ACF脱除SO2/NOx反应器数学模型的建立

在大量试验研究获得数据基础上,结合机理分析,考虑ACF同时脱除多种污染物的主要影响因素,运用气固催化反应动力学方法进行分析,采用"混合模型法"建立ACF反应器数学模型,并用MATLAB软件与实验数据相结合迭代求取了模型参数,求出了宏观反应速率方程,并将计算模拟值与实验值进行比对,发现模拟结果与实验结果基本吻合,证实了模型的可靠性.为ACF反应器从试验研究的成果放大到工业规模的应用奠定了基础.     

Laboratory and field measurements of NOx produced from corona discharge

This research consists of a laboratory study and a field study. The laboratory research reports the formation of NO_x from a point to plane corona discharge. Discharge polarity and relative humidity determined the amount of NO_x that was produced. The positive point discharge caused more NO_x to form than the negative point discharge. For both polarities NO_x production showed a nonlinear increase with current. Relative humidity enhanced the NO_x formation for both polarities. In each case, the amount of NO_x formed was comparable to the quantity of N₂O produced from corona discharge. The research also reports the results from a field study that measured the amounts of 03 and NO₂ produced by corona discharge during a thunderstorm. The study found that the ambient concentrations of 03 and NO₂ increased several fold due to corona discharge and returned to original levels after the thunderstorm.     

High NOx levels and lack of ozone in downtown Caracas

An evaluation of the NO, NO₂ and O₃ concentrations in downtown Caracas atmosphere at two different heights (1.5 and 56 m ) during the dry and wet season was performed.The qualitative variation of NO and NO₂ concentrations throughout the day was the same for all conditions. The profiles are explained considering the automobile emissions and the fates by photochemical reactions and dispersion. The daily mean averages for NO_x exceed all available air quality standards, making the downtown Caracas air polluted with these compounds at harmful levels.The O₃ concentrations are lower than the natural background levels practically all day long for all conditions. This lack of O₃ is explained mainly by the very high continuous NO emissions occuring in Caracas. NO reacts very fast with O₃ consuming all the O₃ produced by photochemical reactions. Possible health implications of the low O₃ levels are pointed out.     

碳纳米管/二氧化钛/壳聚糖催化薄膜光催化活性及苯降解机理

通过X-射线衍射仪(XRD)、扫描电镜(SEM)、透射电镜(TEM)和紫外可见光漫反射谱(UV-vis)对碳纳米管/二氧化钛/壳聚糖复合薄膜的晶体结构和形貌进行表征,以室内空气典型污染物气相苯为模型反应物,研究碳纳米管/二氧化钛/壳聚糖催化薄膜的光催化活性及其对苯的光降解机理。结果表明,制备的碳纳米管/二氧化钛/壳聚糖催化薄膜所具有的良好催化活性归功于碳纳米管、二氧化钛和壳聚糖三者的协调效应;气相苯光降解产生的主要中间产物是乙酸乙酯和十一烷,以及少量的丙烯醛、4-羰基-甲基-苯乙酮、十二烷烃、2,4,-二叔丁基苯酚、二十一烷烃。根据红外光谱分析与GC/MS分析结果,进一步提出了气相苯的降解机理过程。     

Anthropogenic NOx emissions alter the intrinsic water-use efficiency (WUEi) for Quercus cerris stands under Mediterranean climate conditions

We investigated the effect of N deposition (Ndep) on intrinsic water-use efficiency (WUE_i), the ratio of photosynthesis (A) to stomatal conductance (g_s), for two Quercus cerris stands at different distances to an oil refinery in Southern Italy. We used δ¹³C in tree rings for assessing changes in WUE_i; while the influence of climate and NO_x emission was explored through δ¹⁸O and δ¹⁵N, respectively. Differences in WUE_i between the two sites were significant, with trees exposed to different degrees of NO_x emissions showing an abrupt increase with the onset of pollution. Assuming similar g_s at the two sites, as inferred through δ¹⁸O, the higher N availability at the polluted site caused the shift of the A/g_s ratio in favour of A. Overall, our result suggests that an increase of Ndep may enhance tree WUE under a scenario of reduction of precipitation predicted for Mediterranean area.     

Decomposition of chlorinated dioxins, odourous compounds and NOx from MSW incineraton plant by oxidizing catalyst

An experiment was carried out to decompose chlorinated dioxins (PCDDs, PCDFs) Chlorobenzenes, NOx and odourous compounds (H₂S, CH₄S, C₂H₆S₂, C₈H₈, C₂H₆S, C₂H₄O, NH₃) simultaneously using a catalyst in the MSW incineration plant. The experiments were conducted at temperatures from 200°C to 400°C and from 3000h⁻¹ to 6000h⁻¹ at space velocity. A catalyst containing V₂O₅ and WO₃ on the basis of TiO₂ is used, an oxidizing catalyst of the honeycomb type. The average decomposition efficiencis were 95%, 98%, 92% for PCDDs(48CDDs), PCDFs(48CDFs) and Chlorobenzenes(36CLBs) at a reaction temperature of 350°C and a space velocity of 3000h⁻¹, more than 90% for NOx at a reactiont temperature of 300°C and more than 80% for odourous compounds at the reaction temperature of 300°C and a space velocity of 6000h⁻¹. All those compounds were decomposed successfully with increasing contact time and surface. The rate-determing step was the chemical reaction of catalyst surface.     

Decomposition of gas phase 1,3-butadiene by ultraviolet/ozone process

A pilot-scale plug-flow reactor was built to investigate its performance in treating airborne 1,3-butadiene (BD) via ozonation (O3) and ultraviolet (UV)/O3 technologies. Governing factors, such as the initial molar ratio of ozone to BD, UV volumetric electric input power, and moisture content in the influent airstream, were investigated. Experiments were conducted at an influent BD concentration of approximately 50 ppm, an ambient temperature of 26 degrees C, and a gas retention time of 85 sec. Results show that an initial molar ratio of ozone to BD of 3.5 and 2 sufficed to obtain BD decompositions of >90% for ozonation and UV/O3, respectively. The UV irradiance did not directly promote the decomposition of BD, rather, it played a role in promoting the production of secondary oxidants, such as hydroxyl radicals. Kinetic analyses indicate that both types of BD decomposition are peudo-first-order with respect to BD concentrations. Moisture content (relative humidity = 40-99%) and UV volumetric electric input power (0.147 and 0.294 W/L) are both factors that weakly affect the rate of BD decomposition. Economic evaluation factors, including both energy of ozone production and UV electric input power, were also estimated.     

生物膜填料塔净化模拟烟气和电厂烟气中SO2和NOx的对比实验

对生物膜填料塔对模拟烟气和电厂烟气的净化效果进行了实验研究。实验对比分析了在相同的实验条件下生物膜填料塔对不同烟气中SO2和NOx的净化效率。实验结果表明,在循环液温度在24～35℃、空床停留时间（EBRT）为60s、喷淋量为8～10L／h、脱硫塔的pH为0．8～1．5、脱氮塔的pH为7．5～8．0的条件下,生物膜填料塔对模拟烟气和电厂烟气中SO2的净化效率都很高,但模拟烟气条件下的总脱氮率的平均值为80％,而在电厂烟气条件下只有35％。经分析认为,脱氮率产生差异的主要原因是电厂烟气中杂质的影响,以及烟气中氧气含量的不同,同时因为生长条件不同从而驯化出的微生物群体组成也不同。     

膜气体吸收技术分离VOCs/N2混合气性能的研究

以C₆H₆/N₂混合气为代表,疏水性聚丙烯中空纤维膜为气液接触膜,n-甲酰吗啉(NFM,n-formyl morpholine)水溶液为吸收剂,研究了膜气体吸收法分离VOCs/N₂混合气性能。考察了吸收剂流量、吸收剂体积分数、进口气流量、进口气浓度和膜组件结构等诸因素对分离性能的影响。结果表明,在吸收剂流量为20～100 mL/min,进口气流量为40～300 mL/min,进口气浓度为10.2 mg/L的条件下,苯的去除率为65.0 % ～ 99.6 %,总体积传质系数为0.0157～0.08412 s^-1。实验证明,采用疏水性多孔膜气体吸收法,NFM水溶液吸收分离VOCs/N₂混合气具有较高的分离效率和较快的传质速率。     

负载型氧化铁对高毒气体PH3的催化分解

采用沉积-沉淀法制备了碳纳米管(CNTs)和二氧化硅(SiO2)负载的纳米Fe2O3催化剂,将其应用于高毒气体PH3分解反应.通过XRD,TEM,XPS,BET等一系列检测手段,对制备样品的相结构、形貌、组分和比表面积进行了表征.研究结果表明,在PH3催化分解反应过程,极少量的产物P迁移至Fe2O3中,形成金属磷化物FeP作为反应的活性相.与Fe2 O3/SiO2相比,Fe2O3/CNTs显示了较高的催化性能.在440℃反应温度下,Fe2O3/CNTs对PH3分解率达到99.8％.CNTs作为催化剂载体的优秀性能可归因于CNTs良好的导电性能和活性组分在其上的高度分散.     

柱状V/AC催化剂的再生对脱硫活性的影响

使用常压固定床反应器,考察了吸附SO2的柱状V/AC催化剂的热再生和NH3再生行为.结果表明:柱状V/AC催化剂再生过程中生成的SO2主要沿催化剂轴向由内部向外扩散.催化剂350 ℃NH3再生的效率高于热再生的效率.两次热再生后柱状V/AC催化剂的脱硫活性开始下降,而六次NH3再生后的脱硫活性仍保持不变,甚至还稍高于新鲜柱状V/AC催化剂的脱硫活性.柱状V/AC催化剂孔结构和元素分析结果表明,NH3再生使催化剂表面含N官能团增加,保护了催化剂小于1 nm的微孔.     

The application of regenerable sorbents for mercury capture in gas phase

Mercury is a well-known toxic element, and flue gas streams emitted from coal-fired utilities are one of the largest anthropogenic sources of this element. This study briefly reviews the proposed technologies for reducing mercury emissions from coal combustion, focusing on an emerging process which involves the use of regenerable sorbents and especially those loaded with noble metals. Among the mercury species formed during coal combustion, elemental mercury is the most difficult to remove from the flue gases due to its low reactivity and insolubility in water. The widespread interest in using regenerable sorbents with metals is due to their ability to retain elemental mercury. With this technology, not only can efficiencies of 100 % be reached in the retention of elemental mercury but also a way to avoid the generation of new wastes loaded with mercury. This study considers the main aspects that must be taken into account when developing effective regenerable sorbents for mercury capture, with special attention to sorbents containing noble metals. The characteristics of this process are compared with those of other processes in a more advanced state of development.     

高锰酸钾氧化吸收烟气中单质汞的研究

在鼓泡反应器中考察了高锰酸钾氧化单质汞(Hg0)的影响因素和机理,研究结果表明,KMnO4和Hg0的反应很快,去除率随KMnO4增加而增加;汞的进口浓度对汞的去除率影响不大;随pH值的升高汞的去除率先降低后增加,在强酸性(pH=0)下Hg0去除率最大,为92.4％,当pH值超过11随pH值的升高而增加。在不同酸碱体系中...     

NaCl电解氧化吸收液脱除烟气中的NOx

研究了NaCl质量浓度、电解时间对电解生成有效氯组分的影响,并以NaCl电解液作为氧化吸收液在自制的小型鼓泡喷淋吸收塔中进行模拟烟气脱硝实验,进一步研究了有效氯质量浓度、反应体系pH和温度对脱硝效果的影响,同时分析了脱硝机理。结果表明：有效氯质量浓度随着NaCl质量浓度和电解时间的增加逐渐增加,电解反应的主产物是ClO⁻。NO_x去除率随着有效氯质量浓度增加而升高;氧化体系酸度和温度增高有利于NO氧化,但不利于NO_x吸收去除。当烟气流量为2 L·min⁻¹,NO初始质量浓度为1 340 mg·m⁻³,吸收液有效氯初始质量浓度为2.5 g·L⁻¹,反应体系pH为5,温度为30 ℃时,NO的转化率可达91.1%,NO_x去除率可达78.9%,且能在该条件下长时间保持较高的烟气脱硝效果。本研究结果可为低温湿法氧化脱硝技术的工业化应用提供参考。     

The effect of SO2 gas phase oxidation on hydroxyl smog chemistry

A series of smog chamber experiments was conducted to investigate the effect of SO₂ on HO steady-state levels. Various amounts of SO₂ were added to propene-butane-NO_x-H₂O mixtures to simulate polluted air conditions. The addition of SO₂ was found to enhance slightly the rate of NO → NO₂ conversion with resultant increase in ozone formation. Although the addition of SO₂ did not reduce the HO steady state concentration during the early stages of the experiment, a significant (~ 40 %) reduction in HO steady-state concentration was observed at the highest ( ~ 6 ppm) SO₂ concentration during the latter stages. Model calculations were performed to test various mechanistic options. The model calculations indicate that the HO + SO₂ reaction leads predominantly to the production of HO₂ radicals. However, an additional O₃-consuming reaction is proposed to explain the experimental observations.     

钝顶螺旋藻固定模拟烟道气中的CO2

研究了钝顶螺旋藻对模拟烟道气中CO2的固定性能,及其对NOx和SOx水溶形态亚硝态氮、亚硫酸氢根的耐受性。结果显示:随CO2浓度的增加,藻细胞达到最大比生长速率的时间缩短,CO2浓度为15%时藻细胞比生长速率达到最大的时间最短,生物量最终达到最大值4.1 g/L;CO2浓度为15%时藻细胞的固碳率为12.34 mg/(L·h)。研究发现,钝顶螺旋藻能够耐受浓度小于10 mmol/L的亚硝态氮,可将其作为钝顶螺旋藻生长的唯一氮源,但藻生长的延迟期增长。钝顶螺旋藻能够耐受8 mmol/L的亚硫酸氢盐,可将其作为生长的唯一硫源,藻细胞6 d后开始快速增长。     

CuO-CeO_2/AC吸附燃煤烟气中元素汞的实验研究

通过活性炭负载CuO和CeO2来制备吸附剂,采用固定床吸附方式,在不同反应条件下对吸附剂的吸附性能进行测试,筛选出去除效率最好的吸附剂,并通过BET和XRD对吸附剂的理化性质进行分析。结果表明,CuO和CeO2的加入大大改变了原活性炭的比表面积和孔结构,改善了活性炭的吸附性能。CuO-CeO2/AC中CuO和CeO2质量比不同,对汞的去除效率也不同,在1∶2时去除效率最好;CuO-CeO2/AC中所负载的CuO和CeO的总量为5%时,能大大促进汞的吸附效率,增长有效吸附时间;CuO-CeO2/AC对汞的吸附性能随反应温度的增加呈先增加后减小的趋势,在80℃时达到最大值。     

PCDD/PCDF Isomer patterns in waste incinerator flyash and desorbed into the gas phase in relation to temperature

The influence of temperature on the PCDD and PCDF isomer profiles of a municipal waste incinerator flyash and the PCDD/PCDF desorbed from the ash under an inert atmosphere was investigated using a bench-scale reactor. Exposure to temperatures of 250 degrees C and above resulted in significant changes in the distribution of isomers within most dioxin and furan congener groups. The PCDD content tended to become more evenly distributed across the range of isomers than was the case for the raw flyash, while the PCDF content became concentrated across a relatively lower number of isomers. In most cases the desorbed PCDD/PCDF were mainly mono- to tri-chlorinated, and hence had a relatively low I-TEQ value. The isomer profiles of the desorbed species were also influenced by temperature. There were some significant differences between the PCDF isomer profiles of the desorbed species and those of the treated flyashes under the same conditions, but no clear differences between the PCDD isomer profiles.     

EDTA-（NH4）2FeSO4络合剂脱除烟气中的氮氧化物

络合脱硝法是近年来新型的脱除氮氧化物的方法之一,其中EDTA金属络合剂受到了广泛关注,而亚铁络合剂又具有很好的脱除氮氧化物的效果。考查了硫酸亚铁铵与EDTA形成的Fe（II）EDTA这种比较常见的EDTA金属络合剂对NO的吸收容量,并考查温度、络合剂浓度等对Fe（II）EDTA吸收NO的影响。研究结果表明：在相同的实验环境和实验条件下,对于影响Fe（II）EDTA吸收NO的因素最重要的是温度,其余依次为络合剂浓度、气体流速、氧含量、吸收液pH,最适宜吸收条件是反应温度50℃、络合剂浓度0．1mol／L、进气流速600mL／min、氧含量2％、吸收液pH=6。