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Size-activity threshold of titanium dioxide-supported Cu cluster in CO oxidation
2021
Khan, Wasim Ullah | Yu, Iris K.M. | Sun, Yuqing | Polson, Matthew I.J. | Golovko, Vladimir | Lam, Frank L.Y. | Ogino, Isao | Tsang, Daniel C.W. | Yip, Alex C.K.
Development of non-noble metal cluster catalysts, aiming at concurrently high activity and stability, for emission control systems has been challenging because of sintering and overcoating of clusters on the support. In this work, we reported the role of well-dispersed copper nanoclusters supported on TiO₂ in CO oxidation under industrially relevant operating conditions. The catalyst containing 0.15 wt% Cu on TiO₂ (0.15 CT) exhibited a high dispersion (59.1%), a large specific surface area (381 m²/gCᵤ), a small particle size (1.77 nm), and abundant active sites (75.8% Cu₂O). The CO oxidation activity measured by the turnover frequency (TOF) was found to be enhanced from 0.60 × 10⁻³ to 3.22 × 10⁻³ molCO·molCᵤ⁻¹·s⁻¹ as the copper loading decreased from 5 to 0.15 wt%. A CO conversion of approximately 60% was still observed in the supported cluster catalyst with a Cu loading of 5 wt% at 240 °C. No deactivation was observed for catalysts with low copper loading (0.15 and 0.30 CT) after 8 h of time-on-stream, which compares favorably with less stable Au cluster-based catalysts reported in the literature. In contrast, catalysts with high copper loading (0.75 and 5 CT) showed deactivation over time, which was ascribed to the increase in copper particle size due to metal cluster agglomeration. This study elucidated the size-activity threshold of TiO₂-supported Cu cluster catalysts. It also demonstrated the potential of the supported Cu cluster catalyst at a typical temperature range of diesel engines at light-load. The supported Cu cluster catalyst could be a promising alternative to noble metal cluster catalysts for emission control systems.
Show more [+] Less [-]Effects of the antineoplastic drug cyclophosphamide on the biochemical responses of the mussel Mytilus galloprovincialis under different temperatures
2021
Queirós, Vanessa | Azeiteiro, Ulisses M. | Barata, Carlos | Santos, Juan Luis | Alonso, Esteban | Soares, Amadeu M.V.M. | Freitas, Rosa
Cyclophosphamide (CP) is an antineoplastic drug widely used in chemotherapy treatments with high consumption rates and that has been detected in the aquatic environment. After being released into the aquatic environment, CP may cause adverse effects on aquatic organisms since antineoplastics are well-known cytotoxic, genotoxic, mutagenic and teratogenic drugs. Moreover, predicted environmental changes, such as the temperature rising, may alter the impacts caused by CP on organisms. Thus, the present study aimed to assess the effects caused by CP chronic exposure in the mussel Mytilus galloprovincialis, under actual and predicted warming scenarios. Organisms were exposed for 28 days to different concentrations of CP (10, 100, 500 and 1000 ng/L) at control (17 ± 1.0 °C) and increased (21 ± 1.0 °C) temperatures. Biochemical responses related to metabolic capacity, energy reserves, oxidative stress and neurotoxicity were assessed. The results showed that the organisms were able to maintain their metabolic capacity under all exposure conditions. However, their antioxidant defense mechanisms were activated mostly at higher CP concentrations being able to prevent cellular damage, even under the warming scenario. Overall, the present findings suggest that temperature rise may not alter the impacts of CP towards M. galloprovincialis.
Show more [+] Less [-]Bioremediation of aromatic hydrocarbons contaminated soil from industrial site using surface modified amino acid enhanced biosurfactant
2021
Christopher, Judia Magthalin | Sridharan, Rajalakshmi | Somasundaram, Swarnalatha | Ganesan, Sekaran
Surface modified lipopeptide biosurfactant (BS) with enhancement of amino acids was produced using Bacillus Malacitensis. The aromatic hydrocarbons from contaminated soil were removed by BS soil washing process and bioremediation using activated functionalized carbon-BS matrix (AFC-BS). The Central Composite Design (CCD) showed the optimum time100 h; pH 7; temperature 30°C on maximum yield of BS. The amino acid profiling of BS reveals the enhancement of amino acids especially polar amino acids and its importance in the formation of micellar structure for the tight packing of aromatic hydrocarbons from industrial contaminated soil. AFC-BS matrix was implanted directly into the contaminated soil for 28 days and found 61.80 % of Total Petroleum Hydrocarbon (TPH) removal efficiency which is high compared to the AFC treated soil. The compounds were extracted from contaminated soil and AFC-BS matrix, found similar peaks in high performance liquid chromatography, which reveals the ability of BS to remove aromatic contaminants. The soil toxicity was also analyzed by seed germination and found improvement in the growth of seeds. The germination of seeds increased from 60 % to 100 % and the phytotoxicity of root and shoot was reduced from 89.50 %, 88.45 % to12.55 %, 11.87 % respectively.
Show more [+] Less [-]Do dissipation and transformation of γ-HCH and p,p’-DDT in soil respond to a proxy for climate change? Insights from a field study on the eastern Tibetan Plateau
2021
Ding, Yang | Li, Li | Wania, Frank | Huang, Huanfang | Zhang, Yuan | Peng, Bo | Chen, Yingjie | Qi, Shihua
While the influence of climate change on the fate of persistent organic pollutants (POPs) is becoming a topic of global concern, it has yet to be demonstrated how POPs and their transformation products in soil respond to a changing climate at the local scale. We conducted a year-long field experiment with spiked soils to investigate the impact of climate on the dissipation of γ-hexachlorocyclohexane (γ-HCH) and p,p’-dichlorodiphenyltrichloroethane (p,p’-DDT) as well as the formation of their products. Four sites along an elevational gradient on the eastern Tibetan Plateau were selected to represent four scenarios ranging from a dry and cold to a warm and humid climate. Based on the measured concentrations of the two pesticides and their transformation products, we calculated the dissipation rates of γ-HCH and p,p’-DDT in soil using two biphasic kinetic models, and the formation rates of transformation products using a mid-point rectangular approximation method. The spiked γ-HCH generally showed the expected decrease in dissipation from soils with increasing altitudes, and therefore decreasing temperature and precipitation, whereas dissipation of p,p’-DDT was influenced more by photolysis and sequestration in soil. The formation rates of the primary products of γ-HCH (i.e. γ-HCH→PeCCH and γ-HCH→TeCCH) and p,p’-DDT (i.e. p,p’-DDT→p,p’-DDE and p,p’-DDT→p,p’-DDD) indicate that a warmer and wetter climate favors dechloroelimination (anaerobic biodegradation) over dehydrochlorination (aerobic biodegradation). The significantly longer dissipation half-lives of γ-HCH at the coldest site suggests that the fate of POPs in frozen regions (e.g. polar regions) needs more attention. Overall, the fate of more volatile chemicals (e.g. γ-HCH) might be more responsive to the climate change.
Show more [+] Less [-]Quantification of tire tread wear particles in microparticles produced on the road using oleamide as a novel marker
2021
Chae, Eunji | Jung, Uiyeong | Choi, Sung-Seen
In general, tire tread rubber compounds contain oleamide for improvement of manufacturing processibility, mold release characterization, and abrasion resistance. Tire tread wear particles (TWPs) are one of major contributors to microplastic emissions. In this study, a novel analytical method for quantification of TWP in microparticles produced on the road (road dust, MPRs) was developed by employing oleamide as a new marker. MPRs were collected at bus stops in autumn, winter, and summer seasons. MPRs of 38–63, 63–106, 106–212, and 212–500 μm obtained by size separation were employed for the analysis. Rubber components for bus and passenger car tire tread compounds were identified using pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Oleamide was extracted from the MPRs with acetone and was identified using GC/MS. The oleamide concentration was analyzed using GC equipped with flame ionization detector (FID). The TWP contents of the MPRs were determined using the oleamide concentrations and the reference compound formulations. In order to reduce the sampling errors, each experiment was carried out five times and the results were averaged. The TWP contents of the MPRs were 1.4–4.7 wt% and were different according to the sampling seasons and places. The TWP contents were increased by increasing the traffic volume and the temperature.
Show more [+] Less [-]Size−resolved source apportionment of particulate matter from a megacity in northern China based on one-year measurement of inorganic and organic components
2021
Tian, Yingze | Harrison, Roy M. | Feng, Yinchang | Shi, Zongbo | Liang, Yongli | Li, Yixuan | Xue, Qianqian | Xu, Jingsha
This research apportioned size-resolved particulate matter (PM) contributions in a megacity in northern China based on a full year of measurements of both inorganic and organic markers. Ions, elements, carbon fractions, n-alkanes, polycyclic aromatic hydrocarbons (PAHs), hopanes and steranes in 9 p.m. size fractions were analyzed. High molecular weight PAHs concentrated in fine PM, while most other organic compounds showed two peaks. Both two-way and three-way receptor models were used for source apportionment of PM in different size ranges. The three-way receptor model gave a clearer separation of factors than the two-way model, because it uses a combination of chemical composition and size distributions, so that factors with similar composition but distinct size distributions (like more mature and less mature coal combustion) can be resolved. The three-way model resolved six primary and three secondary factors. Gasoline vehicles and coal and biomass combustion, nitrate and high relative humidity related secondary aerosol, and resuspended dust and diesel vehicles (exhaust and non-exhaust) are the top two contributors to pseudo-ultrafine (<0.43 μm), fine (0.43–2.1 μm) and coarse mode (>2.1 μm) PM, respectively. Mass concentration of PM from coal and biomass combustion, industrial emissions, and diesel vehicle sources showed a bimodal size distribution, but gasoline vehicles and resuspended dust exhibited a peak in the fine and coarse mode, separately. Mass concentration of sulphate, nitrate and secondary organic aerosol exhibited a bimodal distribution and were correlated with temperature, indicating strong photochemical processing and repartitioning. High relative humidity related secondary aerosol was strongly associated with size shifts of PM, NO₃⁻ and SO₄²⁻ from the usual 0.43–0.65 μm to 1.1–2.1 μm. Our results demonstrated the dominance of primary combustion sources in the <0.43 μm particle mass, in contrast to that of secondary aerosol in fine particle mass, and dust in coarse particle mass in the Northern China megacity.
Show more [+] Less [-]Atmospheric ammonia and its effect on PM2.5 pollution in urban Chengdu, Sichuan Basin, China
2021
Huang, Xiaojuan | Zhang, Junke | Zhang, Wei | Tang, Guiqian | Wang, Yuesi
Controlling ammonia (NH₃) emissions has been proposed as a strategy to mitigate haze pollution. To explore the role of NH₃ in haze pollution in Sichuan Basin, where agricultural activities are intense, hourly in situ data of NH₃, as well as nitric acid and secondary inorganic aerosols (SIAs) were gathered in Chengdu from April 2017 to March 2018. We found that NH₃ had an annual mean concentration of 9.7 ± 3.5 (mean ± standard deviation) μg m⁻³, and exhibited seasonal variations (spring > summer > autumn and winter) due to changes in emission sources and meteorological conditions (particularly temperature). Chengdu's atmosphere is generally NH₃-sufficient, especially in the warm seasons, implying that the formation of SIAs is more sensitive to the availability of nitric acid. However, an NH₃ “sufficient-to-deficient” transition was found to occur during winter pollution periods, and the frequency of NH₃ deficiency increased with the aggravation of pollution. Under NH₃-deficient conditions, the nitrogen oxidation ratio increased linearly with the increase in free NH₃, implying that NH₃ contributes appreciably to the formation of nitrate and thus to high PM₂.₅ loadings. No relationships of NH₃ with fossil fuel combustion–related pollutants were found. The NH₃ emissions from farmland and livestock waste in the suburbs of Chengdu and regional transport from west of Chengdu probably contribute to the occurrence of high PM₂.₅ loading in winter and spring, respectively. These results suggest that to achieve effective mitigation of PM₂.₅ in Chengdu, local and regional emission control of NH₃ and NOx synergistically would be effective.
Show more [+] Less [-]Are environmental pollution and biodiversity levels associated to the spread and mortality of COVID-19? A four-month global analysis
2021
Fernández, Daniel | Giné-Vázquez, Iago | Liu, Ivy | Yucel, Recai | Nai Ruscone, Marta | Morena, Marianthi | García, Víctor Gerardo | Haro, Josep Maria | Pan, William | Tyrovolas, Stefanos
On March 12th, 2020, the WHO declared COVID-19 as a pandemic. The collective impact of environmental and ecosystem factors, as well as biodiversity, on the spread of COVID-19 and its mortality evolution remain empirically unknown, particularly in regions with a wide ecosystem range. The aim of our study is to assess how those factors impact on the COVID-19 spread and mortality by country. This study compiled a global database merging WHO daily case reports with other publicly available measures from January 21st to May 18th, 2020. We applied spatio-temporal models to identify the influence of biodiversity, temperature, and precipitation and fitted generalized linear mixed models to identify the effects of environmental variables. Additionally, we used count time series to characterize the association between COVID-19 spread and air quality factors. All analyses were adjusted by social demographic, country-income level, and government policy intervention confounders, among 160 countries, globally. Our results reveal a statistically meaningful association between COVID-19 infection and several factors of interest at country and city levels such as the national biodiversity index, air quality, and pollutants elements (PM₁₀, PM₂.₅, and O₃). Particularly, there is a significant relationship of loss of biodiversity, high level of air pollutants, and diminished air quality with COVID-19 infection spread and mortality. Our findings provide an empirical foundation for future studies on the relationship between air quality variables, a country’s biodiversity, and COVID-19 transmission and mortality. The relationships measured in this study can be valuable when governments plan environmental and health policies, as alternative strategy to respond to new COVID-19 outbreaks and prevent future crises.
Show more [+] Less [-]Pyrolysis temperature-dependent carbon retention and stability of biochar with participation of calcium: Implications to carbon sequestration
2021
Nan, Hongyan | Yin, Jianxiang | Yang, Fan | Luo, Ying | Zhao, Ling | Cao, Xinde
Converting biomass waste into biochar by slow pyrolysis with subsequent soil amendment is a prospective approach with multiple environmental benefits including soil contamination remediation, soil amelioration and carbon sequestration. This study selected cow manure as precursor to produce biochar under 300 °C, 400 °C, 500 °C and 600 °C, and a remarkable promotion of carbon (C) retention in biochar by incorporation of exogenous Ca was achieved at all investigated pyrolysis temperatures. The C retention was elevated from 49.2 to 68.3% of pristine biochars to 66.1–79.7% of Ca-composite biochars. It was interesting that extent of this improvement increased gradually with rising of pyrolysis temperature, i.e., doping Ca in biomass promoted pyrolytic C retention in biochar by 16.6%, 23.4%, 29.1% and 31.1% for 300 °C, 400 °C, 500 °C and 600 °C, respectively. Thermogravimetric-mass spectrometer (TG-MS) and X-ray photoelectron spectroscopy (XPS) showed that Ca catalyzed thermal-chemical reactions and simultaneously suppressed the release of small organic molecular substances (C₂–C₇) via physical blocking (CaO, CaCO₃, and CaClOH) and chemical bonding (CO and OC–O). The catalyzation mainly occurred at 200–400 °C, while the suppression was more prominent at higher temperatures. Raman spectra and 2D FTIR analysis on biochar microstructure showed that presence of Ca had negative influence on carbon aromatization and thus weakened biochar's stability, while increasing pyrolysis temperature enhanced the stability of carbon structure. Finally, with integrating “C retention” during pyrolysis and “C stability” in biochar, the maximum C sequestration (56.3%) was achieved at 600 °C with the participation of Ca. The study highlights the importance of both Ca and pyrolysis temperature in enhancing biochar's capacity of sequestrating C.
Show more [+] Less [-]Sustainable functionalized metal-organic framework NH2-MIL-101(Al) for CO2 separation under cryogenic conditions
2021
Bābar, Muḥammad | Mubashir, Muhammad | Mukhtar, Ahmad | Saqib, Sidra | Ullah, Sami | Bustam, Mohamad Azmi | Show, Pau Loke
In this study, a sustainable NH₂-MIL-101(Al) is synthesized and subjected to characterization for cryogenic CO₂ adsorption, isotherms, and thermodynamic study. The morphology revealed a highly porous surface. The XRD showed that NH₂-MIL-101(Al) was crystalline. The NH₂-MIL-101(Al) decomposes at a temperature (>500 °C) indicating excellent thermal stability. The BET investigation revealed the specific surface area of 2530 m²/g and the pore volume of 1.32 cm³/g. The CO₂ adsorption capacity was found to be 9.55 wt% to 2.31 wt% within the investigated temperature range. The isotherms revealed the availability of adsorption sites with favorable adsorption at lower temperatures indicating the thermodynamically controlled process. The thermodynamics showed that the process is non-spontaneous, endothermic, with fewer disorders, chemisorption. Finally, the breakthrough time of NH₂-MIL-101(Al) is 31.25% more than spherical glass beads. The CO₂ captured by the particles was 2.29 kg m⁻³. The CO₂ capture using glass packing was 121% less than NH₂-MIL-101(Al) under similar conditions of temperature and pressure.
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