Optimised start-up strategy for bioelectrochemical systems operating on hydrolysed human urine.

Key nutrients, such as nitrogen measured as total ammonium nitrogen (TAN), could be recycled from hydrolysed human urine back to fertiliser use. Bioelectrochemical systems (BESs) are an interesting, low-energy option for realising this. However, the high TAN concentration (> 5 g L-1) and pH (> 9) of hydrolysed urine can inhibit microbial growth and hinder the enrichment of an electroactive biofilm at the anode. This study investigated a new strategy for bioanode inoculation by mixing real hydrolysed urine with thickened waste activated sludge (TWAS) from a municipal wastewater treatment plant at different volumetric ratios. The addition of TWAS diluted the high TAN concentration of hydrolysed urine (5.2 ± 0.3 g L-1) to 2.6-5.1 g L-1, while the pH of the inoculation mixtures remained > 9 and soluble chemical oxygen demand (sCOD) at 5.6-6.7 g L-1. Despite the high pH, current generation started within 24 h for all reactors, and robust bioanodes tolerant of continuous feeding with undiluted hydrolysed urine were enriched within 11 days of start-up. Current output and Coulombic efficiency decreased with increasing initial hydrolysed urine fraction. The anodes inoculated with the highest sCOD-to-TAN ratio (2.1) performed the best, which suggests that high organics levels can protect microbes from inhibition even at elevated TAN concentrations.

The role of suspended biomass in PFAS enrichment in wastewater treatment foams.

Foaming in aerated bioreactors at wastewater treatment plants (WWTPs) has been identified as an operational issue for decades. However, the affinity of per- and polyfluoroalkyl substances (PFAS) for air-liquid interfaces suggests that foam harvesting has the potential to become a sustainable method for PFAS removal from sewage. Aerated bioreactors' foams are considered three-phase systems, comprising air, aqueous and solid components, the latter consisting of activated sludge biomass. To achieve a comprehensive understanding of the capability of aerated bioreactors' foams to enrich PFAS, we analysed PFAS concentrations from WWTPs in both the solid and aqueous phases of the collapsed foams (foamate) and underlying bulk mixed liquors. Our findings show that PFAS enrichment occurs not only in the aqueous phase but also in the solid phase of the foamate. This suggests that previous field studies that only analysed the aqueous phase may have underestimated the capability of the aerated bioreactors' foams to enrich PFAS. Fractions of PFOA and PFOS sorbed to the solid phase of the foamate can be as high as 60 % and 95 %, respectively. Our findings highlight the importance of implementing effective foamate management strategies that consider both the aqueous and solid phases.

A review of foam fractionation for the removal of per- and polyfluoroalkyl substances (PFAS) from aqueous matrices.

The detection of per- and polyfluoroalkyl substances (PFAS) in aqueous matrices is an emerging environmental concern due to their persistent, bioaccumulative and toxic properties. Foam fractionation has emerged as a viable method for removing and concentrating PFAS from aqueous matrices. The method exploits the surface-active nature of the PFAS to adsorb at the air-liquid interfaces of rising air bubbles, resulting in foam formation at the top of a foam fractionator. The removal of PFAS is then achieved through foam harvesting. Foam fractionation has gained increasing attention owing to its inherent advantages, including simplicity and low operational costs. The coupling of foam fractionation with destructive technologies could potentially serve as a comprehensive treatment train for future PFAS management in aqueous matrices. The PFAS-enriched foam, which has a smaller volume, can be directed to subsequent destructive treatment technologies. In this review, we delve into previous experiences with foam fractionation for PFAS removal from various aqueous matrices and critically analyse their key findings. Then, the recent industry advancements and commercial projects that utilise this technology are identified. Finally, future research needs are suggested based on the current challenges.

Phenanthrene regulates metabolic pathways for hydrogen accumulation in sludge alkaline dark fermentation.

The influence of phenanthrene (PHE), a general polycyclic aromatic hydrocarbon in waste activated sludge, on sludge alkaline dark fermentation for hydrogen accumulation was investigated prospectively. The yield of hydrogen was 16.2 mL/g TSS with 50 mg/kg TSS PHE, which was 1.3-fold greater than that of the control. Mechanism research demonstrated that hydrogen production and the abundance of functional microorganisms were facilitated, whereas those of homoacetogenesis were reduced. The activity of pyruvate ferredoxin oxidoreductase in the conversion of pyruvate to reduced ferredoxin for hydrogen production was promoted by 57.2%, and that of carbon monoxide dehydrogenase and formyltetrahydrofolate synthetase, closely associated with hydrogen consumption, was suppressed by 60.5% and 55.9%, respectively. Moreover, the encoding genes involved in pyruvate metabolism were significantly up-regulated, while genes related to consuming hydrogen to reduce carbon dioxide and produce 5-methyltetrahydrofolate were down-regulated. This study notably illustrates the effect of PHE on hydrogen accumulation from metabolic pathways.

Dioctyl phthalate enhances volatile fatty acids production from sludge anaerobic fermentation: Insights of electron transport and metabolic functions.

As one of the most widely used phthalate plasticizers, dioctyl phthalate (DOP) has been detected in wastewater and accumulates in sludge through wastewater treatment, which may adversely affect further sludge treatment. However, the role of DOP on sludge anaerobic fermentation and its mechanism are not yet clear. Therefore, this study focused on the effect of DOP on the volatile fatty acids (VFAs) generation via the anaerobic fermentation of sludge. The results demonstrated that the presence of DOP had a considerable contribution to the generation of VFAs, and the maximum production of VFAs reached 4769 mg COD/L at 500 mg/kg DOP, which was 1.57 folds that of the control. Mechanistic investigation showed that DOP mainly enhanced the hydrolysis, acidification and related enzymes activities of sludge. VFAs-producing microorganisms (e.g., Clostridium and Conexibacter) were also enriched under DOP exposure. Importantly, the presence of DOP increased the electron transfer activity by 26 %, consequently facilitating the organics conversion and fermentation process. Notably, the functional gene expressions involved in substrate metabolism and VFAs biosynthesis were enhanced with DOP, resulting in increased VFAs production from sludge. The results obtained in this study offered a new strategy for the control of pollutants and the recycling of valuable products from sludge.

Urea hydrolysis and long-term storage of source-separated urine for reuse as fertiliser is insufficient for the removal of anthropogenic micropollutants.

Human and animal source-separated urine, stored and allowed to naturally hydrolyse (the bio-catalysed transformation of urea to ammonia and bicarbonate), has been used for millennia as a fertiliser in agriculture. In a context of growing water scarcity and climate uncertainty, source-separation of urine is facing a strong revival thanks to the emergence of cost-effective waterless collection systems. Concomitantly, urine source-separation can be used as a method for nutrient recovery and subsequent reuse. In its simplest form, such recovery consists of collection followed by urea hydrolysis and storage as sole treatment. Numerous guidelines, including by the World Health Organisation, consider that this is sufficient to stabilise the nutrients and inactivate any potential pathogens in the urine. However, it is still unclear whether said urine is effectively free from other compounds of concern, such as anthropogenic micropollutants with known toxicological effects. Moreover, it is also currently unknown if the metabolites produced by human consumption of these products behave in similar way during short- and long-term storage i.e. whether any changes in chemical structure mean that these could be sorbed and/or precipitated in a different way, or if they can potentially be degraded by the biomass inherently present in urine collection systems. Finally, there is currently no knowledge of whether the observed concentrations of micropollutants in stored hydrolysed urine could potentially have toxicological effects if/when applied to soils and edible crops. To fill these research gaps, 20 commonly consumed compounds were selected in this study and their concentrations in the liquid and solid phases studied in the short- and long-term (up to ≥ 2 years). During the initial process of urea hydrolysis (≤ 5 days), ethyl-glucuronide was the sole compound effectively removed (by deconjugation), while only two other compounds, erythromycin and its metabolite, saw a reduction in their concentration (likely due to biomass sorption). Subsequently, during early storage (≤ 15 days), only three additional compounds were removed: paracetamol (> 99%), acesulfame (11.5%) and carbamazepine-10,11 epoxide (40.7%). Finally, long-term storage of up to 24 months did not result in any further significant removal for any of the measured compounds, indicating that the procedure of hydrolysis + storage is not effective for the removal of anthropogenic micropollutants. The results of this investigation raise strong concerns about the direct reuse of hydrolysed/stored human source-separated urine, and evidence the need for post-processing before implementation as fertiliser into edible crops due to the inherent toxicological risk, particularly to infants.

Modelling and techno-economic assessment of (bio)electrochemical nitrogen removal and recovery from reject water at full WWTP scale.

At conventional wastewater treatment plants (WWTPs), reject waters originating from the dewatering of anaerobically digested sludge contain the highest nitrogen concentrations within the plant and thereby have potential for realising nitrogen recovery in a reusable form. At the same time, nitrogen removal from reject waters has potential to reduce the energetic and chemical demands of the WWTP due to a reduced nutrient load to the activated sludge process. In recent years, (bio)electrochemical methods have been extensively studied for nitrogen recovery from reject waters in laboratory-scale but not yet implemented in real WWTP environments, particularly due to concerns about the need for large capital investments. This study assessed the techno-economic feasibility of retrofitting a (bio)electrochemical nitrogen removal and recovery (NRR) unit into the reject water circulation line of a full-scale WWTP through modelling. Data from laboratory-scale (bio)electroconcentration ((B)EC) experiments was used to construct a simple, semi-empirical model block integrated into the Benchmark Simulation Model No. 2 (BSM2) simulating a generalised WWTP. The effects of nitrogen removal from the reject water on both the effluent quality and operational costs of the WWTP were assessed and compared to the BSM2 performance without an NRR unit. In all studied scenarios, the effluent quality index was improved by 4-11%, while both the aeration (7-19% decrease) and carbon (24-71%) requirements were reduced. The additional energy consumed by the NRR unit increased the total operational cost index by >18%, but the revenue assumed for the generated nutrient product (20 EUR kgN-1) was enough to make the BEC-NRR scenarios at realistically low current densities (1 and 5 A m-2) economically attractive compared to the control. A sensitivity analysis revealed that electricity price and nutrient product value had the most notable effects on the feasibility of the NRR unit. The results suggest a key factor in making (bio)electrochemical NRR economically viable is to reduce its electricity consumption further, while the anticipated increases in nitrogen fertiliser prices can help accelerate the adoption of these methods in larger scale.

Electro-fermentation: Sustainable bioproductions steered by electricity.

The market of biobased products obtainable via fermentation processes has steadily increased over the past few years, driven by the need to create a decarbonized economy. To date, industrial fermentation (IF) employs either pure or mixed microbial cultures (MMC), whereby the type of the microbial catalysts and the used feedstock affect metabolic pathways and, in turn, the type of product(s) generated. In many cases, especially when dealing with MMC, the economic viability of IF is still hindered by factors such as the low attained product titer and selectivity, which ultimately challenge the downstream recovery and purification steps. In this context, electro-fermentation (EF) represents an innovative approach, based on the use of a polarized electrode interface to trigger changes in the rate, yield, titer or product distribution deriving from traditional fermentation processes. In principle, the electrode in EF can act as an electron acceptor (i.e., anodic electro-fermentation, AEF) or donor (i.e., cathodic electro-fermentation, CEF), or simply as a means to control the oxidation-reduction potential of the fermentation broth. However, the molecular and biochemical basis underlying EF are still largely unknown. This review provides a comprehensive overview of recent literature studies including both AEF and CEF examples using pure or mixed microbial cultures. A critical analysis of biochemical, microbiological, and engineering aspects which presently hamper the transition of the EF technology from the laboratory to the market is also presented.

Electrochemical oxidation processes for PFAS removal from contaminated water and wastewater: fundamentals, gaps and opportunities towards practical implementation.

Electrochemical oxidation (EO) is emerging as one of the most promising methods for the degradation of recalcitrant per- and poly-fluoroalkyl substances (PFASs) in water and wastewater, as these compounds cannot be effectively treated with conventional bio- or chemical approaches. This review examines the state of the art of EO for PFASs destruction, and comprehensively compares operating parameters and treatment performance indicators for both synthetic and real contaminated water and wastewater media. The evaluation shows the need to use environmentally-relevant media to properly quantify the effectiveness/efficiency of EO for PFASs treatment. Additionally, there is currently a lack of quantification of sorption losses, resulting in a likely over-estimation of process' efficiencies. Furthermore, the majority of experimental results to date indicate that short-chain PFASs are the most challenging and need to be prioritized as environmental regulations become more stringent. Finally, and with a perspective towards practical implementation, several operational strategies are proposed, including processes combining up-concentration followed by EO destruction.

Impact of source-separation of urine on treatment capacity, process design, and capital expenditure of a decentralised wastewater treatment plant.

In this study, the impact of urine diversion on the treatment capacity, treatment process, and capital costs of a decentralised wastewater treatment plant (WWTP) was simulated using BioWin. The data for simulation including for economic analysis were obtained from a real decentralised WWTP at Sydney. Simulation was conducted for two alternative process design scenarios of a WWTP: membrane bioreactor (MBR) without denitrification and anaerobic MBR in place of aerobic MBR and compared to existing process design. The simulation shows that with about 75% urine diversion (through source separation), the treatment capacity of the existing WWTP can be doubled although above 40% urine diversion, the impact appears less rapid. When the urine diversion exceeds 75%, it was found that the anoxic tank for biological denitrification becomes redundant and the current wastewater treatment process could be replaced with a simpler and much less aeration intensive membrane bioreactor (MBR) producing similar effluent quality with a 24% reduction in capital expenditure (footprint) cost. Anaerobic MBR can be a potential alternative to aerobic MBR although pre-treatment becomes essential before reverse osmosis treatment for water reuse applications. Sensitivity analysis has revealed that by operating the bioreactor at higher mixed liquor suspended solids concentrations (9 g/L instead of 5 g/L) could help increase the WWTP treatment capacity by about 3.5 times at 75% urine diversion. Hence, urine diversion (until nitrogen-limiting conditions occur above 75% urine diversion) can increase the treatment capacity of an existing WWTP and reduce the capital expenses due to reduced plant footprint.

A review of microscopic cell imaging and neural network recognition for synergistic cyanobacteria identification and enumeration.

Real-time cyanobacteria/algal monitoring is a valuable tool for early detection of harmful algal blooms, water treatment efficacy evaluation, and assists tailored water quality risk assessments by considering taxonomy and cell counts. This review evaluates and proposes a synergistic approach using neural network image recognition and microscopic imaging devices by first evaluating published literature for both imaging microscopes and image recognition. Quantitative phase imaging was considered the most promising of the investigated imaging techniques due to the provision of enhanced information relative to alternatives. This information provides significant value to image recognition neural networks, such as the convolutional neural networks discussed within this review. Considering published literature, a cyanobacteria monitoring system and corresponding image processing workflow using in situ sample collection buoys and on-shore sample processing was proposed. This system can be implemented using commercially available equipment to facilitate accurate, real-time water quality monitoring.

Wastewater fertigation in agriculture: Issues and opportunities for improved water management and circular economy.

Water shortages are an issue of growing worldwide concern. Irrigated agriculture accounts for about 70% of total freshwater withdrawals globally, therefore alternatives to use of conventional sources need to be investigated. This paper critically reviews the application of treated wastewater for agricultural fertigation (i.e., water and nutrient recovery) considering different perspectives: legislation, agronomic characteristics, social acceptability, sustainability of treatment technologies. Critical issues that still need further investigation for a wider application of fertigation practices include accumulation of emerging contaminants in soils, microbiological and public health implications, and stakeholders' acceptance. A techno-economic methodological approach for assessing the sustainability of treated wastewater reuse in agriculture is subsequently proposed herein, which considers different possible local conditions (cultivated crops and effluent characteristics). The results showed that tailoring effluent characteristics to the desired nutrient composition could enhance the process economic sustainability; however, water savings have a major economic impact than fertilizers' savings, partly due to limited P reuse efficiency. The developed methodology is based on a practical approach and may be generalized to most agricultural conditions, to evaluate and encourage safe and efficient agricultural wastewater reuse practices.

Fertiliser recovery from source-separated urine via membrane bioreactor and heat localized solar evaporation.

Urine with its abundant macronutrients (N-P-K) is an ideal resource for the production of fertiliser. However, the odor and pathogens in the raw urine must be removed to meet the public acceptance of urine collection systems and to enable its safe reuse as a fertiliser. In this work, real urine was collected and treated through a pilot-scale gravity-driven membrane bioreactor (GDMBR) to remove the malodorous organics and to nitrify almost 50% of the ammonia into nitrate. The stablised urine was subsequently distilled via low-cost heat localized solar evaporation (HLSE) to produce a non-odorous solid fertiliser. The developed HLSE with a small footprint can attract bulk solution into a vertical insulated space and quickly heat it up to 68 °C within 1 h. The HLSE process had vapour flux at 1.3 kg m-2 h-1 as well as high solar to vapour conversion efficiency at 87%. Based on the EDX mapping and XRD analysis, the generated crystals are mainly NaNO3, NH4Cl, NaCl, NH4H2PO4 and K2HPO4, which are ideal nutrients for vegetation. In this study, the produced urine-derived fertilisers have a better performance on the growth of the leafy basil than the all-purpose commercial fertilisers. Generally, the GDMBR-HLSE is a promising cost-effective and green technology for nutrients recovery from urine.

Implementation of a Sulfide-Air Fuel Cell Coupled to a Sulfate-Reducing Biocathode for Elemental Sulfur Recovery.

Bio-electrochemical systems (BES) are a flexible biotechnological platform that can be employed to treat several types of wastewaters and recover valuable products concomitantly. Sulfate-rich wastewaters usually lack an electron donor; for this reason, implementing BES to treat the sulfate and the possibility of recovering the elemental sulfur (S0) offers a solution to this kind of wastewater. This study proposes a novel BES configuration that combines bio-electrochemical sulfate reduction in a biocathode with a sulfide-air fuel cell (FC) to recover S0. The proposed system achieved high elemental sulfur production rates (up to 386 mg S0-S L-1 d-1) with 65% of the sulfate removed recovered as S0 and a 12% lower energy consumption per kg of S0 produced (16.50 ± 0.19 kWh kg-1 S0-S) than a conventional electrochemical S0 recovery system.

Selective Extraction of Medium-Chain Carboxylic Acids by Electrodialysis and Phase Separation.

Carboxylic acids obtained via the microbial electrochemical conversion of waste gases containing carbon dioxide (i.e., microbial electrosynthesis) can be used in lieu of nonrenewable building-block chemicals in the manufacture of a variety of products. When targeting valuable medium-chain carboxylic acids such as caproic acid, electricity-driven fermentations can be limited by the accumulation of fermentation products in the culturing media, often resulting in low volumetric productivities and titers due to direct toxicity or inhibition of the biocatalyst. In this study, we tested the effectiveness of a simple electrodialysis system in upconcentrating carboxylic acids from a model solution mimicking the effluent of a microbial electrochemical system producing short- and medium-chain carboxylic acids. Under batch extraction conditions, the electrodialysis scheme enabled the recovery of 60% (mol mol-1) of the total carboxylic acids present in the model fermentation broth. The particular arrangement of conventional monopolar ion exchange membranes and hydraulic recirculation loops allowed the progressive acidification of the extraction solution, enabling phase separation of caproic acid as an immiscible oil with 76% purity.

Electrochemical biofilm control by reconstructing microbial community in agricultural water distribution systems.

Biofilm causes considerable technical challenges in agricultural water distribution systems. Electrochemical treatment (ECT) is a potential technique for controlling biofilm in the systems. Given the limited information on how ECT performance changes of irrigation systems and microbial biofilm community shifts. In this study, the effect of anti-biofilm was assessed. Illumina Miseq high-throughput sequencing, combined with molecular ecological network analysis, were applied to detect the effects of ECT on attached biofilm microbial communities. We found that ECT effectively mitigated biofilm formation with the fixed-biofilm biomass reduced by 37.5 %-79.9 %. ECT significantly shifted the bacterial community structures in the biofilm, reduced the communities' diversity, and changed the dominant species. Molecular ecological network analysis showed that the complexity and size of bacterial networks were destabilized under ECT and decreased the interactions among bacterial species. The reconstruction in bacterial community and networks were responsible for the decline in extracellular polymer substances and biofilm biomass. However, chlorine-resistant bacteria were found increased after ECT, and higher relative abundance and low biofilm removal was identified in continuous ECT as compared with intermittent ECT. These results aimed to highlight the opportunity for biofouling mitigation by ECT for irrigation systems, and reveal the potential anti-biofilm microbial mechanisms of ECT.

Extracellular electron transfer by Microcystis aeruginosa is solely driven by high pH.

Extracellular electron transfer (EET) by the cyanobacterium Microcystis aeruginosa was investigated. Observations indicate that EET onto an electrode poised at + 0.6 vs. standard hydrogen electrode (SHE) is triggered by high pH, more evidently at pH levels above 9. Light intensity does not appear to affect electricity generation, indicating that this may not be a "biophotovoltaic" process. The generated current density was amplified with stepwise pH increases from approximately 5 mA m-2 at pH 7.8 to 30 mA m-2 at pH 10.5, for dense (0.4 mg mL-1 dry weight) Microcystis aeruginosa suspensions with dissolved CO2 and O2 approaching equilibrium with atmospheric concentrations. The upsurge in current density was more pronounced (from 5 mA m-2 at pH 7.8 to 40 mA m-2 at pH 10.2) in the absence of the cells' natural electron acceptors, dissolved CO2 and O2. However, the latter effect is more likely due to competition for electrons by oxygen than to reductive stress. EET in this species is therefore a light-independent process that is enhanced by increasing pH, with reasons that are still unknown, but either related to the involvement of protons in the last step of electron transfer, or to intracellular pH control.

Urine Treatment on the International Space Station: Current Practice and Novel Approaches.

A reliable, robust, and resilient water recovery system is of paramount importance on board the International Space Station (ISS). Such a system must be able to treat all sources of water, thereby reducing resupply costs and allowing for longer-term space missions. As such, technologies able to dewater urine in microgravity have been investigated by different space agencies. However, despite over 50 years of research and advancements on water extraction from human urine, the Urine Processing Assembly (UPA) and the Water Processor Assembly (WPA) now operating on the ISS still achieve suboptimal water recovery rates and require periodic consumables resupply. Additionally, urine brine from the treatment is collected for disposal and not yet reused. These factors, combined with the need for a life support system capable of tolerating even dormant periods of up to one year, make the research in this field ever more critical. As such, in the last decade, extensive research was conducted on the adaptation of existing or emerging technologies for the ISS context. In virtue of having a strong chemical resistance, small footprint, tuneable selectivity and versatility, novel membrane-based processes have been in focus for treating human urine. Their hybridisation with thermal and biological processes as well as the combination with new nanomaterials have been particularly investigated. This article critically reviews the UPA and WPA processes currently in operation on the ISS, summarising the research directions and needs, highlighted by major space agencies, necessary for allowing life support for missions outside the Low Earth Orbit (LEO). Additionally, it reviews the technologies recently proposed to improve the performance of the system as well as new concepts to allow for the valorisation of the nutrients in urine or the brine after urine dewatering.

Energy recovery through reverse electrodialysis: Harnessing the salinity gradient from the flushing of human urine.

Urine dilution is often performed to avoid clogging or scaling of pipes, which occurs due to urine's Ca2+ and Mg2+ precipitating at the alkaline conditions created by ureolysis. The large salinity gradient between urine and flushing water is, theoretically, a source of potential energy which is currently unexploited. As such, this work explored the use of a compact reverse electrodialysis (RED) system to convert the chemical potential energy of urine dilution into electric energy. Urine' composition and ureolysis state as well as solution pumping costs were all taken into account. Despite having almost double its electric conductivity, real hydrolysed urine obtained net energy recoveries ENet of 0.053-0.039 kWh/m3, which is similar to energy recovered from real fresh urine. The reduced performances of hydrolysed urine were linked to its higher organic fouling potential and possible volatilisation of NH3 due to its high pH. However, the higher-than-expected performance achieved by fresh urine is possibly due to the fast diffusion of uncharged urea to the freshwater side. Real urine was also tested as a novel electrolyte solution and its performance compared with a conventional K4Fe(CN)6/K3Fe(CN)6 couple. While K4Fe(CN)6/K3Fe(CN)6 outperformed urine in terms of power densities and energy recoveries, net chemical reactions seemed to have occurred in urine when used as an electrolyte solution, leading to TOC, ammonia and urea removal of up to 13%, 6% and 4.4%, respectively. Finally, due to the migration of K+, NH4+ and PO43-, the low concentration solution could be utilised for fertigation. Overall, this process has the potential of providing off-grid urine treatment or energy production at a household or building level.

Staged electrochemical treatment guided by modelling allows for targeted recovery of metals and rare earth elements from acid mine drainage.

Acid mine drainage (AMD) is a challenge for current and legacy mining operations worldwide given its potential to severely harm ecosystems and communities if inadequately managed. Treatment costs for AMD are amongst the highest in the industrial wastewater treatment sector, with limited sustainable options available to date. This work demonstrates a novel chemical-free approach to tackle AMD, whereby staged electrochemical neutralisation is employed to treat AMD and concomitantly recover metals as precipitates. This approach was guided by physico-chemical modelling and tested on real AMD from two different legacy mine sites in Australia, and compared against conventional chemical-dosing-based techniques using hydrated lime (Ca(OH)2) and sodium hydroxide (NaOH). The electrochemical treatment demonstrated the same capacity than Ca(OH)2 to neutralise AMD and remove sulfates, and both were significantly better than NaOH. However, the electrochemical approach produced less voluminous and more easily settleable sludge than Ca(OH)2. Moreover, the staged treatment approach demonstrated the potential to produce metal-rich powdered solids with a targeted composition, including rare earth elements and yttrium (REY). REY were recovered in concentrations up to 0.1% of the total solids composition, illustrating a new avenue for AMD remediation coupled with the recovery of critical metals.