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1.
Science ; 384(6693): 333-338, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38669571

RESUMO

Thin-film composite reverse osmosis membranes have remained the gold standard technology for desalination and water purification for nearly half a century. Polyamide films offer excellent water permeability and salt rejection but also suffer from poor chlorine resistance, high fouling propensity, and low boron rejection. We addressed these issues by molecularly designing a polyester thin-film composite reverse osmosis membrane using co-solvent-assisted interfacial polymerization to react 3,5-dihydroxy-4-methylbenzoic acid with trimesoyl chloride. This polyester membrane exhibits substantial water permeability, high rejection for sodium chloride and boron, and complete resistance toward chlorine. The ultrasmooth, low-energy surface of the membrane also prevents fouling and mineral scaling compared with polyamide membranes. These membranes could increasingly challenge polyamide membranes by further optimizing water-salt selectivity, offering a path to considerably reducing pretreatment steps in desalination.

2.
Environ Sci Technol ; 57(15): 6331-6341, 2023 04 18.
Artigo em Inglês | MEDLINE | ID: mdl-37023347

RESUMO

Separation of specific ions from water could enable recovery and reuse of essential metals and nutrients, but established membrane technologies lack the high-precision selectivity needed to facilitate a circular resource economy. In this work, we investigate whether the cation/cation selectivity of a composite cation-exchange membrane (CEM), or a thin polymer selective layer on top of a CEM, may be limited by the mass transfer resistance of the underlying CEM. In our analysis, we utilize a layer-by-layer technique to modify CEMs with a thin polymer selective layer (∼50 nm) that has previously shown high selectivity toward copper over similarly sized metals. While these composite membranes have a CuCl2/MgCl2 selectivity up to 33 times larger than unmodified CEMs in diffusion dialysis, our estimates suggest that eliminating resistance from the underlying CEM could further increase selectivity twofold. In contrast, the CEM base layer has a smaller effect on the selectivity of these composite membranes in electrodialysis, although these effects could become more pronounced for ultrathin or highly conductive selective layers. Our results highlight that base layer resistance prevents selectivity factors from being comparable across diffusion dialysis and electrodialysis, and CEMs with low resistance are necessary for providing highly precise separations with composite CEMs.


Assuntos
Polímeros , Água , Cobre , Cátions
3.
Sci Adv ; 8(9): eabm9436, 2022 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-35245114

RESUMO

State-of-the-art polymeric membranes are unable to perform the high-precision ion separations needed for technologies essential to a circular economy and clean energy future. Coordinative interactions are a mechanism to increase sorption of a target species into a membrane, but the effects of these interactions on membrane permeability and selectivity are poorly understood. We use a multilayered polymer membrane to assess how ion-membrane binding energies affect membrane permeability of similarly sized cations: Cu2+, Ni2+, Zn2+, Co2+, and Mg2+. We report that metals with higher binding energy to iminodiacetate groups of the polymer more selectively permeate through the membrane in multisalt solutions than single-salt solutions. In contrast, weaker binding species are precluded from diffusing into the polymer membrane, which leads to passage proportional to binding energy and independent of membrane thickness. Our findings demonstrate that selectivity of polymeric membranes can markedly increase by tailoring ion-membrane binding energy and minimizing membrane thickness.

4.
Environ Sci Technol ; 56(6): 3313-3323, 2022 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-35235312

RESUMO

Despite decades of dominance in separation technology, progress in the design and development of high-performance polymer-based membranes has been incremental. Recent advances in materials science and chemical synthesis provide opportunities for molecular-level design of next-generation membrane materials. Such designs necessitate a fundamental understanding of transport and separation mechanisms at the molecular scale. Molecular simulations are important tools that could lead to the development of fundamental structure-property-performance relationships for advancing membrane design. In this Perspective, we assess the application and capability of molecular simulations to understand the mechanisms of ion and water transport across polymeric membranes. Additionally, we discuss the reliability of molecular models in mimicking the structure and chemistry of nanochannels and transport pathways in polymeric membranes. We conclude by providing research directions for resolving key knowledge gaps related to transport phenomena in polymeric membranes and for the construction of structure-property-performance relationships for the design of next-generation membranes.


Assuntos
Membranas Artificiais , Polímeros , Osmose , Reprodutibilidade dos Testes
5.
Adv Mater ; 33(38): e2101312, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34396602

RESUMO

Synthetic polymer membranes are enabling components in key technologies at the water-energy nexus, including desalination and energy conversion, because of their high water/salt selectivity or ionic conductivity. However, many applications at the water-energy nexus require ion selectivity, or separation of specific ionic species from other similar species. Here, the ion selectivity of conventional polymeric membrane materials is assessed and recent progress in enhancing selective transport via tailored free volume elements and ion-membrane interactions is described. In view of the limitations of polymeric membranes, three material classes-porous crystalline materials, 2D materials, and discrete biomimetic channels-are highlighted as possible candidates for ion-selective membranes owing to their molecular-level control over physical and chemical properties. Lastly, research directions and critical challenges for developing bioinspired membranes with molecular recognition are provided.

6.
Nat Nanotechnol ; 15(6): 426-436, 2020 06.
Artigo em Inglês | MEDLINE | ID: mdl-32533116

RESUMO

Synthetic membranes with pores at the subnanometre scale are at the core of processes for separating solutes from water, such as water purification and desalination. While these membrane processes have achieved substantial industrial success, the capability of state-of-the-art membranes to selectively separate a single solute from a mixture of solutes is limited. Such high-precision separation would enable fit-for-purpose treatment, improving the sustainability of current water-treatment processes and opening doors for new applications of membrane technologies. Herein, we introduce the challenges of state-of-the-art membranes with subnanometre pores to achieve high selectivity between solutes. We then analyse experimental and theoretical literature to discuss the molecular-level mechanisms that contribute to energy barriers for solute transport through subnanometre pores. We conclude by providing principles and guidelines for designing next-generation single-species selective membranes that are inspired by ion-selective biological channels.

8.
Environ Sci Technol ; 53(8): 4355-4363, 2019 04 16.
Artigo em Inglês | MEDLINE | ID: mdl-30917279

RESUMO

Access to continuous water supply is key for improving health and economic outcomes in rural areas of low- and middle-income countries, but the factors associated with continuous water access in these areas have not been well-characterized. We surveyed 4786 households for evidence of technical, financial, institutional, social, and environmental predictors of rural water service continuity (WSC), defined as the percentage of the year that water is available from a source. Multiple imputed fractional logistic regression models that account for the survey design were used to assess operational risks to WSC for piped supply, tube wells, boreholes, springs, dug wells, and surface water for the rural populations of Bangladesh, Pakistan, Ethiopia, and Mozambique. Multivariable regressions indicate that households using multiple water sources were associated with lower WSC in Bangladesh, Pakistan, and Mozambique. However, the possibility must be considered that households may use more than one water source because services are intermittent. Water scarcity and drought were largely unassociated with WSC, suggesting that service interruptions may not be primarily due to physical water resource constraints. Consistent findings across countries may have broader relevance for meeting established targets for service availability as well as human health.


Assuntos
População Rural , Água , Bangladesh , Etiópia , Humanos , Moçambique , Paquistão , Abastecimento de Água
9.
Nat Nanotechnol ; 14(2): 191, 2019 02.
Artigo em Inglês | MEDLINE | ID: mdl-30675037

RESUMO

In the version of the Supplementary Information file originally published with this Article, the images used for Supplementary Fig. 4 were incorrect and have now been replaced. This does not affect the results of the Article.

10.
Ecol Eng ; 140: 1-105589, 2019 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-32020990

RESUMO

One of the primary functions of green roofs in urban areas is to moderate rainwater runoff, and one of the major impediments to the survival of plants on an extensive green roof (EGR) is a lack of available water during dry periods. Runoff moderation and water storage are both influenced by the composition of the growing media. Here we present a framework for evaluating the hydrologic performance of EGR growing media and also provide hydrologic attribute data for several commonly used EGR media constituents. In this three-phase study, we: 1) measured hydrologic attributes of individual EGR media constituents, 2) predicted attributes of media mixtures using individual constituent data, and 3) tested the seven top-ranking mixtures to evaluate hydrologic performance. Hydrologic attributes included wet weight and water held at maximum retentive capacity, long-term water retention, and hydraulic conductivity. Because perlite was light in weight yet held the greatest amount of water both at its maximum retentive capacity and in the long term, media mixtures dominated by perlite were predicted to have the best overall hydrologic performance. Mixtures dominated by pumice were also predicted to perform relatively well but were heavier. Despite the slightly greater weight and slightly lower performance, pumice may be a preferred alternative to perlite because perlite is a processed constituent with greater estimated embodied energy. Results indicate that performance of mixtures can be adequately predicted using performance of individual constituents for wet weight, water held, and long-term water retention. Hydraulic conductivity was less predictable because the pore volume in mixtures can be unrelated to the pore volume of the individual constituents. The framework presented here can be used to evaluate the performance of other EGR media, and the media attribute data can be used in formulating EGR media mixtures for specific applications. In addition, the attribute data can serve as a benchmark for evaluating other EGR media. Our results underscore the need for standardization of methods for more effective comparisons of EGR substrates, and also reinforce the need to evaluate EGR components using real-world scenarios.

11.
Nat Nanotechnol ; 14(1): 64-71, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30478276

RESUMO

Current technologies for water purification are limited by their contaminant-specific removal capability, requiring multiple processes to meet water quality objectives. Here we show an innovative biomimetic micellar nanocoagulant that imitates the structure of Actinia, a marine predator that uses its tentacles to ensnare food, for the removal of an array of water contaminants with a single treatment step. The Actinia-like micellar nanocoagulant has a core-shell structure and readily disperses in water while maintaining a high stability against aggregation. To achieve effective coagulation, the nanocoagulant everts its configuration, similar to Actinia. The shell hydrolyses into 'flocs' and destabilizes and enmeshes colloidal particles while the core is exposed to water, like the extended tentacles of Actinia, and adsorbs the dissolved contaminants. The technology, with its ability to remove a broad spectrum of contaminants and produce high-quality water, has the potential to be a cost-effective replacement for current water treatment processes.

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