碳黑改性TiO2薄膜光催化剂的研制

通过掺杂碳黑来提高TiO2薄膜光催化剂的吸附性能，消除固定膜反应体系中经常出现的传质限制问题，使催化剂的活性由未经改性的3.2mg/L提高到4.8mg/L，相当于浓度为0.2g/L DegussaP25TiO2悬浮体系的效果，同时研究了影响催化剂活性的主要制备条件，获得的适宜制备条件为浓硝酸添加量1.0mL，热处理温度500℃，热处理时间2h，最佳涂覆次数为8次。     

The hydrocarbon composition of exhaust emitted from gasoline fuelled vehicles

The non-methane hydrocarbon (NMHC) compositions of the exhausts from 67 vehicles in ‘on the road’ condition and driven through an urban driving cycle on a chassis dynamometer, have been determined. The major components were ethylene (11.2% w/w of NMHC), toluene (10.2%), acetylene (8.7%), m,p-Xylenes(6.5%), benzene (5.0%), propylene (5.0%) and i-pentane(4.8%). These compounds have also been reported as significant components in the exhausts from two similar populations of American vehicles.The NMHC compositions were found to be insensitive to the mass emission rates of hydrocarbons from the vehicles, except for the combustion-derived olefins, ethylene and propylene, which were affected by engine modifications introduced to satisfy emission control requirements. A close relationship was found between petrol composition and exhaust composition but this did not correspond simply to emissions of unburnt petrol. The aromatics are enriched relative to the alkanes in exhaust when compared with their proportions in the petrol.     

Morphology and composition of particles emitted from conventional and alternative fuel vehicles

Size, morphology, and composition of airborne particles strongly affect human health and visibility, precipitation, and the kinetic characteristics of particles. In this study, the morphology and chemical composition of particles emitted from conventional (diesel and gasoline) and alternative (CNG and methanol) fuel vehicles were characterized through scanning electron microscopy (SEM) and energy-dispersive X-ray (EDX). The SEM images revealed that the size of primary particles (without agglomeration) was approximately 10 nm in the exhaust from all the tested vehicles. The particles emitted from gasoline vehicle (GV), CNG vehicle (CNGV), and methanol vehicle (MV) had the same median diameter, 62 nm, which was smaller than those from heavy diesel vehicle (HDV) and light diesel vehicle (LDV). Soot was observed in the HDV, LDV, and GV samples but not in the CNGV and MV. The fractal dimension, which was used to quantify the degree of irregularity of soot, was 1.752 ± 0.014, 1.789 ± 0.076, and 1.769 ± 0.006 in the exhaust from HDV, LDV, and GV samples, respectively. The particles discharged by all tested vehicles contained the elements C, O, Fe, and Na. The main element in the samples of HDV, LDV, and GV was C, while O was the main element in the samples of alternative fuel vehicles. The profiles of minor elements were more complex in the emissions of alternative fuel vehicles than those in the emissions of conventional fuel vehicles. The results improved our understanding of the morphology and elemental composition of particles emitted from vehicles powered by diesel, gasoline, CNG, and methanol.

     

Evaluation of solid particle number and black carbon for very low particulate matter emissions standards in light-duty vehicles

To reliably measure at the low particulate matter (PM) levels needed to meet California’s Low Emission Vehicle (LEV III) 3- and 1-mg/mile particulate matter (PM) standards, various approaches other than gravimetric measurement have been suggested for testing purposes. In this work, a feasibility study of solid particle number (SPN, d50 = 23 nm) and black carbon (BC) as alternatives to gravimetric PM mass was conducted, based on the relationship of these two metrics to gravimetric PM mass, as well as the variability of each of these metrics. More than 150 Federal Test Procedure (FTP-75) or Supplemental Federal Test Procedure (US06) tests were conducted on 46 light-duty vehicles, including port-fuel-injected and direct-injected gasoline vehicles, as well as several light-duty diesel vehicles equipped with diesel particle filters (LDD/DPF). For FTP tests, emission variability of gravimetric PM mass was found to be slightly less than that of either SPN or BC, whereas the opposite was observed for US06 tests. Emission variability of PM mass for LDD/DPF was higher than that of both SPN and BC, primarily because of higher PM mass measurement uncertainties (background and precision) near or below 0.1 mg/mile. While strong correlations were observed from both SPN and BC to PM mass, the slopes are dependent on engine technologies and driving cycles, and the proportionality between the metrics can vary over the course of the test. Replacement of the LEV III PM mass emission standard with one other measurement metric may imperil the effectiveness of emission reduction, as a correlation-based relationship may evolve over future technologies for meeting stringent greenhouse standards.

Implications: Solid particle number and black carbon were suggested in place of PM mass for the California LEV III 1-mg/mile FTP standard. Their equivalence, proportionality, and emission variability in comparison to PM mass, based on a large light-duty vehicle fleet examined, are dependent on engine technologies and driving cycles. Such empirical derived correlations exhibit the limitation of using these metrics for enforcement and certification standards as vehicle combustion and after-treatment technologies advance.     

酸析-活性炭纤维吸附预处理精制棉黑液

采用酸析-活性炭纤维吸附工艺去除精制棉黑液中的有机物,先用酸析法去除木质素,再用活性炭纤维吸附黑液中的剩余有机物。采用紫外-可见(UV-vis)吸收光谱、傅立叶转换红外吸收光谱(FTIR)和明亮发光菌水质急性毒性法等手段分析处理前后的精制棉黑液。研究表明,黑液中主要有机成分为愈创基(G-)和羟苯基(H-)木质素。在pH为2.0,活性炭纤维用量为90 g/L,温度为40°C,吸附时间为5 h的条件下,COD去除率可以达到85%。活性炭纤维对酸析后精制棉黑液的吸附热力学符合Redlich-Peterson经验吸附模型,吸附动力学符合伪二级动力学模型,吸附为吸热过程。酸析-吸附过程使精制棉黑液急性毒性去除率达到95%以上,为后续生物法处理提供了有利条件。     

基于自碳黑的水化硅酸钙制备及其磷回收特性

以白碳黑、硅灰、硅藻土和硅胶筛选硅质原料,并与钙质原料电石渣制备了水化硅酸钙。借助XRF、BET、FT—IR等表征手段,通过多次重复除磷实验,研究了硅质原料特性对水化硅酸钙回收磷性能的影响。结果表明,白碳黑具有极高的反应活性,因此可作为制备具有磷回收特性的水化硅酸钙的硅质原料。结合XRD等表征发现,白碳黑的有效利用率是影响水化硅酸钙回收磷性能的关键,该利用率取决于白碳黑与电石渣的摩尔配比以及水热反应温度。当电石渣与白碳黑的摩尔比为1．6：1,反应温度为170℃时,白碳黑具有最佳的利用效率。该条件制备的水化硅酸钙可作为晶种,在其表面结晶形成羟基磷灰石,从而达到磷回收的目的,磷回收后固体物质中的磷含量为19．05％。     

基于白碳黑的水化硅酸钙制备及其磷回收特性简

以白碳黑、硅灰、硅藻土和硅胶筛选硅质原料,并与钙质原料电石渣制备了水化硅酸钙。借助XRF、BET、FTIR等表征手段,通过多次重复除磷实验,研究了硅质原料特性对水化硅酸钙回收磷性能的影响。结果表明,白碳黑具有极高的反应活性,因此可作为制备具有磷回收特性的水化硅酸钙的硅质原料。结合XRD等表征发现,白碳黑的有效利用率是影响水化硅酸钙回收磷性能的关键,该利用率取决于白碳黑与电石渣的摩尔配比以及水热反应温度。当电石渣与白碳黑的摩尔比为1.6：1,反应温度为170℃时,白碳黑具有最佳的利用效率。该条件制备的水化硅酸钙可作为晶种,在其表面结晶形成羟基磷灰石,从而达到磷回收的目的,磷回收后固体物质中的磷含量为19.05%。     

An investigation on the physical,chemical and ecotoxicological characteristics of particulate matter emitted from light-duty vehicles

Particulate matter (PM) emitted from three light-duty vehicles was studied in terms of its physicochemical and ecotoxicological character using Microtox^® bioassay tests. A diesel vehicle equipped with an oxidation catalyst emitted PM which consisted of carbon species at over 97%. PM from a diesel vehicle with a particle filter (DPF) consisted of almost equal amounts of carbon species and ions, while a gasoline vehicle emitted PM consisting of ～90% carbon and ～10% ions. Both the DPF and the gasoline vehicles produced a distinct nucleation mode at 120 km/h. The PM emitted from the DPF and the gasoline vehicles was less ecotoxic than that of conventional diesel, but not in direct proportion to the emission levels of the different vehicles. These results indicate that PM emission reductions are not equally translated into ecotoxicity reductions, implying some deficiencies on the actual environmental impact of emission control technologies and regulations.     

Preparation and characterisation of activated carbon from waste tea by physical activation using steam

ABSTRACT

In this study, the feasibility of preparing activated carbon from waste tea by physical activation using steam was investigated. The effects of activation temperature on yield and pore properties of the prepared activated carbon were studied. The yield decreased with increased activation temperature owing to the decomposition of cellulose and hemicellulose. The specific surface area and pore volume of the activated carbon were estimated using the Brunauer–Emmett–Teller method, Langmuir equation, and t-plot method. The specific surface area and micropore volume increased with increases in activation temperature, as additional volatile materials were released. The specific surface area significantly decreased at first but slightly increased with increasing activation time. The maximum specific surface area reached 995 m²/g at an activation temperature of 800 °C with a water flow rate of 0.075 g/min and a constant hold time of 0.5 hr. According to the nitrogen adsorption isotherms, micropores mainly developed when the activation temperature was below 800 °C, and both micropores and mesopores developed when it was above 800 °C. The results showed that activation temperature significantly affected micropore and mesopore volumes, as well as the specific surface area of the activated carbon. Overall, waste tea was found to be an attractive raw material for producing low-cost activated carbon.

Implications: Every year, a large amount of waste tea is generated after extraction. The high carbon content of waste tea showed that it can be used as raw material to produce activated carbon. This study investigated the feasibility of preparing activated carbon from waste tea by physical activation using steam. Temperature and time were found to have clear effects on pore properties. Our proposed method and raw material are more environmentally friendly and involve low cost. Furthermore, this offers a potential solution to the problems of waste tea disposal and low-cost activated carbon production.     

Soil uptake of carbon monoxide emitted in the exhaust of a gasoline-powered engine

Carbon monoxide (CO) poses dangers to both human and environmental health, sickening thousands of people annually in the United States and decreasing the capacity of the atmosphere to oxidize greenhouse gases. Globally, soil ecosystems with their populations of bacteria, fungi, and algae are estimated to remove 9-36% of total CO emissions, which makes them the second largest CO sink after hydroxyl oxidation. Our aim was determine whether soil ecosystems could remove CO from an atmosphere mixed with gasoline-powered engine exhaust. Sealed microcosms containing no soil (NoSoil), nonvegetated soil (Soil), or vegetated soil (Soil+Veg), were exposed to 800, 100, and 50 ppm of CO for 1 hr. The uptake rate of CO was found to be higher at the 800 ppm level suggesting first-order rate kinetics. Soil+Veg exhibited a significantly higher CO uptake rate than either Soil or NoSoil (P<0.05), and Soil exhibited significantly higher uptake than NoSoil (P<0.05). As a free ecosystem service, the uptake of CO by soil ecosystems needs to be properly valued and ecologically engineered into the urban traffic network in a manner analogous to how wetlands, vegetated swales, and other ecologically based storm water treatment systems have improved urban runoff.     

Determination of elemental carbon component of soot in ambient aerosol samples

A reflectance method for the determination of the elemental carbon component of soot in atmospheric fine particulate matter collected on a filter has been developed. Two instruments are described. One operates continuously as the aerosol sample is being collected, measuring the decrease in reflectance of light from the filter spot through which air is aspirated. The other instrument measures the reflectance of samples mounted after a collection on a filter. The instruments have been calibrated with soot standards of known total non-volatile carbon content determined by the GRALE technique after heating. Limited field data are presented on both the total carbon and soot carbon content of the St. Louis urban fine aerosol.     

Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method

To make progress towards linking the atmosphere and biogeosphere parts of the black carbon (BC) cycle, a chemothermal oxidation method (CTO-375), commonly applied for isolating BC from complex geomatrices such as soils, sediments and aquatic particles, was applied to investigate the BC also in atmospheric particles. Concentrations and ¹⁴C-based source apportionment of CTO-375 based BC was established for a reference aerosol (NIST RM-8785) and for wintertime aerosols collected in Stockholm and in a Swedish background area. The results were compared with thermal–optical (OC/EC) measurements. For NIST RM-8785, a good agreement was found between the BC_CTO-375 concentration and the reported elemental carbon (EC) concentration measured by the “Speciation Trends Network—National Institute of Occupational Safety and Health” method (EC_NIOSH) with BC_CTO-375 of 0.054±0.002 g g⁻¹ and EC_NIOSH of 0.067±0.008 g g⁻¹. In contrast, there was an average factor of ca. 20 difference between BC_CTO-375 and EC_NIOSH for the ambient Scandinavian wintertime aerosols, presumably reflecting a combination of BC_CTO-375 isolating only the recalcitrant soot-BC portion of the BC continuum and the EC_NIOSH metric inadvertently including some intrinsically non-pyrogenic organic matter. Isolation of BC_CTO-375 with subsequent off-line radiocarbon analysis yielded fraction modern values (fM) for total organic carbon (TOC) of 0.93 (aerosols from a Swedish background area), and 0.58 (aerosols collected in Stockholm); whereas the fM for BC_CTO-375 isolates were 1.08 (aerosols from a Swedish background area), and 0.87 (aerosols collected in Stockholm). This radiocarbon-based source apportionment suggests that contribution from biomass combustion to cold-season atmospheric BC_CTO-375 in Stockholm was 70% and in the background area 88%.     

Multiple-year black carbon measurements and source apportionment using delta-C in Rochester, New York

Black carbon (BC), an important component ofthe atmospheric aerosol, has climatic, environmental, and human health significance. In this study, BC was continuously measured using a two-wavelength aethalometer (370 nm and 880 nm) in Rochester; New York, from January 2007 to December 2010. The monitoring site is adjacent to two major urban highways (I-490 and I-590), where 14% to 21% of the total traffic was heavy-duty diesel vehicles. The annual average BC concentrations were 0.76 microg/m3, 0.67 microg/m3, 0.60 microg/m3, and 0.52 microg/m3 in 2007, 2008, 2009, and 2010, respectively. Positive matrix factorization (PMF) modeling was performed using PM2.5 elements, sulfate, nitrate, ammonia, elemental carbon (EC), and organic carbon (OC) data from the US. Environmental Protection Agency (EPA) speciation network and Delta-C (UVBC370nm-BC880nm) data. Delta-C has been previously shown to be a tracer of wood combustion factor It was used as an input variable in source apportionment models for the first time in this study and was found to play an important role in separating traffic (especially diesel) emissions from wood combustion emissions. The result showed the annual average PM2.5 concentrations apportioned to diesel emissions in 2007, 2008, 2009, and 2010 were 1.34 microg/m3, 1.25 microg/m3, 1.13 microg/m3, and 0.97 microg/m3, respectively. The BC conditional probability function (CPF) plots show a large contribution from the highway diesel traffic to elevated BC concentrations. The measurements and modeling results suggest an impact of the US Environmental Protection Agency (EPA) 2007 Heavy-Duty Highway Rule on the decrease ofBC and PM2.5 concentrations during the study period.     

Multiple-year black carbon measurements and source apportionment using Delta-C in Rochester,New York

Black carbon (BC), an important component of the atmospheric aerosol, has climatic, environmental, and human health significance. In this study, BC was continuously measured using a two-wavelength aethalometer (370 nm and 880 nm) in Rochester, New York, from January 2007 to December 2010. The monitoring site is adjacent to two major urban highways (I-490 and I-590), where 14% to 21% of the total traffic was heavy-duty diesel vehicles. The annual average BC concentrations were 0.76 μg/m³, 0.67 μg/m³, 0.60 μg/m³, and 0.52 μg/m³ in 2007, 2008, 2009, and 2010, respectively. Positive matrix factorization (PMF) modeling was performed using PM_2.5 elements, sulfate, nitrate, ammonia, elemental carbon (EC), and organic carbon (OC) data from the U.S. Environmental Protection Agency (EPA) speciation network and Delta-C (UVBC_370nm – BC_880nm) data. Delta-C has been previously shown to be a tracer of wood combustion factor. It was used as an input variable in source apportionment models for the first time in this study and was found to play an important role in separating traffic (especially diesel) emissions from wood combustion emissions. The result showed the annual average PM_2.5 concentrations apportioned to diesel emissions in 2007, 2008, 2009, and 2010 were 1.34 μg/m³, 1.25 μg/m³, 1.13 μg/m³, and 0.97 μg/m³, respectively. The BC conditional probability function (CPF) plots show a large contribution from the highway diesel traffic to elevated BC concentrations. The measurements and modeling results suggest an impact of the U.S Environmental Protection Agency (EPA) 2007 Heavy-Duty Highway Rule on the decrease of BC and PM_2.5 concentrations during the study period.

Implications: This study suggests that there was an observable impact of the U.S EPA 2007 Heavy-Duty Highway Rule on the ambient black carbon concentrations in Rochester, New York. Aethalometer Delta-C was used as an input variable in source apportionment models and it allowed the separation of traffic (especially diesel) emissions from wood combustion emissions.     

Investigation of soot by two-colour four-wave mixing

A novel technique has been used for the temporally resolved investigation of the interaction of laser radiation and soot in a flame. Based on established soot vaporisation models we developed a framework to calculate the two-colour four-wave mixing signal obtained in an acetylene/air diffusion flame at atmospheric pressure. The signal comprises a contribution due to soot and, depending on the wavelength of the probe laser, a contribution because of C2, which is generated by vaporising soot. For both parts of the signal we found a good agreement between measured and calculated power dependency. Furthermore, we measured spatial profiles of the signal in a Wolfhard-Parker slot burner. By analysing the different signal contributions we found that depending on the location within the flame there are particles with different C2 yield.     

混凝——吸附法处理油墨废水工艺研究

采用不同无机混凝剂及氧化还原剂对打印机生产中的油墨废水的混凝及脱色效果进行试验比较,确定了实验室工艺条件及各种混凝剂最佳用量及次序。结果表明,该工艺脱色率达１００％,ＣＯＤｃｒ去除率达５１％。     

The fate of PAHs in the carbon black manufacturing process

This study measured PAHs contained in the feedstock oil, carbon black products, and stack flue gas, then the fate of PAHs was assessed from the mass balance point of view for a carbon black manufacturing process. Results show the carbon black manufacturing process would result in the depletion of total-PAHs and the summation of top three carcinogenic PAH species (i.e., BbF+BaP+DBA) up to 98.15% and 99.83%, respectively. The above results suggest that the carbon black manufacturing process would result in not only the decrease of the amount of total-PAHs, but also the carcinogenic potencies of PAHs originally contained in the feedstock oil. Regarding PAHs contained in the carbon black products and stack flue gas, this study suggest they might be resulted mostly from high-temperature pyrolytic process, rather than the PAHs originally contained in the feedstock oil. For the carbon black manufacturing industry, since the soot (i.e., the carbon black) was completely collected as its final product, therefore most of carbon black-bearing PAHs did not directly release to atmosphere. On the other hand, PAHs contained in the stack flue gas were directly exhausted to the atmosphere and thus were assessed in this study. The results show the emission rates for total-PAHs and BbF+BaP+DBA for the stack flue gas were 2.18 kg/day and 1.50 g/day, respectively, which were approximately 25% and 40% of those exhausted from a municipal incinerator with a treatment capacity of 300 metric tons/day. It is concluded that the carbon black manufacturing process might not be a significant PAHs emission source, as compared to the municipal incinerator.