The co-occurrence of uranyl and arsenate in contaminated water caused by natural processes and mining is a concern for impacted communities, including in Native American lands in the U.S. Southwest. We investigated the simultaneous removal of aqueous uranyl and arsenate after the reaction with limestone and precipitated hydroxyapatite (HAp, Ca10(PO4)6(OH)2). In benchtop experiments with an initial pH of 3.0 and initial concentrations of 1 mM U and As, uranyl and arsenate coprecipitated in the presence of 1 g L−1 limestone. However, related experiments initiated under circumneutral pH conditions showed that uranyl and arsenate remained soluble. Upon addition of 1 mM PO43− and 3 mM Ca2+ in solution (initial concentration of 0.05 mM U and As) resulted in the rapid removal of over 97% of U via Ca−U−P precipitation. In experiments with 2 mM PO4 3− and 10 mM Ca2+ at pH rising from 7.0 to 11.0, aqueous concentrations of As decreased (between 30 and 98%) circa pH 9. HAp precipitation in solids was confirmed by powder X-ray diffraction and scanning electron microscopy/energy dispersive X-ray. Electron microprobe analysis indicated U was coprecipitated with Ca and P, while As was mainly immobilized through HAp adsorption. The results indicate that natural materials, such as HAp and limestone, can effectively remove uranyl and arsenate mixtures.
more »
« less
Nanocrystalline iron hydroxide lignocellulose filters for arsenate remediation
Harmful levels of environmental contaminants, such as arsenic (As), persist readily in the environment, threatening safe drinking water supplies in many parts of the world. In this paper, we present a straightforward and cost-effective filtration technology for the removal of arsenate from potable water. Biocomposite filters comprised of nanocrystalline iron oxides or oxyhydroxides mineralized within lignocellulose scaffolds constitute a promising low cost, low-tech avenue for the removal of these contaminants. Two types of iron oxide mineral phases, 2-line ferrihydrite (Fh) and magnetite (Mt), were synthesized within highly porous balsa wood using an environmentally benign modification process and studied in view of their effective removal of As from contaminated water. The mineral deposition pattern, minerology, as well as crystallinity, were assessed using scanning electron microscopy, transmission electron microscopy, micro-computed X-ray tomography, confocal Raman microscopy, infrared spectroscopy, and X-ray powder diffraction. Our results indicate a preferential distribution of the Fh mineral phase within the micro-porous cell wall and radial parenchyma cells of rays, while Mt is formed primarily at the cell wall/lumen interface of vessels and fibers. Water samples of known As concentrations were subjected to composite filters in batch incubation and gravity-driven flow-through adsorption tests. Eluents were analyzed using microwave plasma optical emission spectroscopy (MPAES) and inductively coupled plasma mass spectrometry (ICP-MS). By subjecting the filters to a flow of contaminated water, the time for As uptake was reduced to minutes rather than hours, while immobilizing the same amount of As. The retention of As within the composite filter was further confirmed through energy-dispersive X-ray mappings. Apart from addressing dangerously high levels of arsenate in potable water, these versatile iron oxide lignocellulosic filters harbor tremendous potential for addressing current and emerging environmental contaminants that are known to adsorb on iron oxide mineral phases, such as phosphate, polycyclic aromatic hydrocarbons or heavy metals.
more »
« less
- Award ID(s):
- 2137663
- PAR ID:
- 10561456
- Publisher / Repository:
- Royal Society of Chemistry
- Date Published:
- Journal Name:
- RSC Sustainability
- Volume:
- 2
- Issue:
- 3
- ISSN:
- 2753-8125
- Page Range / eLocation ID:
- 626 to 634
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
The global presence of pharmaceutical pollutants in water sources represents a burgeoning public health concern. Recent studies underscore the urgency of addressing this class of emerging contaminants. In this context, our work focuses on synthesizing a composite material, FexOy/MAF-32, through a streamlined one-pot reaction process, as an adsorbent for diclofenac, an emerging environmental contaminant frequently found in freshwater environments and linked to potential toxicity towards several organisms such as fish and mussels. A thorough characterization was performed to elucidate the structural composition of the composite. The material presents magnetic properties attributed to its superparamagnetic behavior, which facilitates the recovery efficiency of the composite post-diclofenac adsorption. Our study further involves a comparative analysis between the FexOy/MAF-32 and a non-magnetic counterpart, comprised solely of 2-ethylimidazolate zinc polymer. This comparison aims to discern the relative advantages and disadvantages of incorporating magnetic iron oxide nanoparticles in the contaminant removal process facilitated by a coordination polymer. Our findings reveal that even a minimal incorporation of iron oxide nanoparticles substantially enhanced the composite’s overall performance in pollutant adsorption.more » « less
-
As plastics degrade in the environment, chemical oxidation of the plastic surface enables inorganics to adsorb and form inorganic coatings, likely through a combination of adsorption of minerals and in situ mineral formation. The presence of inorganic coatings on aged plastics has negative implications for plastics fate, hindering our ability to recycle weathered plastics and increasing the potential for plastics to adsorb contaminants. Inorganic coatings formed on terrestrially weathered polyethylene were characterized using synchrotron spectroscopy and microscopy techniques across spatial scales including optical microscopy, nano-X-ray-fluorescence mapping (nano-XRF), nano-X-ray absorption near edge structure (nano-XANES), and high-energy resolution fluorescence detected-XANES (HERFD-XANES). Results indicate a heterogeneous elemental distribution and speciation which includes inorganics common to soil terrestrial environments including iron oxides and oxyhydroxides, aluminosilicates, and carbonates.more » « less
-
Structurally stabilized composites are promising for using phase change materials in high‐temperature thermal energy storage (TES). However, conventional skeleton materials, which typically comprise 30–50 wt% of the composite, mainly provide sensible heat storage and contribute minimally to overall energy density. This study introduces a new class of redox‐active oxide‐molten salt (ROMS) composites that overcome this limitation by combining sensible, latent, and thermochemical heat storage in a single particle. Specifically, porous, redox‐active Ca2AlMnO5+δ(CAM) complex oxide particles were demonstrated as a suitable support matrix, with the pores filled by eutectic NaCl/CaCl2salt. X‐ray diffraction confirms excellent phase compatibility between CAM and the salt. Scanning electron microscopy/energy dispersive X‐ray spectroscopy and nano X‐ray tomography show good salt infiltration and wettability within the CAM pores. Thermogravimetric analysis reveals that a 60 wt% CAM/40 wt% salt composite achieves an energy density of 267 kJ kg−1over a narrow 150 °C window, with ≈50 kJ kg−1from thermochemical storage. Additionally, the composite shows higher thermal conductivity than salt alone, enabling faster energy storage and release. ROMS composites thus represent a novel and efficient solution for high‐performance TES.more » « less
-
Direct contact membrane distillation (DCMD) for desalination is attractive for high salt concentrations if low cost steam/waste heat is available and waste brine disposal cost for inland desalination is factored in. A number of innovations have taken place in DCMD in terms of the structure of the porous hydrophobic membrane. Composite membranes are of increasing interest. Composite membrane structures of great interest include a thin hydrophobic porous layer over a porous hydrophilic layer of polyvinylidene fluoride (PVDF) or a thin porous hydrophobic layer over a more conventional hydrophobic porous membrane. These membranes can be in the form of an integral composite or a stacked composite or a laminated composite. A facile method of fabricating such integral composite membranes is plasma polymerization under vacuum. A class of such membranes yielding quite high water vapor fluxes have been characterized using a variety of characterization techniques: Contact angle, liquid entry pressure (LEP), bubble-point pressure, scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), atomic force microscopy (AFM). Stacked composites of a hydrophobic ePTFE membrane over a hydrophilic PVDF membrane or a hydrophobic PVDF membrane over another hydrophobic PVDF membrane were also studied. Novel conditions created lead to very high water vapor fluxes compared to those from conventional hydrophobic membranes supported on a mesh support.more » « less
An official website of the United States government

