Journal of Environmental Sciences
·
2024
·
IF 5.9
Zijuan Qi,Xiaofeng Huang,Jiajun Jing,Wenya Feng,Ming Xu,Li Yan,Ming Gao,Sijin Liu,Xue-Feng Yu
Iron oxide nanoparticles (IONPs) have wide applications in the biomedical field due to their outstanding physical and chemical properties. However, the potential adverse effects and related mechanisms of IONPs in human organs, especially the lung, are still largely ignored. In this study, we found that group-modified IONPs (carboxylated, aminated and silica coated) induce slight lung cell damage (in terms of the cell cycle, reactive oxygen species (ROS) production, cell membrane integrity and DNA damage) at a sublethal dosage. However, aminated IONPs could release more iron ions in the lysosome than the other two types of IONPs, but the abnormally elevated iron ion concentration did not induce ferroptosis. Intriguingly, amino-modified IONPs aggravated the accumulation of intracellular peroxides induced by the ferroptosis activator RSL3 and thus caused ferroptosis in vitro , and the coadministration of amino-modified IONPs and RSL3 induced more severe lung injury in vivo. Therefore, our data revealed that the surface functionalization of IONPs plays an important role in determining their potential pulmonary toxicity, as surface modification influences their degradation behavior. These results provide guidance for the design of future IONPs and the corresponding safety evaluations and predictions.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Ao Ding,Yupeng He,Fei-Fei Chen,Yan Yu
Bacterial infections result in significant burdens on public health, especially with the increasing prevalence of antibiotic resistance owing to the overuse of antibiotics. The development of the next-generation nanoantibacterial materials as alternatives to antibiotics is urgently needed. Metal–organic frameworks (MOFs) have been emerging as promising antibacterial materials. However, the impact of metal centers on the properties and antibacterial activity of MOFs has not been clarified to date. In this work, five M-MOF nanomaterials (M = Fe, Co, Ni, Cu, Zn) are synthesized with 2-methylimidazole as an organic ligand. Subsequently, the minimum inhibitory concentration (MIC), minimum bactericidal concentration, and time-kill curves are studied to evaluate their antibacterial activity. In addition, the destruction of the bacterial cells after treatment with M-MOFs is observed via scanning electron microscopy. The experimental results demonstrate that the Co-MOF and Zn-MOF polyhedra exhibit optimal antibacterial activity. They can effectively inhibit the growth of both Gram-negative bacteria Escherichia coli and Gram-positive bacteria Staphylococcus aureus at a low concentration. On the other hand, the Fe-MOF irregular particles show the weakest antibacterial activity among five M-MOFs and the antibacterial activity of the Ni-MOF and Cu-MOF nanosheets are comparable to each other. The huge difference in antibacterial activity of M-MOFs is attributed to the difference in the shape and size, specific surface area, surface charge, ion release, and production of reactive oxygen species. Overall, this study clarifies the relationship between metal centers in M-MOFs and their antibacterial activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Guoyu Wei,Jiaxin Chen,Qunfeng Yue,Changhong Guo,Fengyu Qu,Huiming Lin
The pervasive presence of pathogenic bacteria in water environment poses a serious threat to public health. Here, a photocatalytic cascade was developed to reveal great water disinfection. Firstly, N -doped carbon nanosheets ( N -CNSs) about 30–50 nm in size were synthesized by a hydrothermal strategy. It revealed wide-spectrum photocatalysis for H 2 O 2 generation via a typical two-step single-electron process. A Fenton agent (Fe ion) was loaded, N -CNSs-Fe can in-situ convert photocatalytic H 2 O 2 into ·OH with high oxidation potential. Moreover, its Fenton active is three times greater than pure Fe 2+ owing to electron enrichment from N -CNSs to Fe for Fe 3+ /Fe 2+ cycle. Further investigation displayed that Fe loading also could decrease bad gap and promote charge separation to boost photocatalysis. In addition, N -CNSs-Fe possesses positive surface potential to exhibit strong interaction with negative bacteria, facilitating the capture. Therefore, the nanocomposite can effectively inactivate E. coli with a lethality rate of 99.7 % under stimulated sunlight irradiation. In addition, it also was employed to treat a complex lake water sample, revealing great antibacterial (95.1 %) and dye-decolored (92.3 %) efficiency at the same time. With novel biocompatibility and antibacterial ability, N -CNSs-Fe possessed great potential for water disinfection.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yueqian Yan,Xiaohong Zhou,Wen Jin,Xingyuan Wang,Lei Song,Ziyi Luo,Tuqiao Zhang,Miaomiao Ye
Fenton reaction is a traditional advanced oxidation process that has long been used for wastewater treatment. However, the narrow pH range of 2–4, the inefficient utilization of both H 2 O 2 and Fe 2+ , and the large amount of iron sludge formation limit its application. Here, we prepared sodium alginate composite hydrogel spheres with both Fe 2+ and CoS 2 loading (denoted as CoS 2 /Fe/SA hydrogel spheres) to construct a CoS 2 /Fe/SA + H 2 O 2 reaction system. The degradation efficiency of carbamazepine (CBZ) in the CoS 2 /Fe/SA + H 2 O 2 system was significantly enhanced with a first-order kinetic reaction constant of 0.1958 min −1 , which is 8.9 times higher than that in Fe 2+ +H 2 O 2 system. When the initial solution pH was in the range of 2–8, the removal rate of CBZ at 90 min reaction time ranged from 96.5 % to 99.9 %. The enhanced degradation efficiency even in a slightly alkaline aqueous solution was due to the sustained slow release of Fe 2+ from the CoS 2 /Fe/SA hydrogel spheres that enhances the utilization of Fe 2+ and the promotion of Fe 3+ /Fe 2+ cycling via CoS 2 . Moreover, the release amount of Fe 2+ in CoS 2 /Fe/SA hydrogel spheres could be controlled by tuning the Fe 2+ loading amount during preparation, which in turn determines its number of cycling uses.
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WATER RESEARCH
·
2024
·
IF 11.4
Kexin Yin,Xing Xu,Qinyan Yue,Yanan Shang,Yanwei Li,Yue Gao,Baoyu Gao
The limited interaction between pollutants, oxidants, and the surface catalytic sites of single atom catalysts (SACs) restricts the water decontamination effectiveness. Confining catalytic sites within porous structures enables the localized enrichment of reactants for optimized reaction kinetics, while the specific regulatory mechanisms remain unclear. Herein, SACs with porous modification significantly improves the utilization of peroxymonosulfate (PMS) and pollutant degradation activity. Confining catalytic sites in porous structure effectively reduces the mass transfer distance between radicals (SO 4 •- and •OH) and pollutants, thereby improving reaction performance. Pore modulation changes the surface electronic structure, leading to a significant improvement in the electron migration process. The system shows significant potential in effectively oxidizing various common emerging pollutants, and exhibits robust resistance to interference from environmental matrices. Moreover, a quantitative evaluation using life cycle assessment (LCA) indicates that the pFe-SAC/PMS system showcases superior environmental importance and practicality.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Haozheng Hu,Xianghao Meng,Yin Li,Yusong Yang,Yanqiu Xu,Junxian Hu,Yaochun Yao
In the era of extensive deployment of LiFePO4 batteries in energy storage and electric vehicle domains, the recycling of lithium from spent LiFePO4 (SLFP) batteries has emerged as a focus, which helps in alleviating environmental pollution and resource shortages. Traditional recycling techniques, encompassing pyrometallurgical and hydrometallurgical methods, are often marred by low selectivity and extraction efficiency. Herein, an eco-friendly and low-consumption recycling strategy involving potassium pyrosulfate (K2S2O7)-assisted low-temperature roasting and subsequent water leaching has been developed for selectively recycling Fe and Li from SLFP batteries. The proposed strategy, compared to the conventional inorganic acid leaching method, mitigates the environmental hazards caused by acidic wastewater generation and reduces the costs associated with wastewater treatment. Investigations of thermal performance characterization and thermodynamic calculation analyses have revealed that K2S2O7 plays a pivotal role in extracting lithium from the Fe–P–O framework, converting lithium into a soluble sulfate variant and iron into insoluble compounds. This process culminates in the segregation of a lithium-rich leachate and an iron-enriched residue, which are further processed to synthesize Li2CO3 and FePO4. The effects on Li leaching of the mass ratio of K2S2O7 to SLFP, roasting time, roasting temperature, and water leaching time are systematically studied and 95.87% Li was leached in water under optimal conditions. In addition, the feasibility of the strategy was further illustrated by the regeneration of LiFePO4 produced by the recycled Li2CO3 and FePO4. Overall, this recovery strategy stands out for its effective lithium-iron segregation, environmental sustainability, and economic viability, which provide some inspiration for high-efficiency and environmentally friendly recovery metal from spent lithium-ion batteries.
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Molecular Catalysis
·
2024
·
IF 3.9
Zheng Zhou,Meng Miao,Wenzhi Li,Jingting Jin,Liqun Wang,Lulu Zhang,Liang Yuan
The selective conversion of methane is a significant but difficult challenge. We reported a CuFe bimetallic catalyst supported by g-C 3 N 4 for the catalytic oxidation of methane to oxygenated C1 products. Using H 2 O 2 as the oxidant, Cu 0.4 Fe 0.3 -C 3 N 4 catalyst had a C1 yield of 8231 μmol·g cat −1 · h −1 at 70 °C, and 1 H NMR results showed that almost all of the liquid phase products were target C1 products. The methanol selectivity on CuFe-C 3 N 4 was 44.5 %, comparing with 20.2 % methanol selectivity on Cu-C 3 N 4 . The formation of a Cu-O-Fe site on the CuFe-C 3 N 4 was confirmed by in situ DRIFTS and 57 Fe Mössbauer spectroscopy. This Cu-O-Fe site was responsible for the improved catalyst performance. DFT calculations illustrated that at the Cu-O-Fe site, H 2 O 2 dissociated into two ·OH radicals instead of ·H and ·OOH radicals as it did at the Cu-O-Cu site. The ·OH radicals combined with the ·CH 3 radicals from the CH 4 molecules to form methanol. These findings provided valuable insights into the rational design of active sites on carbon nitride materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Anli Liu,Zhixue Zhang,Zhikui Zhou,Chengwan Wang,Yue Yuan,Qinmei Zhong,Sheng-Tao Yang
As commonly observed water pollutants, organophosphates (OPs) can induce eutrophication of water bodies and pose serious risks to the environment and human health. In this study, we investigated the degradation of tetramethylphosphonate (THPS), an OP, using micron-scale iron-copper (Fe/Cu) bimetals activated peracetic acid (PAA) system. Interestingly, the iron groups (i.e., Fe, Fe/Cu and Fe-PAA system) exhibited a biphasic response: an initial rapid response within the first 10 min followed by a slower degradation lasting from 10 to 60 min. However, the copper groups (i.e., Cu, Cu-PAA and Fe/Cu-PAA) exhibited an initial response within the first 10 min coupled with a subsequent plateau with no significant alterations thereafter. In terms of reactive oxidized species (ROS) verification, only hydroxyl radical ( • OH) was detected in the Fe and Fe-PAA systems; only singlet oxygen ( 1 O 2 ) was detected in the Cu system; organic radicals (R-O • ) and 1 O 2 were detected in the Cu-PAA and Fe/Cu-PAA systems respectively; while • OH, R-O • and 1 O 2 were all detected in the Fe/Cu-PAA system. The presence of Cu promoted the release of electrons from iron and strengthened the single-electron transfer mode. Notably, after five consecutive runs, the removal efficiency of THPS remained above 80 %, and the k obs during the first ten minutes (11.28, 10.11, 9.12, 8.29, and 8.45 min −1 ) remained high and stable throughout the cycles. XPS spectra analysis demonstrated that for 5 cycles, the surface content of Fe 0 /Fe 2+ and Cu 0 /Cu + in the utilized materials surpassed that of the pristine Fe/Cu bimetals, indicating the self-renewal of Fe/Cu bimetals. These findings highlight the potential of Fe/Cu bimetals in effectively degrading THPS and reducing its environmental impact.
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Water
·
2024
·Vol. 16
·期 13
·1822
·
IF 3
Dongyuan Zhang,Lin Shi,Edwin Hena Dawolo,Bingfa Chen,Ning Ding,Hong Liu
In this study, magnetic (Fe)-loaded biochar was successfully prepared by a simple impregnation pyrolysis method. Meanwhile, its degradation capability and mechanism for typical antibiotic metronidazole (MNZ) were systematically investigated under different conditions. The characterization of the synthesized material showed that the specific surface area, pore diameter, and pore volume changed significantly. Also, functional groups and metal element Fe were introduced on the surface of the biochar, leading to its better capability to activate peroxymonosulfate (PMS). The degradation experiments showed that the removal of MNZ in the Fe-BC/PMS system can reach up to 95.3% in 60 min under optimal conditions. Free-radical capture experiments showed that there were several active species of •OH, SO4•−, •O2−, and1O2present in the catalyst to synergistically degrade MNZ, among which SO4•−played a major role; it was also found that the material can be easily recycled and was still effective after several uses. Further, the main degradation pathways of MNZ include nitrohydroxylation, hydroxyethyl functional group deletion, carboxylation of the amino functional group of •OH, demethylation, oxidation, and carboxylation. It is obvious that the synthesized magnetic-loaded biochar, Fe-BC, generated from waste rape straw crops, shows high catalytic performance in pollutant degradation, providing an insight into the recycling potential of waste biomass in the catalytic field for pollutant removal.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yourong Wu,Wanqian Cai,Shiqi Zhong,Cong Lin,Mei Lin,Tengfei Lin,Min Gao,Chunlin Zhao,Xiao Wu
Conventional nanomaterials are met with the bottleneck problem of difficult recycling and reuse when applied to water treatment. Carbon aerogel with three-dimensional structure can effectively solve the problem of recycling, however, the preparation of efficient and recyclable aerogel catalyst is still an urgent technical problem. Here, an NH 2 -MIL-88B(Fe)/agarose carbon aerogel (MGA-x) was synthesized at different calcination temperatures (x = 100, 150, 200 and 300 °C) and their changes in structures and photo-electrochemical properties were investigated. As a photo-Fenton catalyst, the aerogel could efficiently activate H 2 O 2 to ultrafast degrade mitoxantrone in water. Within 2 min, the removal efficiency of mitoxantrone in the MGA-200/H 2 O 2 /Light system was 97.6%, which was 85.3 times greater than that in the agarose aerogel/H 2 O 2 /Light system. Notably, the aerogel catalyst could be directly recovered and recycled without additional treatments, and the microstructure and degradation performance were maintained even after five cycles, demonstrating excellent sustainability for applications in practical aquatic environment. The primary active radicals involved in the photocatalytic degradation process were • OH, h + and • O 2 - , which were confirmed through free radical quenching experiments and electron paramagnetic resonance analysis. Additionally, possible degradation pathways for mitoxantrone were proposed based on the results of liquid chromatography-mass spectrometry. This study presents a photocatalytic aerogel with highly efficient degradation ability along with recycling and reuse capacity, exhibiting great potential for application in the remediation of water pollution.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 3
·1-10
·
IF 5.3
Han Hongyu,Huang Yiqun,Miao Junjian,Lai Keqiang
Surface-enhanced Raman spectroscopy (SERS) was combined with stoichiometric analysis to synthesize a AuNPs@MIL-100 (Fe) SERS substrate. This high-performance, and low-cost metal–organic framework-based SERS nano sensor is capable of detecting malachite green (MG) residues in fish. The minimum detectable concentration of MG in standard solutions is 0.1 μg/L, while in fish samples, the detection range spanned from 0.003–0.088 μg/kg. The partial least squares regression (PLSR) and support vector machine regression (SVR) were applied to model the SERS data, enhancing both the precision and reliability of the detection. The results show that compared with the traditional linear regression and PLSR models, the prediction accuracy of the SVR model is an improvement with higher stability. MG standard solutions and three fish samples can be analysed directly or after simple extraction. This method can be used to detect trace harmful substances in different aquatic products. Graphical
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MINERALS ENGINEERING
·
2024
·
IF 4.9
Qinbo Cao,Yan Yan,Heng Zou,Haiyu Zhang,Dianwen Liu,Shuming Wen,Yanjun Li
The separation of galena (PbS) from chalcopyrite (CuFeS 2 ) requires strong oxidants for the depression of PbS, due to the excellent hydrophobicity of PbS. In this work, an advanced oxidation process, i.e., S 2 O 8 2− /Fe 2+ treatment, was employed to selectively depress PbS. The parameters of the S 2 O 8 2− /Fe 2+ process were determined via flotation tests as follows: pH 3, 1:1 S 2 O 8 2− : Fe 2+ molar ratio, and 10 min reaction time. The S 2 O 8 2− /Fe 2+ treatment selectivity decreased the hydrophobicity of the PbS surface. UV–vis spectroscopy results revealed that SO 4 − (major species) and OH radicals were produced in solution by the activation of Fe 2+ . The SO 4 − / OH radicals reacted with the PbS surface, generating the SO 4 2− and PbSO 4 species. These species coated the PbS surface, forming a hydrophilic PbS surface and inhibiting the PbS flotation. By contrast, the S 2 O 8 2− /Fe 2+ treatment generated only a minimal amount of SO 4 2− (5.98 % of the total S species) on the CuFeS 2 surface. Therefore, the CuFeS 2 surface was hydrophobic and CuFeS 2 particles could still be floated into the foam phase. This study provides a promising method for the selective depression of PbS in the PbS-CuFeS 2 mixture.
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