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Mechanism of accelerating soot oxidation by NO2 from diesel engine exhaust
2020
Li, Zehong | Zhang, Wei | Chen, Zhaohui | Jiang, Qianyu
NO₂ oxidation of soot exhausted from engines is more efficient than O₂ under low-temperature conditions, and is crucial for diesel particulate filter to control soot pollution. To explore the principle behind accelerating soot oxidation by NO₂, this paper uses density functional theory to reveal soot oxidation process by NO₂. This study contributes to understanding rules of soot oxidation by NO₂ and perfecting soot oxidation models to develop soot emission control technologies. Results show that NO₂ oxidation of pyrene radical involves three steps. Firstly, NO₂ attacks the C∗ atom to form –C (NO₂) with reaction energy of 306.3 kJ/mol, which decomposes to produce a –C (O) compound. Secondly, another NO₂ molecule climbs over an energy barrier of 8.8 kJ/mol, and changes into a –C (ONO₂) intermediate on –C (O). Finally, the N or O atom of NO₂ attacks –C (O) for a second time to help open aromatic ring for releasing CO or CO₂. Further decomposition of –C (NO₂) and –C (ONO₂) requires activation energies of 81.6 kJ/mol, 75.7 kJ/mol, and 53.5 kJ/mol, respectively, on preferential pathways. Calculations prove that attacks of O atom from NO₂ on C∗ help open the aromatic ring more efficiently than N atom.
Show more [+] Less [-]Importance of the structure and micropores of sedimentary organic matter in the sorption of phenanthrene and nonylphenol
2020
Xu, Decheng | Hu, Shujie | Xiong, Yongqiang | Yang, Yu | Ran, Yong
The demineralized fraction (DM), lipid-free fraction (LF), nonhydrolyzable organic carbon fraction (NHC), and black carbon (BC) were isolated from five marine surface sediments, and they were characterized by elemental analysis as well as CO₂ and N₂ adsorption techniques, respectively. The NHC fractions were characterized using advanced solid-state ¹³C nuclear magnetic resonance (NMR) and x-ray photoelectron spectroscopy (XPS). Then, the sorption isotherms of phenanthrene (Phen) and nonylphenol (NP) on all of the samples were investigated by a batch technique. The CO₂ micropore volumes were corrected for the outer specific surface areas (SSAs) by using the N₂-SSA. Significant correlations between the micropore-filling volumes of Phen and NP and the micropore volumes suggested that the micropore-filling mechanism dominated the Phen and NP sorption. Meanwhile, the (O + N)/C atomic ratios were negatively and significantly correlated with the sorption capacities of Phen and NP, indicating that the sedimentary organic matter (SOM) polarity also played a significant role in the sorption process. In addition, a strong linear correlation was demonstrated between the aromatic C and the sorption capacity of Phen for the NHC fractions. This study demonstrates the importance of the micropores, polarity, and aromaticity on the sorption processes of Phen and NP in the sediments.
Show more [+] Less [-]Compliance of indoor air quality during sleep with legislation and guidelines – A case study of Lisbon dwellings
2020
Canha, Nuno | Alves, Ana Carolina | Marta, Catarina Simão | Lage, Joana | Belo, Joana | Faria, Tiago | Cabo Verde, Sandra | Viegas, Carla | Alves, Célia | Almeida, Susana Marta
This study aimed to provide a comprehensive characterisation of the indoor air quality during the sleeping period of 10 couples at Lisbon dwellings, using a multi-pollutant approach, and to understand how the compliance with legislation and guidelines was to assure a good indoor air quality. The assessment of indoor air quality was conducted in the cold season using real time monitors during the sleeping period for comfort parameters (temperature and relative humidity) and air pollutants (carbon dioxide – CO₂, carbon monoxide – CO, formaldehyde – CH₂O, total volatile organic compounds – VOCs, and particulate matter – PM₂.₅ and PM₁₀), together with active sampling of bioaerosols (fungi and bacteria) before and after the sleeping period. Lower compliance (less than 50% of the cases) with the Portuguese legislation was found for temperature, CO₂ (3440 ± 1610 mg m⁻³), VOCs (1.79 ± 0.99 mg m⁻³) and both bioaerosol types. In 70% of the cases, PM₂.₅ (15.3 ± 9.1 μg m⁻³) exceeded the WHO guideline of 10 μg m⁻³. All bedrooms presented air change rates above the recommended minimum value of 0.7 h⁻¹, highlighting that a good indoor air quality during sleep is not guaranteed.
Show more [+] Less [-]A new experimental setup for measuring greenhouse gas and volatile organic compound emissions of silage during the aerobic storage period in a special silage respiration chamber
2020
Krommweh, Manuel S. | Schmithausen, Alexander J. | Deeken, Hauke F. | Büscher, Wolfgang | Maack, Gerd-Christian
The aim of this study was to develop a new experimental setup to determine parallel the emissions of greenhouse gases (GHG) and volatile organic compounds (VOCs) from silage during the opening as well as the subsequent aerobic storage phase of the complete bale without wrapping film. For this purpose, a special silage respiration chamber was used in which a silage bale could be examined. The gas analysis (CO₂, methanol, ethanol, ethyl acetate) of inlet, ambient and outlet air of the silage respiration chamber was carried out by photoacoustic spectroscopy. The gas samples taken inside the bale were analysed by gas chromatography for CO₂, O₂, CH₄, and N₂O. Three silage bales (grass and lucerne) as the smallest silage unit commonly used in practice were examined. The emission behaviour of the bales was recorded during experimental periods up to 55 days. The results allow a differentiation of the outgassing processes. On the one hand, gases produced during the anaerobic ensiling process (CO₂, CH₄, N₂O) are released once in a large amount during the first experimental hours after opening the silage. On the other hand, a continuous outgassing process takes place, which is particularly true for the VOCs ethanol, methanol, and ethyl acetate, whereby VOC emissions increase with rising ambient air temperatures. In this study, the emissions during the first 600 experimental hours from the grass silage bale and lucerne silage bale were 2313 g and 2612 g CO₂, 17.6 g and 145.2 g methanol, 132.3 g and 675.9 g ethanol, 55.1 g and 66.2 g ethyl acetate, respectively. Nevertheless, the focus of this study was on the technical recording of gas concentrations inside the silage bale itself and the emissions in the ambient air of the bale. For a better interpretation of the data, additional factors should be considered in further investigations.
Show more [+] Less [-]A new perspective of probing the level of pollution in the megacity Delhi affected by crop residue burning using the triple oxygen isotope technique in atmospheric CO2
2020
Laskar, Amzad H. | Maurya, Abhayanand S. | Singh, Vishvendra | Gurjar, Bhola R. | Liang, Mao-Chang
Air quality in the megacity Delhi is affected not only by local emissions but also by pollutants from crop residue burning in the surrounding areas of the city, particularly the rice straw burning in the post monsoon season. As a major burning product, gaseous CO₂, which is rather inert in the polluted atmosphere, provides an alternative solution to characterize the impact of biomass burning from a new perspective that other common tracers such as particulate matters are limited because of their physical and chemical reactiveness. Here, we report conventional ([CO₂], δ¹³C, and δ¹⁸O) and unconventional (Δ¹⁷O) isotope data for CO₂ collected at Connaught Place (CP), a core area in the megacity Delhi, and two surrounding remote regions during a field campaign in October 18–20, 2017. We also measured the isotopic ratios near a rice straw burning site in Taiwan to constrain their end member isotopic compositions. Rice straw burning produces CO₂ with δ¹³C, δ¹⁸O, and Δ¹⁷O values of −29.02 ± 0.65, 19.63 ± 1.16, and 0.05 ± 0.02‰, respectively. The first two isotopic tracers are less distinguishable from those emitted by fossil fuel combustion but the last one is significantly different. We then utilize these end member isotopic ratios, with emphasis on Δ¹⁷O for the reason given above, for partitioning sources that affect the CO₂ level in Delhi. Anthropogenic fraction of CO₂ at CP ranges from 4 to 40%. Further analysis done by employing a three-component (background, rice straw burning, and fuel combustion) mixing model with constraints from the Δ¹⁷O values yields that rice straw burning contributes as much as ∼70% of the total anthropogenic CO₂, which is more than double of the fossil fuel contribution (∼30%), during the study days.
Show more [+] Less [-]Large eddy simulation of vehicle emissions dispersion: Implications for on-road remote sensing measurements
2020
Huang, Yuhan | Ng, Elvin C.Y. | Surawski, Nic C. | Yam, Yat-Shing | Mok, Wai-Chuen | Liu, Chun-Ho | Zhou, John L. | Organ, Bruce | Chan, Edward F.C.
On-road remote sensing technology measures the concentration ratios of pollutants over CO₂ in the exhaust plume in half a second when a vehicle passes by a measurement site, providing a rapid, non-intrusive and economic tool for vehicle emissions monitoring and control. A key assumption in such measurement is that the emission ratios are constant for a given plume. However, there is a lack of study on this assumption, whose validity could be affected by a number of factors, especially the engine operating conditions and turbulence. To guide the development of the next-generation remote sensing system, this study is conducted to investigate the effects of various factors on the emissions dispersion process in the vehicle near-wake region and their effects on remote sensing measurement. The emissions dispersion process is modelled using Large Eddy Simulation (LES). The studied factors include the height of the remote sensing beam, vehicle speed, acceleration and side wind. The results show that the measurable CO₂ and NO exhaust plumes are relatively short at 30 km/h cruising speed, indicating that a large percentage of remote sensing readings within the measurement duration (0.5 s) are below the sensor detection limit which would distort the derived emission ratio. In addition, the valid measurement region of NO/CO₂ emission ratio is even shorter than the measurable plume and is at the tailpipe height. The effect of vehicle speed (30–90 km/h) on the measurable plume length is insignificant. Under deceleration condition, the length of the valid NO/CO₂ measurement region is shorter than under cruising and acceleration conditions. Side winds from the far-tailpipe direction have a significant effect on remote sensing measurements. The implications of these findings are discussed and possible solutions to improve the accuracy of remote sensing measurement are proposed.
Show more [+] Less [-]Low O2 level enhances CH4-derived carbon flow into microbial communities in landfill cover soils
2020
He, Ruo | Su, Yao | Leewis, Mary-Cathrine | Chu, Yi-Xuan | Wang, Jing | Ma, Ruo-Chan | Wu, Donglei | Zhan, Liang-Tong | Herriott, Ian Charold | Leigh, Mary Beth
CH₄ oxidation in landfill cover soils plays a significant role in mitigating CH₄ release to the atmosphere. Oxygen availability and the presence of co-contaminants are potentially important factors affecting CH₄ oxidation rate and the fate of CH₄-derived carbon. In this study, microbial populations that oxidize CH₄ and the subsequent conversion of CH₄-derived carbon into CO₂, soil organic C and biomass C were investigated in landfill cover soils at two O₂ tensions, i.e., O₂ concentrations of 21% (“sufficient”) and 2.5% (“limited”) with and without toluene. CH₄-derived carbon was primarily converted into CO₂ and soil organic C in the landfill cover soils, accounting for more than 80% of CH₄ oxidized. Under the O₂-sufficient condition, 52.9%–59.6% of CH₄-derived carbon was converted into CO₂ (CECO₂₋C), and 29.1%–39.3% was converted into soil organic C (CEₒᵣgₐₙᵢc₋C). A higher CEₒᵣgₐₙᵢc₋C and lower CECO₂₋C occurred in the O₂-limited environment, relative to the O₂-sufficient condition. With the addition of toluene, the carbon conversion efficiency of CH₄ into biomass C and organic C increased slightly, especially in the O₂-limited environment. A more complex microbial network was involved in CH₄ assimilation in the O₂-limited environment than under the O₂-sufficient condition. DNA-based stable isotope probing of the community with ¹³CH₄ revealed that Methylocaldum and Methylosarcina had a higher relative growth rate than other type I methanotrophs in the landfill cover soils, especially at the low O₂ concentration, while Methylosinus was more abundant in the treatment with both the high O₂ concentration and toluene. These results indicated that O₂-limited environments could prompt more CH₄-derived carbon to be deposited into soils in the form of biomass C and organic C, thereby enhancing the contribution of CH₄-derived carbon to soil community biomass and functionality of landfill cover soils (i.e. reduction of CO₂ emission).
Show more [+] Less [-]Biochar amendment mitigates greenhouse gases emission and global warming potential in dairy manure based silage corn in boreal climate
2020
Ashiq, Waqar | Nadeem, Muhammad | Ali, Waqas | Zaeem, Muhammad | Wu, Jianghua | Galagedara, Lakshman | Thomas, Raymond | Kavanagh, Vanessa | Cheema, Mumtaz
About 11% of the global anthropogenic greenhouse gases (GHGs) emissions result from agricultural practices. Dairy manure (DM) application to soil is regarded as a best management practice due to C sequestration and improvement of soil physiochemical properties. However, GHGs emissions from the soil following the DM application could offset its advantages. Biochar (BC) is known to affect N transformation and GHGs emissions from soil. There had been considerably less focus on the BC amendment and its effects on GHGs emissions following DM application under field conditions. The objectives of this study were; i) to determine the temporal patterns and cumulative GHGs fluxes following DM and inorganic nitrogen (IN) application and, ii) to investigate BC amendment impact on DMY, GWP, direct N₂O emission factor (EFd) and the response of CH₄ emissions (RC) in DM based silage corn. To achieve these objectives a two-year field experiment was conducted with these treatments: 1) DM with high N conc. (DM₁: 0.37% N); 2) DM with low N conc. (DM₂: 0.13% N); 3) IN; 4) DM₁+BC; 5) DM₂+BC; 6) IN + BC; and 7) Control (N₀); and were laid out in randomized complete block design with four replications. BC amendment to DM₁, DM₂ and IN significantly reduced cumulative CO₂ emission by 16, 25.5 and 26.5%, CH₄ emission by 184, 200 and 293% and N₂O emission by 95, 86 and 93% respectively. It also reduced area-scaled and yield-scaled GWP, EFd, RC and enhanced DMY. Thus, BC application showed great potential to offset the negative effects of DM application i.e GHGs emissions from the silage corn cropping system. Further research is needed to evaluate soil organic carbon and nitrogen dynamics (substrates for GHG emissions) after DM and BC application on various soil types and cropping systems under field conditions.
Show more [+] Less [-]Elevated CO2 mitigates the negative effect of CeO2 and Cr2O3 nanoparticles on soil bacterial communities by alteration of microbial carbon use
2020
Luo, Jipeng | Song, Yuchao | Liang, Jiabin | Li, Jinxing | Islam, Ejazul | Li, Tingqiang
The interactive effects of elevated atmospheric CO₂ and nanoparticles (NPs) on the structure and function of soil bacterial community remain unknown. Here we compared the impacts of CeO₂ (nCeO₂) and Cr₂O₃ (nCr₂O₃) nanoparticles on the taxonomic compositions and functional attributes of bacterial communities under elevated CO₂ (eCO₂). The stimulated enzyme activities (dehydrogenase, acid phosphatase and urease), increased microbial biomass carbon (MBC), and higher bacterial alpha-diversity were observed under the combined effects of eCO₂ and NPs compared to the single NP treatment, indicating eCO₂ could mitigate the adverse effect of NPs on soil microorganisms. NPs and eCO₂ are important factors influencing the alpha- and beta-diversity (17% and 18% of variations were explained) as well as functional profile (20% and 26% of variations were explained) of bacterial communities. Rising CO₂ level promoted the resilience of NP-resistant bacterial populations, primarily the members of Alphaproteobacteria, Gammaproteobacteria and Bacteroidia, which are also characterized by the fast carbon use capability. Moreover, the significantly (P < 0.05) higher metabolic quotient (qCO₂), reduced available carbon and overrepresented carbon metabolism genes at eCO₂vs. ambient CO₂ (aCO₂) indicate the acceleration of available carbon turnover in NP-exposed soils. Correlation analysis revealed that mitigation of NPs toxicity by eCO₂ could be attributed to the remarkable decline of bioavailable metals disassociated from NPs and available carbon level, as well as promotion of the rapid carbon-metabolizing microbes. Our study pointed out the positive role of eCO₂ in alleviating the adverse effect of NPs on microbiological soil environment, and results can serve as important basis in establishing guidelines for lowering the ecotoxicity of NPs.
Show more [+] Less [-]Environmental investments decreased partial pressure of CO2 in a small eutrophic urban lake: Evidence from long-term measurements
2020
Xiao, Qitao | Duan, Hongtao | Qi, Tianci | Hu, Zhenghua | Liu, Shoudong | Zhang, Mi | Lee, Xuhui
Inland waters emit large amounts of carbon dioxide (CO₂) to the atmosphere, but emissions from urban lakes are poorly understood. This study investigated seasonal and interannual variations in the partial pressure of CO₂ (pCO₂) and CO₂ flux from Lake Wuli, a small eutrophic urban lake in the heart of the Yangtze River Delta, China, based on a long-term (2000–2015) dataset. The results showed that the annual mean pCO₂ was 1030 ± 281 μatm (mean ± standard deviation) with a mean CO₂ flux of 1.1 ± 0.6 g m⁻² d⁻¹ during 2000–2015, suggesting that compared with other lakes globally, Lake Wuli was a significant source of atmospheric CO₂. Substantial interannual variability was observed, and the annual pCO₂ exhibited a decreasing trend due to improvements in water quality driven by environmental investment. Changes in ammonia nitrogen and total phosphorus concentrations together explained 90% of the observed interannual variability in pCO₂ (R² = 0.90, p < 0.01). The lake was dominated by cyanobacterial blooms and showed nonseasonal variation in pCO₂. This finding was different from those of other eutrophic lakes with seasonal variation in pCO₂, mostly because the uptake of CO₂ by algal-derived primary production was counterbalanced by the production of CO₂ by algal-derived organic carbon decomposition. Our results suggested that anthropogenic activities strongly affect lake CO₂ dynamics and that environmental investments, such as ecological restoration and reducing nutrient discharge, can significantly reduce CO₂ emissions from inland lakes. This study provides valuable information on the reduction in carbon emissions from artificially controlled eutrophic lakes and an assessment of the impact of inland water on the global carbon cycle.
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