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1.
大气光化学烟雾反应机理比较(Ⅰ)O3和NOx的比较   总被引:8,自引:0,他引:8       下载免费PDF全文
在相同初始和排放条件下,对四种应用较广的光化学烟雾反应机理(CB4-99,RADM2,RACM,SAPRC99)进行了比较。研究发现:对于O3,在低VOCs/NOx时,四种机理模拟结果相关较小,平均相对标准偏差为7%,在高VOCs/NOx时,平均相对标准偏差为26%,差距较大;对于NOx,多数情况下RACM和RADM2的模拟结果较高,CB4-99和SAPRC99的模拟值偏低,其原因主要来源于不同机理中O3的生成对NOx及VOCs的敏感性不同而造成的。在用模式模拟O3和NOx时,应特别注意机理不同而带来的模拟结果差异。  相似文献   

2.
易挥发有机化合物在Pt/Al_2O_3-Si纤维催化剂上的低温氧化   总被引:4,自引:0,他引:4  
本文合成了一种新型的Pt负载在Al_2O_3涂膜强力富硅纤维载体的催化剂,研究低温下催化易挥发有机化合物的行为.用四种有机化合物检验实验参数对催化剂分解有机化合物分解率的影响.讨论了流速、浓度、有机物的本性、预热温度、反应热等参数的影响,并给出了催化剂对苯、甲苯在特定实验条件下的活化能、反应级数和指前因子的数值.  相似文献   

3.
张业新  王晓  王力  王仲鹏  李倩  张昭良 《环境化学》2013,32(7):1300-1307
利用程序升温脱附(TPD)、程序升温表面反应(TPSR)和原位红外光谱(in situ IR)等技术研究了Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程.结果表明,NOx在Pd-K/MgAlO上主要以硝酸根和亚硝酸根的形式存储.在Pd的催化作用下,部分亚硝酸根被氧化为强酸性的硝酸根,变得更容易存储.由NOx-TPD计算得到Pd-K/MgAlO的NOx存储容量高达890.4 μmol·g-1.此外,在NOx脱附及H2还原的实验中均发现了Pd催化的亚硝酸盐歧化分解反应,该反应通过亚硝酸盐溢流至Pd位实现.亚硝酸盐的溢流产生了两个作用:促进NOx低温脱附及促进H2对存储NOx的还原.此发现为NOx存储物种的溢流机理提供了一个有力的证据.  相似文献   

4.
武汉城区大气中NOx的污染,一日中以早晨最重,下午最轻;一年中,冬季的浓度比夏季高出37.7%.交通稠密区和商业集中区大气中的NOx年日均浓度分别比郊区高5倍和4.3倍.统计研究的结果表明,九年间特别是近六年来,武汉城区大气中NOx年日均值呈上升趋势.从1984年~1989年,大气中的NOx日均浓度平均每年以7%的速度递增,其超标率平均每年以0.8%的速度递增.  相似文献   

5.
This paper identifies a new economic motive for pollution regulations that allow polluting firms to bank and borrow emission permits over time. When aggregate pollution is stochastic, an intertemporal permit trading regime can provide firms with efficient incentives for pollution abatement without the need for costly government enforcement actions that would otherwise be required.  相似文献   

6.
    
● Microwave-assisted catalytic NH3-SCR reaction over spinel oxides is carried out. ● SCR reaction temperature is tremendously lowered in microwave field. ● NO conversion of NiMn2O4 is highly up to 90.6% at 70°C under microwave heating. Microwave-assisted selective catalytic reduction of nitrogen oxides (NOx) was investigated over Ni-based metal oxides. The NiMn2O4 and NiCo2O4 catalysts were synthesized by the co-precipitation method and their activities were evaluated as potential candidate catalysts for low-temperature NH3-SCR in a microwave field. The physicochemical properties and structures of the catalysts were characterized by X-ray diffraction (XRD), Scanning electron microscope (SEM), N2-physisorption, NO adsorption-desorption in the microwave field, H2-temperature programmed reduction (H2-TPR) and NH3-temperature programmed desorption (NH3-TPD). The results verified that microwave radiation reduced the reaction temperature required for NH3-SCR compared to conventional heating, which needed less energy. For the NiMn2O4 catalyst, the catalytic efficiency exceeded 90% at 70 °C and reached 96.8% at 110 °C in the microwave field. Meanwhile, the NiMn2O4 also exhibited excellent low-temperature NH3-SCR reaction performance under conventional heating conditions, which is due to the high BET specific surface area, more suitable redox property, good NO adsorption-desorption in the microwave field and rich acidic sites.  相似文献   

7.
● This study summarizes and evaluates different approaches that indicate O3 formation. ● Isopleth and sensitivity methods are useful but have many prerequisites. ● AOC is a better indicator of photochemical reactions leading to O3 formation. Tropospheric ozone (O3) concentration is increasing in China along with dramatic changes in precursor emissions and meteorological conditions, adversely affecting human health and ecosystems. O3 is formed from the complex nonlinear photochemical reactions from nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs). Although the mechanism of O3 formation is rather clear, describing and analyzing its changes and formation potential at fine spatial and temporal resolution is still a challenge today. In this study, we briefly summarized and evaluated different approaches that indicate O3 formation regimes. We identify that atmospheric oxidation capacity (AOC) is a better indicator of photochemical reactions leading to the formation of O3 and other secondary pollutants. Results show that AOC has a prominent positive relationship to O3 in the major city clusters in China, with a goodness of fit (R2) up to 0.6. This outcome provides a novel perspective in characterizing O3 formation and has significant implications for formulating control strategies of secondary pollutants.  相似文献   

8.
李晓璐  陈欢  周娟  万海勤  万玉秋  郑寿荣 《环境化学》2011,30(10):1705-1710
采用浸渍法合成出Pd/Al2O3催化剂,通过ICP、XRD、TEM和Zeta电位等表征手段对催化剂的组成和形貌进行了表征.在液相催化加氢还原Cr(Ⅵ)的反应中,分别研究了催化剂加入量、Cr(Ⅵ)初始浓度、pH值、Pd负载量等因素的影响.结果表明,该催化剂表面酸性影响催化还原效果,此反应属于吸附抑制型.  相似文献   

9.
    
• Quantification of efficiency and fairness of abatement allocation are optimized. • Allocation results are refined to the different abatement measures of enterprises. • Optimized allocation results reduce abatement costs and tap the abatement space. • Abatement suggestions are given to enterprises with different abatement quotas. For achieving air pollutant emission reduction targets, total pollutant amount control is being continuously promoted in China. However, the traditional pattern of pollutant emission reduction allocation regardless of economic cost often results in unreasonable emission reduction pathways, and industrial enterprises as the main implementers have to pay excessively high costs. Therefore, this study adopted economic efficiency as its main consideration, used specific emission reduction measures (ERMs) of industrial enterprises as minimum allocation units, and constructed an enterprise-level pollutant emission reduction allocation (EPERA) model with minimization of the total abatement cost (TAC) as the objective function, and fairness and feasibility as constraints for emission reduction allocation. Taking City M in China as an example, the EPERA model was used to construct a Pareto optimal frontier and obtain the optimal trade-off result. Results showed that under basic and strict emission reduction regulations, the TAC of the optimal trade-off point was reduced by 46.40% and 45.77%, respectively, in comparison with that achieved when only considering fairness, and the Gini coefficient was 0.26 and 0.31, respectively. The abatement target was attained with controllable cost and relatively fair and reasonable allocation. In addition, enterprises allocated different emission reduction quotas under different ERMs had specific characteristics that required targeted optimization of technology and equipment to enable them to achieve optimal emission reduction effects for the same abatement cost.  相似文献   

10.
董昊  王含月  程龙  赵旭辉  王欢 《环境化学》2022,41(7):2364-2374
为了解芜湖市O3污染变化特征及与主要影响因子相关性,本文对芜湖市环境监测站点和基本气象站点的监测数据进行统计分析。结果表明,芜湖市O3污染程度呈现西南向东北逐步加重的趋势,科创中心、济民医院和四水厂站点月度变化呈现双峰分布的特征,峰值出现在4月和6月,而监测站则是显著单峰型,峰值出现在6月。各站点O3日变化均呈现显著的“单峰单谷”型,在15:00前后达到峰值。在NO2/NO比值区间为10—20时,夜间更易出现高浓度O3,而昼间O3浓度高值更易出现在比值低于10时。PM2.5和O3间的相关性更趋向于非线性关系。温度和相对湿度对O3的影响分别呈现正相关和负相关,O3峰值易出现在温度为25—35 ℃、相对湿度为60%—80%的气象条件下。在东-东南风向下,O3的超标天最多。  相似文献   

11.
废水生物脱氮中N2O和NOx的产生和作用   总被引:5,自引:0,他引:5  
废水生物脱氮中N2O和NOx来源于硝化、反硝化、厌氧氨氧化和化学反硝化等过程.电子受体和供体浓度、pH、缓冲剂类型、有机负荷、微生物种类及其相互作用等都会影响这些气态中间产物的产生.NO2能够氧化氨和强化好氧和厌氧氨氧化,NO能够阻止C2H2对好氧氨氧化活性的抑制,两者对好氧氨氧化活性的恢复至关重要.所有这些表明,废水生物脱氮的气态中问产物N2O和NOx在氮的生物转化中具有重要的正面作用,甚至必不可少.基于NO2曝气技术和Brocadia anammoxidans与Nitrosomonas协同作用的废水生物脱氮新技术开发是今后一段时间的重要研究方向.图4参35  相似文献   

12.
    
● Methanol effectively reduces CO, HC, CO2, PM, and PN emissions of gasoline vehicles. ● Elemental composition of methanol directly affects the reduction of emissions. ● Several physicochemical properties of methanol help reduce vehicle emissions. The transport sector is a significant energy consumer and a major contributor to urban air pollution. At present, the substitution of cleaner fuel is one feasible way to deal with the growing energy demand and environmental pollution. Methanol has been recognized as a good alternative to gasoline due to its good combustion performance. In the past decades, many studies have investigated exhaust emissions using methanol-gasoline blends. However, the conclusions derived from different studies vary significantly, and the explanations for the effects of methanol blending on exhaust emissions are also inconsistent. This review summarizes the characteristics of CO, HC, NOx, CO2, and particulate emissions from methanol-gasoline blended fuels and pure methanol fuel. CO, HC, CO2, particle mass (PM), and particle number (PN) emissions decrease when methanol-blended fuel is used in place of gasoline fuel. NOx emission either decreases or increases depending on the test conditions, i.e., methanol content. Furthermore, this review synthesizes the mechanisms by which methanol-blended fuel influences pollutant emissions. This review provides insight into the pollutant emissions from methanol-blended fuel, which will aid policymakers in making energy strategy decisions that take urban air pollution, climate change, and energy security into account.  相似文献   

13.
论述了英国实现污染物减排环境治理方面的成功经验和做法,其主要有健全完善的法规政策体系,强化运用环境经济手段,建立节能减排的长效机制,建立科学、成熟的战略环评体系(SEA),用最佳可行技术(BAT)防止和减少污染排放,注重公众参与促进全民减排。依据英国实现污染物减排环境治理方面的成功经验和做法,结合目前我国污染物减排工作的实际,对我国污染物减排工作提出了相应的对策与建议。  相似文献   

14.
Excess nitrate in Mississippi River water entering offshore areas is reported to contribute to low oxygen (hypoxia) conditions in the Gulf of Mexico. Excessive algal growth driven by the excess nitrogen results in a decrease in dissolved oxygen in bottom water. Reintroduction of Mississippi River waters into a Louisiana coastal wetland has the potential to reduce the amount of nitrate reaching offshore waters. In this study, reduction in the concentration of added NO3- was determined in sediment-water-columns collected from a wetland site in Breton Sound estuary receiving nutrient inputs from the Mississippi River. The capacity of a wetland to process nitrate in floodwater was determined in the laboratory. The rates of NO3- removal (determined from change in nitrate concentration in the floodwater) averaged 97 mg N m-2 d-1 over 16 d for a 1750-mg NO3-N m-2 addition, and 170 mg N m-2 d-1 over 16 d for a 3500-mg NO3-N m-2 addition. The total N2O-N emissions from the 1750- and 3500-mg NO3-N m-2 additions were 19 and 54 mg N m-2 accounting for 1.1% and 1.5% of the applied NO3-N, respectively. Using the acetylene-inhibition technique, the average denitrification rate was determined to be 57 and 87 mg N m-2 d-1 (21 and 32 g N m-2 yr-1) during the most active denitrification period of 5 d after incubation for 1750 and 3500 mg NO3--N m-2 of added nitrate in floodwater, respectively. The total N evolved over 11 d as N2O + N2 was equivalent to 436 and 921 mg N m-2 (24.9% and 26.3%, respectively, of added N). Increasing the amount of NO3- applied to the overlying water increased the rate of NO3- loss and N2O emission significantly. The thickness of the oxidized surface sediment layer was also influenced by the NO3- application to the floodwater with a significant linear correlation between nitrate addition and thickness of the oxidized layer (r = 0.9998, p = 0.01). This study indicates that wetlands receiving diverted Mississippi River water have the potential to process and remove NO3- in the river water, reducing the amount of NO3- reaching to offshore areas.  相似文献   

15.
    
• Nano Fe2O3 and N-doped graphene was prepared via a one-step ball milling method. • The maximum power density of Fe-N-G in MFC was 390% of that of pristine graphite. • Active sites like nano Fe2O3, pyridinic N and Fe-N groups were formed in Fe-N-G. • The improvement of Fe-N-G was due to full exposure of active sites on graphene. Developing high activity, low-cost and long durability catalysts for oxygen reduction reaction is of great significance for the practical application of microbial fuel cells. The full exposure of active sites in catalysts can enhance catalytic activity dramatically. Here, novel Fe-N-doped graphene is successfully synthesized via a one-step in situ ball milling method. Pristine graphite, ball milling graphene, N-doped graphene and Fe-N-doped graphene are applied in air cathodes, and enhanced performance is observed in microbial fuel cells with graphene-based catalysts. Particularly, Fe-N-doped graphene achieves the highest oxygen reduction reaction activity, with a maximum power density of 1380±20 mW/m2 in microbial fuel cells and a current density of 23.8 A/m2 at –0.16 V in electrochemical tests, which are comparable to commercial Pt and 390% and 640% of those of pristine graphite. An investigation of the material characteristics reveals that the superior performance of Fe-N-doped graphene results from the full exposure of Fe2O3 nanoparticles, pyrrolic N, pyridinic N and excellent Fe-N-G active sites on the graphene matrix. This work not only suggests the strategy of maximally exposing active sites to optimize the potential of catalysts but also provides promising catalysts for the use of microbial fuel cells in sustainable energy generation.  相似文献   

16.
Lake eutrophication leading to water pollution is a major global concern. In recent years, rapid economic growth and the increase in the intensity of resource exploitation in China have caused the influx of nitrogen and phosphorus into lakes. This in turn has led to more severe lake eutrophication, more frequent outbreaks of algal blooms, and the degradation of lake ecosystems. An effective plan balancing economic growth with the reduction of nitrogen and phosphorus emissions is greatly needed. The design and implementation of such a plan requires the collection and analysis of pertinent data. In this paper, we use the environmental computable general equilibrium (ECGE) model to identify the most effective way to balance economic growth with the reduction of nitrogen and phosphorus emissions. For the multiregional analysis, we use social accounting matrices (SAMs) and a provincial trade matrix based on the assumptions of the gravity model. We consider the Poyang Lake Watershed as a case study to illustrate the utility of the model. Based on present conditions in the Poyang Lake Watershed, restricting nitrogen and phosphorus emissions from sectors with the highest emissions is more effective for balancing economic growth and the reduction of nitrogen and phosphorus emissions than restricting nitrogen and phosphorus emissions from all sectors.  相似文献   

17.
    
• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst. • The surface acidity and reducibility were highly improved, as well as the pore structure. • The enrichment of the surface Fe2+ and the adsorbed oxygen account for the improvement. Our previous study proved that the acid-pretreatment process could efficiently activate red mud (RM) for the selective catalytic reduction (SCR) of NOx. However, in terms of the molding process, which is the key step determining whether it can be applied in large-scale industrial, the surface acidity and reducibility of catalyst always decreased dramatically, and part of surface area and pore structure were lost. In this study, we prepared monolithic honeycomb red mud (MHRM) catalysts with activated carbon (AC) as an accelerant and investigated the effect of AC on the MHRM. The results showed that the MHRM with 3 wt.% of AC (MHRM-AC3) exhibited the best SCR performance, and kept more than 80% NOx conversion in the range of 325°C–400°C. Compared with the MHRM, MHRM-AC1, and HMRM-AC5, the MHRM-AC3 has more mesoporous and macroporous structures, which can provide more adsorption active sites. The AC significantly improved NH3 adsorption and surface reducibility, which was mainly due to the increase of the surface acid sites (especially the Brönsted acid sites), the concentration of Fe(II), and the surface adsorbed oxygen. The presence of more Fe(II) enriched the surface oxygen vacancies, as well as the surface adsorbed oxygen, due to the charge imbalance and unsaturated chemical bond. And surface adsorbed oxygen exhibited more active than lattice oxygen owing to its higher mobility, which was conducive to NOx reduction in the SCR reaction.  相似文献   

18.
    
Reduced perovskite HCa2Ta3O10 nanosheets loaded with Pt and Cu are synthesized for sunlight‐driven conversion of CO2 with water vapor into valuable fuels. Perovskite nanosheets are prepared by exfoliating layered perovskite CsCa2Ta3O10 via tetra butyl ammonium ion exchange, followed by liquid ultrasonic exfoliation. The obtained nanosheets exhibits a high specific surface area (>200 m2 g−1). The photocatalytic performance of the resulting reduced perovskite nanosheets is evaluated for CO2 photoreduction under sunlight in the presence of saturated water vapor. The reduced nanosheets exhibit much higher photoactivity than the nonreduced ones. This can be ascribed to their unique structure. The hydrogen treatment in the presence of platinum induces a considerable amount of Ta+4 and oxygen vacancies, which apparently improves the visible light absorption of perovskite nanosheets. Moreover, the introduction of CuO nanoparticles significantly improves the electron–hole separation through the formation of a p–n junction. It also enhances the adsorption of CO2 and stabilizes C1 intermediates which are favorable for C C coupling to form C2 products (e.g., ethanol). The formation rates of ethanol and methanol are 113 and 7.4 µmol g−1 h−1, respectively, while only methanol is obtained at the rate of 125.9 µmol g−1 h−1 in the absence of CuO nanoparticles.  相似文献   

19.
    
Developing a high-performance photocatalyst is important for realizing efficient photocatalytic H2O2 generation. Herein, a novel step-scheme (S-scheme) heterojunction photocatalyst C3N4/PDA (CNP) comprised of ultrathin g-C3N4 (U-CN) and polydopamine (PDA) is constructed by in situ self-polymerization. The optimal photocatalyst presents an excellent H2O2 production rate of 3801.25 µmol g−1 h−1 under light irradiation, which is about 2 and 11 times higher than that of pure U-CN and PDA, respectively, and exceeds most of the reported C3N4-based photocatalysts. The improvement of photocatalytic activity is ascribed to the synergistic effect of improved light absorption and promoted charge separation and transfer induced by the S-scheme heterojunction. In situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) reveals that the charge transfer route matches the S-scheme mechanism. Rotating disk electrode (RDE) measurements and electron spin resonance (ESR) spectroscopy verify that H2O2 is produced by a two-step one-electron process. This work highlights a promising method to construct high-performance S-scheme heterojunction photocatalysts through the hybridization of PDA and C3N4.  相似文献   

20.
To assess the impact of three different emission reduction scenarios on PM10 concentrations in Northern Italy, the TCAM multiphase model has been applied in the framework of the CityDelta III-CAFE EU project. The considered domain, that is characterized by high urban and industrial emissions and a dense road traffic, due to frequently stagnating meteorological conditions is often affected by severe PM10 levels, far from the European standard regulations. The impact evaluation has been performed in terms of both yearly mean values and 50 g/m3 exceedance days for the 2004 Base Case simulation. The results show that the three selected emission reduction scenarios up to 2020 improve air quality all over the domain, in particular, in the area with higher emission density.  相似文献   

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