Just add water and salt: the optimisation of petrogenic hydrocarbon biodegradation in soils from semi-arid Barrow Island, Western Australia

We investigated the potential of soil moisture and nutrient amendments to enhance the biodegradation of oil in the soils from an ecologically unique semi-arid island. This was achieved using a series of controlled laboratory incubations where moisture or nutrient levels were experimentally manipulated. Respired CO2 increased sharply with moisture amendment reflecting the severe moisture limitation of these porous and semi-arid soils. The greatest levels of CO2 respiration were generally obtained with a soil pore water saturation of 50–70%. Biodegradation in these nutrient poor soils was also promoted by the moderate addition of a nitrogen fertiliser. Increased biodegradation was greater at the lowest amendment rate (100 mg N kg−1 soil) than the higher levels (500 or 1,000 mg N kg−1 soil), suggesting the higher application rates may introduce N toxicity. Addition of phosphorous alone had little effect, but a combined 500 mg N and 200 mg P kg−1 soil amendment led to a synergistic increase in CO2 respiration (3.0×), suggesting P can limit the biodegradation of hydrocarbons following exogenous N amendment.

When smoke gets in our eyes: The multiple impacts of atmospheric black carbon on climate, air quality and health

With both climate change and air quality on political and social agendas from local to global scale, the links between these hitherto separate fields are becoming more apparent. Black carbon, largely from combustion processes, scatters and absorbs incoming solar radiation, contributes to poor air quality and induces respiratory and cardiovascular problems. Uncertainties in the amount, location, size and shape of atmospheric black carbon cause large uncertainty in both climate change estimates and toxicology studies alike. Increased research has led to new effects and areas of uncertainty being uncovered. Here we draw together recent results and explore the increasing opportunities for synergistic research that will lead to improved confidence in the impact of black carbon on climate change, air quality and human health. Topics of mutual interest include better information on spatial distribution, size, mixing state and measuring and monitoring. (c) 2006 Elsevier Ltd. All rights reserved.

Direct estimates of emissions from the megacity of Lagos

We report here top-down emissions estimates for an African megacity. A boundary layer circumnavigation of Lagos, Nigeria was completed using the FAAM BAe146 aircraft as part of the AMMA project. These observations together with an inferred boundary layer height allow the flux of pollutants to be calculated. Extrapolation gives annual emissions for CO, NOx, and VOCs of 1.44 Tg yr−1, 0.03 Tg yr−1 and 0.37 Tg yr−1 respectively with uncertainties of +250/−60%. These inferred emissions are consistent with bottom-up estimates for other developing megacities and are attributed to the evaporation of fuels, mobile combustion and natural gas emissions.

Direct estimates of emissions from the megacity of Lagos

We report here top-down emissions estimates for an African megacity. A boundary layer circumnavigation of Lagos, Nigeria was completed using the FAAM BAe146 aircraft as part of the AMMA project. These observations together with an inferred boundary layer height allow the flux of pollutants to be calculated. Extrapolation gives annual emissions for CO, NOx, and VOCs of 1.44 Tg yr(-1), 0.03 Tg yr(-1) and 0.37 Tg yr(-1) respectively with uncertainties of (+250)/(-60%). These inferred emissions are consistent with bottom-up estimates for other developing megacities and are attributed to the evaporation of fuels, mobile combustion and natural gas emissions.

Aerogel-coated metal nanoparticle colloids as novel entities for the synthesis of defined supported metal catalysts

Nanometer metal particles of tailored size (3-5 nm) and composition prepared via inverse microemulsion were encapsulated by ultrathin coatings (<2.5 nm) of inorganic porous aerogels covered with surface -OH groups. These composite materials formed metastable colloids in solvent(s), and the organic surfactant molecules were subsequently removed without leading to aggregation (the ethanolic colloid solution was shown to be stable against flocculation for at least weeks). We demonstrate that the totally inorganic-based composite colloids, after the removal of surfactant, can be anchored to conventional solid supports (gamma-alumina, carbons) upon mixing. Application of a high temperature resulted in the formation of strong covalent linkages between the colloids and the support because of the condensation of surface groups at the interface. Detailed characterizations (X-ray diffraction (XRD), pore analysis, transmission electron microscopy (TEM), CO chemisorption) and catalytic testing (butane combustion) showed that there was no significant metal aggregation from the fine metal particles individually coated with porous aerogel oxide. Most of these metal sites on the coated nanoparticles with and without support are fully accessible by small molecules hence giving extremely active metal catalysts. Thus, the product and technology described may be suitable to synthesize these precursor entities of defined metal sizes (as inks) for wash coat/impregnation applications in catalysis. The advantages of developing inorganic nanocomposite chemical precursors are also discussed.

Life cycle analysis of UK coal fired power plants

This paper examines the life cycle GHG emissions from existing UK pulverized coal power plants. The life cycle of the electricity Generation plant includes construction, operation and decommissioning. The operation phase is extended to upstream and downstream processes. Upstream processes include the mining and transport of coal including methane leakage and the production and transport of limestone and ammonia, which are necessary for flue gas clean up. Downstream processes, on the other hand, include waste disposal and the recovery of land used for surface mining. The methodology used is material based process analysis that allows calculation of the total emissions for each process involved. A simple model for predicting the energy and material requirements of the power plant is developed. Preliminary calculations reveal that for a typical UK coal fired plant, the life cycle emissions amount to 990 g CO2-e/kWh of electricity generated, which compares well with previous UK studies. The majority of these emissions result from direct fuel combustion (882 g/kWh 89%) with methane leakage from mining operations accounting for 60% of indirect emissions. In total, mining operations (including methane leakage) account for 67.4% of indirect emissions, while limestone and other material production and transport account for 31.5%. The methodology developed is also applied to a typical IGCC power plant. It is found that IGCC life cycle emissions are 15% less than those from PC power plants. Furthermore, upon investigating the influence of power plant parameters on life cycle emissions, it is determined that, while the effect of changing the load factor is negligible, increasing efficiency from 35% to 38% can reduce emissions by 7.6%. The current study is funded by the UK National Environment Research Council (NERC) and is undertaken as part of the UK Carbon Capture and Storage Consortium (UKCCSC). Future work will investigate the life cycle emissions from other power generation technologies with and without carbon capture and storage. The current paper reveals that it might be possible that, when CCS is employed. the emissions during generation decrease to a level where the emissions from upstream processes (i.e. coal production and transport) become dominant, and so, the life cycle efficiency of the CCS system can be significantly reduced. The location of coal, coal composition and mining method are important in determining the overall impacts. In addition to studying the net emissions from CCS systems, future work will also investigate the feasibility and technoeconomics of these systems as a means of carbon abatement.

Controls of carbon dioxide concentrations and fluxes above central London

Eddy-covariance measurements of carbon dioxide fluxes were taken semi-continuously between October 2006 and May 2008 at 190 m height in central London (UK) to quantify emissions and study their controls. Inner London, with a population of 8.2 million (~5000 inhabitants per km2) is heavily built up with 8% vegetation cover within the central boroughs. CO2 emissions were found to be mainly controlled by fossil fuel combustion (e.g. traffic, commercial and domestic heating). The measurement period allowed investigation of both diurnal patterns and seasonal trends. Diurnal averages of CO2 fluxes were found to be highly correlated to traffic. However changes in heating-related natural gas consumption and, to a lesser extent, photosynthetic activity that controlled the seasonal variability. Despite measurements being taken at ca. 22 times the mean building height, coupling with street level was adequate, especially during daytime. Night-time saw a higher occurrence of stable or neutral stratification, especially in autumn and winter, which resulted in data loss in post-processing. No significant difference was found between the annual estimate of net exchange of CO2 for the expected measurement footprint and the values derived from the National Atmospheric Emissions Inventory (NAEI), with daytime fluxes differing by only 3%. This agreement with NAEI data also supported the use of the simple flux footprint model which was applied to the London site; this also suggests that individual roughness elements did not significantly affect the measurements due to the large ratio of measurement height to mean building height.

Radicals from the atmospheric pressure pyrolysis and oxidative pyrolysis of hydroquinone, catechol, and phenol

The burning of tobacco creates various types of free radicals that have been reported to be biologically active. Some radicals are transient but can initiate catalytic cycles that generate other free radicals. Other radicals are environmentally persistent and can exist in total particulate matter (TPM) for extended periods. In spite of their importance, little is known concerning the precursors of these radicals or under what pyrolysis/combustion conditions they are formed. We performed studies of the formation of radicals from the gas-phase pyrolysis and oxidative pyrolysis of hydroquinone (HQ) and catechol (CT) between 750 and 1000 °C and phenol from 500 to 1000 °C. The initial electron paramagnetic resonance (EPR) spectra were complex, indicating the presence of multiple radicals. Using matrix annealing and microwave power saturation techniques, phenoxyl, cyclopentadienyl, and peroxyl radicals were identifiable, but only cyclopentadienyl radicals were stable above 750 °C.

Design and development of a low NOx Coanda ejector burner

Small gaseous combustion systems are being targeted by strict pollution legislation which will provide challenges to reduce the NOx being emitted. A novel type of gas burner has been successfully designed and developed which incorporates a Coanda ejector to promote recirculation of flue gas from the burner exit. This provides a combustion system which gives very low emissions of NOx and CO, whilst maintaining a high degree of flame stability over a range of air/fuel ratios and fuel flow rates. Recirculation of flue gas was obtained by manipulating the aerodynamics of the system, without the aid of external duct work or moving parts. The design of the burner allowed very low pollutant emissions near stoichiometric conditions, resulting in high temperatures of the exit gas. Potential applications of this type of burner are in small and intermediate furnaces where low NOx emissions are required. Moreover, very high-temperature applications, such as glass furnaces could benefit in both cost and pollutant emissions from such a burner.

Co-fuelling of peat with meat and bone meal in a pilot scale bubbling bed reactor

Co-combustion performance trials of Meat and Bone Meal (MBM) and peat were conducted using a bubbling fluidized bed (BFB) reactor. In the combustion performance trials the effects of the co-combustion of MBM and peat on flue gas emissions, bed fluidization, ash agglomeration tendency in the bed and the composition and quality of the ash were studied. MBM was mixed with peat at 6 levels between 15% and 100%. Emissions were predominantly below regulatory limits. CO concentrations in the flue gas only exceeded the 100 mg/m3 limit upon combustion of pure MBM. SO2 emissions were found to be over the limit of 50 mg/m3, while in all trials NOx emissions were below the limit of 300 mg/m3. The HCl content of the flue gases was found to vary near the limit of 30 mg/m3. VOCs however were within their limits. The problem of bed agglomeration was avoided when the bed temperature was about 850 °C and only 20% MBM was co-combusted. This study indicates that a pilot scale BFB reactor can, under optimum conditions, be operated within emission limits when MBM is used as a co-fuel with peat. This can provide a basis for further scale-up development work in industrial scale BFB applications

Adjoint methods in data assimilation for estimating model error

Data assimilation aims to incorporate measured observations into a dynamical system model in order to produce accurate estimates of all the current (and future) state variables of the system. The optimal estimates minimize a variational principle and can be found using adjoint methods. The model equations are treated as strong constraints on the problem. In reality, the model does not represent the system behaviour exactly and errors arise due to lack of resolution and inaccuracies in physical parameters, boundary conditions and forcing terms. A technique for estimating systematic and time-correlated errors as part of the variational assimilation procedure is described here. The modified method determines a correction term that compensates for model error and leads to improved predictions of the system states. The technique is illustrated in two test cases. Applications to the 1-D nonlinear shallow water equations demonstrate the effectiveness of the new procedure.

On increasing global temperatures: 75 years after Callendar

In 1938, Guy Stewart Callendar was the first to demonstrate that the Earth’s land surface was warming. Callendar also suggested that the production of carbon dioxide by the combustion of fossil fuels was responsible for much of this modern change in climate. This short note marks the 75th anniversary of Callendar’s landmark study and demonstrates that his global land temperature estimates agree remarkably well with more recent analyses.

Bounding the role of black carbon in the climate system: a scientific assessment

Black carbon aerosol plays a unique and important role in Earth’s climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr�-1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m�-2 with 90% uncertainty bounds of (+0.08, +1.27)Wm�-2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m�-2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m�-2 with 90% uncertainty bounds of +0.17 to +2.1 W m�-2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m�-2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (�-0.50 to +1.08) W m-�2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (�-0.06 W m�-2 with 90% uncertainty bounds of �-1.45 to +1.29 W m�-2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

Yield and nitrogen accumulation and partitioning in winter wheat under elevated CO2: A 3-year free-air CO2 enrichment experiment

Fossil fuel combustion and deforestation have resulted in a rapid increase in atmospheric [CO2] since the 1950’s, and it will reach about 550 μmol mol−1 in 2050. Field experiments were conducted at the Free-air CO2 Enrichment facility in Beijing, China. Winter wheat was grown to maturity under elevated [CO2] (550 ± 17 μmol mol−1) and ambient [CO2] (415 ± 16 μmol mol−1), with high nitrogen (N) supply (HN, 170 kg N ha−1) and low nitrogen supply (LN, 100 kg N ha−1) for three growing seasons from 2007 to 2010. Elevated [CO2] increased wheat grain yield by 11.4% across the three years. [CO2]-induced yield enhancements were 10.8% and 11.9% under low N and high N supply, respectively. Nitrogen accumulation under elevated [CO2] was increased by 12.9% and 9.2% at the half-way anthesis and ripening stage across three years, respectively. Winter wheat had higher nitrogen demand under elevated [CO2] than ambient [CO2], and grain yield had a stronger correlation with plant N uptake after anthesis than before anthesis at high [CO2]. Our results suggest that regulating on the N application rate and time, is likely important for sustainable grain production under future CO2 climate.

The hidden organic carbon in deep mineral soils

Aims Current estimates of soil organic carbon (SOC) are based largely on surficial measurements to depths of 0.3 to 1 m. Many of the world’s soils greatly exceed 1 m depth and there are numerous reports of biological activity to depths of many metres. Although SOC storage to depths of up to 8 m has been previously reported, the extent to which SOC is stored at deeper depths in soil profiles is currently unknown. This paper aims to provide the first detailed analysis of these previously unreported stores of SOC. Methods Soils from five sites in the deeply weathered regolith in the Yilgarn Craton of south-western Australia were sampled and analysed for total organic carbon by combustion chromatography. These soils ranged between 5 and 38 m (mean 21 m) depth to bedrock and had been either recently reforested with Pinus pinaster or were under agriculture. Sites had a mean annual rainfall of between 399 and 583 mm yr−1. Results The mean SOC concentration across all sites was 2.30 ± 0.26 % (s.e.), 0.41 ± 0.05 % and 0.23 ± 0.04 % in the surface 0.1, 0.1–0.5 and 0.5 to 1.0 m increments, respectively. The mean value between 1 and 5 m was 0.12 ± 0.01 %, whereas between 5 and 35 m the values decreased from 0.04 ± 0.002 % to 0.03 ± 0.003 %. Mean SOC mass densities for each of the five locations varied from 21.8–37.5 kg C m−2, and were in toto two to five times greater than would be reported with sampling to a depth of 0.5 m. Conclusions This finding may have major implications for estimates of global carbon storage and modelling of the potential global impacts of climate change and land-use change on carbon cycles. The paper demonstrates the need for a reassessment of the current arbitrary shallow soil sampling depths for assessing carbon stocks, a revision of global SOC estimates and elucidation of the composition and fate of deep carbon in response to land use and climate change