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1.
Proc Natl Acad Sci U S A ; 118(23)2021 06 08.
Artigo em Inglês | MEDLINE | ID: mdl-34088843

RESUMO

Aqueous phosphate pollution can dramatically impact ecosystems, introducing a variety of environmental, economic, and public health problems. While novel remediation tactics based on nanoparticle binding have shown considerable promise in nutrient recovery from water, they are challenging to deploy at scale. To bridge the gap between the laboratory-scale nature of these nanostructure solutions and the practical benchmarks for deploying an environmental remediation tool, we have developed a nanocomposite material. Here, an economical, readily available, porous substrate is dip coated using scalable, water-based processes with a slurry of nanostructures. These nanomaterials have tailored affinity for specific adsorption of pollutants. Our Phosphate Elimination and Recovery Lightweight (PEARL) membrane can selectively sequester up to 99% of phosphate ions from polluted waters at environmentally relevant concentrations. Moreover, mild tuning of pH promotes at will adsorption and desorption of nutrients. This timed release allows for phosphate recovery and reuse of the PEARL membrane repeatedly for numerous cycles. We combine correlative microscopy and spectroscopy techniques to characterize the complex microstructure of the PEARL membrane and to unravel the mechanism of phosphate sorption. More broadly, through the example of phosphate pollution, this work describes a platform membrane approach based on nanostructures with specific affinity coated on a porous structure. Such a strategy can be tuned to address other environmental remediation challenges through the incorporation of other nanomaterials.


Assuntos
Recuperação e Remediação Ambiental , Membranas Artificiais , Nanocompostos/química , Fosfatos/química , Poluentes Químicos da Água/química , Poluição da Água
2.
Langmuir ; 39(21): 7514-7523, 2023 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-37196238

RESUMO

We investigate the usage of polyelectrolyte complex materials for water remediation purposes, specifically their ability to remove nanoplastics from water, on which there is currently little to no prior research. We demonstrate that oppositely charged random copolymers are effective at quantitatively removing nanoplastic contamination from aqueous solution. The mechanisms underlying this remediation ability are explored through computational simulations, with corroborating quartz crystal microbalance adsorption experiments. We find that hydrophobic nanostructures and interactions likely play an important role.

3.
Environ Sci Technol ; 57(50): 21080-21091, 2023 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-37788016

RESUMO

Developing materials that can more efficiently and cheaply capture carbon dioxide from ambient atmospheric conditions is essential for improving negative emission technologies. This study builds on the promising moisture-swing modality for direct air capture of carbon dioxide by investigating the use of several new anions─orthosilicate, borate, pyrophosphate, tripolyphosphate, and dibasic phosphate─that when introduced into ion-exchange resins allow for the cyclable capture of CO2 under dry conditions and its release under wet conditions. These ions, as well as many others that failed to show moisture-swing performance, are tested and directly compared thermodynamically and kinetically to understand their differences. This includes the use of analytical approaches new to the carbon capture field, such as the correlation of adsorption isotherms to moisture-swing performance, the use of phase lag kinetics, the examination of the humidity-carbon capture hysteresis of the sorbents, and the precise quantification of ion loading using inductively coupled plasma-optical emission spectroscopy. Phosphate dibasic was found to have the largest mass-normalized CO2 moisture-swing capacity, whereas phosphate tribasic had the best performance when factoring in kinetics, and pyrophosphate had the highest swing capacity when normalizing on a per-ion or per-unit-charge basis. This work not only sheds light on ways to improve DAC but also provides insights pertinent to the advancement of gas separation, negative emission technologies, and sorbent materials.


Assuntos
Dióxido de Carbono , Difosfatos , Dióxido de Carbono/química , Clima , Umidade
4.
J Phys Chem B ; 119(28): 8764-72, 2015 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-26090562

RESUMO

Iodide-based ionic liquids have been widely employed as iodide sources in electrolytes for applications utilizing the triiodide/iodide redox couple. While adding a low-viscosity solvent such as water to ionic liquids can greatly enhance their usefulness, mixtures of highly viscous iodide-containing ILs with water have never been studied. This paper investigates, for the first time, mixtures of water and the ionic liquid 1-butyl-3-methylimidazolium iodide ([BMIM][I]) through a combined experimental and molecular dynamics study. The density, melting point, viscosity, and conductivity of these mixtures were measured by experiment. The composition region below 50% water by mole was found to differ dramatically from the region above 50% water, with trends in density and melting point differing before and after that point. Water was found to have a profound effect on viscosity and conductivity of the IL, and the effect of hydrogen bonding was discussed. Molecular dynamics simulations representing the same mixture compositions were performed. Molecular ordering was observed, as were changes in this ordering corresponding to water content. Molecular ordering was related to the experimentally measured mixture properties, providing a possible explanation for the two distinct composition regions identified by experiment.

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