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Fluoride (F) is an emerging pollutant that originates from multiple sources and adversely affects plant growth and nutrient bioavailability in soil. This greenhouse study investigated the effects of soil F (0, 10, 20, 50, 100, 200 mg kg-1) on morpho-physiological growth characteristics of wheat, soil F contents, and bioavailability and uptake of F, phosphorus (P), sulphur (S), potassium (K), calcium (Ca), magnesium (Mg), aluminium (Al), iron (Fe), manganese (Mn), silicon (Si) and zinc (Zn) by wheat. Higher F significantly reduced plant height and number of leaves particularly at early growth stages and increased visible leaf injury index. Powdery mildew infestation coincided with leafy injury and was higher in elevated soil F treatments. Fluoride treatments (>50 mg kg-1) significantly increased water (H2O)- and calcium chloride (CaCl2)-extractable F contents in soil. Water-extractable soil F contents from soil in all concentration were higher than CaCl2-extractable F. This increased F bioavailability resulted in significantly higher F uptake and accumulation in live leaves, dead leaves and grains of wheat which followed order: live leaves > dead leaves > grains. Leaf injury index and number of dead leaves correlated significantly positively with soil H2O- and CaCl2-extractable F contents. Patterns of nutrient (P, K, S) and trace metals (Al, Ca, Mg, Fe, Mn, Si, Zn) varied significantly with F concentrations and between live and dead leaves, and grains except for Zn. Dead leaves generally had higher nutrients and trace metals than live leaves and grains. Fluoride contents in live leaves, dead leaves and grains showed positive correlations with nutrient elements but negative with trace metals. Number of dead leaves correlated negatively with Al, Ca, Fe, Mg, S and Si but positively with P and Zn contents in dead leaves whereas leaf injury index showed positive correlation with Fe, K, P, Si, Zn, S but negative with Al, Ca and Mg contents. These observations provided evidence of higher F uptake and associated impairment in nutrient and trace metal accumulation which caused leaf injury accompanied by powdery mildew infestation in wheat. However, further research in the region is required to confirm the relationship between F pollution, leaf injury and trace metal accumulation in crops under field conditions.

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Atmospheric nitrogen (N) deposition is believed to accelerate dissolved organic carbon (DOC) production and could lead to increased heavy metal mobility into water resources. We sampled intact soil cores from the Isle of Skye with low background N deposition history and having Serpentine rock known for its higher heavy metal concentrations including zinc (Zn), copper (Cu), nickel (Ni) and lead (Pb). The effects of 16 (16kgN) and 32 kg N ha-1 year-1 (32kgN), and liming with 32kgN (32kgN+Lime) on soil solution chemistry and heavy metal mobilization were investigated over the 15-month study. Nitrogen in deposition load was added at five ammonium (NH4+) to nitrate (NO3-) ratios of 9:1, 5:1, 1:1, 1:5 and 1:9 along NO3-dominance. We found significant effects of load on Cu and NH4+/NO3- ratio on pH, DOC and Zn in soil solution. However, under lime and ratio experimental factors, liming significantly influenced pH, DOC, Cu and Pb, and NH4+/NO3- ratio pH, DOC, Ni and Zn whereas interactions between lime and ratio was significant for Ni and Cu. pH and DOC increased with N load, liming and NO3- dominance, and both correlated significantly positively. Liming under NH4+ dominance enhanced DOC production due to supply of base cations in lime. Mobilization of Cu, Ni and Pb was driven by DOC concentrations and, therefore, increased with load, liming and NO3- dominance in deposition. However, in contrast, low pH and high NH4+ dominance was associated with Zn mobilization in soil solution. On the contrary, despite of some patterns, heavy metals in soil HNO3 extracts were devoid of any load, lime and NH4+/NO3- ratio effects. Our study suggests that the effects of N load and forms in deposition on sites with high accumulated loads of metals need to be better quantified through soil solution partitioning models.

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The adverse effects of soil acidification are extensive and may result in hampered ecosystem functioning. Admixture of tree species with nutrient rich litter has been proposed to restore acidified forest soils and improve forest vitality, productivity and resilience. However, it is common belief that litter effects are insufficiently functional for restoration of poorly buffered sandy soils. Therefore we examined the effect of leaf litter on the forest floor, soil chemistry and soil biota in temperate forest stands along a range of sandy soil types in Belgium, the Netherlands and Germany. Specifically, we address: i) Which tree litter properties contribute most to the mitigation of soil acidification effects and ii) Do rich litter species have the potential to improve the belowground nutrient status of poorly buffered, sandy soils? Our analysis using structural equation modelling shows that litter base cation concentration is the decisive trait for the dominating soil buffering mechanism in forests that are heavily influenced by atmospheric nitrogen (N) deposition. This is in contrast with studies in which leaf litter quality is summarized by C/N ratio. We suggest that the concept of rich litter is context dependent and should consider Liebig's law of the most limiting: if N is not limiting in the ecosystem, litter C/N becomes of low importance, while base cations (calcium, magnesium, potassium) become determining. We further find that on poorly buffered soils, tree species with rich litter induce fast nutrient cycling, sustain higher earthworm biomass and keep topsoil base saturation above a threshold of 30%. Hence, rich litter can trigger a regime shift to the exchange buffer domain in sandy soils. This highlights that admixing tree species with litter rich in base cations is a promising measure to remediate soil properties on acidified sandy soils that receive, or have received, high inputs of N via deposition.

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A significant body of knowledge suggests that soil solution pH and dissolved organic carbon (DOC) strongly influence metal concentrations and speciation in porewater, however, these effects vary between different metals. This study investigated the factors influencing soil and soil solution concentrations of copper (Cu), lead (Pb), nickel (Ni) and zinc (Zn) under field conditions in upland soils from UK having a wide range of pH, DOC and organic matter contents. The study primarily focussed on predicting soil and soil solution metal concentrations from the data on total soil metal concentrations (HNO3 extracts) and soil and soil solution properties (pH, DOC and organic matter content). We tested the multiple regression models proposed by Tipping et al. (2003) to predict heavy metal concentrations in soil solutions and the results indicated a better fit (higher R2 values) in both studies for Pb compared to the Zn and Cu concentrations. Both studies observed consistent negative relationships of metals with pH and loss on ignition (LOI) suggesting an increase in soil solution metal concentrations with increasing acidity. The positive relationship between Pb concentrations in porewater and HNO3 extracts was similar for both studies, however, similar relationships were not found for the Zn and Cu concentrations because of the negative coefficients for these metals in our study. The results of this study conclude that the predictive equations of Tipping et al. (2003) may not be applicable to the field sites where the range of DOC and metal concentrations is much lower than their study. Our study also suggests that the extent to which metals are partitioned into soil solution is lower in soils with a higher organic matter contents due to binding of these metals to soil organic matter.

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Pristine bogs, peatlands in which vegetation is exclusively fed by rainwater (ombrotrophic), typically have a low atmospheric deposition of reactive nitrogen (N) (<0.5kgha-1y-1). An important additional N source is N2 fixation by symbiotic microorganisms (diazotrophs) in peat and mosses. Although the effects of increased total airborne N by anthropogenic emissions on bog vegetation are well documented, the important question remains how different N forms (ammonium, NH4+, versus nitrate, NO3-) affect N cycling, as their relative contribution to the total load strongly varies among regions globally. Here, we studied the effects of 11years of experimentally increased deposition (32 versus 8kgNha-1y-1) of either NH4+ or NO3- on N accumulation in three moss and one lichen species (Sphagnum capillifolium, S. papillosum, Pleurozium schreberi and Cladonia portentosa), N2 fixation rates of their symbionts, and potential N losses to peat soil and atmosphere, in a bog in Scotland. Increased input of both N forms led to 15-90% increase in N content for all moss species, without affecting their cover. The keystone species S. capillifolium showed 4 times higher N allocation into free amino acids, indicating N stress, but only in response to increased NH4+. In contrast, NO3- addition resulted in enhanced peat N mineralization linked to microbial NO3- reduction, increasing soil pH, N concentrations and N losses via denitrification. Unexpectedly, increased deposition from 8 to 32kgha-1y-1 in both N forms did not affect N2 fixation rates for any of the moss species and corresponded to an additional input of 5kgNha-1y-1 with a 100% S. capillifolium cover. Since both N forms clearly show differential effects on living Sphagnum and biogeochemical processes in the underlying peat, N form should be included in the assessment of the effects of N pollution on peatlands.

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Nitrogen (N) deposition impacts natural and semi-natural ecosystems globally. The responses of vegetation to N deposition may, however, differ strongly between habitats and may be mediated by the form of N. Although much attention has been focused on the impact of total N deposition, the effects of reduced and oxidised N, independent of the total N deposition, have received less attention. In this paper, we present new analyses of national monitoring data in the UK to provide an extensive evaluation of whether there are differences in the effects of reduced and oxidised N deposition across eight habitat types (acid, calcareous and mesotrophic grasslands, upland and lowland heaths, bogs and mires, base-rich mires, woodlands). We analysed data from 6860 plots in the British Countryside Survey 2007 for effects of total N deposition and N form on species richness, Ellenberg N values and grass:forb ratio. Our results provide clear evidence that N deposition affects species richness in all habitats except base-rich mires, after factoring out correlated explanatory variables (climate and sulphur deposition). In addition, the form of N in deposition appears important for the biodiversity of grasslands and woodlands but not mires and heaths. Ellenberg N increased more in relation to NHx deposition than NOy deposition in all but one habitat type. Relationships between species richness and N form were habitat-specific: acid and mesotrophic grasslands appear more sensitive to NHx deposition while calcareous grasslands and woodlands appeared more responsive to NOy deposition. These relationships are likely driven by the preferences of the component plant species for oxidised or reduced forms of N, rather than by soil acidification.

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Emissions of gaseous and particulate pollutants from burning of wheat straw, rice straw, cotton straw, and bagasse were studied for the two agricultural-activity-dominated provinces of Pakistan: the Punjab and Sindh. Emission estimates, inventory, and allocation maps indicated distinct patterns of pollutant emissions in the two provinces. Comparative pollutant emission analysis revealed that the Punjab province produced higher pollutants from agricultural biomass burning than Sindh province. Total emissions from these two provinces were estimated to be 16,084.04 Gg (16.08 Tg) for the year 2006/2007. Wheat straw was found to be the dominant source of CO, CO2, SO2, NOx, and EC emissions in the both provinces. However, for the emissions of CH4, NH3, EC, and OC, the Punjab and Sindh provinces differed markedly for the crop residue share in these pollutant emissions. Rice straw was found to be the largest contributor of CH4 (51%) and NH3 (65%) in Sindh province. When total emissions from biomass burning were considered at provincial level, wheat straw and bagasse were the major crop residues which accounted for 72 and 14% of pollutant emissions, respectively, in the Punjab province, whereas, in Sindh province, the order of crop residue contribution in total emission was as follows: wheat (59%) > bagasse (19%) > rice (14%) > cotton (7%). Emission inventory data of total pollutants per unit area under cultivation (Mg ha(-1)) revealed that Sindh province produced higher emissions per hectare for wheat straw, rice straw, and bagasse than the Punjab province.

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Peat forming Sphagnum mosses are able to prevent the dominance of vascular plants under ombrotrophic conditions by efficiently scavenging atmospherically deposited nitrogen (N). N-uptake kinetics of these mosses are therefore expected to play a key role in differential N availability, plant competition, and carbon sequestration in Sphagnum peatlands. The interacting effects of rain N concentration and exposure time on moss N-uptake rates are, however, poorly understood. We investigated the effects of N-concentration (1, 5, 10, 50, 100, 500 µM), N-form ((15)N-ammonium or nitrate) and exposure time (0.5, 2, 72 h) on uptake kinetics for Sphagnum magellanicum from a pristine bog in Patagonia (Argentina) and from a Dutch bog exposed to decades of N-pollution. Uptake rates for ammonium were higher than for nitrate, and N-binding at adsorption sites was negligible. During the first 0.5 h, N-uptake followed saturation kinetics revealing a high affinity (Km 3.5-6.5 µM). Ammonium was taken up 8 times faster than nitrate, whereas over 72 hours this was only 2 times. Uptake rates decreased drastically with increasing exposure times, which implies that many short-term N-uptake experiments in literature may well have overestimated long-term uptake rates and ecosystem retention. Sphagnum from the polluted site (i.e. long-term N exposure) showed lower uptake rates than mosses from the pristine site, indicating an adaptive response. Sphagnum therefore appears to be highly efficient in using short N pulses (e.g. rainfall in pristine areas). This strategy has important ecological and evolutionary implications: at high N input rates, the risk of N-toxicity seems to be reduced by lower uptake rates of Sphagnum, at the expense of its long-term filter capacity and related competitive advantage over vascular plants. As shown by our conceptual model, interacting effects of N-deposition and climate change (changes in rainfall) will seriously alter the functioning of Sphagnum peatlands.

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Wet deposition of nitrogen (N) occurs in oxidized (nitrate) and reduced (ammonium) forms. Whether one form drives vegetation change more than the other is widely debated, as field evidence has been lacking. We are manipulating N form in wet deposition to an ombrotrophic bog, Whim (Scottish Borders), and here report nine years of results. Ammonium and nitrate were provided in rainwater spray as NH4 Cl or NaNO3 at 8, 24 or 56 kg N ha(-1)  yr(-1) , plus a rainwater only control, via an automated system coupled to site meteorology. Detrimental N effects were observed in sensitive nonvascular plant species, with higher cumulative N loads leading to more damage at lower annual doses. Cover responses to N addition, both in relation to form and dose, were species specific and mostly dependent on N dose. Some species were generally indifferent to N form and dose, while others were dose sensitive. Calluna vulgaris showed a preference for higher N doses as ammonium N and Hypnum jutlandicum for nitrate N. However, after 9 years, the magnitude of change from wet deposited N on overall species cover is small, indicating only a slow decline in key species. Nitrogen treatment effects on soil N availability were likewise small and rarely correlated with species cover. Ammonium caused most N accumulation and damage to sensitive species at lower N loads, but toxic effects also occurred with nitrate. However, because different species respond differently to N form, setting of ecosystem level critical loads by N form is challenging. We recommend implementing the lowest value of the critical load range where communities include sensitive nonvascular plants and where ammonium dominates wet deposition chemistry. In the context of parallel assessment at the same site, N treatments for wet deposition showed overall much smaller effects than corresponding inputs of dry deposition as ammonia.

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Although ozone is well-documented to reduce crop yields in the densely populated Indo-Gangetic Plain, there is little knowledge of its effects in other parts of south Asia. We surveyed crops close to the city of Peshawar, in north-west Pakistan, for visible injury, linking this to passive measurements of ozone concentrations. Foliar injury was found on potato, onion and cotton when mean monthly ozone concentrations exceeded 45 ppb. The symptoms on onion were reproduced in ozone fumigation experiments, which also showed that daytime ozone concentrations of 60 ppb significantly reduce the growth of a major Pakistani onion variety. Aphid infestation on spinach was also reduced at these elevated ozone concentrations. The ozone concentrations measured in April-May in Peshawar, and used in the fumigation experiment, are comparable to those that have been modelled to occur over many parts of south Asia, where ozone may be a significant threat to sensitive crops.

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Given the lack of studies which measured dissolved organic carbon (DOC) over long periods, especially in non-forest habitat, the aim of this study was to expand the existing datasets with data of mainly non-forest sites that were representative of the major soil and habitat types in the UK. A further aim was to predict DOC concentrations from a number of biotic and abiotic explanatory variables such as rainfall, temperature, vegetation type and soil type in a multivariate way. Pore water was sampled using Rhizon or Prenart samplers at two to three week intervals for 1 year. DOC, pH, organic carbon, carbon/nitrogen (C:N) ratios of soils and slope were measured and data on vegetation, soil type, temperature and precipitation were obtained. The majority of the variation in DOC concentrations between the UK sites could be explained by simple empirical models that included annual precipitation, and soil C:N ratio with precipitation being negatively related to DOC concentrations and C:N ratio being positively related to DOC concentrations. Our study adds significantly to the data reporting DOC concentrations in soils, especially in grasslands, heathlands and moorlands. Broad climatic and site factors have been identified as key factors influencing DOC concentrations.

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The rapid urbanisation of many cities in south and south-east Asia has increased the demand for bricks, which are typically supplied from brick kilns in peri-urban areas. We report visible foliar damage to mango, apricot and plum trees in the vicinity of traditional Bull's Trench brick kilns in Peshawar, Pakistan. Visible injury symptoms, hydrogen fluoride concentrations in air, and foliar fluoride concentrations were all greater in the vicinity of brick kilns than at more distant sites, indicating that fluoride emissions from brick kilns were the main cause of damage. Interviews with local farmers established the significant impact of this damage on their livelihoods. Since poorly regulated brick kilns are often found close to important peri-urban agricultural areas, we suggest that this may be a growing but unrecognised environmental problem in regions of Asia where emission control in brick kilns has not been improved.

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While it is well established that ecosystems display strong responses to elevated nitrogen deposition, the importance of the ratio between the dominant forms of deposited nitrogen (NH(x) and NO(y)) in determining ecosystem response is poorly understood. As large changes in the ratio of oxidised and reduced nitrogen inputs are occurring, this oversight requires attention. One reason for this knowledge gap is that plants experience a different NH(x):NO(y) ratio in soil to that seen in atmospheric deposits because atmospheric inputs are modified by soil transformations, mediated by soil pH. Consequently species of neutral and alkaline habitats are less likely to encounter high NH(4)(+) concentrations than species from acid soils. We suggest that the response of vascular plant species to changing ratios of NH(x):NO(y) deposits will be driven primarily by a combination of soil pH and nitrification rates. Testing this hypothesis requires a combination of experimental and survey work in a range of systems.

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The adaptive responses to atmospheric nitrogen deposition for different European accessions of Arabidopsis lyrata petraea were analysed using populations along a strong atmospheric N-deposition gradient. Plants were exposed to three N-deposition rates, reflecting the rates at the different locations, in a full factorial design. Differences between accessions in the response to N were found for important phenological and physiological response variables. For example, plants from low-deposition areas had higher nitrogen-use efficiencies (NUE) and C : N ratios than plants from areas high in N deposition when grown at low N-deposition rates. The NUE decreased in all accessions at higher experimental deposition rates. However, plants from high-deposition areas showed a limited capacity to increase their NUE at lower experimental deposition rates. Plants from low-deposition areas had faster growth rates, higher leaf turnover rates and shorter times to flowering, and showed a greater increase in growth rate in response to N deposition than those from high-deposition areas. Indications for adaptation to N deposition were found, and results suggest that adaptation of plants from areas high in N deposition to increased N deposition has resulted in the loss of plasticity.

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Mesocosms filled with dune sand were planted with graminoid (Calamagrostis epigejos, Carex arenaria) and herbaceous species (Carlina vulgaris, Galium verum). Strong effects of nitrogen addition on the vegetation were found within two to three years. The above-ground biomass of C. epigejos and C. arenaria increased at deposition rates between 10 and 80 kg N ha(-1) yr(-1). Both grasses were limited by N. In latter stages P limitation was suggested for C. arenaria. At high N-levels, C. epigejos dominated the vegetation within two years. C. vulgaris and G. verum declined drastically as a result of increased competition for light by the highly competitive grass C. epigejos. It is concluded that increased (ambient) N inputs are of major importance for the increased dominance of tall grasses in stable dune grasslands.

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The effects of increasing ammonium concentrations in combination with different pH levels were studied on five heathland plant species to determine whether their occurrence and decline could be attributed to ammonium toxicity and/or pH levels. Plants were grown in growth media amended with four different ammonium concentrations (10, 100, 500 and 1000 micromol l(-1)) and two pH levels resembling acidified (pH 3.5 or 4) and weakly buffered (pH 5 or 5.5) situations. Survival of Antennaria dioica and Succisa pratensis was reduced by low pH in combination with high ammonium concentrations. Biomass decreased with increased ammonium concentrations and decreasing pH levels. Internal pH of the plants decreased with increasing ammonium concentrations. Survival of Calluna vulgaris, Deschampsia flexuosa and Gentiana pneumonanthe was not affected by ammonium. Moreover, biomass increased with increasing ammonium concentrations. Biomass production of G. pneumonanthe reduced at low pH levels. A decline of acid-sensitive species in heathlands was attributed to ammonium toxicity effects in combination with a low pH.

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