Water Cycle
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2026
·
IF 7.9
Yuze Li,Wei Li,Yue Yuan,Jian Zhang,Ningruo Wang,Heng Zhang,Xuejia Li,Yujia Xiang,Bo Lai,Peng Zhou,Chuanshu He,Yang Liu
The inherent inefficiency associated with the utilization of micro-concentration hydrogen peroxide (H 2 O 2 ) in conventional Fenton systems arises from the sluggish cycling between Fe(III) and Fe(II). To address this fundamental limitation, the present study demonstrates that complexes formed between Fe(III) and fulvic acid (FA) can effectively harness visible-light-driven ligand-to-metal charge transfer (LMCT). This photochemical process facilitates a synergistic dual-pathway activation of H 2 O 2 : 1) Fe(II) generated through intramolecular electron transfer reduction of the Fe(III)-FA complex directly activated H 2 O 2 ; 2) In the photoexcited *Fe(III)-FA complex, the reduction of the key intermediate *OOH lowered the activation energy barrier, facilitating the formation of ∙OH and O 2 ·- radicals. Moreover, at a stoichiometric molar ratio of H 2 O 2 to contaminant set at 1:1, contaminant removal efficiency achieves an impressive 95%. This light-enhanced mechanism establishes a new paradigm for efficient micro-concentration -level oxidation using H 2 O 2 , demonstrating exceptional effectiveness in eliminating trace pollutants.
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Fashuai Yang,Peiren Ding,Minghan Wang,Yang Liu,Xiaowen Zhang,Yulong Yuan,Yuankui Sun,Xiaohong Guan
Hierarchically porous 3D Fe 0 aerogel overcomes agglomeration and passivation of Fe 0 nanoparticles. • Aerogel achieves 9590.25 mg/g uranium capacity which is 1.5 times that of conventional Fe 0 nanoparticles. • Electric field drives dynamic Fe(II)/Fe(III) cycling on the aerogel to sustain active site regeneration for uranyl reduction. • Hierarchical pores create a localized microenvironment that enhances active site accessibility and Fe(II) retention. Electrochemical uranium extraction (EUE) is a promising strategy, yet conventional Zero-Valent Iron (Fe 0 ) nanoparticles suffer from severe agglomeration and surface passivation. Herein, we designed a hierarchically porous 3D Fe 0 aerogel that overcomes these limitations by providing an interconnected conductive network and abundant accessible active sites. At −0.2 V vs. RHE and an initial U(VI) concentration of 500 mg/L, the Fe 0 aerogel exhibited a maximum capacity of 9590.25 mg/g after 48 h electrolysis, which is approximately 1.5 times that of conventional Fe 0 nanoparticles under identical conditions. The aerogel also exhibited excellent selectivity against competing ions and good tolerance to carbonate interference. Operando Raman spectroscopy and quasi-operando XPS revealed that the external electric field drove the dynamic Fe(II)/Fe(III) redox cycle at the solid-liquid interface, which enabled the continuous in-situ regeneration of Fe(II) as the active electron-shuttling mediator for uranyl reduction. This electrochemically mediated mechanism effectively mitigates the severe surface passivation that plagues conventional iron-based electrodes. In-situ FTIR spectroscopy hinted at the formation of a distinct interfacial microenvironment within the porous architecture, potentially involving enhanced hydrogen-bonding interactions, which may further contribute to the extraction performance. Additionally, a continuous-flow reactor employing the aerogel as a flow-through cathode operated steadily in natural seawater for 10 days, achieving a stable extraction rate of 1.26 mg/g/day. This work elucidates the molecular-scale mechanisms of interfacial electroreduction, providing an innovative paradigm for the scalable mining of critical nuclear resources from real aquatic environments. Schematic illustration of efficient uranium extraction by Fe 0 aerogels via dynamic Fe(II)/Fe(III) cycling. Download: Download high-res image (410KB) Download: Download full-size image
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Desalination and Water Treatment
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2026
·
IF 1
Yuqiong Gao,Qingqing Yang,Jiaxin Ma,Juxiang Chen,Cong Li,Naiyun Gao
This study employs the Fe(III)/CaSO 3 system to degrade ibuprofen (IBP) and elucidate the key factors and mechanisms. Negligible IBP degradation is observed when CaSO 3 and Fe(III) are applied individually, but their combination significantly enhances it. At initial pH 3, 40 μΜ Fe(III), and 200 μM sulfite, 92.2 % of IBP was removed within 20 min. Quenching experiments indicated that SO 4 •– , •OH, and 1 O 2 collectively governed the degradation of IBP in the Fe(III)/CaSO 3 system. Additionally, dissolved oxygen is essential in the system by initiating the radical chain reactions. The degradation of IBP by the Fe(III)/CaSO 3 system is influenced by key operational parameters and the water matrix. Typically, the process exhibits optimal Fe(III) and sulfite concentrations and initial pH, an activation energy of 51.2 kJ·mol -1 , and is inhibited by common water constituents like humic acid (HA), Cl⁻, Br⁻ and Mg 2+ . Integrated LC/TOF/MS and DFT calculations identified hydroxylation and decarboxylation as the primary pathways for IBP degradation, with bioassays confirming decreased antibacterial activity due to toxic products. Overall, our finding indicate that the Fe(III)/CaSO 3 system is effective for the oxidation of IBP, but the process parameters need further optimization to enhance IBP degradation efficiency and reduce potential environmental risks.
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Catalysts
·
2026
·Vol. 16
·期 9
·769
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IF 4.5
Jingsi Liu,Fan Yang,He Guo
Sulfamethoxazole (SMX), a persistent sulfonamide antibiotic widespread in aquatic environments, resists conventional water treatment degradation. This work developed a NaOAc/Fe3+/O3homogeneous ozonation system for SMX abatement. Four comparative reaction groups confirmed significant synergism between trace Fe3+and sodium acetate. Under optimized near-neutral conditions, 96.19% SMX was removed within 30 min with kobs= 0.107 min−1, outperforming sole O3, O3/NaOAc and O3/Fe3+by 11.0%, 31.0% and 21.9% respectively. Single-factor tests revealed excess Fe3+or acetate suppressed catalytic activity, while alkaline conditions accelerated degradation yet aggravated iron precipitation. Radical quenching and p-CBA probing indicated that acetate coordination did not increase bulk ·OH exposure, while the stronger TEMP-derived TEMPO response after acetate addition was consistent with enhanced1O2-associated oxidation, suggesting that acetate altered the relative contributions of ozone-derived oxidation pathways. Post acetate background deduction, the ternary system achieved higher TOC/COD elimination. Twelve SMX intermediates were identified via LC-MS, with three ring-opening degradation pathways proposed. QSAR toxicity evaluation indicated that most intermediates possessed lower bioconcentration and developmental risks than raw SMX. Overall, the results indicate that weak acetate ligands can alter iron-mediated ozone oxidation pathways, providing a low-dose and economical strategy for antibiotic wastewater treatment.
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Materials Today Communications
·
2023
·
IF 3.8
Yushu Han,Rui Bao,Jianhong Yi,Hongdong Li,Liang Liu,Shuyu Huang,Zhaojie Li,Wenfu Zhang,Deqi Min
Carbonized polymer dots (CPDs) have drawn a lot of attention in the past ten years because of their excellent selectivity and sensitivity. In this study, tungsten was doped into CPDs (W-CPDs) using a simple hydrothermal technique for the first time. With an excitation/emission maximum of 365/455 nm and excitation-independent emission, W-CPDs exhibit blue fluorescence and have an average particle diameter of 2.33 nm. Because of the dynamic quenching between Fe (III) and W-CPDs, there is a good linear relationship between the Fe (III) concentration and the limit of detection (LOD) of 0.012 μM for W-CPD fluorescence intensity. The intensity of the W-CPDs fluorescence is also found to be linearly correlated with pH values between 5.0 and 10.0. This technique enables quick detection of Fe (III) in drinking water and is expected to lower the risk of Fe (III) ingestion by humans. In addition, the creation of fluorescent flexible devices and information encryption are fascinating applications for W-CPDs.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xianxian Sheng,Yulong Liu,Mudassir Habib,Shuguang Lyu
In the advanced oxidation process for the remediation of organic contaminated water and soil, sodium percarbonate (SPC) is regarded as a potential oxidant. Iron sulfide (FeS) was chosen as an activator in this work for assisting fluoranthene (FLT) removal, with Fe(III) addition overcoming the solution pH constraint on FLT removal in the SPC/FeS process. At the optimal chemical dosages, SPC/FeS (pH = 3.0) and SPC/FeS/Fe(III) (pH = 5.7) processes removed approximately 100% and 92.8% of FLT, respectively. Based on the results of scavenging trials and electron paramagnetic resonance analysis, HO• was the dominant reactive oxygen species in FLT removal by SPC/FeS and SPC/FeS/Fe(III) processes. Dissolved oxygen (DO) played a crucial role in FLT removal, and SPC/FeS/Fe(III) process was more dependent on DO than SPC/FeS process. Both processes overcame the limitation of Cl – on the application of SPC-induced oxidation process. In actual groundwater experiments, 95.5% of FLT was removed in SPC/FeS/Fe(III) process at an initial solution pH of 5.0. In soil slurry trials, 12 h was the optimal reaction time for FLT removal, and the SPC/FeS and SPC/FeS/Fe(III) processes degraded 85.6% and 86.7% of FLT, respectively. In conclusion, the FeS-activated SPC-induced oxidation process offers perspectives for PAHs contaminated field decontamination and contributes to the optimization of modern oxidation methods.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 26
·7741-7751
·
IF 4.478
Liu Yuqian,Hu Xianyun,Liang Fangyuan,Cao Yajing
Exploring sensors based on Förster resonance energy transfer (FRET) systems enables the continuous development of biological sensing technologies. Herein, we report the construction of a FRET sensor with dual-emissive quantum dots (QDs) and meso -tetra(4-sulfonatophenyl) porphine (TSPP). The sensor is composed of mesial green-emissive QDs with a thick silica shell (gQD@SiO 2 ) and circumjacent blue-emissive QDs coated with ultra-thin silica spacer, on which is linked TSPP (bQD@SiO 2 -TSPP). The gQD@SiO 2 endows the sensor with a fluorescent background. Due to the ultra-thin silica spacing, coupled with the superior resonance effect of bQD fluorescence and the Soret-band absorption of TSPP, the FRET efficiency is highly sensitive to the chelation state of TSPP. Relying on the absorbance transition of TSPP complexed with Fe(III), the FRET sensor is applied for ultra-sensitive Fe(III) detection. In aqueous solution, the sensor is demonstrated to linearly detect Fe(III) in the range of 0–1 μM, with a limit of detection (LOD) of 40 nM. More importantly, reliable Fe(III) detection can be achieved via the specific complexation of Fe(III) by TSPP and the ratiometric fluorescent response. As such, the inter-/intra-day precisions in standard samples, as well as the recovery rate in biological matrices, are fully validated. The excellent analytical performance, in combination with the excellent biocompatibility of the FRET sensor, allows semi-quantitative Fe(III) imaging in living cells. Graphical abstract
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Ling Wu,Feng Li,Haidong Yu,Luping Shen,Mingxi Wang
Spectrophotometry is an economic and rapid method for detecting oxalic acid (OA), while the reported methods have some drawbacks, such as narrow linear range, long response time, delicate operation and required expensive reagents. Herein, we found that the as-synthesized Fe(III)-sulfosalicylate (FeSSA) could be used as an efficient colorimetric chemosensor to detect OA, and the established FeSSA-based fading spectrophotometry showed prominent advantages over the existing ones in detecting OA. The as-established method has wider linear range of 0.80–160 mg/L with regression coefficient ≥ 0.999, while the widest linear range is just 2.7–54 mg/L among the reported ones. Moreover, the method has low limit of detection (0.74 mg/L), extremely fast response (several seconds), satisfactory selectivity, high accuracy and precision. Most importantly, its reliability was further verified by employing it to determine OA concentration during the degradation process of organic pollutants. The measured OA concentration at any time interval was perfectly consistent with those determined by the well-recognized high performance liquid chromatography (HPLC). These confirmed that the FeSSA-based fading spectrophotometry is an efficient, simple, fast, accurate and economic method to determine OA in a wide concentration range.
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RSC Advances
·
2022
·Vol. 12
·期 27
·17237-17248
·
IF 4.036
Dongqing Feng,Jianxin Shou,Sen Guo,Mengna Ya,Jianfa Li,Huaping Dong,Yimin Li
Activation of hydrogen peroxide (H2O2) with biochar is a sustainable and low-cost approach for advanced oxidation of organic pollutants, but faces the challenge of a low yield of hydroxyl radical (˙OH). Herein, we hypothesize that the activation efficiency of H2O2 can be enhanced through co-catalysis of trace dissolved iron (Fe) with biochar. Two biochar samples derived from different feedstock, namely LB from liquor-making residue and WB from wood sawdust, were tested in the co-catalytic systems using trace Fe(III) (0.3 mg L−1). The cumulative ˙OH production in [Fe(III) + LB]/H2O2 was measured to be 3.28 times that in LB/H2O2, while the cumulative ˙OH production in [Fe(III) + WB]/H2O2 was 11.9 times that in WB/H2O2. No extra consumption of H2O2 was observed in LB/H2O2 or WB/H2O2 after addition of trace Fe(III). Consequently, the reaction rate constants (kobs) for oxidation of pollutants (2,4-dichlorophenoxyacetic acid and sulfamethazine) were enhanced by 3.13–9.16 times. Other iron species including dissolved Fe(II) and iron minerals showed a similar effect on catalyzing 2,4-D oxidation by biochar/H2O2. The interactions involved in adsorption and reduction of Fe(III) by biochar in which the defects acted as electron donors and oxygen-containing functional groups bridged the electron transfer. The fast regeneration of Fe(II) in the co-catalytic system resulted in the sustainable ˙OH production, thus the efficient oxidation of pollutants comparable to other advanced oxidation processes was achieved by using dissolved iron at a concentration as low as the concentration that can be found in natural water.
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Analytical Methods
·
2022
·Vol. 14
·期 25
·2541-2548
·
IF 3.532
Lixia Su,Yonghuan Su,Bingqian Liu
A new ratiometric electrochemical strategy for immobilization-free detection of Escherichia coli (E. coli) was constructed by using a capture DNA-polyaniline/copper ferrite nanoparticles/graphene oxide (cDNA-PANI/CuFe2O4/GO) composite as capture probes, which has a high specific surface area and good magnetic properties. Then trigger DNA/Au nanoparticles (tDNA/Au NPs) were used as signal amplification labels, and Pt (IV) and Fe (III) were chosen as the signal probes. In the presence of targets, the sandwich format among cDNA-PANI/CuFe2O4/GO, E. coli and auxiliary DNA (aDNA) was realized by using the aptamer recognition system. Then, the tDNA/Au binding could be anchored on the sandwich format due to the principle of base complementation between unpaired aDNA and tDNA. And the unbounded tDNA of tDNA/Au NPs could bind an amount of Pt (IV). After separation using a magnet, a handful of unbound Pt (IV) which remained in the supernatant reacted with a large number of Fe (III) ions, leading to a markedly increased IFe(III)/IPt(IV) value. Oppositely, the sandwich format could not appear in the absence of targets, and even the tDNA/Au could not be immobilized on it. So, the redox reaction between a large amount of Pt (IV) residue in the supernatant and Fe (III) was significantly successful, causing a low IFe(III)/IPt(IV) value. Under optimal conditions, we found that IFe(III)/IPt(IV) was linearly related to the logarithmic E. coli concentration with a low limit of detection (1.862 × 103 cfu mL−1). This devised ratiometric electrochemical method may develop into a powerful and effective means for the detection of E. coli in real samples, which may also be developed as a universal tool for another microorganism.
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CHEMICAL GEOLOGY
·
2021
·
IF 4.015
ChunYan Luo,ShuaiLong Wen,YueHan Lu,JiaRu Dai,YingXun Du
The coprecipitation of dissolved organic matter (DOM) and phosphate with Fe(III) at the sediment-water interface plays an important role in the biogeochemical cycle of organic carbon (OC) and phosphorus (P) in aquatic ecosystems . However, studies remain limited towards understanding the strength of ternary DOM-phosphate-Fe(III) coprecipitation in sequestering OC and P. Here, we investigated the behaviors of humic acid (HA) and phosphate during their coprecipitation with Fe(III) and compared the coprecipitation behaviors with those during the adsorption process. The results showed that the coprecipitation of HA and phosphate with Fe(III) enhanced as pH decreased or initial Fe(III) concentrations increased. The presence of phosphate had a moderate inhibition effect on HA coprecipitation, leading to 3%–37% of reduction in precipitated HA. Changes in optical properties of DOM (i.e., SUVA 254 , E 2 /E 3 , and fluorescent components) showed that macromolecular, aromatic molecules preferentially coprecipitated, and this selectivity pattern was not influenced by the presence of phosphate. Compared to the adsorption of HA and phosphate to goethite , coprecipitation with Fe(III) displayed stronger binding ability, sequestering more than10 times of HA and phosphate, and was more efficient in sequestering protein-like compounds. The inhibitory effect of phosphate on HA sequestration was weaker during coprecipitation than during adsorption. Moreover, coprecipitation led to a lower degree of compositional fractionation of HA than adsorption, which may be explained by that inclusion, an important pathway for coprecipitation, has low selectivity for chemical compositions. Collectively, our results demonstrate that coprecipitation plays a crucial role in sequestering both OC and P in aquatic systems, arguing that the formation of ternary OC-Fe-P coprecipitates may be an important pathway for sequestering OC and P over a long term and reducing the internal loading of P in eutrophic lakes.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2019
·
IF 2.931
Aiwen Yu,Yiping Tang,Kai Li,Jinwei Gao,Yuhui Zheng,Zhi Zeng
Fluorescence has been well documented and the optical feature of carbon dots generates considerable interests. Here the nitrogen-doped carbon dots with a relative quantum yield of 25% have been prepared. It displays stable blue emission based on the excitation at 355 nm. The carbon nanomaterial is highly dispersible in aqueous solution and can be employed as an effective optical probe for label-free detection of Fe 3+ (0.87 μM) via a switched off change. Additionally, such sensing nanoplatform can be recovered in the presence of pyrophosphate (PPi) and an “off-on” process has been identified. It is expected that this on-off-on strategy will allow new possibilities for developing efficient sensors in industrial fields.
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