Cationic organobismuth complex as an effective catalyst for conversion of CO2 into cyclic carbonates

In order to achieve high-efficiency conversion of CO₂ into valuable chemicals, and to exploit new applications of organobismuth compounds, cationic organobismuth complex with 5,6,7,12-tetrahydrodibenz[c,f][1,5] azabismocine framework was examined for the first time for the coupling of CO₂ into cyclic carbonates, using terminal epoxides as substrates and tetrabutylammonium halide as co-catalyst in a solvent-free environment under mild conditions. It is shown that the catalyst exhibited high activity and selectivity for the coupling reaction of CO₂ with a wide range of terminal epoxide. The selectivity of propylene carbonates could reach 100%, and the maximum turnover frequency was up to 10740 h^?1 at 120°C and 3 MPa CO₂ pressure when tetrabutylammonium iodide was used as co-catalyst. Moreover, the catalyst is environment friendly, resistant to air and water, and can be readily reused and recycled without any loss of activity, demonstrating a potential in industrial application.     

有机胺调控的CO2吸附材料的研究进展

当前,CO_2排放量急剧增加,空气中CO_2浓度正逐年增大.利用固体材料进行CO_2吸附可以实现CO_2减排的目的.CO_2吸附剂中,有机胺调控的固体材料因具有吸附量较大、对设备腐蚀性较小等特点而备受关注.然而,目前所报道的大部分有机胺调控的固体材料中N原子利用率较低,吸附速率较慢.在CO_2吸附体系中引入水分,使其参与CO_2捕集,有利于提高CO_2与氨基的反应摩尔比,增大N原子利用率,提高CO_2吸附性能.将含羟基的聚合物引入至有机胺调控的CO_2吸附材料之中,也可以获得相似的效果.本文综述了近年来有机胺调控的CO_2吸附材料的设计及"构-效"关系,具体包括有机胺调控的氧化物、多孔碳材料、硅基分子筛和金属-有机框架材料的合成及CO_2吸附机理.同时,展望了有机胺调控的CO_2吸附材料面临的科学挑战及发展机遇.     

14C of grasses as an indicator of fossil fuel CO2 pollution

Measuring the amount of fossil fuel carbon stored in the vegetation is now crucial to understand the mechanisms ruling climate changes. In this respect, highly polluted areas such as major towns represent “natural” laboratories because fossil fuel CO₂ (¹⁴C-free) is isotopically distinct from mean atmospheric CO₂ (¹⁴C-labeled). Here, a¹⁴C study of urban grasses near a major highway in Paris, France, shows that plants store up to 13% of fossil fuel carbon. The ¹⁴C composition of urban grasses is thus a novel parameter to assess the fossil fuel CO₂ pollution.     

Elevated CO2 affects the behavior of an ecologically and economically important coral reef fish

We tested the effect of near-future CO₂ levels (≈490, 570, 700, and 960 μatm CO₂) on the olfactory responses and activity levels of juvenile coral trout, Plectropomus leopardus, a piscivorous reef fish that is also one of the most important fisheries species on the Great Barrier Reef, Australia. Juvenile coral trout reared for 4 weeks at 570 μatm CO₂ exhibited similar sensory responses and behaviors to juveniles reared at 490 μatm CO₂ (control). In contrast, juveniles reared at 700 and 960 μatm CO₂ exhibited dramatically altered sensory function and behaviors. At these higher CO₂ concentrations, juveniles became attracted to the odor of potential predators, as has been observed in other reef fishes. They were more active, spent less time in shelter, ventured further from shelter, and were bolder than fish reared at 490 or 570 μatm CO₂. These results demonstrate that behavioral impairment of coral trout is unlikely if pCO₂ remains below 600 μatm; however, at higher levels, there are significant impacts on juvenile performance that are likely to affect survival and energy budgets, with consequences for predator–prey interactions and commercial fisheries.     

High Cu and Cd pollution in sediments from Sisimiut, Greenland. Adsorption to organic matter and fine particles

High concentrations of Cu of up to 200 mg/kg, and Cd of up to 4.0 mg/kg, were found in sediments from the aquatic environment around Sisimiut, Greenland. These concentrations are four times higher than the limiting concentration where toxicological effects are expected. The pollution could be linked to human activities in Sisimiut, a link that have not been investigated previously in Greenland. Except from the most polluted samples there was good correlation between heavy metal concentration and organic matter. Also some relationship between fine fraction and heavy metal concentration was observed.     

Eddy covariance CO2 flux measurements in nocturnal conditions: an analysis of the problem

A detailed analysis of the various processes at work in stable boundary layers was made. It pointed out that two main mechanisms may affect eddy covariance measurements in stable conditions and that their impacts were different. On one hand, intermittent turbulence produces strongly nonstationary events during which the validity of turbulent transport and storage measurements is uncertain. On the other hand, during breeze and drainage flow events, significant advection takes place and competes with turbulent flux and storage. Intermittent turbulence questions both the ability of eddy covariance systems to adequately capture turbulent flux and storage and the representativeness of the measurements. Ability of the systems to capture the fluxes could be improved by adapting the averaging time period or the high pass filtering characteristics. However, beyond this, the question of representativeness of the flux remains open as the flux measured during an intermittent turbulence event represents not only the source term, but also the removal of CO2 that built up in the control volume and that cannot be simply related to the source term. In these conditions, the u* discrimination is likely to be insufficient and should be completed with a stationarity criterion. Further research should allow determining better selection criteria. Advection occurs mainly in presence of flows associated with topographical slopes (drainage flows) or with land use changes (breezes). Direct advection measurements were performed at several sites, but the results were shown to be strongly site dependent. A classification based on the general flow pattern and on the source intensity evolution along streamlines was proposed here. Five different patterns were identified that helped to classify the different observations. The classification was found to be a fairly good fit for the observations. This could serve as a tool to better understand and quantify the fluxes at sites subjected to repeatable patterns.     

Resolving CO2 and methane hydrate formation kinetics

We analyse the kinetics of CO₂ and methane hydrate formation. The characteristic formation times are associated with different steps of the formation process. Conditions for minimising these rate times are identified while maintaining a regime where CO₂ hydrate is formed and methane remains predominantly gaseous. This involves a rapid pressurisation routine and accesses points well above the phase boundary in order to enable faster kinetics. Conditions for optimising rates and times, to obtain maximum CO₂ uptake with respect to CH₄, were identified as (1) stirring faster than 1,000 rpm, (2) rapid pressurisation to a partial pressure of around 50 bar for CO₂ and (3) re-use of contaminated as opposed to fresh water.     

Biopolymer-based membranes from polysaccharides for CO2 separation: a review

Environmental Chemistry Letters - The application of natural biopolymers such as polysaccharides for the fabrication of bio-based membranes has recently attracted attention for CO2...     

Bimetallic atomic site catalysts for CO2 reduction reactions: a review

Environmental Chemistry Letters - Carbon neutral becomes one of the most important environmental goals due to the excessive emission of CO2. The reduction of CO2 into valuable chemicals or fuels is...     

Long-term CO2 enrichment of a forest ecosystem: implications for forest regeneration and succession.

The composition and successional status of a forest affect carbon storage and net ecosystem productivity, yet it remains unclear whether elevated atmospheric carbon dioxide (CO2) will impact rates and trajectories of forest succession. We examined how CO2 enrichment (+200 microL CO2/L air differential) affects forest succession through growth and survivorship of tree seedlings, as part of the Duke Forest free-air CO2 enrichment (FACE) experiment in North Carolina, USA. We planted 2352 seedlings of 14 species in the low light forest understory and determined effects of elevated CO2 on individual plant growth, survival, and total sample biomass accumulation, an integrator of plant growth and survivorship over time, for six years. We used a hierarchical Bayes framework to accommodate the uncertainty associated with the availability of light and the variability in growth among individual plants. We found that most species did not exhibit strong responses to CO2. Ulmus alata (+21%), Quercus alba (+9.5%), and nitrogen-fixing Robinia pseudoacacia (+230%) exhibited greater mean annual relative growth rates under elevated CO2 than under ambient conditions. The effects of CO2 were small relative to variability within populations; however, some species grew better under low light conditions when exposed to elevated CO2 than they did under ambient conditions. These species include shade-intolerant Liriodendron tulipifera and Liquidambar styraciflua, intermediate-tolerant Quercus velutina, and shade-tolerant Acer barbatum, A. rubrum, Prunus serotina, Ulmus alata, and Cercis canadensis. Contrary to our expectation, shade-intolerant trees did not survive better with CO2 enrichment, and population-scale responses to CO2 were influenced by survival probabilities in low light. CO2 enrichment did not increase rates of sample biomass accumulation for most species, but it did stimulate biomass growth of shade-tolerant taxa, particularly Acer barbatum and Ulmus alata. Our data suggest a small CO2 fertilization effect on tree productivity, and the possibility of reduced carbon accumulation rates relative to today's forests due to changes in species composition.     

Development and characterization of an anaerobic microcosm for reductive dechlorination of PCBs

The toxic and recalcitrant polychlorinated biphenyls (PCBs) adversely affect human and biota by bioaccumulation and biomagnification through food chain. In this study, an anaerobic microcosm was developed to extensively dechlorinate hexa- and hepta-CBs in Aroclor 1260. After 4 months of incubation in defined mineral salts medium amended PCBs (70 mmol·L^–1) and lactate (10 mmol·L^–1), the culture dechlorinated hexa-CBs from 40.2% to 8.7% and hepta-CBs 33.6% to 11.6%, with dechlorination efficiencies of 78.3% and 65.5%, respectively (all in moL ratio). This dechlorination process led to tetra-CBs (46.4%) as the predominant dechlorination products, followed by penta-(22.1%) and tri-CBs (5.4%). The number of meta chlorines per biphenyl decreased from 2.50 to 1.41. Results of quantitative real-time PCR show that Dehalococcoides cells increased from 2.39 ×10⁵±0.5 × 10⁵ to 4.99 × 10⁷±0.32 × 10⁷ copies mL^–1 after 120 days of incubation, suggesting that Dehalococcoides play a major role in reductive dechlorination of PCBs. This study could prove the feasibility of anaerobic reductive culture enrichment for the dehalogenation of highly chlorinated PCBs, which is prior to be applied for in situ bioremediation of notorious halogenated compounds.

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大气CO2与植物氮素营养的关系

大气CO2浓度升高对植物吸收氮素,以及对植物和土壤中的氮浓度、C/N比和氮循环都存在着影响。大气CO2浓度与植物氮素营养之间存在着交互作用。大气CO2浓度升高对植物氮素营养影响的结果与氮浓度、氮形态等因素有关。     

Co-pyrolysis of sewage sludge and biomass for stabilizing heavy metals and reducing biochar toxicity: A review

The huge amounts of sewage sludge produced by municipal wastewater treatment plants induce major environmental and economical issues, calling for advanced disposal methods. Traditional methods for sewage sludge disposal increase greenhouse gas emissions and pollution. Moreover, biochar created from sewage sludge often cannot be used directly in soil applications due to elevated levels of heavy metals and other toxic compounds, which alter soil biota and earthworms. This has limited the application of sewage sludge-derived biochar as a fertilizer. Here, we review biomass and sewage sludge co-pyrolysis with a focus on the stabilization of heavy metals and toxicity reduction of the sludge-derived biochar. We observed that co-pyrolyzing sewage sludge with biomass materials reduced heavy metal concentrations and decreased the environmental risk of sludge-derived biochar by up to 93%. Biochar produced from sewage sludge and biomass co-pyrolysis could enhance the reproduction stimulation of soil biota by 20‒98%. Heavy metals immobilization and transformation are controlled by the co-feed material mixing ratio, pyrolysis temperature, and pyrolysis atmosphere.

     

CO2-enrichment and nutrient availability alter ectomycorrhizal fungal communities

Ectomycorrhizal fungi (EMF), a phylogenetically and physiologically diverse guild, form symbiotic associations with many trees and greatly enhance their uptake of nutrients and water. Elevated CO2, which increases plant carbon supply and demand for mineral nutrients, may change the composition of the EMF community, possibly altering nutrient uptake and ultimately forest productivity. To assess CO2 effects on EMF communities, we sampled mycorrhizae from the FACTS-I (Forest-Atmosphere Carbon Transfer and Storage) research site in Duke Forest, Orange County, North Carolina, USA, where Pinus taeda forest plots are maintained at either ambient or elevated CO2 (200 ppm above ambient) concentrations. Mycorrhizae were identified by DNA sequence similarity of the internal transcribed spacer ribosomal RNA gene region. EMF richness was very high; 72 distinct phylotypes were detected from 411 mycorrhizal samples. Overall EMF richness and diversity were not affected by elevated CO2, but increased CO2 concentrations altered the relative abundances of particular EMF taxa colonizing fine roots, increased prevalence of unique EMF species, and led to greater EMF community dissimilarity among individual study plots. Natural variation among plots in mean potential net nitrogen (N) mineralization rates was a key determinant of EMF community structure; increasing net N mineralization rate was negatively correlated with EMF richness and had differential effects on the abundance of particular EMF taxa. Our results predict that, at CO2 concentrations comparable to that predicted for the year 2050, EMF community composition and structure will change, but diversity will be maintained. In contrast, high soil N concentrations can negatively affect EMF diversity; this underscores the importance of considering CO2 effects on forest ecosystems in the context of background soil chemical parameters and other environmental perturbations such as acid deposition or fertilizer runoff.