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A rapid reaction occurs near the exhaust nozzle when vehicle emissions contact the air. Twenty diesel vehicles were studied using a new multipoint sampling system that is suitable for studying the exhaust plume near the exhaust nozzle. The variation characteristics of fine particle matter (PM2.5) and its components in diesel vehicle exhaust plumes were analyzed. The PM2.5 emissions gradually increased with increasing distance from the nozzle in the plume. Elemental carbon emissions remained basically unchanged, organic carbon and total carbon (TC) increased with increasing distance. The concentrations of SO42-, NO3- and NH4+ (SNA) directly emitted by the vehicles were very low but increased rapidly in the exhaust plume. The selective catalytic reduction (SCR) reduced 42.7% TC, 40% NO3- emissions, but increased 104% SO42- and 36% NH4+ emissions, respectively. In summary, the SCR reduced 29% primary PM2.5 emissions for the tested diesel vehicles. The NH4NO3 particle formation maybe more important in the plume, and there maybe other forms of formation of NH4+ (eg. NH4Cl). The generation of secondary organic carbon (SOC) plays a leading role in the generation of secondary PM2.5. The SCR enhanced the formation of SOC and SNA in the plume, but comprehensive analysis shows that the SCR more enhanced the SNA formation in the plume, which is mainly new particles formation process. The inconsistency between secondary organic aerosol (SOA) and primary organic aerosol definitions is one of the important reasons for the difference between SOA simulation and observation.

Ion exchange membranes (IEMs) are widely used in water treatment applications such as electrodialysis. However, the exploration of IEMs as effective antibacterial food contact materials (e.g., food packaging membranes) against pathogenic bacteria to ensure food safety has not been reported. Here, we report a simple but effective method to prepare high performance antibacterial membranes via ion exchange coupled with in-situ reduction. The general membrane properties are characterized using SEM, EDS, FTIR, XPS, XRD, DSC, TGA, water uptake, etc. The distribution of silver and copper in the membranes are generally in line with the distribution of sulfur, indicating that the antibacterial ions are introduced into the membranes via ion exchange and are bonded with the sulfonate groups in the membranes. The antibacterial performance is investigated using zone of inhibition tests and continuous bacteria growth inhibition tests. All of the prepared membranes show obvious antibacterial activities compared to the bare cation exchange membranes. The diameters of inhibition zone against Staphylococcus aureus (S. aureus) are all larger than those of Escherichia coli (E. coli), indicating that the prepared membranes are more efficient in inhibiting S. aureus compared to E. coli. Furthermore, the silver-based membrane shows more sustainable antibacterial activities compared to the copper-based membrane. Especially, the results clearly reveal that the silver-based membrane is capable of killing bacteria instead of just inhibiting the growth of bacteria. We have shown for the first time that membranes derived from IEMs have the potential as food contact materials to inhibit the growth of pathogenic bacteria so as to eliminate the risk of bacterial infections and meanwhile delay food spoilage due to bacteria growth.

In order to make clear the role of intercalated anions in layered double hydroxides (LDHs) for catalytic hydrolysis of carbonyl sulfide (COS), the adsorption and reaction characteristics of COS over the simple Mg2Al-Cl-LDH model catalyst were studied by both theoretical and experimental methods. Density functional theory (DFT) calculations by CASTEP found that the chloride ions in LDH function as the key Bronsted base sites to activate the adsorbed H2O with enlarged bond length and angle, facilitate the dissociative adsorption of intermediates including mono-thiocarbonic acid (MTA) and hydrogen thiocarbonic acid (HTA), and participate in the formation of transient states and subsequent hydrogen transfer process with decreased energy barriers during COS hydrolysis. COS hydrolysis will preferentially go through the dissociated intermediates of mono-thiocarbonates (MT) and hydrogen thiocarbonates (HT) with dramatically decreased energy barriers, and the rate-determining step of COS hydrolysis over Mg2Al-Cl-LDH will be the nucleophilic addition of C=O in COS by H2O (Ea = 1.10 eV). The experimental results further revealed that the apparent activation energy (0.89 eV) of COS hydrolysis over Mg2Al-Cl-LDH is close to theoretical value (1.10 eV), and the accumulated intermediates of MT, HT, or carbonate were also observed by FT-IR around 1363 cm−1 on the used Mg2Al-Cl-LDH, which are well in accordance with the theoretical prediction. The demonstrated participation of intercalated chlorine anions in the evolution of intermediates and transient states as Bronsted base sites during COS hydrolysis will give new insight into the basic sites in LDH materials.

Medium-flow atmospheric samplers were used to collect particulate (PM2.5) and gaseous samples from the indoor kitchen of each of 35 randomly selected rural houses in North China while a meal was being cooked. The concentrations of 16 polycyclic aromatic hydrocarbons (PAHs) and 9 nitro-PAHs (NPAHs) in the samples were quantified by high-performance liquid chromatography (HPLC). This study provided the real PAH and NPAH pollution characteristics and carcinogenic risk produced by cooking in rural indoor kitchens in North China. The mean PAH and NPAH concentrations in air in the indoor kitchens during cooking periods were 4049.1 and 1741.6 ng/m3, respectively. The PAH and NPAH concentrations were lower in the particulate phase than the gaseous phase. The mean PAH and NPAH concentrations were much higher for cooking using coal than for cooking using liquefied petroleum gas (LPG) or electricity. The PAH and NPAH benzo[a]pyrene toxic equivalent (TEQBaP) concentrations for cooking using coal were 1823.3 and 2760.9 ng/m3, respectively. Lower PAH and NPAH concentrations were found in kitchens with than without range hoods. Range hoods decreased the PAH and NPAH TEQBaP concentrations by 68.8% and 61.9%, respectively. Appropriate fuel and ventilation choice will improve air pollution in indoor kitchens during cooking. The results provide important evidence for changing cooking habits and developing policies for cooking in rural China.

In order to reduce foodborne diseases caused by bacterial infections, antibacterial membranes have received increasing research interests in recent years. In this study, highly effective antibacterial membranes were prepared using biodegradable polymers, including polylactic acid (PLA), polybutylene adipate terephthalate (PBAT), and carboxymethyl cellulose (CMC). The cation exchange property of CMC was utilized to introduce silver to prepare antibacterial materials. The presence of silver in the membranes was confirmed by EDS mapping, and the reduction of silver ions to metallic silver was confirmed by the Ag3d XPS spectrum which displayed peaks at 374.46 eV and 368.45 eV, revealing that the oxidation state of silver changed to zero. Two common pathogenic bacteria, Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli), were used to investigate the antibacterial performance of the prepared membranes. Zone of inhibition and bacteria-killing tests revealed that the antibacterial membranes were efficient in inhibiting the growth of bacteria (diameters of inhibition zone ranged from 16 mm to 19 mm for fresh membranes) and capable of killing 100% of bacteria under suitable conditions. Furthermore, after 10 cycles of continuous zone of inhibition tests, the membranes still showed noticeable antibacterial activities, which disclosed the sustainable antibacterial properties of the membranes.

To study the formation process of secondary organic aerosols (SOA) in a vehicle exhaust plume near the exhaust gas discharge outlet, a new multipoint sampling system was established. The system has five sampling heads and includes a particulate matter multi-channel film sampling system, a CO2/CO analyzer system, a volatile organic compound (VOC) sampling system, a particulate matter real-time analyzer system, and sensor interfaces. The vehicle exhaust near the exhaust nozzle can be sampled at multiple locations simultaneously using the new multipoint sampling system. Additionally, the system can be used to measure and analyze variations in the fine particulate matter, including the carbonaceous and ionic components, and organic compounds in the plume near the exhaust nozzle. This paper introduces the construction and application of the multipoint sampling system. The motor vehicle exhaust multipoint sampling system is reliable and can accurately capture the characteristics of the exhaust plume near the discharge outlet area. Changes in the CO2 concentration were used to determine whether exhaust was accurately collected at the sampling points. The relationship between the dilution rate and distance was calculated on the basis of on-road test results using the following equation: DR = 21.4X1.16. This equation can be used for modeling purposes, especially in comparisons of model results and observations and in the evaluation of dispersion models.

Polycyclic aromatic hydrocarbon (PAH) and nitro-polycyclic aromatic hydrocarbon (NPAH) emissions from 18 diesel trucks of different sizes and with different emission standards were tested in Beijing using a portable emission measurement system (PEMS). Both the gaseous- and particulate-phase PAHs and NPAHs were quantified by high-performance liquid chromatography (HPLC) in the laboratory. The emission factors (EFs) of the total PAHs from light-duty diesel trucks (LDDTs), medium-duty diesel trucks (MDDTs) and heavy-duty diesel trucks (HDDTs) were 82229.11 ± 41906.06, 52867.43 ± 18946.47 and 93837.35 ± 32193.14 μg/km, respectively, much higher than the respective values of total NPAHs from their counterpart vehicles. The gaseous phase had an important contribution to the total PAHs and NPAHs, with a share rate of approximately 69% and 97% on average, respectively. The driving cycle had important impacts on the emissions of PAHs and NPAHs, especially for LDDTs and HDDTs. Higher emissions of PAHs and NPAHs were detected on non-highway roads compared to that on highways for these two types of vehicles. Compared to the results of different studies, the difference in the EFs of PAHs and NPAHs can reach several orders of magnitudes, which would introduce errors in the development of an emission inventory of PAHs and NPAHs.

Biofuel stoves are an important source of black carbon (BC) emissions, which have adverse effects on the environment and human health, especially in rural areas. However, there have been only limited studies of BC emissions from residential biofuel stoves based on real-time measurements. In this study, a photo-acoustic extinctiometer (PAX)-based real-time measurement system was employed to monitor the emission characteristics of corncobs, corn stalks, cotton stalks and poplar branches in simple or improved stoves (with a total of 16 units) in Hebei Province, China. The real-time and phased emissions of BC, fine particulate matter (PM2.5), carbon monoxide (CO) and carbon dioxide (CO2) were assessed, and the effects of stove type and fuel on emissions were analyzed. Under the same conditions, polar branches were associated with the highest BC emission factors (EFs) of up to 2.64 ± 0.42 g kg−1, while the EFs for improved stoves were higher than those for simple stoves. During the ignition phase, BC emissions were found to be low, while the later addition of fuel dramatically increased emissions, followed by a gradual decrease until the next fuel addition. The phased results show that the flaming phase had the highest BC emission rate, the fuel addition phase was associated with the highest BC EF. The BC emission rates and EFs for the ignition, fuel addition, flaming and smoldering phases ranged from 0.0014–0.014, 0.11–6.32, 0.18–2.24 and 0.03–0.32 mg s−1, and from 0.04–0.18, 0.38–9.53, 0.45–3.55 and 0.12–1.01 g kg−1, respectively. This study assessed the BC emissions from residential biofuel stoves using a larger sample size than in prior work. The results increase our understanding of the BC emissions process, which is helpful in terms of improving the accuracy of BC EF estimations. The real-time measurement process described herein is also expected to provide new approaches to minimizing BC emissions.

This study is the third in a series of three papers aimed at characterizing the VOC emissions of vehicles in Beijing. In this study, 30 light-duty vehicles fueled with gasoline were evaluated using a portable emission measurement system (PEMS) as they were driven on a predesigned, fixed test route. All of the tested vehicles were rented from private vehicle owners and spanned regulatory compliance guidelines ranging from Pre-China I to China IV. Alkanes, alkenes, aromatics and some additional species in the exhaust were collected in Tedlar bags and analyzed using gas chromatography/mass spectrometry (GC–MS). Carbonyls were collected on 2,4-dinitrophenyhydrazine (DNPH) cartridges and analyzed using high-performance liquid chromatography (HPLC). Overall, 74 VOC species were detected from the tested vehicles, including 22 alkanes, 6 alkenes, 1 alkyne, 16 aromatics, 3 cyclanes, 10 halohydrocarbons, 12 carbonyls and 4 other compounds. Alkanes, aromatics and carbonyls were the dominant VOCs with weight percentages of approximately 36.4%, 33.1% and 17.4%, respectively. The average VOC emission factors and standard deviations of the Pre-China I, China I, China II, China III and China IV vehicles were 469.3 ± 200.1, 80.7 ± 46.1, 56.8 ± 37.4, 25.6 ± 11.7 and 14.9 ± 8.2 mg/km, respectively, which indicated that the VOC emissions significantly decreased under stricter vehicular emission standards. Driving cycles also influenced the VOC emissions from the tested vehicles. The average VOC emission factors based on the travel distances of the tested vehicles under urban driving cycles were greater than those under highway driving cycles. In addition, we calculated the ozone formation potential (OFP) using the maximum incremental reactivity (MIR) method. The results of this study will be helpful for understanding the true emission levels of light-duty gasoline vehicles and will provide information for controlling VOC emissions from vehicles in Beijing, China.

This work assessed the effects of biodiesel on carbonyl emissions from diesel trucks. Biodiesel converted from waste cooking oil was employed and mixed with commercial fossil diesel to produce four blends: B0 (pure conventional diesel fuel), B5 (5% v/v biodiesel), B20 (20% v/v biodiesel) and B100 (pure biodiesel). Four diesel trucks were tested under real-world conditions using a portable emissions measurement system, including one China III light-duty diesel truck (LDDT), one China IV LDDT, one China III heavy-duty diesel truck (HDDT) and one China IV HDDT. A driving cycle including highway (HW) and non-highway (NHW) driving conditions was employed and carbonyls were sampled using 2,4-dinitrophenylhydrazine cartridges and analyzed via high performance liquid chromatography. Seven carbonyl compounds were detected, and formaldehyde, acetaldehyde, acetone and butyraldehyde were the primary carbonyls. Total carbonyl emissions from the China III LDDT, China III HDDT and China IV HDDT vehicles with selective catalytic reduction decreased monotonically with increases in the biodiesel proportion, while the China IV LDDT with a particle oxidation catalyst system showed an increasing trend. With increases in the biodiesel proportions, complementary variations were observed in the proportions of formaldehyde and butyraldehyde obtained using the China III LDDT, China IV LDDT and China III HDDT vehicles. However, in the case of the China IV HDDT trials, the formaldehyde and acetaldehyde emissions exhibited complementary variations. Under different driving conditions, the effects of adding biodiesel on carbonyl emission factors were different. In China III LDDT trials, biodiesel reduced carbonyl emissions to a greater extent under HW conditions, but the opposite occurred in China III HDDT tests. Using the China IV LDDT vehicle, the emission factors did not increase as much during HW trials compared with NHW trials when the B5 and B20 fuels were used, but were significantly higher than the NHW values when pure biodiesel was employed. In China III LDDT data, the proportions of formaldehyde, acetaldehyde and butyraldehyde showed opposite variations under the two driving conditions. Using the China IV LDDT vehicle, a significant increase in formaldehyde and decrease in butyraldehyde were found during HW trials, but not NHW trials. Ozone formation potentials were obtained from carbonyls emission factors using the maximum incremental reactivity method and their variations were similar to those of the carbonyl emission factors.

A considerable amount of volatile organic compounds (VOCs) is emitted, and a vast amount of citric acid residue (CAR) waste is simultaneously produced during citric acid production. Thus, a suitable method realizing the clean production of citric acid must be developed. This study investigated the adsorption of the multicomponent VOCs in a homemade CAR waste-based activated carbon (CAR-AC). A fixed-bed experimental setup was used to explore the adsorption and desorption of single- and multi-component VOCs. Surface adsorption and diffusion molecular models with different defects were built to study the underlying adsorption and diffusion mechanisms of multicomponent VOCs on CAR-AC. The adsorption amount of ethyl acetate in CAR-AC from multicomponent VOCs was 3.04 and 5.91 times higher than those of acetone and acetaldehyde, respectively, and the interaction energy between ethyl acetate and C surfaces was low at −13.41 kcal/mol. During desorption, the most weakly adsorbed acetaldehyde desorbed from the surface of CAR-AC first, followed by acetone and ethyl acetate. The regeneration efficiencies of acetaldehyde, acetone, and ethyl acetate reached 88.77, 85.55, and 91.46 %, respectively, after four adsorption/desorption cycles. We aimed to provide a new strategy to realize the recycle use of CAR and the clean production of citric acid.

The polycyclic aromatic hydrocarbon (PAH) and nitro-polycyclic aromatic hydrocarbon (NPAH) emissions from 16 gasoline passenger cars, encompassing five emission standards and two driving conditions, were tested using a portable emission measurement system (PEMS) in Beijing under on-road conditions. In total, 16 PAHs and 9 NPAHs were quantified in both the gaseous and particulate phases by high-performance liquid chromatography (HPLC). The results indicated that lower PAH and NPAH emissions were observed with improved emission standards, especially for China 3 to China 5 vehicles (P 0.05). Higher emission factors (EFs) were detected on nonhighway roads than on highway roads due to incomplete combustion. Although most PAHs and NPAHs were in the gas-phase, the TEQ

Heavy-duty diesel trucks (HDDTs) are gaining more attention because of their contribution to NOX and PM2.5 emissions. To evaluate their contribution to ambient fine particulate matter (PM2.5), not only their emission factors, but also their source profile is required. We conducted on-road emissions tests to characterize the PM2.5 emission, documenting per second mass emission rates from in-use HDDTs in China, using portable emissions measurement systems. The average PM2.5 emission factors for pre-EURO and EURO 1 HDDTs were 1.104 g/km and 0.822 g/km, equivalent to 6.106 g/kg and 3.132 g/kg based on fuel consumption. Element carbon (EC) and organic carbon (OC) were the major components: EC accounted for 45–65% of PM2.5 for pre-EURO HDDTs and 36–69% for EURO 1 HDDTs, while the OC fraction for pre-EURO and EURO 1 HDDTs ranged from 20 to 31% and 19–31%, respectively. Thus, the average EC emission factors for pre-EURO and EURO 1 HDDTs were 0.667 g/km and 0.502 g/km, showing that implementation of tighter emission standards resulted in a 25% EC output reduction from pre-EURO to EURO 1 vehicles. Sulfate, comprising about 1% of PM2.5 mass, is still an abundant species in PM2.5 from HDDTs because of the high sulfur content in diesel fuel in China. Using these data, we updated national PM2.5 emission profiles for pre-EURO and EURO 1 HDDTs.

This paper is the second in a series of papers aimed at understanding volatile organic compound (VOC) emissions from motor vehicles in Beijing using on-board emission measurements, focusing specifically on rural vehicles (RVs). In this work, 13 RVs, including 6 different 3-wheel (3-W) RVs and 7 different 4-wheel (4-W) RVs, were examined using a portable emissions measurement system (PEMS) as the vehicles were driven on predesigned fixed test routes in rural areas of Beijing. Overall, 50 VOC species were quantified in this study, including 18 alkanes, 5 alkenes, 11 aromatics, 13 carbonyls and 3 other compounds. The average emission factor (EF) of the total VOCs for the 4-W RVs based on the distance traveled was 326.2 ± 129.3 mg/km, which is 2.5 times greater than that of the 3-W RVs. However, the VOC emissions for the 3-W RVs had higher EFs based on their CO2 emissions due to the different fuel economies of the two types of RVs. Formaldehyde, toluene, acetaldehyde, m-xylene, p-xylene, isopentane, benzene, ethylbenzene, n-pentane, 2-methoxy-2-methylpropane and butenal were the dominant VOC species from the RVs, accounting for an average of 68.6% of the total VOC emissions. Overall, the RVs had high proportions of aromatics and carbonyls. The ozone formation potentials (OFPs) were 670.6 ± 227.2 and 1454.1 ± 643.0 mg O3/km for the 3-W and 4-W RVs, respectively, and approximately 60%–70% of the OFP resulted from carbonyls. We estimated that the 3-W and 4-W RVs accounted for approximately 50% and 10%, respectively, of the total OFP caused by diesel vehicles (including diesel trucks and RVs) in Beijing in 2012. Thus, more attention should be given to VOC emissions and their impact on ozone formation.

This paper is the first in our series of papers aimed at understanding the volatile organic compound (VOC) emissions of vehicles in Beijing by conducting on-board emission measurements. This paper focuses on diesel vehicles. In this work, 18 China III diesel vehicles, including seven light-duty diesel trucks (LDDTs), four medium-duty diesel trucks (MDDTs) and seven heavy-duty diesel trucks (HDDTs), were examined when the vehicles were driven on predesigned fixed test routes in Beijing in China using a portable emissions measurement system (PEMS). Tedlar bag sampling and 2,4-dinitrophenyhydrazine (DNPH) cartridge sampling were used to collect VOC species, and gas chromatography-mass spectrometry (GC/MS) and high-performance liquid chromatography (HPLC) were used to analyze these samples. We obtained the VOC emission factors and relative compositions for diesel trucks of different sizes under different driving patterns. In total, 64 VOC species were quantified in this study, including 25 alkanes, four alkenes, 13 aromatics, 13 carbonyls and nine other compounds. The emission factors of the total VOCs based on mileage traveled for HDDTs were higher than those of LDDTs and MDDTs. Carbonyls, aromatics and alkanes were the dominant VOC species. Carbonyls accounted for 42.7%–69.2% of the total VOCs in the three types of tested diesel trucks. The total VOC emission factors of the tested vehicles that were driven on non-highway routes were 1.5–2.0 times higher than those of the vehicles driven on the highway. As for the OFP calculation results, with increased vehicle size, the ozone formation potential presented an increasing trend. Among the VOC components, carbonyls were the primary contributor to OFP. In addition, the OFPs under non-highway driving cycles were 1.3–1.7 times those under highway driving cycles. The results of this study will be helpful in improving our understanding of VOCs emitted from on-road diesel trucks in China.

To study the emission characteristics of carbonyl compounds for in-use diesel vehicles on real roads, nine in-use heavy-duty diesel trucks (HDDTs) representing different emission standards from China 0 to China 3 were tested on roads in Xiamen using an on-board carbonyl compound sampling system with a 2,4-DNPH cartridge. High-performance liquid chromatography (HPLC) was used to quantify the carbonyl compound emission factors. In total, 10 carbonyl compounds were detected for all the tested vehicles in this work. Formaldehyde, acetaldehyde and propanal were the three largest contributors of carbonyl emissions, accounting for 47.9%, 21.0% and 9.9% of the total carbonyls, respectively. The emission standards had a significant effect on the emission factors and profiles of the carbonyl compounds from the test vehicles. The total emissions of carbonyls from the test vehicles with China 0, China 1, China 2 and China 3 emission standards were 318.4, 232.8, 108.1 and 88.8 mg/km, respectively. The relative contribution of formaldehyde to the total carbonyl emissions increased with increasing stringency of the emission standards. Driving patterns also affected the vehicular carbonyl emissions. The total carbonyl emissions under highway driving cycles were lower than those under non-highway driving cycles. In addition, the ozone-formation potential of the carbonyls from the tested diesel vehicles was analyzed. This work represents a preliminary step in measuring carbonyl emission characteristics using portable emission measurement systems (PEMS). More attention should be paid to carbonyl emissions from HDDTs.