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Catalytic hydrogenolysis of plastic to liquid hydrocarbons over a nickel-based catalyst
2022
Zhao, Zhigang | Li, Zheng | Zhang, Xiangkun | Li, Tan | Li, Yuqing | Chen, Xingkun | Wang, Kaige
The catalytic hydrogenolysis of a typical model compound of mulching film waste, polyethylene, was investigated as a potential way to improve economic efficiency of mulching film recycling. Nickel-based heterogeneous catalysts are proposed for polyethylene hydrogenolysis to produce liquid hydrocarbons. Among catalysts supported on various carriers, Ni/SiO₂ catalyst shows the highest activity which may due to the interactions between nickel and silica with the formation of nickel phyllosilicate. As high as 81.18% total gasoline and diesel range hydrocarbon was obtained from the polyethylene hydrogenolysis at relatively mild condition of 280 °C, and 3 MPa cold hydrogen pressure. The result is comparable to what have been reported in previous studies using noble metal catalysts. The gasoline and diesel range hydrocarbon are n-alkanes with a distribution at a range of C₄–C₂₂. The gas products are primarily CH₄ along with a small amount of C₂H₆ and C₃H₈. High yield of CH₄ as much as 9.68% was observed for the cleavage of molecule occurs along the alkane chain.
Show more [+] Less [-]Effects of ocean acidification and tralopyril on bivalve biomineralization and carbon cycling: A study of the Pacific Oyster (Crassostrea gigas)
2022
Wang, Xu | Li, Ping | Cao, Xuqian | Liu, Bin | He, Shuwen | Cao, Zhihan | Xing, Shaoying | Liu, Ling | Li, Zhi-Hua
The combined effects of emerging pollutants and ocean acidification (OA) on marine organisms and marine ecosystems have attracted increasing attention. However, the combined effects of tralopyril and OA on marine organisms and marine ecosystems remain unclear. In this study, Crassostrea gigas (C. gigas) were exposed to tralopyril (1 μg/L) and/or OA (PH = 7.7) for 21 days and a 14-day recovery acclimation. To investigate the stress response and potential molecular mechanisms of C. gigas to OA and tralopyril exposure alone or in combination, as well as the effects of OA and/or tralopyril on bivalve biomineralization and marine carbon cycling. The results showed that the combined toxicity was between that of acidification and tralopyril alone. Single or combined exposure activated the general stress defense responses of C. gigas mantle, affected energy metabolism and biomineralization of the organism and the carbon cycle of the marine ecosystem. Moreover, acidification-induced and tralopyril-induced toxicity showed potential recoverability at molecular and biochemical levels. This study provides a new perspective on the molecular mechanisms of tralopyril toxicity to bivalve shellfish and reveals the potential role of tralopyril and OA on marine carbon cycling.
Show more [+] Less [-]Impacts of changes in environmental exposures and health behaviours due to the COVID-19 pandemic on cardiovascular and mental health: A comparison of Barcelona, Vienna, and Stockholm
2022
Koch, Sarah | Khomenko, Sasha | Cirach, Marta | Ubalde-Lopez, Mònica | Baclet, Sacha | Daher, Carolyn | Hidalgo, Laura | Lõhmus, Mare | Rizzuto, Debora | Rumpler, Romain | Susilo, Yusak | Venkataraman, Siddharth | Wegener, Sandra | Wellenius, Gregory A. | Woodcock, Jim | Nieuwenhuijsen, Mark
Responses to COVID-19 altered environmental exposures and health behaviours associated with non-communicable diseases. We aimed to (1) quantify changes in nitrogen dioxide (NO₂), noise, physical activity, and greenspace visits associated with COVID-19 policies in the spring of 2020 in Barcelona (Spain), Vienna (Austria), and Stockholm (Sweden), and (2) estimated the number of additional and prevented diagnoses of myocardial infarction (MI), stroke, depression, and anxiety based on these changes. We calculated differences in NO₂, noise, physical activity, and greenspace visits between pre-pandemic (baseline) and pandemic (counterfactual) levels. With two counterfactual scenarios, we distinguished between Acute Period (March 15th – April 26th, 2020) and Deconfinement Period (May 2nd – June 30th, 2020) assuming counterfactual scenarios were extended for 12 months. Relative risks for each exposure difference were estimated with exposure-risk functions. In the Acute Period, reductions in NO₂ (range of change from −16.9 μg/m³ to −1.1 μg/m³), noise (from −5 dB(A) to −2 dB(A)), physical activity (from −659 MET*min/wk to −183 MET*min/wk) and greenspace visits (from −20.2 h/m to 1.1 h/m) were largest in Barcelona and smallest in Stockholm. In the Deconfinement Period, NO₂ (from −13.9 μg/m³ to −3.1 μg/m³), noise (from −3 dB(A) to −1 dB(A)), and physical activity levels (from −524 MET*min/wk to −83 MET*min/wk) remained below pre-pandemic levels in all cities. Greatest impacts were caused by physical activity reductions. If physical activity levels in Barcelona remained at Acute Period levels, increases in annual diagnoses for MI (mean: 572 (95% CI: 224, 943)), stroke (585 (6, 1156)), depression (7903 (5202, 10,936)), and anxiety (16,677 (926, 27,002)) would be anticipated. To decrease cardiovascular and mental health impacts, reductions in NO₂ and noise from the first COVID-19 surge should be sustained, but without reducing physical activity. Focusing on cities’ connectivity that promotes active transportation and reduces motor vehicle use assists in achieving this goal.
Show more [+] Less [-]Local environment modulates whole-transcriptome expression in the seagrass Posidonia oceanica under warming and nutrients excess
2022
Pazzaglia, Jessica | Santillán-Sarmiento, Alex | Ruocco, Miriam | Dattolo, Emanuela | Ambrosino, Luca | Marín-Guirao, Lazaro | Procaccini, Gabriele
The intensification of anomalous events of seawater warming and the co-occurrence with local anthropogenic stressors are threatening coastal marine habitats, including seagrasses, which form extensive underwater meadows. Eutrophication highly affects coastal environments, potentially summing up to the widespread effects of global climate changes. In the present study, we investigated for the first time in seagrasses, the transcriptional response of different plant organs (i.e., leaf and shoot apical meristem, SAM) of the Mediterranean seagrass Posidonia oceanica growing in environments with a different history of nutrient enrichment. To this end, a mesocosm experiment exposing plants to single (nutrient enrichment or temperature increase) and multiple stressors (nutrient enrichment plus temperature increase), was performed. Results revealed a differential transcriptome regulation of plants under single and multiple stressors, showing an organ-specific sensitivity depending on plants' origin. While leaf tissues were more responsive to nutrient stress, SAM revealed a higher sensitivity to temperature treatments, especially in plants already impacted in their native environment. The exposure to stress conditions induced the modulation of different biological processes. Plants living in an oligotrophic environment were more responsive to nutrients compared to plants from a eutrophic environment. Evidences that epigenetic mechanisms were involved in the regulation of transcriptional reprogramming were also observed in both plants’ organs. These results represent a further step in the comprehension of seagrass response to abiotic stressors pointing out the importance of local pressures in a global warming scenario.
Show more [+] Less [-]Fragility of nocturnal interactions: Pollination intensity increases with distance to light pollution sources but decreases with increasing environmental suitability
2022
Soteras, Florencia | Camps, Gonzalo Andrés | Costas, Santiago Martín | Giaquinta, Adrián | Peralta, Guadalupe | Cocucci, Andrea Arístides
Light pollution represents a widespread long-established human-made disturbance and an important threat to nocturnal pollination. Distance from the niche centroid where optimal environmental conditions join may be related to species sensitivity to habitat change. We estimated the environmental suitability of the plant species Erythrostemon gilliesii and of its guild of hawkmoth pollinators. We considered the overlap of suitability maps of both partners as the environmental suitability of the interaction. We used a three-year record of ten E. gilliesii populations to calculate pollination intensity as the number of individuals that received pollen per population. In addition, for each population, we measured the distance to the high light pollution source around a buffer of 15 km radius. Finally, we predicted pollination intensity values for environmental suitability ranging from 0 to 1, and distance to high light pollution sources ranging from 0 to 56 Km. Pollination intensity decreased along an axis of increasing environmental suitability and increased with distance to sources of light pollution. The highest values of pollination intensity were observed at greatest distances to sources of light pollution and where environmental suitability of the interaction was lowest. The prediction model evidenced that, when environmental suitability was lowest, pollination intensity increased with distance to sources of high light pollution. However, when environmental suitability was intermediate or high, pollination intensity decreased away and until 28 km from the sources of high light pollution. Beyond 28 km from the sources of high light pollution, pollination intensity remained low and constant. Populations under conditions of low environmental suitability might be more likely to respond to disturbances that affect pollinators than populations under conditions of high environmental suitability.
Show more [+] Less [-]Suspect and non-targeted screening-based human biomonitoring identified 74 biomarkers of exposure in urine of Slovenian children
2022
Tkalec, Žiga | Codling, Garry | Tratnik, Janja Snoj | Mazej, Darja | Klánová, Jana | Horvat, Milena | Kosjek, Tina
Human exposure to organic contaminants is widespread. Many of these contaminants show adverse health effects on human population. Human biomonitoring (HBM) follows the levels and the distribution of biomarkers of exposure (BoE), but it is usually done in a targeted manner. Suspect and non-targeted screening (SS/NTS) tend to find BoE in an agnostic way, without preselection of compounds, and include finding evidence of exposure to predicted, unpredicted known and unknown chemicals. This study describes the application of high-resolution mass spectrometry (HRMS)-based SS/NTS workflow for revealing organic contaminants in urine of a cohort of 200 children from Slovenia, aged 6–9 years. The children originated from two regions, urban and rural, and the latter were sampled in two time periods, summer and winter. We tentatively identified 74 BoE at the confidence levels of 2 and 3. These BoE belong to several classes of pharmaceuticals, personal care products, plasticizers and plastic related products, volatile organic compounds, nicotine, caffeine and pesticides. The risk of three pesticides, atrazine, amitraz and diazinon is of particular concern since their use was limited in the EU. Among BoE we tentatively identified compounds that have not yet been monitored in HBM schemes and demonstrate limited exposure data, such as bisphenol G, polyethylene glycols and their ethers. Furthermore, 7 compounds with unknown use and sources of exposure were tentatively identified, either indicating the entry of new chemicals into the market, or their metabolites and transformation products. Interestingly, several BoE showed location and time dependency. Globally, this study presents high-throughput approach to SS/NTS for HBM. The results shed a light on the exposure of Slovenian children and raise questions on potential adverse health effects of such mixtures on this vulnerable population.
Show more [+] Less [-]Effective Sb(V) removal from aqueous solution using phosphogypsum-modified biochar
2022
Li, Ling | Liao, Lu | Wang, Bing | Li, Wei | Liu, Taoze | Wu, Pan | Xu, Qingya | Liu, Shirong
Antimonate is the dominant form of antimony (Sb) in Sb mine water. The treatment of high-Sb mine water essentially reduces the discharge of antimonate oxyanions ([Sb(OH)₆]⁻) in it. Biochar obtained from phosphogypsum-modified anaerobic digested distillers’ grain (PADC) can effectively adsorb antimonate from water. In this work, using batch adsorption experiments, mathematical models, and characterization methods, the mechanism of Sb(V) adsorption by PADC was studied. Compared with pristine biochar, PADC biochar showed abundant lamellar and vesicular structures with significant calcium ion loading on the surface. The kinetics data of the adsorption of Sb(V) on the PADC biochar followed the Elovich equation (R² = 0.992), indicating that heterogeneous adsorption had occurred. The results also showed that intraparticle diffusion played an important role in controlling Sb(V) adsorption by PADC biochar. The Redlich–Peterson model best fit the Sb(V) adsorption isotherm (R² = 0.997), indicating that the adsorption was a combination of the Langmuir and Freundlich models. The maximum adsorption capacity of PADC biochar for Sb(V) is 8123 mg/kg, which is more than twice that of the pristine biochar (3487 mg/kg) and is sufficient for Sb(V) treatment in most mine water. Fourier transform infrared (FTIR) spectra, X-ray photoelectron spectroscopy (XPS), X-ray diffractometry (XRD), and Transmission electron microscopy with energy dispersive X-ray spectroscopy (TEM-EDS) analyses revealed that the dominant mechanism of Sb(V) removal by PADC biochar was the formation of Ca–O–Sb complexes or amorphous surface precipitation as well as electrostatic adsorption. This work demonstrated the potential of PADC biochar in the treatment of Sb-contaminated mine water.
Show more [+] Less [-]Severe cyanobacteria accumulation potentially induces methylotrophic methane producing pathway in eutrophic lakes
2022
Zhou, Chuanqiao | Peng, Yu | Yu, Miaotong | Deng, Yang | Chen, Li | Zhang, Lanqing | Xu, Xiaoguang | Zhang, Siyuan | Yan, Yan | Wang, Guoxiang
Although cyanobacteria blooms lead to an increase in methane (CH₄) emissions in eutrophic lakes have been intensively studied, the methane production pathways and driving mechanisms of the associated CH₄ emissions are still unclear. In this study, the hypereutrophic Lake Taihu, which has extreme cyanobacteria accumulation, was selected to test hypothesis of a potential methylotrophic CH₄ production pathway. Field observation displayed that the CH₄ emission flux from the area with cyanobacteria accumulation was 867.01 μg m⁻²·min⁻¹, much higher than the flux of 3.44 μg m⁻²·min⁻¹ in the non-cyanobacteria accumulation area. The corresponding abundance of methane-producing archaea (MPA) in the cyanobacteria-concentrated area was 77.33% higher than that in the non-concentrated area via RT-qPCR technologies. Synchronously, sediments from these areas were incubated in anaerobic bottles, and results exhibited the high CH₄ emission potential of the cyanobacteria concentrated area versus the non-concentrated area (1199.26 vs. 205.76 μmol/L) and more active biological processes (CO₂ emission, 2072.8 vs. −714.62 μmol/L). We also found evidence for the methylotrophic methane producing pathway, which contributed to the high CH₄ emission flux from the cyanobacteria accumulation area. Firstly, cyanobacteria decomposition provided the prerequisite of abundant methyl thioether substances, including DMS, DMDS, and DMTS. Results showed that the content of methyl thioethers increased with the biomass of cyanobacteria, and the released DMS, DMDS, and DMTS was up to 96.35, 3.22 and 13.61 μg/L, respectively, in the highly concentrated 25000 g/cm³ cyanobacteria treatment. Then, cyanobacteria decomposition created anaerobic microenvironments (DO 0.06 mg/L and Eh −304.8Mv) for methylotrophic methane production. Lastly, the relative abundance of Methanosarcinales was increased from 7.67% at the initial stage to 36.02% at the final stage within a sediment treatment with 10 mmol/L N(CH₃)₃. Quantitatively, the proportion of the methylotrophic methane production pathway was as high as 32.58%. This finding is crucial for accurately evaluating the methane emission flux, and evaluating future management strategies of eutrophic lakes.
Show more [+] Less [-]Deep insight into the Sb(III) and Sb(V) removal mechanism by Fe–Cu-chitosan material
2022
Wang, Tianning | Jiao, Yonghong | He, Mengchang | Ouyang, Wei | Lin, Chunye | Liu, Xitao | Xie, Haijiao
Currently, alleviating antimony (Sb) contamination in aqueous solutions is crucial for restoring and recovering ecological and environmental health. Due to its toxicity, bioaccumulation and mobile characteristics, developing an efficient technique for antimony decontamination is imperative. Herein, we prepared a Fe–Cu-chitosan (FCC) composite by a one-step coprecipitation method, in which nanoscale Fe/Cu acts as the active sites and the whole structure is exhibited as porous microscale particles. A Fe/Cu proportion of 2/1 (FCC-2/1) was determined to be the optimum proportion for antimony adsorption, specifically 34.5 mg g⁻¹ for Sb(III) and 26.8 mg g⁻¹ for Sb(V) (initial concentration: 5.0 mg L⁻¹). Spectral characterization, batch experiments and density functional theory (DFT) simulations were applied to determine the adsorption mechanism, in which surface hydroxyls (-OH) were responsible for antimony complexion and Fe–Cu coupling was a major contributor to adsorption enhancement. According to kinetic analysis, Cu provided an electrostatic attraction during the adsorption process, which facilitated the transportation of antimony molecules to the material interface. In the meantime, the FCC electronic structure was modified due to the optimization of the Fe–Cu interface coupling. Based on the Mullikan net charge, the intrinsic Fe–O–Cu bond might favor interfacial electronic redistribution. When the antimony molecule contacted the adsorption interface, the electrons transferred swiftly as Fe/Cu 3d and O 2p orbital hybridization occurred, thus inducing a stabilizing effect. This work may offer a new perspective for binary oxide construction and its adsorption mechanism analysis.
Show more [+] Less [-]Microplastics in arid soils: Impact of different cropping systems (Altay, Xinjiang)
2022
Liu, Hao | Wang, Xiyuan | Shi, Qingdong | Liu, Yuying | Lei, Haifeng | Chen, Yutong
Although microplastic pollution in the soil environment is currently an important research topic, few studies have focused on farmland soil in arid regions. This study investigated the abundances, sizes, polymer compositions, and forms of microplastics across nine agricultural plots cultivated with maize, sunflower, and potato (three of each crop) plants to determine the influences of different cropping characteristics and agricultural practices. The study area was within the arid region of the Ulungur River basin in Qinghe County, Altay, Xinjiang, China. The main forms of microplastics were fragments and fibers, and polyethylene was the dominant polymer (91.6%). The microplastic abundance ranged from 11 347 items/kgdw to 78 061 items/kgdw (mean of 52 081.7 items/kgdw). The abundance and proportion of microplastics with a diameter of <0.2 mm were significantly higher in the sunflower and maize plots (i.e., tall crops) than in the potato plots (i.e., short crops) (p < 0.05). This is due to straw residues affecting the migration and recovery of the mulch. The abundance and fragmentation of microplastics were significantly higher in the sunflower and maize plots where plastic mulch was extensively used because these tall crops anchored the mulch near their stem–root systems. The mulch was then slowly aged (e.g., via wind erosion) before being fragmented due to agricultural practices (e.g., mechanical plowing and residue retention). Although microplastics sourced from mulch are probably immobilized by straw residues in the short term, fragile and easily broken pieces of mulch are eventually released into the soil due to agricultural practices. The findings suggest that different cropping characteristics can affect the abundance and fragmentation of microplastics in agricultural soils, even within the same region, and thus the level and type of microplastic pollution. Traditional plastic mulch should be replaced with biodegradable mulch to reduce microplastic pollution in agricultural fields.
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