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Sustainable utilization of waste glycerol for 1,3-propanediol production over Pt/WOx/Al2O3 catalysts: Effects of catalyst pore sizes and optimization of synthesis conditions Texto completo
2021
Numpilai, Thanapha | Cheng, Chin Kui | Seubsai, Anusorn | Faungnawakij, Kajornsak | Limtrakul, Jumras | Witoon, Thongthai
Recycling of waste glycerol derived from biodiesel production to high value-added chemicals is essential for sustainable development of Bio-Circular-Green Economy. This work studied the conversion of glycerol to 1,3-propanediol over Pt/WOₓ/Al₂O₃ catalysts, pointing out the impacts of catalyst pore sizes and operating conditions for maximizing the yield of 1,3-propanediol. The results suggested that both pore confinement effect and number of available reactive metals as well as operating conditions determined the glycerol conversion and 1,3-propanediol selectivity. The small-pore 5Pt/WOₓ/S–Al₂O₃ catalyst (6.1 nm) gave a higher Pt dispersion (32.0%), a smaller Pt crystallite size (3.5 nm) and a higher number of acidity (0.47 mmol NH₃ g⁻¹) compared to those of the large-pore 5Pt/WOₓ/L-Al₂O₃ catalyst (40.3 nm). However, glycerol conversion and 1,3-propanediol yield over the small-pore 5Pt/WOₓ/S–Al₂O₃ catalyst were significantly lower than those of the large-pore Pt/WOₓ/L-Al₂O₃ catalyst, suggesting that the diffusional restriction within the small-pore catalyst suppressed transportation of molecules to expose catalytic active sites, favoring the excessive hydrogenolysis of 1,3-propanediol, giving rise to undesirable products. The best 1,3-propanediol yield of 32.8% at 78% glycerol conversion were achieved over the 5Pt/WOₓ/L-Al₂O₃ under optimal reaction condition of 220 °C, 6 MPa, 5 h reaction time and amount of catalyst to glycerol ratio of 0.25 g mL⁻¹. However, the 1,3-propanediol yield and glycerol conversion decreased to 19.6% and 51% after the 4th reaction-regeneration which were attributed to the carbonaceous deposition and the agglomeration of Pt particles.
Mostrar más [+] Menos [-]The atmospheric concentrations and emissions of major halocarbons in China during 2009–2019 Texto completo
2021
Yi, Liying | Wu, Jing | An, Minde | Xu, Weiguang | Fang, Xuekun | Yao, Bo | Li, Yixi | Gao, Ding | Zhao, Xingchen | Hu, Jianxin
Due to the characteristics of ozone-depleting and high global warming potential, chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs) and hydrofluorocarbons (HFCs) have been restricted by the Montreal Protocol and its amendments over the world. Considering that China is one of the main contributors to the emission of halocarbons, a long-term atmospheric observation on major substances including CFC-11 (CCl₃F), CFC-12 (CCl₂F₂), HCFC-22 (CHClF₂), HCFC-141b (CH₃CCl₂F), HCFC-142b (CH₃CClF₂) and HFC-134a (CH₂FCF₃) was conducted in five cities (Beijing, Hangzhou, Guangzhou, Lanzhou and Chengdu) of China during 2009–2019. The atmospheric concentrations of CFC-11, CFC-12, HCFC-141b and HCFC-142b all showed declining trends on the whole while those of HCFC-22 and HFC-134a were opposite. A paired sample t-test showed that the ambient mixing ratios of HCFC-22 and HFC-134a in cities were 41.9% and 25.7% higher on average than those in suburban areas, respectively, while the other substances did not show significant regional differences. The annual emissions of halocarbons were calculated using an interspecies correlation method and the results were generally consistent with the published estimates. Discrepancies between bottom-up inventories and the estimates in this study for CFCs emissions were found. Among the most consumed ozone depleting substances (ODSs) in China, CFCs accounted for 75.1% of the ozone depletion potential (ODP)-weighted emissions while HCFCs contributed a larger proportion (58.6%) of CO₂-equivalent emissions in 2019. China's emissions of HCFC-141b and HCFC-142b contributed the most to the global emission (17.8%–48.0%). The elimination of HCFCs in China will have a crucial impact on the HCFCs phase-out in the world.
Mostrar más [+] Menos [-]Saline mine-water alters the structure and function of prokaryote communities in shallow groundwater below a tropical stream Texto completo
2021
Chandler, Lisa | Harford, Andrew J. | Hose, Grant C. | Humphrey, Chris L. | Chariton, Anthony | Greenfield, Paul | O'Neill, Jenny
Bacteria and archaea (prokaryotes) are vital components for maintaining healthy function of groundwater ecosystems. The prokaryotic community composition and associated putative functional processes were examined in a shallow sandy aquifer in a wet-dry tropical environment. The aquifer had a contaminated gradient of saline mine-water, which primarily consisted of elevated magnesium (Mg²⁺) and sulfate (SO₄²⁻), although other major ions and trace metals were also present. Groundwaters were sampled from piezometers, approximately 2 m in depth, located in the creek channel upstream and downstream of the mine-water influence. Sampling occurred during the dry-season when only subsurface water flow was present. Next generation sequencing was used to analyse the prokaryote assemblages using 16S rDNA and metabolic functions were predicted with FAPROTAX. Significant changes in community composition and functional processes were observed with exposure to mine-waters. Communities in the exposed sites had significantly lower relative abundance of methanotrophs such as Methylococcaceae and methanogens (Methanobacteriaceae), but higher abundance in Nitrososphaeraceae, associated with nitrification, indicating potentially important changes in the biogeochemistry of the exposed sites. The changes were most strongly correlated with concentrations of SO₄²⁻, Mg²⁺ and Na⁺. This knowledge allows an assessment of the risk of mine-water contamination to groundwater ecosystem function and aids mine-water management.
Mostrar más [+] Menos [-]Ambient viral and bacterial distribution during long-range transport in Northern Taiwan Texto completo
2021
Chen, Nai-Tzu | Cheong, Ngok-Song | Lin, Chuan-Yao | Tseng, Chun-Chieh | Su, Huey-Jen
Long-range transport (LRT) reportedly carries air pollutants and microorganisms to downwind areas. LRT can be of various types, such as dust storm (DS) and frontal pollution (FP); however, studies comparing their effects on bioaerosols are lacking. This study evaluated the effect of LRT on viral and bacterial concentrations in Northern Taiwan. When LRT occurred and possibly affected Taiwan from August 2013 to April 2014, air samples (before, during, and after LRT) were collected in Cape Fugui (CF, Taiwan’s northernmost point) and National Taiwan University (NTU). Reverse-transcription quantitative polymerase chain reaction (RT-qPCR) was applied to quantify influenza A virus. qPCR and qPCR coupled with propidium monoazide were, respectively, used to quantify total and viable bacteria. Types and occurrence of LRT were confirmed according to the changing patterns of meteorological factors and air pollution, air mass sources (HYSPLIT model), and satellite images. Two Asian DS and three FP cases were included in this study. Influenza A virus was detected only on days before and during FP occurred on January 3–5, 2014, with concentrations of 0.87 and 10.19 copies/m³, respectively. For bacteria, the increase in concentrations of total and viable cells during Asian DSs (17–19 and 25–29 November 2013) was found at CF only (from 3.13 to 3.40 and from 2.62 to 2.85 log copies/m³, respectively). However, bacterial levels at NTU and CF both increased during FP and lasted for 2 days after FP. In conclusion, LRT increased the levels of influenza A virus and bacteria in the ambient air of Northern Taiwan, particularly at CF. During and 2 days (at least) after LRT, people should avoid outdoor activities, especially in case of FP.
Mostrar más [+] Menos [-]Identification of novel halogenated naturally occurring compounds in marine biota by high-resolution mass spectrometry and combined screening approaches Texto completo
2021
Belova, Lidia | Fujii, Yukiko | Cleys, Paulien | Śmiełowska, Monika | Haraguchi, Koichi | Covaci, Adrian
Marine animals, plants or bacteria are a source of bioactive naturally-occurring halogenated compounds (NHCs) such as bromophenols (BPs), bromoanisoles (BAs) and hydroxylated or methoxylated analogues of polybrominated diphenyl ethers (HO-PBDEs, MeO-PBDEs) and bromobiphenyls (HO-BBs, MeO-BBs). This study applied a comprehensive screening approach using liquid chromatography high-resolution mass spectrometry and combining target, suspect and non-target screening with the aim to identify new hydroxylated NHCs which might be missed by commonly applied gas chromatographic methods. 24 alga samples, 4 sea sponge samples and 7 samples of other invertebrates were screened. Target screening was based on 19 available reference standards of BPs, (di)OH-BDEs and diOH-BBs and yielded seven unequivocally identified compounds. 6-OH-BDE47 was the most frequently detected compound with a detection frequency of 31%. Suspect screening yielded two additional compounds identified in alga samples as well as 17 and 8 compounds identified in sea sponge samples of Lamellodysidea sp. and Callyspongia sp., respectively. The suspect screening results presented here confirmed the findings of previous studies conducted on sea sponge samples of Lamellodysidea sp. and Callyspongia sp. Additionally, in Lamellodysidea sp. and Callyspongia sp. 13 and 4 newly identified NHCs are reported including heptabrominated diOH-BDE, monochlorinated pentabrominated diOH-BDE, hexabrominated OH–MeO-BDE and others. Non-target screening allowed the identification of 31 and 20 polyhalogenated compounds in Lamellodysidea sp. and Callyspongia sp. samples, respectively. Based on the obtained fragmentation spectra, polybrominated dihydroxylated diphenoxybenzenes (diOH-PBDPBs), such as hepta-, octa- and nonabrominated diOH-BDPBs, could be identified in both species. To our knowledge, this study is the first report on the environmental presence of OH-PBDPBs.
Mostrar más [+] Menos [-]Cd bioavailability and nitrogen cycling microbes interaction affected by mixed amendments under paddy-pak choi continued planting Texto completo
2021
Li, Houfu | Abbas, Touqeer | Cai, Mei | Zhang, Qichun | Wang, Jingwen | Li, Yong | Di, Hongjie | Ṭāhir, Muḥammad
Cadmium (Cd) is the most concerning soil pollutant, and a threat to human health, especially in China. The in-situ immobilization of Cadmium by amendments is one of the most widely adopted methods to remedy soil contamination. The study was designed to evaluate the effect of organo-chemical amendments on soil Cd bioavailability and nitrogen cycling microbes under continuous planting of rice (Oryza sativa) and pak choi (Brassica chinensis L.). The experiment was carried out using four amendments, Lime, Zeolite, Superphosphate, and Biochar, at two different ratios; M1: at the ratio of 47:47:5:1, and M2 at the ratio of 71:23:5:1, respectively. Moreover, both M1 and M2 were enriched at four levels (T1: 0.5%; T2: 1%; T3: 2%; T4: 4%). Results showed that compared with CK (Cd enriched soils), the yield of rice under treatments of M1T1 and M2T1 increased by 8.93% and 8.36%, respectively. While the biomass (fresh weight) of pak choi under M1 and M2 amendments increased by 2.52–2.98 times and 0.76–2.89 times respectively, under enrichment treatments T1, T2, and T3. The total Cd concentrations in rice grains treated with M1T3 and M2T3 decreased by 89.25% and 93.16%, respectively, compared with CK. On the other hand, the total Cd concentrations in pak choi under M1T3 and M2T2 decreased by 92.86% and 90.23%, respectively. The results showed that soil pH was the main factor affecting Cd bioavailability in rice and pak choi. The Variance partitioning analysis (VPA) of rice and pak choi showed that soil pH was the most significant contributing factor. In the rice season, the contribution of soil pH (P) on Cd bioavailability was 10.14% (P = 0.102), and in the pak choi season, the contribution of soil pH was 8.38% (P = 0.133). Furthermore, the abundance of ammonia oxidation and denitrifying microorganisms had significantly correlation with soil pH and exchange Cd. In rice season, when the enrichment level of amendments increased from 0.5% (T1) to 2% (T3), the gene abundance of AOA, AOB, nirK, nirS and nosZ (І) tended to decrease. While in pak choi season, when the enrichment level increased at the level of 0.5% (T1), 1% (T2), and 2% (T3), the gene abundance of AOB, nirS, and nosZ (І) increased. Additionally, the gene abundance of AOA and nirK showed a reduction in the pak choi season contrasting to rice. And the mixed amendment M2 performed better at reducing Cd uptake than M1, which may have correlation with the ratio of lime and zeolite in them. Finally, we conclude that between these two amendments, when applied at a moderate level M2 type performed better than M1 in reducing Cd uptake, and also showed positive effects on both gene abundance and increase soil pH.
Mostrar más [+] Menos [-]Exposure to outdoor light at night and risk of breast cancer: A systematic review and meta-analysis of observational studies Texto completo
2021
Wu, Yue | Gui, Si-Yu | Fang, Yuan | Zhang, Mei | Hu, Cheng-Yang
Recent epidemiological studies have explored effects of light at night (LAN) exposure on breast cancer, but reported inconsistent findings. We performed a systematic review and meta-analysis of available evidence regarding the association of LAN assessed by satellite data with breast cancer. We conducted a systematic PubMed, Web of Science, and EMBASE database literature search until August 2020. Random-effects meta-analysis was applied to synthesis risk estimates. Heterogeneity was measured using statistics of Cochran’s Q, I², and Tau² (τ²). We assessed publication bias through funnel plot and Egger’s test. Moreover, subgroup analyses according to study design and menopausal status were performed. Risk of bias (RoB) of each included study was assessed using a domain-based RoB assessment tool. The confidence in the body of evidence was appraised using the GRADE approach for level-of-evidence translation. A total of 1157 studies were identified referring to LAN and breast cancer, from which 6 were included for quantitative synthesis. We found a significantly higher odds of breast cancer in the highest versus the lowest category of LAN exposure (OR = 1.11, 95% CI: 1.06, 1.16; I² = 0.0%). In the subgroup analyses stratified by menopausal status and study design, significant association was found in postmenopausal women (OR = 1.07, 95% CI = 1.00, 1.13) and cohort studies (OR = 1.11, 95% CI = 1.05, 1.18), while the summary estimates of premenopausal women and case-control studies showed no significance. The level of evidence for the association of LAN exposure and breast cancer risk was graded as “moderate” with “probably low” RoB according to the NTP/OHAT framework. In conclusion, this study suggests a link of LAN exposure with risk of breast cancer. Further high-quality prospective studies, especially performed in low-to middle-income countries with improvement in the area of LAN exposure assessment are needed to advance this field.
Mostrar más [+] Menos [-]Biochar amendment mitigated N2O emissions from paddy field during the wheat growing season Texto completo
2021
Zhang, Qianqian | Wu, Zhen | Zhang, Xi | Duan, Pengpeng | Shen, Haojie | Gunina, Anna | Yan, Xiaoyuan | Xiong, Zhengqin
Biochar may variably impact nitrogen (N) transformation and N-cycle-related microbial activities. Yet the mechanism of biochar amendment on nitrous oxide (N₂O) emissions from agricultural ecosystems remains unclear. Based on a 6-year long-term biochar amendment experiment, we applied a dual isotope (¹⁵N–¹⁸O) labeling technique with tracing transcriptional genes to differentiate the contribution of nitrifier nitrification (NN), nitrifier denitrification (ND), nitrification-coupled denitrification (NCD) and heterotrophic denitrification (HD) pathway to N₂O production. Then the field experiment provided quantitative data on dynamic N₂O emissions, soil mineral N and key functional marker gene abundances during the wheat growing season. By using ¹⁵N–¹⁸O isotope, biochar decreased N₂O emission derived from ND (by 45–94%), HD (by 35–46%) and NCD (by 30–64%) compared to the values under N application. Biochar increased the relative contribution of NN to total N₂O production as evidenced by the increase in ammonia-oxidizing bacteria, but did not influence the cumulative NN-derived N₂O. The field experiment found that the majority of the N₂O emissions peaked following fertilization, in parallel with soil NH₄⁺ and nitrite dynamics. Soil N₂O emissions during the wheat growing stage were effectively decreased (by 38–48%) by biochar amendment. Based on the correlation analyses and random forest analysis in both microcosm and field experiments, the decrease in nitrite concentration (by 62–65%) and increase in N₂O consumption were mainly responsible for net N₂O mitigation, as evidenced by the decrease in the ratios of nitrite reductase genes/transcripts (nirS, nirK and fungal nirK) and N₂O reductase gene/transcripts (nosZI and nosZII). Based on the extrapolation from microcosm to field, biochar significantly mitigated N₂O emissions by weakening the ND processes, since NCD and HD contributed little during the N₂O emission “peaks” following urea fertilization. Therefore, emphasis should be put on the ND process and nitrite accumulation during N₂O emission peaks and extrapolated to all agroecosystems.
Mostrar más [+] Menos [-]Source contribution analysis of nutrient pollution in a P-rich watershed: Implications for integrated water quality management Texto completo
2021
Han, Jianxu | Xin, Zhuohang | Han, Feng | Xu, Bo | Wang, Longfan | Zhang, Chi | Zheng, Yi
It is still a great challenge to address nutrient pollution issues caused by various point sources and non-point sources on the watershed scale. Source contribution analysis based on watershed modeling can help watershed managers identify major pollution sources, propose effective management plans and make smart decisions. This study demonstrated a technical procedure for addressing watershed-scale water pollution problems in an agriculture-dominated watershed, using the Dengsha River Watershed (DRW) in Dalian, China as an example. The SWAT model was improved by considering the constraints of soil nutrient concentration, i.e., nitrogen (N) and phosphorus (P), when modeling the nutrient uptake by a typical crop, corn. Then the modified SWAT model was used to quantify the contributions of all known pollution sources to the N and P pollution in the DRW. The results showed that crop production and trans-administrative wastewater discharge were the two dominant sources of nutrient pollution. This study further examined the responses of nutrient loss and crop yield to different fertilizer application schemes. The results showed that N fertilizer was the limiting factor for crop yield and that excessive levels of P were stored in the agricultural soils of the DRW. An N fertilizer application rate of approximately 40% of the current rate was suggested to balance water quality and environmental protection with crop production. The long-term impact of legacy P was investigated with a 100-year future simulation that showed the crop growth could maintain for 12 years even after P fertilization ceased. Our study highlights the need to consider source attribution, fertilizer application and legacy P impacts in agriculture-dominated watersheds. The analysis framework used in this study can provide a scientifically sound procedure for formulating adaptive and sustainable nutrient management strategies in other study areas.
Mostrar más [+] Menos [-]Deep winter intrusions of urban black carbon into a canyon near Santiago, Chile: A pathway towards Andean glaciers Texto completo
2021
Huneeus, Nicolás | Lapere, Rémy | Mazzeo, Andrea | Ordóñez Morales, César Eduardo | Donoso, Nicolás | Munoz, Ricardo | Rutllant, José A.
Black carbon transport from the Santiago Metropolitan Area, Chile, up to the adjacent Andes Cordillera and its glaciers is of major concern. Its deposition accelerates the melting of the snowpack, which could lead to stress on water supply in addition to climate feedback. A proposed pathway for this transport is the channelling through the network of canyons that connect the urban basin to the elevated summits, as suggested by modelling studies, although no observations have validated this hypothesis so far. In this work, atmospheric measurements from a dedicated field campaign conducted in winter 2015, under severe urban pollution conditions, in Santiago and the Maipo canyon, southeast of Santiago, are analysed. Wind (speed and direction) and particulate matter concentrations measured at the surface and along vertical profiles, demonstrate intrusions of thick layers (up to 600 m above ground) of urban black carbon deep into the canyon on several occasions. Transport of PM down-valley occurs mostly through shallow layers at the surface except in connection with deep valley intrusions, when a secondary layer in altitude with return flow (down-valley) at night is observed. The transported particulate matter is mostly from the vicinity of the entrance to the canyon and uncorrelated to concentrations observed in downtown Santiago. Reanalyses data show that for 10% of the wintertime days, deep intrusions into the Maipo canyon are prevented by easterly winds advecting air pollutants away from the Andes. Also, in 23% of the cases, intrusions proceed towards a secondary north-eastward branch of the Maipo canyon, leaving 67% of the cases with favourable conditions for deep penetrations into the main Maipo canyon. Reanalyses show that the wind directions associated to the 33% anomalous cases are related to thick cloud cover and/or the development of coastal lows.
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