The Future of Municipal Wastewater Reuse Concentrate Management: Drivers, Challenges, and Opportunities.

Water reuse is rapidly becoming an integral feature of resilient water systems, where municipal wastewater undergoes advanced treatment, typically involving a sequence of ultrafiltration (UF), reverse osmosis (RO), and an advanced oxidation process (AOP). When RO is used, a concentrated waste stream is produced that is elevated in not only total dissolved solids but also metals, nutrients, and micropollutants that have passed through conventional wastewater treatment. Management of this RO concentrate─dubbed municipal wastewater reuse concentrate (MWRC)─will be critical to address, especially as water reuse practices become more widespread. Building on existing brine management practices, this review explores MWRC management options by identifying infrastructural needs and opportunities for multi-beneficial disposal. To safeguard environmental systems from the potential hazards of MWRC, disposal, monitoring, and regulatory techniques are discussed to promote the safety and affordability of implementing MWRC management. Furthermore, opportunities for resource recovery and valorization are differentiated, while economic techniques to revamp cost-benefit analysis for MWRC management are examined. The goal of this critical review is to create a common foundation for researchers, practitioners, and regulators by providing an interdisciplinary set of tools and frameworks to address the impending challenges and emerging opportunities of MWRC management.

High-impact innovations for high-salinity membrane desalination.

Reducing the cost of high-salinity (>75 g/L total dissolved solids) brine concentration technology would unlock the potential for vast inland water supplies and promote the safe management of concentrated aqueous waste streams. Impactful innovation will target component performance improvements and cost reductions that yield the highest impact on system costs, but the desalination community lacks methods for quantitatively evaluating the value of innovation or the robustness of technology platforms relative to competing technologies. This work proposes a suite of methods built on process-based cost optimization models that explicitly address the complexities of membrane-separation processes, namely that these processes comprise dozens of nonlinearly interacting components and that innovation can occur in more than one component at a time. We begin by demonstrating the merit of performing simple parametric sensitivity analysis on component performance and cost to guide the selection of materials and manufacturing methods that reduce system costs. A more rigorous implementation of this approach relates improvements in component performance to increases in component costs, helping to further discern high-impact innovation trajectories. The most advanced implementation includes a stochastic simulation of the value of innovation that accounts for both the expected impact of a component innovation on reducing system costs and the potential for improvements in other components. Finally, we apply these methods to identify innovations with the highest probability of substantially reducing the levelized cost of water from emerging membrane processes for high-salinity brine treatment.

Integrated Energy Flexibility Management at Wastewater Treatment Facilities.

On-site batteries, low-pressure biogas storage, and wastewater storage could position wastewater resource recovery facilities as a widespread source of industrial energy demand flexibility. This work introduces a digital twin method that simulates the coordinated operation of current and future energy flexibility resources. We combine process models and statistical learning on 15 min resolution sensor data to construct a facility's energy and water flows. We then value energy flexibility interventions and use an iterative search algorithm to optimize energy flexibility upgrades. Results from a California facility with anaerobic sludge digestion and biogas cogeneration predict a 17% reduction in electricity bills and an annualized 3% return on investment. A national analysis suggests substantial benefit from using existing flexibility resources, such as wet-weather storage, to reduce electricity bills but finds that new energy flexibility investments are much less profitable in electricity markets without time-of-use incentives and plants without existing cogeneration facilities. Profitability of a range of energy flexibility interventions may increase as a larger number of utilities place a premium on energy flexibility, and cogeneration is more widely adopted. Our findings suggest that policies are needed to incentivize the sector's energy flexibility and provide subsidized lending to finance it.

Multicriteria Suitability Index for Prioritizing Early-Stage Deployments of Wastewater-Derived Fertilizers in Sub-Saharan Africa.

Recycling nutrients from wastewater could simultaneously decrease the carbon intensity of traditional ammonia supply chains and increase the accessibility of local fertilizer. Despite the theoretical potential, techno-economic viability of wastewater nutrient recovery in sub-Saharan Africa has been poorly characterized at subnational scales. This work proposes a multicriteria suitability index to describe techno-economic viability of wastewater-derived fertilizer technologies with district-scale resolution. This index, with a range from 0 to 1 (highest suitability), incorporates key drivers, including population density, soil conditions, sanitation levels, and fertilizer prices. We found that suitability varies widely within and across countries in sub-Saharan Africa and that the primary limiting factor is the absence of sanitation infrastructure. Regions with a minimum of 10% cropland area and a suitability index of at least 0.9 were identified as highly suitable target regions for initial deployment. While they comprise only 1% of the analyzed area, these regions are home to 39 million people and contain up to 3.7 million hectares of cropland. Wastewater-derived fertilizer technologies could deliver an average of 25 kg of nitrogen per hectare of cropland, generating additional food equivalent to the annual consumption of 6 million people. Screening for high suitability can inform selection of effective lighthouse demonstration sites that derisk technology deployment and promote the transition to a more circular nutrient economy.

High-Resolution Carbon Accounting Framework for Urban Water Supply Systems.

Decarbonization of urban infrastructure systems is imperative to meeting global climate goals. Urban water supply systems (UWSSs) account for 1-3% of urban electricity consumption in the U.S., a value expected to increase, as municipalities tap nontraditional water supplies that are either more distant or require more energy-intensive treatment. Reducing the carbon intensity of UWSSs will require a combination of infrastructure upgrades, operational modifications, and behavioral interventions, but urban water planners, water treatment system operators, and consumers lack transparent tools for quantifying the carbon emission implications of these decisions. We propose a high-resolution carbon accounting framework that allows for attribution of carbon emissions to individual water sources, water system components, or individual consumers in a UWSS. The high temporal resolution of this framework also enables rapid assessment of the potential for operational and behavioral interventions to reduce the carbon intensity of UWSSs. We demonstrate this carbon accounting framework on a real-world UWSS serving a city of roughly 100 000 residents. The high spatial and temporal resolution, coupled with the scalability of this approach, makes it a valuable tool for consulting engineers, operators, and consumers seeking to deliver Net Zero water supplies.

Unraveling pH Effects on Ultrafiltration Membrane Fouling by Extracellular Polymeric Substances: Adsorption and Conformation Analyzed with Localized Surface Plasmon Resonance.

Extracellular polymeric substances (EPSs) can conform and orient on the surface according to the applied aquatic conditions. While pH elevation usually removes EPSs from membranes, small changes in pH can change the adsorbed EPS conformation and orientation, resulting in a decrease in membrane permeability. Accordingly, EPS layers were tested with localized surface plasmon resonance (LSPR) sensing and quartz crystal microbalance with dissipation monitoring (QCM-D) using a hybrid sensor. A novel membrane-mimetic hybrid QCM-D-LSPR sensor was designed to indicate both "dry" mass and mechanical load ("wet" mass) of the adsorbed EPS. The effect of pH on the EPS layer's viscoelastic properties and hydrated thickness analyzed by QCM-D corroborates with the shift in EPS areal concentration, ΓS, and the associated EPS conformation, analyzed by LSPR. As pH elevates, the processes of (i) elevation in EPS layer's thickness (QCM-D) and (ii) decrease in the EPS areal density, ΓS (LSPR), provide a clear indication for changes in EPS conformation, which decrease the effective ultrafiltration (UF) membrane pore diameter. This decrease in the pore diameter together with the increase in surface hydrophobicity elevates UF membrane hydraulic resistance.

Effects of meteorological and land surface modeling uncertainty on errors in winegrape ET calculated with SIMS.

Characterization of model errors is important when applying satellite-driven evapotranspiration (ET) models to water resource management problems. This study examines how uncertainty in meteorological forcing data and land surface modeling propagate through to errors in final ET data calculated using the Satellite Irrigation Management Support (SIMS) model, a computationally efficient ET model driven with satellite surface reflectance values. The model is applied to three instrumented winegrape vineyards over the 2017-2020 time period and the spatial and temporal variation in errors are analyzed. We illustrate how meteorological data inputs can introduce biases that vary in space and at seasonal timescales, but that can persist from year to year. We also observe that errors in SIMS estimates of land surface conductance can have a particularly strong dependence on time of year. Overall, meteorological inputs introduced RMSE of 0.33-0.65 mm/day (7-27%) across sites, while SIMS introduced RMSE of 0.55-0.83 mm/day (19-24%). The relative error contribution from meteorological inputs versus SIMS varied across sites; errors from SIMS were larger at one site, errors from meteorological inputs were larger at a second site, and the error contributions were of equal magnitude at the third site. The similar magnitude of error contributions is significant given that many satellite-driven ET models differ in their approaches to estimating land surface conductance, but often rely on similar or identical meteorological forcing data. The finding is particularly notable given that SIMS makes assumptions about the land surface (no soil evaporation or plant water stress) that do not always hold in practice. The results of this study show that improving SIMS by eliminating these assumptions would result in meteorological inputs dominating the error budget of the model on the whole. This finding underscores the need for further work on characterizing spatial uncertainty in the meteorological forcing of ET. Supplementary Information: The online version contains supplementary material available at 10.1007/s00271-022-00808-9.

Energy-Optimal Siting of Decentralized Water Recycling Systems.

Decentralized water recycling systems (DWRS) have emerged as a viable option for incrementally augmenting water supply in water-stressed regions, but DWRS are generally more energy-intensive than traditional centralized water treatment systems. When DWRS are deployed incrementally in small batches, the marginal energy intensity (MEI) of water supply quantifies the location-specific energy footprint of centralized water supply and serves as a robust metric measuring the energy implications of replacing centralized supply with DWRS supply. This research develops and applies a MEI-based decision framework that identifies the energy-optimal siting of DWRS to minimize the overall system operational energy consumption given a target fraction of water demand to be met by newly deployed DWRS. In a small benchmark water supply system where the energy intensity of the intended DWRS is 5.3% higher than the current system average energy intensity of centralized supply, we demonstrate that the optimal siting of DWRS to offset 10% of the system-wide water demand reduces the overall system energy consumption by 0.77%. In contrast, the naive and worst-case siting of the same DWRS increases the energy consumption of the overall system by 0.65 and 2.0%, respectively. The proposed MEI-based decision framework is particularly valuable for application in large multi-source systems, where an optimization-based approach is computationally intractable. This study highlights the importance of accounting for both distribution and treatment energy intensity when evaluating new water sources and demonstrates the viability of DWRS as an energy-efficient tool for augmenting water supply.

Energy and CO2 Emissions Penalty Ranges for Geologic Carbon Storage Brine Management.

Safe and cost-effective geologic carbon storage will require active CO2 reservoir management, including brine extraction to minimize subsurface pressure accumulation. While past simulation and experimental efforts have estimated brine extraction volumes, carbon management policies must also assess the energy or emissions penalties of managing and disposing of this brine. We estimate energy and CO2 emission penalties of extracted brine management on a per tonne of CO2 stored basis by spatially integrating CO2 emissions from U.S. coal-fired electric generating units, CO2 storage reservoirs, and brine salinity data sets under several carbon and water management scenarios. We estimate a median energy penalty of 4.4-35 kWh/tonne CO2 stored, suggesting that brine management will be the largest post capture and compression energy sink in the carbon storage process. These estimates of energy demand for brine management are useful for evaluating end-uses for treated brine, assessing the cost of CO2 storage at the reservoir level, and optimizing national CO2 transport and storage infrastructure.

Flue Gas Desulfurization Wastewater Composition and Implications for Regulatory and Treatment Train Design.

The U.S. Environmental Protection Agency is currently revising its regulations on trace element discharges from flue gas desulfurization (FGD) wastewater. In this work, we expand a predictive model of trace element behavior at coal-fired power plants (CFPPs) to estimate the trace element concentration of FGD wastewater at the plant level. We demonstrate that variation in trace element concentrations in FGD wastewater can span several orders of magnitude and is a function of both coal rank and installed air pollution control devices. This conclusion suggests that the benefits and costs of FGD wastewater treatment for the median plant will poorly describe the actual benefits and costs over the full range of existing CFPPs. Our model can be used to identify different "classes" of CFPPs for future regulatory and technology development efforts and to evaluate the robustness of proposed treatment technologies in light of large intraplant variability. The model can also elucidate new compliance pathways that exploit empirical and mechanistic relationships between coal concentration, trace element partitioning, and FGD wastewater composition.

Performance Loss of Activated Carbon Electrodes in Capacitive Deionization: Mechanisms and Material Property Predictors.

Understanding the material property origins of performance decay in carbon electrodes is critical to maximizing the longevity of capacitive deionization (CDI) systems. This study investigates the cycling stability of electrodes fabricated from six commercial and two post-processed activated carbons. We find that the capacity decay rate of electrodes in half cells is positively correlated with the specific surface area and total surface acidity of the activated carbons. We also demonstrate that half-cell cycling stability is consistent with full cell desalination performance durability. Additionally, our results suggest that increase in internal resistance and physical pore blockage resulting from extensive cycling may be important mechanisms for the specific capacitance decay of activated carbon electrodes in this study. Our findings provide crucial guidelines for selecting activated carbon electrodes for stable CDI performance over long-term operation and insight into appropriate parameters for electrode performance and longevity in models assessing the techno-economic viability of CDI. Finally, our half-cell cycling protocol also offers a method for evaluating the stability of new electrode materials without preparing large, freestanding electrodes.

Spatially resolved air-water emissions tradeoffs improve regulatory impact analyses for electricity generation.

Coal-fired power plants (CFPPs) generate air, water, and solids emissions that impose substantial human health, environmental, and climate change (HEC) damages. This work demonstrates the importance of accounting for cross-media emissions tradeoffs, plant and regional emissions factors, and spatially variation in the marginal damages of air emissions when performing regulatory impact analyses for electric power generation. As a case study, we assess the benefits and costs of treating wet flue gas desulfurization (FGD) wastewater at US CFPPs using the two best available treatment technology options specified in the 2015 Effluent Limitation Guidelines (ELGs). We perform a life-cycle inventory of electricity and chemical inputs to FGD wastewater treatment processes and quantify the marginal HEC damages of associated air emissions. We combine these spatially resolved damage estimates with Environmental Protection Agency estimates of water quality benefits, fuel-switching benefits, and regulatory compliance costs. We estimate that the ELGs will impose average net costs of $3.01 per cubic meter for chemical precipitation and biological wastewater treatment and $11.26 per cubic meter for zero-liquid discharge wastewater treatment (expected cost-benefit ratios of 1.8 and 1.7, respectively), with damages concentrated in regions containing a high fraction of coal generation or a large chemical manufacturing industry. Findings of net cost for FGD wastewater treatment are robust to uncertainty in auxiliary power source, location of chemical manufacturing, and binding air emissions limits in noncompliant regions, among other variables. Future regulatory design will minimize compliance costs and HEC tradeoffs by regulating air, water, and solids emissions simultaneously and performing regulatory assessments that account for spatial variation in emissions impacts.

Trace Element Mass Flow Rates from U.S. Coal Fired Power Plants.

Trace elements (TEs) exit coal-fired power plants (CFPPs) via solid, liquid, and gaseous waste streams. Estimating the TE concentrations of these waste streams is essential to selecting pollution controls and estimating emission reduction benefits. This work introduces a generalizable mass balance model for estimating TE mass flow rates in CFPP waste streams and evaluates model accuracy for the U.S. coal fleet given current data constraints. We stochastically estimate, using a bootstrapping approach, the 2015 plant-level mass flow rates of Hg, Se, As, and Cl to solid, liquid, and gas phase waste streams by combining publicly available data for combusted coal TE concentrations with estimates of TE partitioning within installed air pollution control processes. When compared with measured and reported data on TE mass flow rates, this model generally overestimates masses by 30-50%, with larger errors for Hg. The partitioning estimates are consistent for Se, As, and Cl removal from flue gas, but tend to underestimate Hg removal. While our model is suitable for first-order estimates of TE mass flows, future work to improve model performance should focus on collecting and using new data on TE concentrations in the coal blend, where data quality is the weakest.

Air Emission Reduction Benefits of Biogas Electricity Generation at Municipal Wastewater Treatment Plants.

Conventional processes for municipal wastewater treatment facilities are energy and materially intensive. This work quantifies the air emission implications of energy consumption, chemical use, and direct pollutant release at municipal wastewater treatment facilities across the U.S. and assesses the potential to avoid these damages by generating electricity and heat from the combustion of biogas produced during anaerobic sludge digestion. We find that embedded and on-site air emissions from municipal wastewater treatment imposed human health, environmental, and climate (HEC) damages on the order of $1.63 billion USD in 2012, with 85% of these damages attributed to the estimated consumption of 19 500 GWh of electricity by treatment processes annually, or 0.53% of the US electricity demand. An additional 11.8 million tons of biogenic CO2 are directly emitted by wastewater treatment and sludge digestion processes currently installed at plants. Retrofitting existing wastewater treatment facilities with anaerobic sludge digestion for biogas production and biogas-fueled heat and electricity generation has the potential to reduce HEC damages by up to 24.9% relative to baseline emissions. Retrofitting only large plants (>5 MGD), where biogas generation is more likely to be economically viable, would generate HEC benefits of $254 annually. These findings reinforce the importance of accounting for use-phase embedded air emissions and spatially resolved marginal damage estimates when designing sustainable infrastructure systems.

Cost Optimization of Osmotically Assisted Reverse Osmosis.

We develop a nonlinear optimization model to identify minimum cost designs for osmotically assisted reverse osmosis (OARO), a multistaged membrane-based process for desalinating high-salinity brines. The optimization model enables comprehensive evaluation of a complex process configuration and operational decision space that includes nonlinear process performance and implicit relationships among membrane stages, saline sweep cycles, and makeup, purge, and recycle streams. The objective function minimizes cost, rather than energy or capital expenditures, to accurately account for the trade-offs in capital and operational expenses inherent in multistaged membrane processes. Generally, we find that cost-optimal OARO processes minimize the number of stages, eliminate the use of saline makeup streams, purge from the first sweep cycle, and successively decrease stage membrane area and sweep flow rates. The optimal OARO configuration for treating feed salinities of 50-125 g/L total dissolved solids with water recoveries between 30-70% results in costs less than or equal to $6 per m3 of product water. Sensitivity analysis suggests that future research to minimize OARO costs should focus on minimizing the membrane structural parameter while maximizing the membrane burst pressure and reducing the membrane unit cost.

Mechanisms of Humic Acid Fouling on Capacitive and Insertion Electrodes for Electrochemical Desalination.

Though electrochemical deionization technologies have been widely explored for brackish water desalination and selective ion removal, their sustained performance in the presence of foulants common to environmental waters remains unclear. This study investigates the fundamental mechanisms by which carbonaceous electrodes used in capacitive deionization and insertion electrodes used for high-capacity selective ion removal are affected by the presence of humic acid (HA). We evaluate HA adsorption behavior and the resulting impact on the ion storage capacity and cycling stability of the electrode materials. We find that HA is primarily adsorbed to the mesopores of two carbonaceous electrodes with distinctly different pore structures, but that the ion storage and transport properties of the electrodes are not significantly impacted by HA adsorption. In contrast, HA adsorption resulted in sharp capacity decay for the insertion (Na4Mn9O18) electrode. We attribute this decay to both hindered Na+ ion diffusion to the insertion interface in the presence of adsorbed HA, as well as HA mediated electrode dissolution. These findings highlight the contrasting mechanisms for HA fouling of capacitive and insertion electrodes and suggest that insertion electrodes may be more susceptible to performance decline in electrochemical deionization of environmental waters.

Air Emissions Damages from Municipal Drinking Water Treatment Under Current and Proposed Regulatory Standards.

Water treatment processes present intersectoral and cross-media risk trade-offs that are not presently considered in Safe Drinking Water Act regulatory analyses. This paper develops a method for assessing the air emission implications of common municipal water treatment processes used to comply with recently promulgated and proposed regulatory standards, including concentration limits for, lead and copper, disinfection byproducts, chromium(VI), strontium, and PFOA/PFOS. Life-cycle models of electricity and chemical consumption for individual drinking water unit processes are used to estimate embedded NOx, SO2, PM2.5, and CO2 emissions on a cubic meter basis. We estimate air emission damages from currently installed treatment processes at U.S. drinking water facilities to be on the order of $500 million USD annually. Fully complying with six promulgated and proposed rules would increase baseline air emission damages by approximately 50%, with three-quarters of these damages originating from chemical manufacturing. Despite the magnitude of these air emission damages, the net benefit of currently implemented rules remains positive. For some proposed rules, however, the promise of net benefits remains contingent on technology choice.

Allocating Damage Compensation in a Federalist System: Lessons from Spatially Resolved Air Emissions in the Marcellus.

The benefits and impacts of unconventional natural gas development are realized at different spatial scales, calling into question the appropriate jurisdictional level at which to set and enforce environmental policy. This paper evaluates impact fee allocation under Pennsylvania Act 13, which authorizes Commonwealth payments to Pennsylvania counties to offset damages from unconventional natural gas extraction in exchange for consolidated state-level regulatory authority. We evaluate the adequacy of damage compensation allocation for impacts that are spatially and temporally removed from the well site, using the air emissions associated with natural gas wastewater transport as a case study. Wastewater transport from wells eligible for 2011 impact fee disbursement calculations generated an estimated $11.6 million in air emission damages from 2004 to 2013, with 35% of damages occurring out-of-state and an average of 94% of damages occurring out-of-county. We find that compensatory payments from Pennsylvania Act 13, which are based upon the number of wells drilled in a county in a single year, inadequately account for spatially and temporally distributed impacts from wastewater transport. This case study of Pennsylvania Act 13 highlights potential issues associated with central regulators using compensatory payments as a means of resolving jurisdictional conflict. In cases where the central regulator benefits from the polluting activity, we argue that there is incentive to focus compensation on local damages and undervalue regional and spatially distributed damages in compensation algorithms.

Magnetically Directed Two-Dimensional Crystallization of OmpF Membrane Proteins in Block Copolymers.

Two-dimensional (2D) alignment and crystallization of membrane proteins (MPs) is increasingly important in characterizing their three-dimensional (3D) structure, in designing pharmacological agents, and in leveraging MPs for biomimetic devices. Large, highly ordered MP 2D crystals in block copolymer (BCP) matrices are challenging to fabricate, but a facile and scalable technique for aligning and crystallizing MPs in thin-film geometries would rapidly translate into applications. This work introduces a novel method to grow larger and potentially better ordered 2D crystals by performing the crystallization process in the presence of a strong magnetic field. We demonstrate the efficacy of this approach using a ß-barrel MP, outer membrane protein F (OmpF), in short-chain polybutadiene-poly(ethylene oxide) (PB-PEO) membranes. Crystals grown in a magnetic field were up to 5 times larger than conventionally grown crystals, and a signal-to-noise (SNR) analysis of diffraction peaks in Fourier transforms of specimens imaged by negative-stain electron microscopy (EM) and cryo-EM showed twice as many high-SNR diffraction peaks, indicating that the magnetic field also improves crystal order.

Quantity, Quality, and Availability of Waste Heat from United States Thermal Power Generation.

Secondary application of unconverted heat produced during electric power generation has the potential to improve the life-cycle fuel efficiency of the electric power industry and the sectors it serves. This work quantifies the residual heat (also known as waste heat) generated by U.S. thermal power plants and assesses the intermittency and transport issues that must be considered when planning to utilize this heat. Combining Energy Information Administration plant-level data with literature-reported process efficiency data, we develop estimates of the unconverted heat flux from individual U.S. thermal power plants in 2012. Together these power plants discharged an estimated 18.9 billion GJ(th) of residual heat in 2012, 4% of which was discharged at temperatures greater than 90 °C. We also characterize the temperature, spatial distribution, and temporal availability of this residual heat at the plant level and model the implications for the technical and economic feasibility of its end use. Increased implementation of flue gas desulfurization technologies at coal-fired facilities and the higher quality heat generated in the exhaust of natural gas fuel cycles are expected to increase the availability of residual heat generated by 10.6% in 2040.