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1.
J Hazard Mater ; 469: 133612, 2024 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-38422728

RESUMO

Zeolitic imidazolate framework-8 (ZIF-8) exhibits excellent performance in capturing iodine. However, the solvent-based procedures and raw materials for ZIF-8 synthesis often lead to secondary pollution. We developed a solvent-minimizing method for preparing ZIF-8 via ball milling of raw material obtained from spent alkaline batteries, and studied its iodine-capture performance and structural changes. Exposure of the ZIF-8 to iodine vapor for 60 min demonstrated that it exhibited industrially competitive iodine-capture performance (the adsorbed amount reaches to 1123 mg g-1 within 60 min). Spectroscopic studies showed that ZIF-8 underwent a structural transformation upon iodine loading. Iodine molecules were adsorbed onto the surface of ZIF-8 and also formed C-I bond with the methyl groups on the imidazole rings, reducing iodine release. This work represents a comprehensive revelation of long-range order and short-range order evolution of ZIF-8 during iodine vapor adsorption over time. Moreover, this green synthesis of ZIF-8 is of lower cost and generates fewer harmful by-products than existing methods, and the produced ZIF-8 effectively entraps toxic iodine vapor. Thus, this synthesis enables a sustainable and circular material flow for beneficial utilization of waste materials.

2.
Front Chem ; 11: 1292979, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38124703

RESUMO

Nuclear power has emerged as a pivotal contributor to the global electricity supply owing to its high efficiency and low-carbon characteristics. However, the rapid expansion of the nuclear industry has resulted in the production of a significant amount of hazardous effluents that contain various radionuclides, such as 137Cs and 90Sr. Effectively removing 137Cs and 90Sr from radioactive effluents prior to discharge is a critical challenge. Layered metal sulfides exhibit significant potential as ion exchangers for the efficient uptake of Cs+ and Sr2+ from aqueous solutions owing to their open and exchangeable frameworks and the distinctive properties of their soft S2- ligands. This review provides a detailed account of layered metal sulfides with MaSb c- frameworks (M = Sb, In, Sn), including their synthesis methods, structural characteristics, and Cs+ and Sr2+ removal efficiencies. Furthermore, we highlight the advantages of layered metal sulfides, such as their relatively high ion exchange capacities, broad active pH ranges, and structural stability against acid and radiation, through a comparative evaluation with other conventional ion exchangers. Finally, we discuss the challenges regarding the practical application of layered metal sulfides in radionuclide scavenging.

3.
Water Res ; 245: 120628, 2023 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-37716294

RESUMO

Electrocatalytic oxidation is an appealing treatment option for emerging micropollutants in wastewater, however, the limited reactive surface area and short service lifetime of planar electrodes hinder their industrial applications. This study introduces an innovative electrochemical wastewater treatment technology that employs packed bead-electrodes (PBE) as a dynamic electrocatalytic filter on a dimensionally stable anode (DSA) acting as a current collector. By using PBE, the electroactive volume is expanded beyond the vicinity of the common planar anode to the thick porous media of PBE with a vast electrocatalytic surface area. This greatly enhances the efficiency of electrochemical degradation of micropollutants. The OV-SnO2-Sb PBE filter achieved a nearly 100 % degradation of moxifloxacin (MOX) in under 2 min of single-pass filtration, with a degradation rate over an order of magnitude higher than the conventional electrochemical oxidation processes. The generation of abundant radical species (•OH) and non-radical species (1O2 and O3), along with the enhanced direct oxidation, led to the outstanding performance of the charged PBE system in MOX degradation. The OV-SnO2-Sb PBE was remarkably stable, and the separation between the electroactive PBE layer and the base Ti anode allows for easy renewal of the bead-electrode materials and scaling up of the system for practical applications. Overall, our study presents a dynamic electroactive PBE that advances the electrocatalytic oxidation technology for effective control of emerging pollutants in the water environment. This technology has the potential to revolutionize electrochemical wastewater treatment and contribute to a more sustainable future environment.

4.
Waste Manag ; 168: 272-280, 2023 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-37329833

RESUMO

Due to ecotoxicity, zinc (Zn) as a heavy metal from electronic waste (e-waste) has been a source of pollution to soil and water for several decades. This study proposes a solution to this serious environmental problem via a self-consumed strategy to stabilize Zn in anode residues. This unique method uses cathode residues from spent zinc-manganese oxide (Zn-Mn) batteries as a stabilized matrix via thermal treatment. More specifically, the strategy incorporates zinc metal into a chemically durable matrix comprised of a lattice of AB2O4 compounds. Results demonstrate that 5-20 wt% of anode residue were fully incorporated into the cathode residue to form a Mn3-xZnxO4 solid solution after sintering at 1300 ℃ for 3 h. The lattice parameters of the Mn3-xZnxO4 solid solution reveal an approximately linear decreasing evolution with the addition of anode residue. To determine the occupancy of Zn in the crystal structure of the products, we used Raman and Rietveld refinement processes; the results reveal that Mn2+ in the 4a site was gradually replaced by Zn2+. We then used a prolonged toxicity leaching procedure to evaluate the Zn stabilization effect after phase transformation; this showed that the Zn leachability of sintered anode-doped cathode sample was over 40 folds lower than that of untreated anode residue. Therefore, this study presents an economical and effective strategy for mitigating the presence of heavy metal pollutants derived from e-waste.


Assuntos
Poluentes Ambientais , Metais Pesados , Zinco/química , Metais Pesados/química , Manganês , Poluentes Ambientais/análise , Poluentes Ambientais/química , Ácidos , Eletrodos
5.
Sci Total Environ ; 877: 162871, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-36933740

RESUMO

The disposal of wastewater sludge is one of the most challenging environmental problems for large cities. Wastewater sludge may be utilized as a feasible substitute for clay to sinter ceramics, given their similar mineralogical composition. However, the organics in sludge will be wasted, while their release during sintering will leave cracks in the ceramic products. In this research, after the thermal treatment for effective organic recovery, the thermally hydrolyzed sludge (THS) is incorporated with clay for the sintering of construction ceramics. The experimental results showed that a THS dosing ratio up to 40 % can be achieved for mixing with montmorillonite clay to make ceramic tiles. The sintered tiles (THS-40) had an intact shape and structure, and the tile performance was close to that made from single montmorillonite (THS-0), with water absorption of 0.4 % vs. 0.2 %, compressive strength of 136.8 vs. 140.7 MPa, and undetected heavy metal leaching. Further addition of THS would lead to a considerable deterioration of the quality of the tiles to a compressive strength of as low as 5.0 MPa for the THS only product (THS-100). Comparing with the tiles incorporated with raw sludge (RS-40), the THS-40 tiles had a more intact and denser structure with a 10 % improved compressive strength. Cristobalite, aluminum phosphate, mullite, and hematite dominated in the THS-born ceramics, which are typical components of ceramics, and the amount of hematite increased with the THS dosing ratio. Sintering at a high temperature of 1200 °C enabled efficient phase transformation from quartz to cristobalite and from muscovite to mullite, which ensured the toughness and compactness of the THS-born ceramic tiles.

6.
Inorg Chem ; 58(23): 15880-15888, 2019 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-31718174

RESUMO

Graphitic carbon nitride (g-C3N4)-based materials have attracted interdisciplinary attention from many fields. However, their crystal structures have not yet been described well. Poly(triazine imide)/LiCl (PTI/LiCl) of good crystallinity synthesized from salt melts enables a confident structural solution for a better understanding of g-C3N4-based materials. In this study, we synthesize PTI/LiCl of high crystallinity in air without byproducts and confirm the orthorhombic feature, which is not observed in powder X-ray diffraction (PXRD) patterns at room temperature, by employing low-temperature synchrotron PXRD. Together with spectroscopic techniques (X-ray photoelectron spectroscopy, solid-state nuclear magnetic resonance, and Fourier-transform infrared/Raman), the orthorhombic structure (space group Cmc21, No. 36) was determined and found to be a superstructure of the previously reported hexagonal structure, as confirmed by electron diffraction. The temperature-dependent synchrotron PXRD data also reveal a highly anisotropic expansion. This work also shows the much higher activity of PTI/LiCl than of g-C3N4 for the photocatalytic degradation of methyl orange under ultraviolet irradiation, especially so for PTI/LiCl with a densely packed (001) plane. This study demonstrates the structural complexity of the g-C3N4 class of materials and illustrates how their temperature-dependent anisotropies facilitate the discovery of the structural features in resolving the structure of g-C3N4-related materials and their structure-property relationship.

7.
Environ Pollut ; 249: 144-151, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30884393

RESUMO

Red mud, which is from the aluminum industry, is a potentially under-utilized resource. Technological processes for using low-cost red mud as an alternative precursor for detoxifying metal pollutants urgently need to be developed. In this study, we systematically investigated the feasibility of using red mud to detoxify metal-containing wastes (e.g., fly ash) via the formation of preferable crystalline phases. To understand the mechanism of metal detoxification by red mud, CuO, NiO, and ZnO were blended with red mud at different weight ratios and the mixtures were then subjected to ceramic-sintering. After sintering, the X-ray diffraction results revealed that all of the metals (i.e., Cu, Ni, and Zn) were able to be crystallographically incorporated into spinel lattices. Sintering the red mud at 1100 °C for 3 h effectively converted the metals into spinels. The mixing weight ratios strongly affected the efficiency of the metal incorporation. The red mud was able to incorporate 15 wt% of metal oxides. The incorporation mechanisms mainly occurred between the metal oxide(s) and hematite. Modified TCLP tests were conducted to further evaluate the metal stabilization performance of the red mud, which demonstrated the leachabilities of ZnO and the sintered red mud + ZnO product. The concentration of leached metal was substantially reduced after the incorporation process, thus demonstrating that red mud can be successfully used to detoxify metals. The results of this study reveal that waste red mud can be feasibly reused as a promising waste-to-resource strategy for stabilizing heavy metal wastes.


Assuntos
Óxido de Alumínio/química , Óxido de Magnésio/química , Metais Pesados/química , Poluentes do Solo/química , Alumínio/química , Cerâmica/química , Cinza de Carvão , Cobre/química , Poluentes Ambientais/química , Recuperação e Remediação Ambiental/métodos , Compostos Férricos , Níquel/química , Difração de Raios X , Zinco/química
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