Hg~0 removal. SO2 and NH_3were observed to weaken Hg~0 removal because of competitive adsorption. NO first facilitated Hg~0 removal and then had an inhibiting effect as NO concentration increased without O_2, and it exhibited weak inhibition of Hg~0 removal efficiency in the presence of O_2. The oxidation of Hg~0 on Mn O x/TiO_2 follows the Mars–Maessen and Langmuir–Hinshelwood mechanisms.     

Torpor in the Patagonian opossum (Lestodelphys halli): implications for the evolution of daily torpor and hibernation

Hibernation and daily torpor are two distinct forms of torpor, and although they are related, it is not known how and in which sequence they evolved. As the pattern of torpor expressed by the oldest marsupial order the opossums (Didelphimorphia) may provide insights into the evolution of torpor, we aimed to provide the first quantitative data on the thermal biology and torpor expression of the rare Patagonian opossum (Lestodelphys halli). It is the opossum with the southernmost distribution, has a propensity of autumnal fattening, and therefore, is likely to hibernate. We captured two male Lestodelphys, which while in captivity displayed strong daily fluctuations of body temperatures (T_b) measured with implanted miniature data loggers even when they remained normothermic. In autumn and early winter, torpor was expressed occasionally when food was available, but cold exposure and food withdrawal increased torpor use. The mean T_b throughout the study was 32.2?±?1.4 °C, the minimum T_b measured in torpid Lestodelphys was 7.7 °C, average torpor bout duration was 10.3 h, and the maximum torpor bout duration was 42.5 h. Thus, the pattern of torpor expressed by Lestodelphys was intermediate between that of daily heterotherms and hibernators suggesting that it may represent an ancestral opportunistic torpor pattern from which the derived patterns of daily torpor and seasonal hibernation diverged.     

铜铈复合氧化物上石化行业典型VOCs的氧化行为与动力学

采用共沉淀法和等体积浸渍法制备了CuCeO x复合催化剂,对材料的物化性质进行了XRD、低温N2吸脱附、H2-TPR和O2-TPD表征.以石化行业典型VOCs(苯、甲苯和正己烷)为探针污染物,研究了污染物组成与浓度、反应空速、O2浓度、H2O浓度和催化剂种类对其氧化行为的影响,并对反应动力学参数进行了模型拟合.共沉淀得到的催化剂具有均匀的活性相、好的低温可还原性能和较多的活性表面氧物种.甲苯氧化率随着污染物浓度升高而降低,高转化率下苯浓度与其氧化率无相关性,正己烷的氧化率与入口浓度呈正比.苯能够显著抑制甲苯的氧化,而甲苯加入有利于苯的氧化.正己烷对苯氧化的影响较小,但能够促进甲苯的转化,苯系物对正己烷氧化有明显的抑制作用.低空速和高氧浓度都有利于污染物的氧化,氧浓度的变化对正己烷和苯的氧化影响较小.水汽对甲苯的氧化有明显的抑制作用,而对苯和正己烷氧化有明显的促进作用.共沉淀催化剂具有更好的甲苯和苯氧化性能,而无水条件下浸渍催化剂具有更好的正己烷氧化性能.拟一级动力学模型能够很好地模拟不同条件下污染物的氧化行为.     

等离子体催化降解甲苯途径的原位红外研究

考察了在常温常压条件下,等离子体分别协同SiO₂、Al₂O₃、NiO/Al₂O₃降解甲苯的性能,并从材料的介电常数、对甲苯的吸附性及臭氧分解能力等角度分析了不同活性表现的原因,同时,采用原位红外技术研究了甲苯降解过程中催化剂表面吸附物种的变化.结果表明,当甲苯浓度为100 ppm,气体流量为100 mL·min^-1时,一定范围内,甲苯降解率随着能量密度、介电常数、吸附性及臭氧分解能力的提高而提高.甲苯在催化剂表面的吸附对其降解途径有十分重要的影响:在放电区域中加入SiO₂,甲苯仍然在气相中完成降解;而存在Al₂O₃ 及NiO/Al₂O₃时,甲苯氧化成苯甲酸的过程主要发生在催化剂表面,是甲苯催化降解的关键步骤,苯甲酸在活性位点的积累将降低催化剂的反应活性.