The need to integrate legacy nitrogen storage dynamics and time lags into policy and practice.

Increased fluxes of reactive nitrogen (Nr), often associated with N fertilizer use in agriculture, have resulted in negative environmental consequences, including eutrophication, which cost billions of dollars per year globally. To address this, best management practices (BMPs) to reduce Nr loading to the environment have been introduced in many locations. However, improvements in water quality associated with BMP implementation have not always been realised over expected timescales. There is a now a significant body of scientific evidence showing that the dynamics of legacy Nr storage and associated time lags invalidate the assumptions of many models used by policymakers for decision making regarding Nr BMPs. Building on this evidence, we believe that the concepts of legacy Nr storage dynamics and time lags need to be included in these models. We believe the biogeochemical research community could play a more proactive role in advocating for this change through both awareness raising and direct collaboration with policymakers to develop improved datasets and models. We anticipate that this will result in more realistic expectations of timescales for water quality improvements associated with BMPs. Given the need for multi-nutrient policy responses to tackle challenges such as eutrophication, integration of N stores will have the further benefit of aligning both researchers and policymakers in the N community with the phosphorus and carbon communities, where estimation of stores is more widespread. Ultimately, we anticipate that integrating legacy Nr storage dynamics and time lags into policy frameworks will better meet the needs of human and environmental health.

Observed controls on resilience of groundwater to climate variability in sub-Saharan Africa.

Groundwater in sub-Saharan Africa supports livelihoods and poverty alleviation1,2, maintains vital ecosystems, and strongly influences terrestrial water and energy budgets3. Yet the hydrological processes that govern groundwater recharge and sustainability-and their sensitivity to climatic variability-are poorly constrained4,5. Given the absence of firm observational constraints, it remains to be seen whether model-based projections of decreased water resources in dry parts of the region4 are justified. Here we show, through analysis of multidecadal groundwater hydrographs across sub-Saharan Africa, that levels of aridity dictate the predominant recharge processes, whereas local hydrogeology influences the type and sensitivity of precipitation-recharge relationships. Recharge in some humid locations varies by as little as five per cent (by coefficient of variation) across a wide range of annual precipitation values. Other regions, by contrast, show roughly linear precipitation-recharge relationships, with precipitation thresholds (of roughly ten millimetres or less per day) governing the initiation of recharge. These thresholds tend to rise as aridity increases, and recharge in drylands is more episodic and increasingly dominated by focused recharge through losses from ephemeral overland flows. Extreme annual recharge is commonly associated with intense rainfall and flooding events, themselves often driven by large-scale climate controls. Intense precipitation, even during years of lower overall precipitation, produces some of the largest years of recharge in some dry subtropical locations. Our results therefore challenge the 'high certainty' consensus regarding decreasing water resources4 in such regions of sub-Saharan Africa. The potential resilience of groundwater to climate variability in many areas that is revealed by these precipitation-recharge relationships is essential for informing reliable predictions of climate-change impacts and adaptation strategies.

Provenance of drinking water revealed through compliance sampling.

Understanding drinking water hydrochemistry is essential for maintaining safe drinking water supplies. Whilst targeted research surveys have characterised drinking water hydrochemistry, vast compliance datasets are routinely collected but are not interrogated amidst concerns regarding the impact of mixed water sources, treatment, the distribution network and customer pipework. In this paper, we examine whether compliance samples retain hydrochemical signatures of their provenance. We first created and subsequently undertook the first hydrochemical analysis of a novel national database of publically available drinking water compliance analyses (n = 3 873 941) reported for 2015 across England and Wales. k-means cluster analysis revealed three spatially coherent clusters. Cluster 1 is dominated by groundwater sources, with high nitrate concentrations and mineralisation, and lower organic carbon, residual chlorine and THM formation. Cluster 2 was dominated by surface water sources and characterised by low mineralisation (low conductivity and major ion concentrations), low nitrate and high organic carbon concentrations (and hence residual chlorine and THM formation). Cluster 3 shows a mixture of groundwater overlain by confining layers and superficial deposits (resulting in higher trace metal concentrations and mineralisation) and surface water sources. These analyses demonstrate that, despite extensive processing of drinking water, at the national scale signatures of the provenance of drinking water remain. Analysis of compliance samples is therefore likely to be a helpful tool in the characterisation of processes that may affect drinking water chemistry. The methodology used is generic and can be applied in any area where drinking water chemistry samples are taken.

Public Water Supply Is Responsible for Significant Fluxes of Inorganic Nitrogen in the Environment.

Understanding anthropogenic disturbance of macronutrient cycles is essential for assessing the risks facing ecosystems. For the first time, we quantified inorganic nitrogen (N) fluxes associated with abstraction, mains water leakage, and transfers of treated water related to public water supply. In England, the mass of nitrate-N removed from aquatic environments by abstraction (ABS-NO3-N) was estimated to be 24.2 kt N/year. This is equal to six times the estimates of organic N removal by abstraction, 15 times in-channel storage of organic N, and 30 times floodplain storage of organic N. ABS-NO3-N is also between 3 and 39% of N removal by denitrification in the hydrosphere. Mains water leakage of nitrate-N (MWL-NO3-N) returns 3.62 kt N/year to the environment, equating to approximately 15% of ABS-NO3-N. In urban areas, MWL-NO3-N can represent up to 20% of the total N inputs. MWL-NO3-N is predicted to increase by up to 66% by 2020 following implementation of treated water transfers. ABS-NO3-N and MWL-NO3-N should be considered in future assessments of N fluxes, in order to accurately quantify anthropogenic disturbances to N cycles. The methodology we developed is transferable, uses widely available datasets, and could be used to quantify N fluxes associated with public water supply across the world.

Mains water leakage: Implications for phosphorus source apportionment and policy responses in catchments.

Effective strategies to reduce phosphorus (P)-enrichment of aquatic ecosystems require accurate quantification of the absolute and relative importance of individual sources of P. In this paper, we quantify the potential significance of a source of P that has been neglected to date. Phosphate dosing of raw water supplies to reduce lead and copper concentrations in drinking water is a common practice globally. However, mains water leakage (MWL) potentially leads to a direct input of P into the environment, bypassing wastewater treatment. We develop a new approach to estimate the spatial distribution and time-variant flux of MWL-P, demonstrating this approach for a 30-year period within the exemplar of the River Thames catchment in the UK. Our analyses suggest that MWL-P could be equivalent to up to c.24% of the P load entering the River Thames from sewage treatment works and up to c.16% of the riverine P load derived from agricultural non-point sources. We consider a range of policy responses that could reduce MWL-P loads to the environment, including incorporating the environmental damage costs associated with P in setting targets for MWL reduction, alongside inclusion of MWL-P within catchment-wide P permits.

Isotopic Fingerprint for Phosphorus in Drinking Water Supplies.

Phosphate dosing of drinking water supplies, coupled with leakage from distribution networks, represents a significant input of phosphorus to the environment. The oxygen isotope composition of phosphate (δ(18)OPO4), a novel stable isotope tracer for phosphorus, offers new opportunities to understand the importance of phosphorus derived from sources such as drinking water. We report the first assessment of δ(18)OPO4 within drinking water supplies. A total of 40 samples from phosphate-dosed distribution networks were analyzed from across England and Wales. In addition, samples of the source orthophosphoric acid used for dosing were also analyzed. Two distinct isotopic signatures for drinking water were identified (average = +13.2 or +19.7‰), primarily determined by δ(18)OPO4 of the source acid (average = +12.4 or +19.7‰). Dependent upon the source acid used, drinking water δ(18)OPO4 appears isotopically distinct from a number of other phosphorus sources. Isotopic offsets from the source acid ranging from -0.9 to +2.8‰ were observed. There was little evidence that equilibrium isotope fractionation dominated within the networks, with offsets from temperature-dependent equilibrium ranging from -4.8 to +4.2‰. While partial equilibrium fractionation may have occurred, kinetic effects associated with microbial uptake of phosphorus or abiotic sorption and dissolution reactions may also contribute to δ(18)OPO4 within drinking water supplies.