The effect of thermodynamic data on computer model predictions of uranium speciation in natural water systems

Computer models have found widespread application in order to help elucidate and predict changes in environmental systems. One such application is the prediction of trace metal speciation in aqueous systems. This is achieved by solving a set of non-linear equations involving equilibrium constants for all the components in the system, within mass and charge balance constraints. In this study a comparison of the predicted uranium speciation from two computer programs, WHAM and PHREEQCI, is used to illustrate the effect variations in thermodynamic data can have on the models produced. Using the original thermodynamic data provided with the models, WHAM predicted the UO2(2+) ion as the major species (84%) while PHREEQCI predicted UO2(HPO4)2(2-) as the major species (86%). Substituting uranium data from the Nuclear Energy Agency Thermochemical Database project (NEA-TDB) into both programs produced similar results from each program, with UO2F+ predicted to dominate (68%) in a groundwater sample. Natural water samples often contain humic substances. The possible interaction of such substances with uranium was also modelled. The WHAM program includes a discreet site electrostatic humic substance model, however in order to use the PHREEQCI program to model humic substance interactions, a 'model fulvic acid' dataset was added to the program. These models predicted 85 to 98% uranium-humic substance species at neutral pH. This indicates that humic substances do need to be taken into account when modelling uranium speciation in natural water samples.     

Uranium speciation in moorland river water samples: a comparison of experimental results and computer model predictions

An on-line method has been developed for separating inorganic and organic bound uranium species present in river water samples. The method utilised a small chelating resin (Hyphan) column incorporated into the sample introduction manifold of an ICP-MS instrument. The method was evaluated for samples from rivers on Dartmoor (Devon, UK), an area of granite overlain with peat bogs. The results indicate that organic-uranium species form a major proportion (80%) of the total dissolved uranium present. Further work with synthetic water samples indicated that the level of dissolved organic carbon played a greater role in determining the level of organic-uranium species than did sample pH. Computer models for the water samples were constructed using the WHAM program (incorporating uranium data from the Nuclear Energy Agency Thermochemical Database project) in order to predict the levels of organic-uranium species that would form. By varying the proportion of humic and fulvic acids used in the humic component, predictions within 10% of the experimental results were obtained. The program did exhibit a low bias at higher pH values (7.5) and low organic carbon concentrations (0.5 microg ml(-1)), but under the natural conditions prevalent in the Dartmoor water samples, the model predictions were successful.     

The US freshwater supply shortage: Experiences with desalination as part of the solution

Parts of the USA are facing impending shortages of freshwater. One proposed solution is the construction of desalination plants to turn seawater into freshwater. Although seawater desalination plants are widely used in the Middle East, especially Saudi Arabia, there are few desalination plants in the USA. In 2003, Tampa Bay Water built the largest desalination plant in North America. Persistent operating problems and escalating costs have caused the utility to re-evaluate its reliance on the seawater desalination plant as part of a long-term regional water supply strategy. In addition, environmental effects of the plant are uncertain. Advances in reverse osmosis technology have significantly reduced desalination costs. However, desalination of seawater is still more expensive than other freshwater supply sources and demand management measures. With time and research, seawater desalination may prove to be a sustainable, cost-effective source of new freshwater supplies, especially if plants are coupled with renewable energy sources. Until then, the development of small-scale groundwater desalination plants, the re-use of water, water conservation, and a more efficient allocation of water through higher prices and rising block rates will be important strategies in meeting growing water demand. Moreover, it is important to improve the coordination between water supply planning and land use planning as populations continue to increase.     

Using expert elicitation to define successful adaptation to climate change

This paper develops definitions of adaptation and successful adaptation to climate change, with a view to evaluating adaptations. There is little consensus on the definition of adapting to climate change in existing debates or on the criteria by which adaptation actions can be deemed successful or sustainable. In this paper, a variant of the Delphi technique is used to elicit expert opinion on a definition of successful adaptation to climate change. Through an iterative process, expert respondents coalesced around a definition based on risk and vulnerability and agreed that a transparent and acceptable definition should reflect impacts on sustainability. According to the final definition, agreed by the Delphi panel, successful adaptation is any adjustment that reduces the risks associated with climate change, or vulnerability to climate change impacts, to a predetermined level, without compromising economic, social, and environmental sustainability.     

Plant species differ in their ability to reduce allocation to non-beneficial arbuscular mycorrhizal fungi

Theory suggests that cheaters threaten the persistence of mutualisms, but that sanctions to prevent cheating can stabilize mutualisms. In the arbuscular mycorrhizal symbiosis, reports of parasitism suggest that reductions in plant carbon allocation are not universally effective. I asked whether plant species differences in mycorrhizal responsiveness would affect both their susceptibility to parasitism and their reduction in allocation to non-beneficial arbuscular mycorrhizal fungi (AMF) in high-phosphorus soils. In a greenhouse experiment, I found that two C3 grasses, Bromus inermis and Elymus repens, effectively suppressed root colonization and AMF hyphal abundance. Increases in soil phosphorus did not reduce the degree to which AMF increased plant biomass. In contrast, two C4 grasses, Andropogon gerardii and Schizachyrium scoparium, more weakly reduced root colonization and failed to suppress AMF hyphal abundance. Consequently, they experienced strong declines in their response to AMF, and one species suffered parasitism. Thus, species differ in susceptibility to parasitism and their reduction in allocation to non-beneficial AMF. These differences may affect the distribution and abundance of plants and AMF, as well as the stability of the mutualism.     

An opinion on the distribution and behavior of chemicals in response to climate change,with particular reference to the Asia-Pacific region

There is a general lack of knowledge as regards the effects of climate change on pollutant behavior. This is particularly true of the Asia-Pacific Region (APR). This region has major significance in terms of global pollutant emission and also displays a wide variety of environments. This review presents the authors’ opinions on possible implications of climate change for pollutant behavior in the APR. Although differing responses can be expected across the region, there are clear implications as regards the short- and long-term behavior of pollutants. Effects can be predicted through modeling, but further data are required for model calibration. Nevertheless, it can be predicted that climate change will affect processes including global distillation of persistent organic pollutants, airborne transport of heavy metals, half-life of readily degradable pollutants, and eutrophication in water bodies. Particulates are expected to play a central role in mediating the effects of climate change, and successful predictive models will need to be based on particulate-mediated transport and behavior. Climate change also has the potential to cause an increase in the intensity and frequency of harmful algal blooms in aquatic environments throughout the region, with significant implications for supply of both food and drinking water.     

水环境中的微塑料：环境危害的本证和反证及主要研究空白

科学界与公众对微塑料(microplastics, MPs)的污染越来越重视。我们对文献进行了系统综述,以评价MPs对环境危害的证据权重。我们发现MPs在地表水和沉积物中均有存在。主要以珠状组成为主的碎片和纤维只是检测到的MP形态中的一小部分。检测出的MPs环境浓度很低,与能够影响生物分子水平上的毒性终点、以及摄食、繁殖、生长、组织炎症和死亡率的浓度有数量级的差别。MPs作为疏水性有机化合物的携带者使其在生物体中富集的作用很弱。现有数据表明MPs对环境造成的危害并不明显。实验室毒性实验中使用的MPs与环境中检测到的MPs在颗粒形态、尺寸范围和浓度等方面都有差距。研究中环境介质的选择少受关注。我们亟需开展更高质量的整体监测和更多实际环境效应的研究。只有这样,我们才能够全面表征MPs的环境风险,以便制定实施真正改善环境质量的管控措施。 精选自Emily E. Burns, Alistair B.A. Boxall. Microplastics in the aquatic environment: Evidence for or against adverse impacts and major knowledge gaps. Environmental Toxicology and Chemistry,2018,37:2776–2796.
详情请见 https://doi.org/10.1002/etc.4268
     

Observations of urban airborne particle number concentrations during rush-hour conditions: analysis of the number based size distributions and modal parameters

A summertime study of the number concentration and the size distribution of combustion derived nanometre sized particles (termed nanoparticles) from diesel and spark-ignition (SI) engine emissions were made under rush-hour and free-flow traffic conditions at an urban roadside location in Leeds, UK in July 2003. The measured total particle number concentrations (N(TOTAL)) were of the order 1.8 x 10(4) to 3.4 x 10(4) cm(-3), and tended to follow the diurnal traffic flow patterns. The N(TOTAL) was dominated by particles < or =100 nm in diameter which accounted for between 89-93% of the measured particle number. By use of a log-normal fitting procedure, the modal parameters of the number based particle size distribution of urban airborne particulates were derived from the roadside measurements. Four component modes were identified. Two nucleation modes were found, with a smaller, more minor, mode composed principally of sub-11 nm particles, believed to be derived from particles formed from the nucleation of gaseous species in the atmosphere. A second mode, much larger in terms of number, was composed of particles within the size range of 10-20 nm. This second mode was believed to be principally derived from the condensation of the unburned fuel and lube oil (the solvent organic fraction or SOF) as it cooled on leaving the engine exhaust. Third and fourth modes were noted within the size ranges of 28-65 nm and 100-160 nm, respectively. The third mode was believed to be representative of internally mixed Aitken mode particles composed of a soot/ash core with an adsorbed layer of readily volatilisable material. The fourth mode was believed to be composed of chemically aged, secondary particles. The larger nucleation and Aitken modes accounted for between 80-90% of the measured N(TOTAL), and the particles in these modes were believed to be derived from SI and diesel engine emissions. The overall size distribution, particularly in modes II-IV, was observed to be strongly related to the number of primary particle emissions, with larger count median diameters observed under conditions where low numbers of primary soot based particles were present.