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1.
J Agric Food Chem ; 72(14): 7672-7683, 2024 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-38530782

RESUMEN

Agrochemical residues and nitrous oxide (N2O) emissions have caused considerable threats to agricultural soil ecology. Nanoscale zerovalent iron (nZVI) and nitrification inhibitors might be complementary to each other to diminish soil agrochemical residues and N2O emissions and enhance soil bacterial community diversities. Compared to the control, the nZVI application declined soil paclobutrazol residues by 5.9% but also decreased the bacterial community co-occurrence network node. Combined nZVI and Dicyandiamide applications significantly decreased soil N2O emission rates and paclobutrazol residues but promoted Shannon diversity of the bacterial community. The increased soil pH, ammonium nitrogen, and Actinobacteriota could promote soil paclobutrazol dissipation. The nZVI generated double-edged sword effects of positively decreasing paclobutrazol residues and N2O emissions but negatively influencing soil multifunctionalities. The nZVI and Dicyandiamide could be complementary to each other in diminishing soil agrochemical residues and N2O emission rates but promoting soil bacterial community diversities simultaneously.


Asunto(s)
Guanidinas , Óxido Nitroso , Suelo , Triazoles , Suelo/química , Óxido Nitroso/química , Nitrificación , Agricultura , Bacterias/genética , Fertilizantes/análisis , Agroquímicos/farmacología , Nitrógeno/química
2.
Environ Pollut ; 301: 118993, 2022 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-35183669

RESUMEN

Nitrogen (N) and phosphorous (P) enrichment play an important role in regulating soil N2O emission, but their interactive effect remains elusive (i.e. whether the effect of P or N enrichment on soil N2O emission varies between ambient and elevated soil N or P conditions). Here, we conducted a Bayesian meta-analysis across the global natural ecosystems to determine this effect. Our results showed that P enrichment significantly decreased soil N2O emission by 13.9% at ambient soil N condition. This N2O mitigation is likely due to the decreased soil NO3--N content (-17.6%) derived by the enhanced plant uptake when the P limitation was alleviated by P enrichment. However, this P-induced N2O (and NO3--N) mitigation was not found at elevated soil N condition. Additionally, N enrichment significantly increased soil N2O emission by 101.4%, which was associated with the increased soil NH4+-N (+41.0%) and NO3--N (+82.3%). However, the effect of N enrichment on soil N2O emission did not differ between ambient and elevated soil P subgroups, indicating that the P-derived N2O mitigation could be masked by N enrichment. Further analysis showed that manipulated N rate, soil texture, soil dissolved organic nitrogen, soil total nitrogen, soil organic carbon, soil pH, aboveground plant biomass, belowground plant biomass, and plant biomass nitrogen were the main factors affecting soil N2O emission under N enrichment. Taken together, our study provides evidence that P enrichment has the potential to reduce soil N2O emission from natural ecosystems, but this mitigation effect could be masked by N enrichment.


Asunto(s)
Nitrógeno , Suelo , Teorema de Bayes , Carbono , Ecosistema , Nitrógeno/química , Óxido Nitroso/química , Fósforo , Suelo/química
3.
Ecotoxicol Environ Saf ; 221: 112451, 2021 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-34174737

RESUMEN

Manganese oxides and iron oxides have been widely introduced in constructed wetlands (CWs) for sewage treatment due to their extensiveness in nature and their ability to participate in various reactions, but their effects on greenhouse gas (GHG) emissions remain unclear. Here, a set of vertical subsurface-flow CWs (Control, Fe-VSSCWs, and Mn-VSSCWs) was established to comprehensively evaluate which are the better metal substrate materials for CWs, iron oxides or manganese oxides, through water quality and the global warming potential (GWP) of nitrous oxide (N2O), methane (CH4), and carbon dioxide (CO2). The results revealed that the removal efficiencies of chemical oxygen demand (COD), total nitrogen (TN), and total phosphorus (TP) in Mn-VSSCWs were all higher than that in Fe-VSSCWs, and manganese oxides could almost completely suppress the CH4 production and reduce GWP (from 8.15 CO2-eq/m2/h to 7.17 mg CO2-eq/m2/h), however, iron oxides promoted GWP (from 8.15 CO2-eq/m2/h to 10.84 mg CO2-eq/m2/h), so manganese oxides are the better CW substrate materials to achieve effective sewage treatment while reducing the greenhouse gas effect.


Asunto(s)
Contaminantes Atmosféricos/química , Compuestos Férricos/química , Efecto Invernadero/prevención & control , Compuestos de Manganeso/química , Óxidos/química , Purificación del Agua/métodos , Humedales , Análisis de la Demanda Biológica de Oxígeno , Dióxido de Carbono/química , Metano/química , Nitrógeno/química , Óxido Nitroso/química , Fósforo/química , Contaminantes del Agua/química , Calidad del Agua
4.
PLoS One ; 14(5): e0216244, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31048904

RESUMEN

Alpine wetlands are important ecosystems, but an increased availability of soil nutrients may affect their soil nitrous oxide (N2O) fluxes and key enzyme activities. We undertook a 3-year experiment of observing nitrogen (N) and/or phosphorus (P) addition to alpine wetland soils of the Tibetan Plateau, China, with measurements made of soil extracellular enzyme activities and soil N2O fluxes. Our study showed that soil N2O flux was significantly increased by 72% and 102% following N and N+P additions, respectively. N addition significantly increased acid phosphatase (AP) and ß-1, 4-N-acetyl-glucosaminidase (NAG) activities by 32% and 26%, respectively. P addition alone exerted a neutral effect on soil AP activities, while increasing NAG activities. We inferred that microbes produce enzymes based on 'resource allocation theory', but that a series of constitutive enzymes or the treatment duration interfere with this response. Our findings suggest that N addition increases N- and P-cycling enzyme activities and soil N2O flux, whereas P addition exerts a neutral effect on P-cycling enzyme activities and N2O flux after 3 years of nutrient applications to an alpine wetland.


Asunto(s)
Nitrógeno/química , Óxido Nitroso/química , Fósforo/química , Suelo/química , Humedales , Fosfatasa Ácida/química , Hexosaminidasas/química , Tibet
5.
Bioresour Technol ; 226: 211-219, 2017 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-28002781

RESUMEN

In this study nitrogen removal via nitrite >80% was achieved after approximately 80days in a sequencing batch reactor (SBR) treating pre-treated industrial wastewater originating from the potato industry. Thereafter, SBR performance was investigated during the formation of aerobic nitrite granules (ANG). The first granules appeared after 26days leading to full granulation after 64days. ANG showed excellent settling properties, as the Sludge Volume Index (SVI) went down to 16mL/g and a SVI10/SVI30=1 was obtained. qPCR analysis showed that slow growing organisms, especially polyphosphate accumulating organisms (PAO) were stimulated by an anaerobic feeding strategy. The average nitrogen removal was 95.3% over the entire operational period, and it mainly followed the "nitrite-route". Moreover, with ANG also phosphorus removal efficiencies up to 65.7% could be achieved. However, it has to be mentioned that nitrous oxide was an important denitrification product, which implies some environmental concerns.


Asunto(s)
Reactores Biológicos , Nitritos/análisis , Aguas del Alcantarillado/análisis , Solanum tuberosum , Eliminación de Residuos Líquidos/métodos , Aguas Residuales/análisis , Agricultura , Desnitrificación , Diseño de Equipo , Nitrógeno/análisis , Nitrógeno/química , Óxido Nitroso/análisis , Óxido Nitroso/química , Fósforo/química
6.
Environ Sci Pollut Res Int ; 23(15): 15657-64, 2016 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-27137189

RESUMEN

The short- and long-term influences of ferric iron (Fe(III)) on nutrients removal and nitrous oxide (N2O) emission during SNDPR process were evaluated. According to the continuous cycle experiments, it was concluded that the addition of Fe(III) could lower the nitrogen removal of the following cycle during SNDPR process, which was mainly induced by the chemical removal of phosphorus. However, the impacts were transitory, and simultaneous nitrogen and phosphorus removal would recover from the inhibition of Fe(III) after running certain cycles. Moreover, the addition of Fe(III) could stimulate N2O emission transitorily during SNDPR process. However, if Fe(III) was added into reactor continuously, the nitrogen removal would be improved, especially at low Fe load condition. It was because that the activity of NO reductase was enhanced by the addition of Fe. However, the low Fe load in reactor would induce more N2O emission. When Fe(III) load was 40 mg/L in the reactor, the N2O yield was 10 % higher than control. The TN removal was weakened when Fe(III) load reached to 60 mg/L, and the N2O yield was lower than control, due to the inhibition of the high Fe load on denitrification enzymes.


Asunto(s)
Desnitrificación , Hierro/química , Nitrificación , Óxido Nitroso/química , Fósforo/química , Nitrógeno/química
7.
Adv Appl Microbiol ; 94: 109-59, 2016.
Artículo en Inglés | MEDLINE | ID: mdl-26917243

RESUMEN

Soil amendments with biochar to improve soil fertility and increase soil carbon stocks have received some high-level attention. Physical and chemical analyses of amended soils and biochars from various feedstocks are reported, alongside some evaluations of plant growth promotion capabilities. Fewer studies investigated the soil microbiota and their potential to increase cycling and mobilization of nutrients in biochar-amended soils. This review is discussing the latest findings in the bacterial contribution to cycling and mobilizing nitrogen, phosphorus, and sulfur in biochar-amended soils and potential contributions to plant growth promotion. Depending on feedstock, pyrolysis, soil type, and plant cover, changes in the bacterial community structure were observed for a majority of the studies using amplicon sequencing or genetic fingerprinting methods. Prokaryotic nitrification largely depends on the availability of ammonium and can vary considerably under soil biochar amendment. However, denitrification to di-nitrogen and in particular, nitrous oxide reductase activity is commonly enhanced, resulting in reduced nitrous oxide emissions. Likewise, bacterial fixation of di-nitrogen appears to be regularly enhanced. A paucity of studies suggests that bacterial mobilization of phosphorus and sulfur is enhanced as well. However, most studies only tested for extracellular sulfatase and phosphatase activity. Further research is needed to reveal details of the bacterial nutrient mobilizing capabilities and this is in particular the case for the mobilization of phosphorus and sulfur.


Asunto(s)
Bacterias/metabolismo , Carbón Orgánico/química , Fertilizantes , Nitrógeno/metabolismo , Fósforo/química , Azufre/química , Reactores Biológicos/microbiología , Desnitrificación , Nitrificación , Óxido Nitroso/química , Oxidorreductasas/metabolismo , Suelo/química , Microbiología del Suelo
8.
Bioresour Technol ; 200: 380-7, 2016 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-26512862

RESUMEN

The aim of this study was to evaluate the feasibility of achieving nitrogen (N) removal using a lab-scale sequencing batch reactor (SBR) exposed to anoxic/aerobic (AN/OX) phases, focusing to achieve aerobic denitrification. This process will minimize emissions of N2O greenhouse gas. The effects of different operating parameters on the reactor performance were studied: cycle duration, AN/OX ratio, pH, dissolved oxygen concentration (DOC), and organic load. The highest inorganic N removal (NiR), close to 70%, was obtained at pH=7.5, low organic load (440mgCOD/(Lday)) and high aeration given by 12h cycle, AN/OX ratio=0.5:1.0 and DOC higher than 4.0mgO2/L. Nitrification followed by high-rate aerobic denitrification took place during the aerobic phase. Aerobic denitrification could be attributed to Tetrad-forming organisms (TFOs) with phenotype of glycogen accumulating organisms using polyhydroxyalkanoate and/or glycogen storage. The proposed AN/OX system constitutes an eco-friendly N removal process providing N2 as the end product.


Asunto(s)
Reactores Biológicos , Desnitrificación , Nitrificación , Óxido Nitroso/química , Diseño de Equipo , Gases , Glucógeno/química , Concentración de Iones de Hidrógeno , Nitrógeno/química , Oxígeno/química , Fenotipo , Fósforo/química , Aguas Residuales
9.
Ying Yong Sheng Tai Xue Bao ; 26(7): 1954-60, 2015 Jul.
Artículo en Chino | MEDLINE | ID: mdl-26710619

RESUMEN

To clarify the effects of biochar addition (0.5%, 1.5%, 2.5%, 3.5%) on the emission of carbon dioxide (CO2) and nitrous oxide (N2O), pH and microbial communities of the tea garden soil, an indoor incubation experiment was conducted using the acidulated tea-planted soil. Results showed that the emissions of CO2 and N2O and the rate of C, N mineralization were increased in a short term after the addition of biochar compared with the control, while the promoting effect was weakened along with increasing the addition of biochar. The pH, dehydrogenase activity and microbial biomass carbon were increased in the biochar treatments. Phospholi-pid fatty acid (PLFA) with different markers was measured and the most PLFA was detected in the group in the 1.5% biochar treatment with significant differences (P<0.05) compared with the control. In addition, the higher levels of 16:0, 14:0 (bacteria), 18:lω9c (fungi), l0Me18:0 (actinomycetes) groups were observed and there were significant differences (P <0.05) in individual phospholipid fatty acid among the different treatments. Taken together, the acidulated tea-planted soil, soil microbial biomass and microbial number were improved after addition of biochar.


Asunto(s)
Dióxido de Carbono/química , Carbón Orgánico/química , Óxido Nitroso/química , Microbiología del Suelo , Suelo/química , Agricultura , Bacterias/crecimiento & desarrollo , Biomasa , Camellia sinensis , Hongos/crecimiento & desarrollo
10.
J Hazard Mater ; 286: 15-29, 2015 Apr 09.
Artículo en Inglés | MEDLINE | ID: mdl-25550080

RESUMEN

Biological wastewater treatment processes (WWTPs), by nature of their reliance on biological entities to degrade organics and sometimes remove nutrients, are vulnerable to toxicants present in their influent. Various toxicity measurement methods have been adopted for biological WWTPs, but most are performed off-line, and cannot be adapted to on-line monitoring tools to provide an early warning for WWTP operators. However, the past decade has seen a rapid expansion in the research and development of biosensors that can be used for toxicity assessment of aquatic environments. Some of these biosensors have also been shown to be effective for use in biological WWTPs. Nevertheless, more research is needed to: examine the sensitivity of assays and sensors based on single organisms to various toxicants and develop a matrix of biosensors or a biosensor incorporating multiple organisms that can protect WWTPs; test the micro fuel cell (MFC)-based biosensors with real wastewaters and correlate the results with the well-established oxygen uptake rate (OUR)-based or CH4-based toxicity assay; and, develop advanced data processing methods for interpreting the results of on-line toxicity sensors in real WWTPs to reduce the noise due to the normal fluctuation in influent quality and quantity.


Asunto(s)
Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Adenosina Trifosfato/química , Compuestos de Amonio/química , Animales , Bacillus subtilis/efectos de los fármacos , Técnicas Biosensibles , Dióxido de Carbono/química , Daphnia , Electroquímica , Escherichia coli/efectos de los fármacos , Metano/química , Pruebas de Sensibilidad Microbiana , Nitrógeno/química , Óxido Nitroso/química , Oxidorreductasas/química , Oxígeno/química , Saccharomyces cerevisiae/efectos de los fármacos , Aguas del Alcantarillado , Eliminación de Residuos Líquidos/métodos , Aguas Residuales
11.
Environ Sci Pollut Res Int ; 22(6): 4173-82, 2015 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-25273518

RESUMEN

Aerobic denitrification is the main process for high N2O production in acid tea field soil. However, the biological mechanisms for the high emission are not fully understood. In this study, we examined N2O emission and denitrifier communities in 100-year-old tea soils with four pH levels (3.71, 5.11, 6.19, and 7.41) and four nitrate concentration (0, 50, 200, and 1000 mg kg(-1) of NO3 (-)-N) addition. Results showed the highest N2O emission (10.1 mg kg(-1) over 21 days) from the soil at pH 3.71 with 1000 mg kg(-1) NO3 (-) addition. The N2O reduction and denitrification enzyme activity in the acid soils (pH <7.0) were significantly higher than that of soils at pH 7.41. Moreover, TRF 78 of nirS and TRF 187 of nosZ dominated in soils of pH 3.71, suggesting an important role of acidophilic denitrifiers in N2O production and reduction. CCA analysis also showed a negative correlation between the dominant denitrifier ecotypes (nirS TRF 78, nosZ TRF 187) and soil pH. The representative sequences were identical to those of cultivated denitrifiers from acidic soils via phylogenetic tree analysis. Our results showed that the acidophilic denitrifier adaptation to the acid environment results in high N2O emission in this highly acidic tea soil.


Asunto(s)
Bacterias/metabolismo , Camellia sinensis/fisiología , Óxido Nitroso/metabolismo , Microbiología del Suelo , Suelo/química , Bacterias/clasificación , Bacterias/genética , Secuencia de Bases , Desnitrificación , Concentración de Iones de Hidrógeno , Nitratos , Óxido Nitroso/química , Filogenia
12.
Environ Sci Technol ; 48(17): 10354-62, 2014 Sep 02.
Artículo en Inglés | MEDLINE | ID: mdl-25105802

RESUMEN

The mechanism of N2O formation during the low-temperature selective catalytic reduction reaction (SCR) over Mn-Fe spinel was studied. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and transient reaction studies demonstrated that the Eley-Rideal mechanism (i.e., the reaction of adsorbed NH3 species with gaseous NO) and the Langmuir-Hinshelwood mechanism (i.e., the reaction of adsorbed NH3 species with adsorbed NOx species) both contributed to N2O formation. However, N2O selectivity of NO reduction over Mn-Fe spinel through the Langmuir-Hinshelwood mechanism was much less than that through the Eley-Rideal mechanism. The ratio of NO reduction over Mn-Fe spinel through the Langmuir-Hinshelwood mechanism remarkably increased; therefore, N2O selectivity of NO reduction over Mn-Fe spinel decreased with the decrease of the gas hourly space velocity (GHSV). As the gaseous NH3 concentration increased, N2O selectivity of NO reduction over Mn-Fe spinel increased because of the promotion of NO reduction through the Eley-Rideal mechanism. Meanwhile, N2O selectivity of NO reduction over Mn-Fe spinel decreased with the increase of the gaseous NO concentration because the formation of NH on Mn-Fe spinel was restrained. Therefore, N2O selectivity of NO reduction over Mn-Fe spinel was related to the GHSV and concentrations of reactants.


Asunto(s)
Óxido de Aluminio/química , Amoníaco/química , Frío , Hierro/química , Óxido de Magnesio/química , Manganeso/química , Óxido Nítrico/química , Óxido Nitroso/química , Adsorción , Catálisis , Oxidación-Reducción , Espectroscopía Infrarroja por Transformada de Fourier
13.
Chemosphere ; 109: 56-63, 2014 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-24873707

RESUMEN

Although wastewater biological nutrient removal can be achieved by alternating the anaerobic-oxic-anoxic phases, significant amount of nitrous oxide (N2O) is generated in oxic phases, where ammonia-oxidizing bacteria (AOB) rather than heterotrophic denitrifiers are the main contributors. Here a new efficient strategy to remarkably reduce N2O generation was reported. It was found that by cancelling the anaerobic phase and extending the idle phase the N2O generation was reduced by 42% using synthetic wastewater, whereas the total nitrogen and phosphorus removals were unaffected. The mechanistic investigations revealed that the cancelling of anaerobic phase benefited heterotrophic denitrifiers instead of AOB to be responsible for nitrogen removal in the oxic phases, increased the ratio of total nitrogen removal driven by external carbon source, and decreased nitrite accumulation. Quantitative real-time polymerase chain reaction and fluorescence in situ hybridization analyses further showed that the new strategy increased the number of N2O reducing bacteria but decreased the abundance of glycogen accumulating organisms, with N2O as their primary denitrification product. It was also determined that the ratio of nitric oxide reductase activity to N2O reductase activity was significantly decreased after anaerobic phase was cancelled. All these observations were in accord with the reduction of N2O production. The feasibility of this strategy to minimize the generation of N2O was finally confirmed for a real municipal wastewater. The results reported in this paper provide a new viewpoint to reduce N2O generation from wastewater biological nutrient removal.


Asunto(s)
Bacterias/metabolismo , Reactores Biológicos/microbiología , Nitrógeno/metabolismo , Óxido Nitroso/metabolismo , Eliminación de Residuos Líquidos/métodos , Aguas Residuales/química , Amoníaco/química , Amoníaco/metabolismo , Bacterias/crecimiento & desarrollo , Fenómenos Fisiológicos Bacterianos , Desnitrificación , Nitrógeno/química , Óxido Nitroso/química , Fósforo/química , Fósforo/metabolismo , Eliminación de Residuos Líquidos/instrumentación
14.
J Environ Sci (China) ; 25(7): 1338-45, 2013 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-24218845

RESUMEN

A laboratory scale experiment of composting in a forced aeration system using pig manure with cornstalks was carried out to investigate the effects of both phosphogypsum and dicyandiamide (DCD, C2H4N4) as additives on gaseous emissions and compost quality. Besides a control, there were three amended treatments with different amounts of additives. The results indicated that the phosphogypsum addition at the rate of 10% of mixture dry weight decreased NH3 and CH4 emissions significantly during composting. The addition of DCD at the rate of 0.2% of mixture dry weight together with 10% of phosphogypsum further reduced the N2O emission by affecting the nitrification process. Reducing the phosphogypsum addition to 5% in the presence of 0.2% DCD moderately increased the NH3 emissions but not N2O emission. The additives increased the ammonium content and electrical conductivity significantly in the final compost. No adverse effect on organic matter degradation or the germination index of the compost was found in the amended treatments. It was recommended that phosphogypsum and DCD could be used in composting for the purpose of reducing NH3, CH4 and N2O emissions. Optimal conditions and dose of DCD additive during composting should be determined with different materials and composting systems in further study.


Asunto(s)
Contaminantes Atmosféricos/análisis , Amoníaco/análisis , Sulfato de Calcio/química , Guanidinas/química , Metano/análisis , Óxido Nitroso/análisis , Fósforo/química , Contaminantes Atmosféricos/química , Contaminación del Aire/prevención & control , Amoníaco/química , Animales , Estiércol , Metano/química , Óxido Nitroso/química , Tallos de la Planta , Suelo/química , Porcinos , Zea mays
15.
Water Res ; 47(3): 1390-8, 2013 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-23276427

RESUMEN

Stormwater treatment ponds provide a variety of functions including sediment retention, organic and nutrient removal, and habitat restoration. The treatment ponds are, however, also a source of greenhouse gases. The objectives of this study were to assess greenhouse gas (CH(4), CO(2) and N(2)O) emissions in duckweed treatment ponds (DWPs) treating simulated stormwater and to determine the role of ammonia-oxidizing organisms in nutrient removal and methanogens in greenhouse gas emissions. Two replicated DWPs operated at a hydraulic retention time (HRT) of 10 days were able to remove 84% (± 4% [standard deviation]) chemical oxygen demand (COD), 79% (± 3%) NH(4)(+)-N, 86% (± 2%) NO(3)(-)-N and 56% (± 7%) orthophosphate. CH(4) emission rates in the DWPs ranged from 502 to 1900 mg CH(4) m(-2) d(-1) while those of nitrous oxide (N(2)O) ranged from 0.63 to 4 mg N(2)O m(-2) d(-1). The CO(2) emission rates ranged from 1700 to 3300 mg CO(2) m(-2) day(-1). Duckweed coverage on water surface along with the continued deposit of duckweed debris in the DWPs and low-nutrient influent water created a low dissolved oxygen environment for the growth of unique ammonia-oxidizing organisms and methanogens. Archaeal and bacterial amoA abundance in the DWPs ranged from (1.5 ± 0.2) × 10(7) to (1.7 ± 0.2) × 10(8) copies/g dry soil and from (1.0 ± 0.3) × 10(3) to (1.5 ± 0.4) × 10(6) copies/g dry soil, respectively. The 16S rRNA acetoclastic and hydrogenotrophic methanogens ranged from (5.2 ± 0.2) × 10(5) to (9.0 ± 0.3) × 10(6) copies/g dry soil and from (1.0 ± 0.1) × 10(2) to (5.5 ± 0.4) × 10(3) copies/g dry soil, respectively. Ammonia-oxidizing archaea (AOA) appeared to be the dominant nitrifiers and acetoclastic Methanosaeta was the major methanogenic genus. The results suggest that methane is the predominant (>90%) greenhouse gas in the DWPs, where the relatively low stormwater nutrient inputs facilitate the growth of K-strategists such as AOA and Methanosaeta that may be responsible for ammonia removal and greenhouse gas emissions, respectively.


Asunto(s)
Araceae , Metano/química , Archaea , Dióxido de Carbono/química , Óxido Nitroso/química , Estanques , Purificación del Agua
16.
Acc Chem Res ; 45(2): 276-87, 2012 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-21875073

RESUMEN

Small-molecule activation by transition metals is essential to numerous organic transformations, both biological and industrial. Creating useful metal-mediated activation systems often depends on stabilizing the metal with uncommon low oxidation states and low coordination numbers. This provides a redox-active metal center with vacant coordination sites well suited for interacting with small molecules. Monovalent nickel species, with their d(9) electronic configuration, are moderately strong one-electron reducing agents that are synthetically attractive if they can be isolated. They represent suitable reagents for closing the knowledge gap in nickel-mediated activation of small molecules. Recently, the first strikingly stable dinuclear ß-diketiminate nickel(I) precursor complexes were synthesized, proving to be suitable promoters for small-molecule binding and activation. They have led to many unprecedented nickel complexes bearing activated small molecules in different reduction stages. In this Account, we describe selected achievements in the activation of nitrous oxide (N(2)O), O(2), the heavier chalcogens (S, Se, and Te), and white phosphorus (P(4)) through this ß-diketiminatonickel(I) precursor species. We emphasize the reductive activation of O(2), owing to its promise in oxidation processes. The one-electron-reduced O(2) activation product, that is, the corresponding ß-diketiminato-supported Ni-O(2) complex, is a genuine superoxonickel(II) complex, representing an important intermediate in the early stages of O(2) activation. It selectively acts as an oxygen-atom transfer agent, hydrogen-atom scavenger, or both towards exogenous organic substrates to yield oxidation products. The one-electron reduction of the superoxonickel(II) moiety was examined by using elemental potassium, ß-diketiminatozinc(II) chloride, and ß-diketiminatoiron(I) complexes, affording the first heterobimetallic complexes featuring a [NiO(2)M] subunit (M is K, Zn, or Fe). Through density functional theory (DFT) calculations, the geometric and electronic structures of these complexes were established and their distinctive reactivity, including the unprecedented monooxygenase-like activity of a bis(µ-oxo)nickel-iron complex, was studied. The studies have further led to other heterobimetallic complexes containing a [NiO(2)M] core, which are useful for understanding the influence of the heterometal on structure-reactivity relationships. The activation of N(2)O led directly to the hydrogen-atom abstraction product bis(µ-hydroxo)nickel(II) species and prevented isolation of any intermediate. In contrast, the activation of elemental S, Se, and Te with the same nickel(I) reagent furnished activation products with superchalcogenido E(2)(-) (E is S, Se, or Te) and dichalcogenido E(2)(2-) ligand in different activation stages. The isolable supersulfidonickel(II) subunit may serve as a versatile building block for the synthesis of heterobimetallic disulfidonickel(II) complexes with a [NiS(2)M] core. In the case of white phosphorus, the P(4) molecule has been coordinated to the nickel(I) center of dinuclear ß-diketiminatonickel(I) precursor complexes; however, the whole P(4) subunit is a weaker electron acceptor than the dichalcogen ligands E(2), thus remaining unreduced. This P(4) binding mode is rare and could open new doors for subsequent functionalization of P(4). Our advances in understanding how these small molecules are bound to a nickel(I) center and are activated for further transformation offer promise for designing new catalysts. These nickel-containing complexes offer exceptional potential for nickel-mediated transformations of organic molecules and as model compounds for mimicking active sites of nickel-containing metalloenzymes.


Asunto(s)
Níquel/química , Calcógenos/química , Electrones , Estructura Molecular , Óxido Nitroso/química , Oxidación-Reducción , Oxígeno/química , Fósforo/química , Selenio/química , Telurio/química , Elementos de Transición/química
17.
Pak J Biol Sci ; 15(7): 325-32, 2012 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-24163958

RESUMEN

Caesalpinia pulcherrima L. Swartz (Caesalpiniaceae) is an ornamental plant also used as a common medicinal plant in India, Taiwan and South-East Asian countries. Majority of the diseases/disorders are mainly linked to oxidative stress due to free radicals. The aims of this study were to screen for phytochemical constituents, evaluate cytotoxicity, in vitro antioxidant activity and estimation of total phenolic content of extracts of pods of Caesalpinia pulcherrima. Phytochemical analysis revealed the presence of tannins, flavonoids, steroids and alkaloids. Brine Shrimp Lethality (BSL) bioassay was used to investigate the cytotoxic effects. The LC50(microg mL(-1)) values obtained for extracts as 750 microg mL(-1) for petroleum ether extract, 800 microg mL(-1) for chloroform extract and 900 microg mL(-1) for methanol extract. The total phenolic content of the methanolic extract was 38.04% w/w, equivalent to gallic acid. Petroleum ether, chloroform and methanolic extracts of Caesalpinia pulcherrima and standard ascorbic acid were found to be scavenger of DPPH radical with an IC50 of 124.75, 112.08, 54.34 and 13.86 microg mL(-1), respectively. Methanolic extract was good scavenger of DPPH radical. Petroleum ether, chloroform, ethyl acetate soluble fraction of methanolic extracts of pods of Caesalpinia pulcherrima and ascorbic acid were found to be scavenger of nitric oxide radical with an IC50 of 93.32, 65.12, 54.83 and 12.59 microg mL(-1), respectively. Ethyl acetate soluble fraction was found to be good scavenger of nitric oxide radical. Our conclusion provides support that the crude extracts of C. pulcherrima is a probable source of natural antioxidants and this justified its uses in folkloric medicines.


Asunto(s)
Antioxidantes/farmacología , Caesalpinia , Fenoles/farmacología , Extractos Vegetales/farmacología , Animales , Antioxidantes/química , Antioxidantes/aislamiento & purificación , Antioxidantes/toxicidad , Artemia/efectos de los fármacos , Compuestos de Bifenilo/química , Caesalpinia/química , Frutas , Dosificación Letal Mediana , Óxido Nitroso/química , Fenoles/química , Fenoles/aislamiento & purificación , Fenoles/toxicidad , Fitoterapia , Picratos/química , Extractos Vegetales/química , Extractos Vegetales/aislamiento & purificación , Extractos Vegetales/toxicidad , Plantas Medicinales , Solventes/química
18.
J Environ Sci (China) ; 24(9): 1616-23, 2012.
Artículo en Inglés | MEDLINE | ID: mdl-23520869

RESUMEN

Nitrous oxide (N2O) emission has been reported to be enhanced during denitrification when internally-stored compounds are used as carbon sources. However, negligible N2O emissions have been detected in the few studies where polyhydroxyalkanoates (PHA) were specifically used. This study investigated and compared the potential enhancement of N2O production, based on utilization of an internally-stored polymer and external carbon (acetate) by a denitrifying phosphorus removal culture. Results indicated that at relatively low chemical oxygen demand-to-nitrogen (COD/N) ratios, more nitrite was reduced to N2O in the presence of an external carbon source as compared to an internal carbon source (PHA). At relatively higher COD/N ratios, similar N2O reduction rates were obtained in all cases regardless of the type of carbon source available. N2O reduction rates were, however, generally higher in the presence of an internal carbon source. Results from the study imply that when the presence of an external carbon source is not sufficient to support denitrification, it is likely competitively utilized by different metabolic pathways of denitrifying polyphosphate accumulating organisms (DPAOs) and other ordinary denitrifiers. This study also reveals that the consumption of PHA is potentially the rate-limiting step for N2O reduction during denitrification.


Asunto(s)
Carbono/metabolismo , Óxido Nitroso/química , Fósforo/metabolismo , Polihidroxialcanoatos/química , Contaminantes Atmosféricos , Biomarcadores , Carbono/química , Efecto Invernadero , Fósforo/química
19.
Anesth Analg ; 111(1): 92-8, 2010 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-20519425

RESUMEN

BACKGROUND: Inhaled anesthetics are recognized greenhouse gases. Calculating their relative impact during common clinical usage will allow comparison to each other and to carbon dioxide emissions in general. METHODS: We determined infrared absorption cross-sections for sevoflurane and isoflurane. Twenty-year global warming potential (GWP(20)) values for desflurane, sevoflurane, and isoflurane were then calculated using the present and previously published infrared results, and best estimate atmospheric lifetimes were determined. The total quantity of each anesthetic used in 1 minimal alveolar concentration (MAC)-hour was then multiplied by the calculated GWP(20) for that anesthetic, and expressed as "carbon dioxide equivalent" (CDE(20)) in grams. Common fresh gas flows and carrier gases, both air/oxygen and nitrous oxide (N2O)/oxygen, were considered in the calculations to allow these examples to represent common clinical use of inhaled anesthetics. RESULTS: GWP(20) values for the inhaled anesthetics were: sevoflurane 349, isoflurane 1401, and desflurane 3714. CDE(20) values for 1 MAC-hour at 2 L fresh gas flow were: sevoflurane 6980 g, isoflurane 15,551 g, and desflurane 187,186 g. Comparison among these anesthetics produced a ratio of sevoflurane 1, isoflurane 2.2, and desflurane 26.8. When 60% N2O/40% oxygen replaced air/oxygen as a carrier gas combination, and inhaled anesthetic delivery was adjusted to deliver 1 MAC-hour of anesthetic, sevoflurane CDE(20) values were 5.9 times higher with N2O than when carried with air/O2, isoflurane values were 2.9 times higher, and desflurane values were 0.4 times lower. On a 100-year time horizon with 60% N2O, the sevoflurane CDE(100) values were 19 times higher than when carried in air/O2, isoflurane values were 9 times higher, and desflurane values were equal with and without N2O. CONCLUSIONS: Under comparable and common clinical conditions, desflurane has a greater potential impact on global warming than either isoflurane or sevoflurane. N2O alone produces a sizable greenhouse gas contribution relative to sevoflurane or isoflurane. Additionally, 60% N2O combined with potent inhaled anesthetics to deliver 1 MAC of anesthetic substantially increases the environmental impact of sevoflurane and isoflurane, and decreases that of desflurane. N2O is destructive to the ozone layer as well as possessing GWP; it continues to have impact over a longer timeframe, and may not be an environmentally sound tradeoff for desflurane. From our calculations, avoiding N2O and unnecessarily high fresh gas flow rates can reduce the environmental impact of inhaled anesthetics.


Asunto(s)
Anestesia por Inhalación , Anestésicos por Inhalación/química , Calentamiento Global , Algoritmos , Desflurano , Isoflurano/análogos & derivados , Isoflurano/química , Éteres Metílicos/química , Óxido Nitroso/química , Pautas de la Práctica en Medicina , Sevoflurano , Espectrofotometría Infrarroja
20.
J Environ Qual ; 38(5): 2147-58, 2009.
Artículo en Inglés | MEDLINE | ID: mdl-19704157

RESUMEN

Restoration of wetland hydrology can produce ecological benefits but may have unintended consequences. We examined effects of altered water level on release of dissolved reactive phosphorus (DRP) and greenhouse gases (GHG) in soil cores from a marsh being evaluated for restoration. We also measured field concentrations of DRP and other constituents in wetland porewater. Intact cores from a sampling location with higher Fe and lower calcium carbonate (CaCO(3)) contents released more DRP than another location, and displayed higher DRP under completely saturated compared to partly drained conditions. Porewater samples collected from the high-Fe location also contained higher DRP levels. Chemical data suggest that redox-driven reactions largely controlled DRP levels at the high-Fe site, while CaCO(3) adsorption was more important at the low-Fe site. Over the long term, water table elevation may attenuate P draining from the wetland due to decreased mineralization. However, such measures may increase P release in the short term. Raising the water level in soil cores resulted in decreased nitrous oxide (N(2)O) emissions, increased methane (CH(4)) emissions, and an overall increase in total global warming potential (GWP). The proportion of total GWP contributed by N(2)O decreased from 14% to < or = 1% as water level was raised, while the proportion contributed by CH(4) increased from 10 to 20% to 60 to 80%. Restoration of hydrology in the Rice Lake wetland has the potential to affect both local water quality and global air quality. These combined effects complicate the cost-to-benefit analysis of such wetland restoration efforts.


Asunto(s)
Efecto Invernadero , Metano/análisis , Óxido Nitroso/análisis , Fósforo/análisis , Contaminantes del Suelo/análisis , Humedales , Conservación de los Recursos Naturales , Metano/química , Minnesota , Óxido Nitroso/química , Fósforo/química
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