Availability of different forms of sulphur fertilisers to wheat and oilseed rape

A pot experiment was conducted to compare the availability and efficiency of three sulphur (S) fertilisers to wheat in the first year and oilseed rape in the second year, using six agricultural soils. Four treatments were applied in the initial year: control (no S), two forms of elemental S (either micronised S° particles or a bentonite + S° mixture) and a sulphate fertiliser (ammonium sulphate). In the first year, the micronised S° was as effective as the sulphate fertiliser, both producing similar increases of wheat grain yield (on average 36%) and S uptake (on average 164%) over the control. In contrast, responses to the bentonite + S° form were minimal, indicating a limited S supply. In the second year the control treatment failed to produce seeds in most soils, whereas the micronised S° and sulphate treatments increased seed yields of oilseed rape to an average of 13.4 and 12.9 g pot^-1, respectively. The performance of the bentonite + S° varied between soils: two soils produced yields similar to those of the other S fertilisers, while the remaining soils had low yields. To test whether the poor performance of the bentonite clay + S° fertiliser was due to the lack of exposure of the prills to physical weathering in the glasshouse, the effect of freeze-thaw action on the fertilisers performance was assessed in a separate pot experiment. The responses in wheat yield and S uptake showed that freeze-thaw did not enhance the physical disruption of the prills or fertiliser effectiveness. These results suggest that the release of available S from the bentonite + S° mixture was too slow to meet the requirement of wheat and oilseed rape. This revised version was published online in June 2006 with corrections to the Cover Date.     

Stable sulphur isotopes in plants: a review

The determination of the natural abundances of stable isotopes has become a useful method by which to study the transformations of elements in biological and ecological studies as well as to investigate the mechanisms of chemical reactions. Unlike carbon and nitrogen isotopes, however, stable sulphur isotopes are used infrequently, and their potential as tracers in biochemical and physiological studies are only beginning to be realized. This review provides an overview of research involving stable sulphur isotopes in studies of plant metabolism and pollution. Topics discussed include the mechanisms and accompanying isotopic fractionations involved during the uptake and assimilation of inorganic sulphur compounds by plants, the utility of plants as bioindicators of environmental sulphur pollution, and the emission of isotopically light H₂S by plants in response to high concentations of sulphur. Future advances in the field are proposed.     

Acidity controls on dissolved organic carbon mobility in organic soils

Dissolved organic carbon (DOC) concentrations in surface waters have increased across much of Europe and North America, with implications for the terrestrial carbon balance, aquatic ecosystem functioning, water treatment costs and human health. Over the past decade, many hypotheses have been put forward to explain this phenomenon, from changing climate and land management to eutrophication and acid deposition. Resolution of this debate has been hindered by a reliance on correlative analyses of time series data, and a lack of robust experimental testing of proposed mechanisms. In a 4 year, four‐site replicated field experiment involving both acidifying and deacidifying treatments, we tested the hypothesis that DOC leaching was previously suppressed by high levels of soil acidity in peat and organo‐mineral soils, and therefore that observed DOC increases a consequence of decreasing soil acidity. We observed a consistent, positive relationship between DOC and acidity change at all sites. Responses were described by similar hyperbolic relationships between standardized changes in DOC and hydrogen ion concentrations at all sites, suggesting potentially general applicability. These relationships explained a substantial proportion of observed changes in peak DOC concentrations in nearby monitoring streams, and application to a UK‐wide upland soil pH dataset suggests that recovery from acidification alone could have led to soil solution DOC increases in the range 46–126% by habitat type since 1978. Our findings raise the possibility that changing soil acidity may have wider impacts on ecosystem carbon balances. Decreasing sulphur deposition may be accelerating terrestrial carbon loss, and returning surface waters to a natural, high‐DOC condition.     

Responses of two wheat varieties to sulphur addition and diagnosis of sulphur deficiency

Sulphur deficiency has become increasingly widespread in wheat in the U.K. Growth, nutrient content and biochemical responses to S and N supply of a breadmaking wheat variety (Hereward) and a non-breadmaking variety (Riband) were investigated in a pot experiment. Shoot dry matter (DM) at stem extension (Zadok's GS 37) and at maturity was increased markedly by S. Grain production of the Riband variety was more susceptible to the imbalance of N to S than the Hereward variety. At GS 37, the concentrations of total S and sulphate-S of shoots, chlorophyll meter readings and the concentrations of glutathione of the uppermost fully expanded leaves were increased significantly by increasing S supply, whereas the concentrations of nitrate and amides were decreased by S. The greatest relative changes in response to S supply were those of the glutathione and asparagine concentrations. Riband also showed greater response to S than Hereward. Critical values of various diagnostic indices at GS 37 were derived from the relationships between DM yield and different indices. The two varieties showed similar diagnostic curves except that for the ratio of total N to total S (N:S) in shoots. Either total S or sulphate-S can be used alone as a good indicator of deficiency, and with values of 1500 and 190 mg kg^-1 DM in shoots for the two indices respectively. There was also a well defined relationship between DM yield and the glutathione concentration, with a critical value of 240 nmol g^-1 FW. There were no advantages of using % of total S as sulphate-S. Shoot N:S ratio was found to be less accurate in predicting S deficiency than total S or sulphate-S. For prognostic purposes, a much higher S status at GS 37 was required to ensure no losses of DM yield due to S deficiency at maturity.     

Differential responses of freshwater wetland soils to sulphate pollution

Sulphate (SO₄ ^2-)reduction rates are generally low in freshwaterwetlands and are regulated by the scarceavailability of the ion. Increasedconcentrations of this electron acceptor due tosulphur (S) pollution of groundwater andsurface water may, however, lead to highSO₄ ^2- reduction rates now regulatedby the availability of appropriate electrondonors. Due to variations in this availability,the response to S pollution (e.g. from surfacewater or groundwater) is expected to differbetween soils. This hypothesis was tested inlaboratory mesocosm experiments by comparingtwo wetland soil types with distinctlydifferent humus profiles: a Hydromoder and aRhizomull type. In the first type, expected tohave a higher availability of degradable soilorganic matter (SOM), SO₄ ^2-availability appeared to be rate limiting forSO₄ ^2- reduction. In the Rhizomullsoils, in contrast, the electron acceptor didnot limit SO₄ ^2- reduction rates athigher concentrations. These differences inresponse could not, however, be attributed todifferences in the various SOM fractions or inSOM densities. Eutrophication and free sulphideaccumulation, two major biogeochemical problemscaused by SO₄ ^2- pollution, occurredin both types. The absolute extent ofphosphorus mobilisation was determined by theconcentration of this element in the soil (C/Pratio), while the level of sulphideaccumulation was governed by the concentrationof dissolved iron in the pore water. It wastherefore concluded that neither the humusprofile nor the concentrations of different SOMfractions in the soils are reliable indicatorsfor the sensitivity of wetland types to Spollution.     

Dissolved organic sulphur in soil water under <Emphasis Type="Italic">Pinus sylvestris</Emphasis> L. and <Emphasis Type="Italic">Fagus sylvatica</Emphasis> L. stands in northeastern Bavaria,Germany variations with seasons and soil depth

Organically bound species have been identified as prominent and mobile forms of nitrogen and phosphorus in soils. Since a large portion of sulphur (S) in soil is bonded to carbon (C) also dissolved organic S likely is a significant constituent in soil water. To investigate the role of dissolved organic forms in leaching and cycling of S in forest soils, we examined concentrations, fluxes, and chemical composition of organic S in forest floor leachates and in soil solutions of Rendzic Leptosols under 90-year-old European beech (Fagus sylvatica L.) and Haplic Arenosols under 160-year-old Scots pine (Pinus sylvestris L.) for 27 months. These soils are low in adsorbed SO₄^2- and receive little atmospheric S depositions at present. The chemical composition of organic S was estimated by fractionation with XAD-8 and wet-chemical characterisation (HI reduction) of binding forms. Although not as prominent as the organic forms of other nutrient elements, organic S proved to be an important contributor to S dissolved in forest floor leachates and in mineral soil solutions. Dissolved organic matter contained on average 29% of total S in forest floor leachates at the pine site and 34% at the beech site. The largest portion of organic S occurred in the subsoil solutions under beech in summer and autumn (up to 53%). Mean concentrations of organic S peaked (up to 1.1 mg l^-1) in summer after rainstorms that followed dry periods. Fluxes with forest floor leachates and at 90 cm soil depth were largest in autumn because of huge amounts of rainfall. Organic S contributed significantly to the fluxes of S in the subsoils under beech comprising on average 39% of total dissolved S at 90 cm depth. Organic S produced in the forest floor layers was mainly in the hydrophilic fraction of dissolved organic matter (62 ± 6% at the pine site, 85 ± 4% at the beech site). The major binding form of organic S in the hydrophobic fraction was C-bonded S while in the hydrophilic fraction ester sulphate S, possibly associated with carbohydrates, was more prominent. Since the hydrophobic fraction increased in summer and autumn, C-bonded S was of greater importance during that time of the year than in winter and spring. With depth, concentrations and composition of organic S (and also of C) hardly changed at the pine site because of little retention of dissolved organic matter, presumably because of the small sorption capability of that soil. At the beech where organic C showed a marked decrease with depth, only a slight decrease in organic S, exclusively from the hydrophobic fraction, was found indicating that organic S was mobile compared with organic C. This was probably due to the concentration of S in the hydrophilic fraction of dissolved organic matter. Because of being concentrated in the mobile hydrophilic fraction, ester sulphate S was more mobile in the soil under beech than C-bonded S.     

The sulphate-S/total S ratio in plants as an index of their sulphur status

Summary Several authors are advocating the use of the SO₄–S/total S ratio in the plant as the best index of S status. We have traced the arguments put forward in support of this index, and we show that they are based either on unfair comparisons with other indices, such as SO₄–S or total S alone, or inappropriate statistical treatment.The SO₄–S/total S index has two fundamental disadvantages compared with SO₄–S or total S alone: (1) the numerator (SO₄–S) is the major variable in the denominator, so the ratio is likely to be less sensitive than either of the measurements alone; (2) its determination involves twice as much analytical work as either measurement alone.Examination of some of the source references indicates that SO₄–S by itself is the most satisfactory S index. Whenever whole plants are analysed, any index which includes organic S is subject to variation due to tissue age.     

Sulphur fractionation in calcareous soils and bioavailability to plants

Sulphur fractionation and availability to plants are poorly understood in calcareous soils. Sixty-four calcareous soils containing varying amounts of CaCO₃ were collected from ten provinces in China and their S fractions determined. Organic S was the predominant fraction of S, accounting for on average 77% of the soil total S. The amounts of adsorbed sulphate were found to be negligible. 1 M HCl extracted substantially more sulphate than either 0.01 M CaCl₂ or 0.016 M KH₂PO₄, indicating the existence of water-insoluble but acid-soluble sulphate, probably in the form of sulphate co-precipitated with CaCO₃. The concentrations of water-insoluble sulphate correlated positively with the contents of CaCO₃ and accounted for 0.03–40.3% (mean 11.7%) of soil total S. To test the bioavailability of water-insoluble sulphate, a sulphate-CaCO₃ co-precipitate labelled with ³⁵S was prepared and added to a calcareous soil in a pot experiment with either NH₄⁺ or NO₃^– as the N source. In 29 days, wheat plants took up 10.6% and 3.0% of the ³⁵S added to the soil in the NH₄⁺ and NO₃^– treatments, respectively. At the end of the pot experiment, the decrease of water-insoluble, acid-soluble, sulphate was more apparent in the NH₄⁺ than in the NO₃^– treatment. The results indicate that sulphate co-precipitated with CaCO₃ in calcareous soils may become partly available for plant uptake, depending on rhizosphere pH, if the field precipitate is similar to the laboratory prepared sample studied.     

Turnover of organic nitrogen in soils and its availability to crops

The root development of barley seedlings grown for one week in an aerated nutrient solution was studied in the presence of dissolved organic matter from an aqueous chestnut leaf litter extract. In particular, the different effects of low and high molecular weight fractions (small molecules: molecular weight <1000; large molecules: >10,000) of the leaf litter extract were examined. In the presence of large molecules root growth was inhibited, an irregular root tip morphology was observed, and Ca and Mg concentrations in the shoots were lower than in control plants. These phytotoxic effects were not caused by the formation of an impermeable layer of large molecules on the root surfaces that lower accessibility for nutrient cations as inferred from voltammetric experiments. A germination assay using spruce seeds, however, indicated allelochemical effects of large molecules, which exhibit a higher aromaticity than the small molecules as indicated by spectroscopic characterisation. In the growth experiments with small molecules, no influence on the root development of barley was evident, but an increase of Ca and Mg in the shoots was detected. During these growth experiments, a large amount of the small molecules, mainly simple phenols and amino acids, disappeared from the nutrient solution. The loss of small molecules was most likely the effect of mineralisation.Abbreviations DOC dissolved organic carbon - DOM dissolved organic matter - LLE leaf litter extract - MW molecular weight - HMDE hanging mercury drop electrode     

Low-molecular-weight organic acids in rhizosphere soils of durum wheat and their effect on cadmium bioaccumulation

Cadmium (Cd) accumulation has been found to vary between cultivars of durum wheat (Triticum turgidum var. durum), and it is hypothesized that low-molecular-weight organic acids (LMWOAs) produced at the soil-root interface (rhizosphere) may play an important role in the availability and uptake of Cd by these plants. The objective of this study, therefore, was to (1) investigate the nature and quantity of LMWOAs present in the rhizosphere of durum wheat cultivars Arcola (low Cd accumulator) and Kyle (high Cd accumulator) grown in three different soils: Yorkton, Sutherland and Waitville, and (2) determine the relationship between Cd accumulation in these plants and LMWOAs present in the rhizosphere. Plants were grown for two weeks in pot-cultures under growth chamber conditions. Oxalic, fumaric, succinic, L-malic, tartaric, citric, acetic, propionic and butyric acids were found and quantified in the water extracts of rhizosphere soil, with acetic and succinic acids being predominant. No water extractable LMWOAs were identified in the bulk soil. Total amount of LMWOAs in the rhizosphere soil of the high Cd accumulator (Kyle) was significantly higher than that for the low Cd accumulator (Arcola) in all three soils. Furthermore, large differences in amounts of LMWOAs were found in the rhizosphere soil for the same cultivars grown in different soils and followed the pattern: Sutherland > Waitville > Yorkton. Extractable soil Cd (M NH4Cl) and Cd accumulation in the plants also followed the same soil sequence as LMWOA production. Cadmium accumulation by the high and low Cd accumulating cultivars was proportional to the levels of LMWOAs found in the rhizosphere soil of each cultivar. These results suggest that the differing levels of LMWOAs present in the rhizosphere soil played an important role in the solubilization of particulate-bound Cd into soil solution and its subsequent phytoaccumulation by the high and low Cd accumulating cultivars.     

A sulphur deficiency-induced gene, sdi1, involved in the utilization of stored sulphate pools under sulphur-limiting conditions has potential as a diagnostic indicator of sulphur nutritional status

A sulphate deficiency-induced gene, sdi1 , has been identified by cDNA-amplified fragment length polymorphism (AFLP) analysis utilizing field-grown, nutrient-deficient wheat ( Triticum aestivum var. Hereward). The expression of sdi1 was specifically induced in leaf and root tissues in response to sulphate deficiency, but was not induced by nitrogen, phosphorus, potassium or magnesium deficiency. Expression was also shown to increase in plant tissues as the external sulphate concentration in hydroponically grown plants was reduced from 1.0 to 0.0 m m . On this basis, sdi1 gene expression has potential as a sensitive indicator of sulphur nutritional status in wheat. Genome-walking techniques were used to clone the 2.7-kb region upstream of sdi1 from genomic DNA, revealing several cis -element motifs previously identified as being associated with sulphur responses in plants. The Arabidopsis thaliana gene most highly homologous to sdi1 is At5g48850, which was also demonstrated to be induced by sulphur deficiency, an observation confirmed by the analysis of microarray data available in the public domain. The expression of Atsdi1 was induced more rapidly than previously characterized sulphur-responsive genes in the period immediately following the transfer of plants to sulphur-deficient medium. Atsdi1 T-DNA 'knockout' mutants were shown to maintain higher tissue sulphate concentrations than wild-type plants under sulphur-limiting conditions, indicating a role in the utilization of stored sulphate under sulphur-deficient conditions. The structural features of the sdi1 gene and its application in the genetic determination of the sulphur nutritional status of wheat crops are discussed.     

土壤中铁锰的形态分布及其有效性研究

以乌鲁木齐雅马里克山的土壤为研究对象,采用Tessier连续提取法对土壤铁、锰各种化学形态进行浸提.研究了土壤中有效铁、锰和土壤的理化性质与土壤铁、锰形态之间的关系,及对铁、锰在土壤中存在形态的影响;并通过盆栽试验对铁、锰的植物有效性进行了分析.结果表明,土壤铁主要以残渣态为主,占全铁的92.3%,其它形态含量均小于全量的8%.土壤锰主要是以铁锰氧化态和残渣态为主,分别占全锰的49%和41.6%,其它形态含量均小于全量的10%.用二级出水灌溉处理可增加铁、锰的有效性,原污水灌溉不利于铁、锰的供应,土壤缺铁、锰的现象可通过施加一定量的铁盐和锰盐而得以改善.相关分析还表明,土壤的理化性质与铁锰形态之间有一定的相关性.供试土壤的pH值、CaCO3含量、有机质及阳离子交换态等对土壤铁、锰的有效性影响较大.逐步回归分析表明,铁的氧化物结合态对植物最为有效,锰的有机结合态对植物有效性贡献最大.     

Transformation of urea and ammonium sulphate in different soils

Summary The transformation of urea and ammonium sulphate in Ladwa sandy loam and Balsamand sand was studied in laboratory. Urea took at least one week in sandy loam and 2 weeks in sandy soils to hydrolyse completely. The process of hydrolysis was faster in finer soil with high organic matter than in coarse soil having low organic matter. There was no nitrification upto 3 days in sandy loam and upto 7 days in sandy soils, respectively, but there was immobilization of NO₃-N during these initial periods. The NO₃-N content at the end of incubation period (35 days) was more in case of urea than in case of ammonium sulphate treated samples in sandy loam soil and reverse was true in sandy soil. The hydrolysis of urea did not follow zero or first order kinetics as proposed in previous studies.     

The roles of three functional sulphate transporters involved in uptake and translocation of sulphate in Arabidopsis thaliana

To investigate the uptake and long-distance translocation of sulphate in plants, we have characterized three cell-type-specific sulphate transporters, Sultr1;1, Sultr2;1 and Sultr2;2 in Arabidopsis thaliana. Heterologous expression in the yeast sulphate transporter mutant indicated that Sultr1;1 encodes a high-affinity sulphate transporter (Km for sulphate 3.6 +/- 0.6 microM), whereas Sultr2;1 and Sultr2;2 encode low-affinity sulphate transporters (Km for sulphate 0.41 +/- 0.07 mM and >/= 1.2 mM, respectively). In Arabidopsis plants expressing the fusion gene construct of the Sultr1;1 promoter and green fluorescent protein (GFP), GFP was localized in the lateral root cap, root hairs, epidermis and cortex of roots. beta-glucuronidase (GUS) expressed with the Sultr2;1 promoter was specifically accumulated in the xylem parenchyma cells of roots and leaves, and in the root pericycles and leaf phloem. Expression of the Sultr2;2 promoter-GFP fusion gene showed specific localization of GFP in the root phloem and leaf vascular bundle sheath cells. Plants continuously grown with low sulphate concentrations accumulated high levels of Sultr1;1 and Sultr2;1 mRNA in roots and Sultr2;2 mRNA in leaves. The abundance of Sultr1;1 and Sultr2;1 mRNA was increased remarkably in roots by short-term stress caused by withdrawal of sulphate. Addition of selenate in the sulphate-sufficient medium increased the sulphate uptake capacity, tissue sulphate content and the abundance of Sultr1;1 and Sultr2;1 mRNA in roots. Concomitant decrease of the tissue thiol content after selenate treatment was consistent with the suggested role of glutathione (GSH) as a repressive effector for the expression of sulphate transporter genes.     

The capacity of soils to preserve organic C and N by their association with clay and silt particles

Although it has been recognized that the adsorption of organics to clay and silt particles is an important determinant of the stability of organic matter in soils, no attempts have been made to quantify the amounts of C and N that can be preserved in this way in different soils. Our hypothesis is that the amounts of C and N that can be associated with clay and silt particles is limited. This study quantifies the relationships between soil texture and the maximum amounts of C and N that can be preserved in the soil by their association with clay and silt particles. To estimate the maximum amounts of C and N that can be associated with clay and silt particles we compared the amounts of clay- and silt-associated C and N in Dutch grassland soils with corresponding Dutch arable soils. Secondly, we compared the amounts of clay- and silt-associated C and N in the Dutch soils with clay and silt-associated C and N in uncultivated soils of temperate and tropical regions.We observed that although the Dutch arable soils contained less C and N than the corresponding grassland soils, the amounts of C and N associated with clay and silt particles was the same indicating that the amounts of C and N that can become associated with this fraction had reached a maximum. We also observed close positive relationships between the proportion of primary particles < 20 m in a soil and the amounts of C and N that were associated with this fraction in the top 10 cm of soils from both temperate and tropical regions. The observed relationships were assumed to estimate the capacity of a soil to preserve C and N by their association with clay and silt particles. The observed relationships did not seem to be affected by the dominant type of clay mineral. The only exception were Australian soils, which had on average more than two times lower amounts of C and N associated with clay and silt particles than other soils. This was probably due to the combination of low precipitation and high temperature leading to low inputs of organic C and N.The amount of C and N in the fraction > 20 m was not correlated with soil texture. Cultivation decreased the amount of C and N in the fraction > 20 m to a greater extent than in the fraction < 20 m, indicating that C and N associated with the fraction < 20 m is better protected against decomposition.The finding of a given soil having a maximum capacity to preserve organic C and N will improve our estimations of the amounts of C and N that can become stabilized in soils. It has important consequences for the contribution of different soils to serve as a sink or source for C and N in the long term.     

Sulphate reduction and sulphur cycling in lake sediments: a review

1. The concentration of sulphate is low in lakes and sulphur cycling has often been neglected in studies of organic matter diagenesis in lake sediments. The cycling of sulphur is, however, both spatially and temporally dynamic and strongly influences many biogeochemical reactions in sediments, such as the binding of phosphorus. This review examines the control of sulphate reduction and sulphur cycling in sediments of lakes with different trophic status. 2. The factors that control the rate of sulphate reduction have not been identified with certainty in the various environments because many factors are involved, e.g. oxygen and sulphate concentrations, temperature and organic matter availability. 3. Sulphate reduction is less significant under oligotrophic conditions, where mineralization is dominated by oxic decomposition. The supply of organic matter may not be sufficient to support sulphate reduction in the anoxic parts of sediments and, also, sulphate availability may control the rate as the concentration is generally low in oligotrophic lakes. 4. There is a potential for significant sulphate reduction in eutrophic lakes, as both the availability of organic matter and sulphate concentration are often higher than in oligotrophic lakes. Sulphate is rapidly depleted with sediment depth, however, and methanogenesis is generally the most important process in overall carbon mineralization. Sulphate reduction is generally low in acidic lakes because of low sulphate availability and reduced microbial activity. 5. It is still unclear which of the forms of sulphur deposits are the most important and under which conditions burial occurs. Sulphur deposition is controlled by the rate of sulphate reduction and reoxidation. Reoxidation of sulphides occurs rapidly through several pathways, both under oxic and anoxic conditions. Only a few studies have been able to examine the importance of reoxidation, but it is hypothesized that most of the reoxidation takes place under anoxic conditions and that disproportionation is often involved. The presence of sulphide oxidizing bacteria, benthic fauna and rooted macrophytes may substantially enhance oxic reoxidation. Deposition of sulphur is generally higher in eutrophic than in oligotrophic lakes because of a number of factors: a higher rate of sulphate reduction, enhanced sedimentation of organic sulphur and less reoxidation as a result of reduced penetration of oxygen into the sediments, a lack of faunal activity and rooted macrophytes.     

Alternative explanations for rising dissolved organic carbon export from organic soils

Since 1988, there has been, on average, a 91% increase in dissolved organic carbon (DOC) concentrations of UK lakes and streams in the Acid Waters Monitoring Network (AWMN). Similar DOC increases have been observed in surface waters across much of Europe and North America. Much of the debate about the causes of rising DOC has, as in other studies relating to the carbon cycle, focused on factors related to climate change. Data from our peat‐core experiments support an influence of climate on DOC, notably an increase in production with temperature under aerobic, and to a lesser extent anaerobic, conditions. However, we argue that climatic factors may not be the dominant drivers of DOC change. DOC solubility is suppressed by high soil water acidity and ionic strength, both of which have decreased as a result of declining sulphur deposition since the 1980s, augmented during the 1990s in the United Kingdom by a cyclical decline in sea‐salt deposition. Our observational and experimental data demonstrate a clear, inverse and quantitatively important link between DOC and sulphate concentrations in soil solution. Statistical analysis of 11 AWMN lakes suggests that rising temperature, declining sulphur deposition and changing sea‐salt loading can account for the majority of the observed DOC trend. This combination of evidence points to the changing chemical composition of atmospheric deposition, particularly the substantial reduction in anthropogenic sulphur emissions during the last 20 years, as a key cause of rising DOC. The implications of rising DOC export for the carbon cycle will be very different if linked primarily to decreasing acid deposition, rather than to changes in climate, suggesting that these systems may be recovering rather than destabilising.