INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Mengqian Yuan,Fan Tian,Guangfang Li,Huiping Zhao,Yunling Liu,Rong Chen
In this work, hierarchical nanostructures Fe(III)-modified BiOBr were successfully prepared via a facile one-step route at room temperature. Compared with pure BiOBr, Fe(III)-modified BiOBr samples possess enhanced photocatalytic abilities for benzyl alcohol oxidation and organic dye degradation in the presence of H2O2 upon light illumination. The improved photocatalytic oxidation and degradation ability of Fe(III)-modified BiOBr is ascribed to the enhanced photogenerated carriers separation efficiency and promoted production of ·OH due to the generation of Fe2+ ions via interfacial charge transfer from Fe3+ ions. This work provides a facial approach to improve photocatalytic efficiency for organic synthesis and environmental remediation.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Yulu Xu,Yu Mei,Yanjun Li,Chenye Fu,Yuantai Li,Yuheng Zhong,Junxi Song,Gang Yang,Shihuai Deng,Xiaohui Lu,Jiali Peng,Bo Lai
The iron-activated periodate (PI) process may be limited by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. Herein, tungsten boride (WB), serving as a co-catalyst, can effectively overcome the inherent drawback of oxidation reactions. The WB/Fe(III)/PI system exhibited different removal efficiencies toward sulfisoxazole (SIZ) under varying PI concentrations. Based on the qualitative and semiquantitative tests, the generation of reactive species changes with various PI concentrations. Specifically, at low PI concentration, Fe(IV), generated via Fe(II)-mediated PI activation following WB-driven Fe(III) reduction, was the primary reactive species responsible for rapid SIZ removal. However, at high PI concentrations, the limited generation of Fe(IV) contributes only marginally to SIZ removal. In situ Raman characterization and electrochemical tests revealed that at high PI concentration, WB could react with PI and Fe(III) to form high-potential metastable intermediates (WB-Fe(III)-PI*), facilitating direct electron transfer pathway (ETP) from the SIZ to PI. Density functional theory (DFT) calculations further confirmed the interactions among WB, Fe(III), and PI. Besides, at low PI concentrations, the WB/Fe(III)/PI system selectively and rapidly oxidized oxygen-transfer-prone pollutants, while at high PI concentrations, it favored sustained oxidation of electron-rich pollutants. Additionally, WB exhibits excellent reusability during cyclic use. This comprehensive investigation deepens insight into PI-based co-catalytic process and offers an efficient strategy for selecting appropriate oxidant concentrations for wastewater treatment.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jiahang Liu,Yingying Chu,Xiaoyang Li,Mengying Qian,Weiming Zhang
The co-catalytic effect of hydroquinone/quinone electron shuttle has received great attention in the area of Fenton-like reaction. However, the crucial roles of phenolic or hydroquinone moieties in the chemical structures of organic pollutants have always been overlooked. In this study, we discovered that the introduction of rifampicin (RIF), a representative of rifamycin antibiotics, could trigger complete degradation of atrazine (ATZ) in the Fe(III)/H 2 O 2 system. By exploring the influences of initial Fe(III), H 2 O 2 , RIF concentrations and pH values on ATZ degradation efficiency, key components affecting metal ion valence transitions in the system were identified. Quenching experiments, probe tests and EPR analysis verified that •OH served as the primary active species, while HO 2 •/O 2 •− was also generated. Through monitoring Fe(II) concentration variations and employing mass spectrometric analyses, the oxidation pathway of RIF was elucidated: When mixed with Fe(III), the naphthohydroquinone moiety of RIF immediately acted as a direct electron donor to reduce Fe(III) to Fe(II), while itself being oxidized to RIF-Q. Upon H 2 O 2 addition, it rapidly triggered the classical Fenton reaction with Fe(II) to generate •OH, enabling ATZ degradation. Simultaneously, RIF-Q underwent further oxidative breakdown, with some degradation products retaining the capacity to continuously donate electrons to Fe(III), thereby promoting its reduction. This study provides new insights for the co-catalytic effect of pollutant-derived electron shuttles on the transition of metal ion valences.
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RENEWABLE ENERGY
·
2024
·
IF 9
Yuming Huang,Wei Zhou,Liang Xie,Junfeng Li,Xiaoxiao Meng,Xuewei Zhang,Yang Yu,Miaoting Sun,Jiaxiang Chen,Lijie Wang,Jihui Gao,Guangbo Zhao
Integrating the hydrogen evolution reaction (HER) with the carbon oxidation reaction (COR) is a promising method for producing H₂ with lower energy consumption. However, due to the passivation effect of oxygen functional groups (OFGs) for COR and Fe³⁺, achieving efficient and sustainable carbon oxidation to assist water electrolysis for hydrogen production remains a challenge over the past decades. This study introduced [EDTA·Fe(III)] – as a mediator to promote COR. [EDTA·Fe(III)] – effectively prevented the oxidation layer on the carbon surface from anchoring Fe (III) and reactivated the carbon that had been passivated by the oxidation layer. Density functional theory calculations indicated that the notable COR activity resulted from [EDTA·Fe(III)] – effectively lowering the vertical ionization potential of carbon, without being affected by OFGs. Notably, in the HER||COR-[EDTA·Fe(III)] – system, a cell voltage of merely 0.74 V is sufficient to reach a current density of 10 mA cm −2 , with the corresponding energy consumption being 1.76 kWh Nm −3 (H 2 ). This strategy offers new insights into achieving stable, low-energy hydrogen production via water electrolysis.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Zhihao Shen,Shuming Wen,Yongchao Miao,Han Wang,Qicheng Feng
Unavoidable metal ions commonly exist in the pulp during flotation. These ions can affect the floatability of minerals, and they can also result in the differences in the surface features between different minerals. In this study, how Fe 3+ affected the flotation behavior of cerussite was investigated by micro-flotation tests. The corresponding adsorption characteristics of the sulfidizing agent and collector on the surfaces of cerussite were investigated by surface-analysis techniques. The results of micro-flotation tests showed that the floatability of cerussite significantly decreased when Fe 3+ was added before Na 2 S and xanthate. The flotation recovery of cerussite decreased compared with that obtained without participation of Fe 3+ . Additionally, the results of xanthate and Na 2 S adsorption tests, X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectrometry (ToF-SIMS) and zeta potential measurements verified that Fe 3+ and its hydrophilic hydroxyl derivatives (Fe-OH compounds) resulted in reduced amounts and reactive activities of S-bearing species adsorbed on the surfaces of cerussite. This decreased the adsorption capacity of subsequently added xanthate, resulting in the difficulty in effectively recovering cerussite in the sulfidization-xanthate system.
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RSC Advances
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2017
·Vol. 7
·期 65
·40952-40956
·
IF 3.108
Chunlin Tan,Xiuya Su,Chao Zhou,Baoju Wang,Qiuqiang Zhan,Sailing He
Red-emitting carbon dots (C-dots) were synthesized from p-phenylenediamine (p-PD) aqueous solution with nitric acid (HNO3) assistance by hydrothermal reaction at 200 °C for 2 h. p-PD aqueous solution can be transferred to C-dots (or poly(p-PD)) with (or without) the addition of acid. Different acid systems, such as HNO3, H3PO4 and HF, can directly synthesize red-emitting C-dots, and the fluorescence can be enhanced by increasing the strength of acids. N-CDs, 3.46 nm-average-sized C-dots, prepared in dilute HNO3, have a quantum yield of 15.8% with unique, excitation-wavelength independent emission in the red region (600 and 680 nm) and a broad visible excitation band. Carboxyl, ester and hydroxyl groups on the C-dots surface directly lead to red emission. N-CDs have a certain selective specificity for Fe3+ detection and the linear range is 10–300 nmol L−1 with a limit of determination of 1.9 nmol L−1.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Yao Huang,Shufeng Zhao,Hui Liu,Rong Chen,Lei Zhao,Shan Liu
Abiotic Fe (II) oxidation widely occurs in the natural subsurface environment and engineered dynamic processes, which possibly impacts the growth of indigenous microbes. As previously discovered, the oxidation of aqueous Fe 2+ at neutral pH effectively inactivates iron-reducing bacteria Shewanella oneidensis strain MR-1 (MR-1). Herein, the impacts of co-existing iron mineral on the oxidation of aqueous Fe 2+ and the subsequent disinfection activity on MR-1 were investigated with siderite selected as a representative iron mineral in the subsurface environment. The oxidation rate of aqueous Fe 2+ and the amount of generated OH radical increased as the content of siderite increased, while the MR-1 inactivation was alleviated. An initial concentration of 2.0 × 10 6 CFU/mL MR-1 was inactivated by about 2.7 orders of magnitude during oxidation of 0.2 mM FeSO 4 alone for 30 min, which was reduced to only about 0.6 orders of magnitude in the presence of 4.3 mM co-existing siderite. ROS scavenging results confirmed that the OH radical generated in the bulk solution was not the leading role for the inactivation of MR-1. Morphological changes of the cells observed by SEM demonstrated that the disruption of the cell membrane was alleviated by siderite, which was further supported by the XRD and FTIR spectra. The underlying mechanism was proposed to be the reduced contact time of Fe 2+ and MR-1 cells due to the accelerated oxidation. This work provides new insights into the disinfection behavior of heterogeneous Fe (II) oxidation on iron cycling bacterial in the natural environment.
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CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Hang Cui,Xiaogang Gu,Shuguang Lu,Xiaori Fu,Xiang Zhang,George Y. Fu,Zhaofu Qiu,Qian Sui
Ethylbenzene (EB) degradation performance in (S,S)-ethylenediamine-N,N-disuccinic acid (EDDS) chelated Fe(III) activated sodium percarbonate (SPC) system was investigated in this study. The effects of various factors, such as the dosages of SPC and Fe(III), molar ratio of EDDS/Fe(III), anions (Cl − , HCO 3 − , SO 4 2− , and NO 3 − ) concentration, natural organic matters (NOM), and initial solution pH were evaluated. The results showed that the addition of EDDS remarkably improved the EB removal in Fe(III)/SPC system. Both HCO 3 − anions and NOM had significantly inhibitive effect, while the influence of SO 4 2− , Cl − and NO 3 − could be negligible on EB degradation. The EB removal was inhibited at extremely low and high initial solution pH. Moreover, the results of free radical probe tests, scavenger tests and electron paramagnetic resonance (EPR) detection indicated that OH was the predominant species responsible for EB degradation even though both OH and O 2 − were generated in the SPC/EDDS–Fe(III) system. The oxidation products were analyzed and possible EB degradation pathways were proposed. In conclusion, this study provides an important insight into the application of SPC/EDDS–Fe(III) system in the removal of EB contaminant, especially for in situ remediation of BTEX-contaminated groundwater.
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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Qiang Zhao,Dandan Li,Guofeng Gao,Wen Yuan,Genyan Hao,Jinping Li
We describe the preparation of three partially ordered iron-based catalyst films (Fe-OAc, Fe-Pro, Fe-But) with nanoporous structure by electrodeposition from organate electrolytes containing Fe 2+ . The anions of the organic acids assisted the partial ordering of the nanostructured Fe(III) catalysts for water oxidation. A model involving an electrical double layer is invoked to explain the role of the organate electrolyte system in their formation. Analytical results have revealed the main component of the iron-based films to be a β-FeOOH structure. The Fe-But catalyst catalyzed water oxidation in 0.1 m potassium carbonate solution with an average activity of 1.48 mA cm −2 and an overpotential of 433 mV.
研究领域:
无机化学
·
材料科学
·
电化学
·
催化化学
·
能源材料
·
纳米科技
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Analytical Methods
·
2023
·Vol. 15
·期 19
·2334-2342
·
IF 3.1
Qian Li,Jing Yang,Wenzhan Yu,Liqiong He,Renlong Zhou,Changming Nie,Lifu Liao,Xilin Xiao
Monocrotophos (MP), an organophosphorus pesticide, poses a serious threat to human health, so a rapid and simple technique is needed to detect it. In this study, two novel optical sensors for MP detection were created using the Fe(III) Salophen complex and Eu(III) Salophen complex, respectively. One sensor is an Fe(III) Salophen complex (I-N-Sal), which can bind MP selectively and form a supramolecule, resulting in a strong resonance light scattering (RLS) signal at 300 nm. Under the optimum conditions, the detection limit was 30 nM, the linear range was 0.1–1.1 μM, the correlation coefficient R2 = 0.9919, and the recovery rate range was 97.0–103.1%. Interaction properties between the sensor I-N-Sal and MP and the RLS mechanism were investigated using density functional theory (DFT). And another sensor is based on the Eu(III) Salophen complex and 5-aminofluorescein derivatives. The Eu(III) Salophen complex was immobilized on the surface of amino-silica gel (Sigel-NH2) particles as the solid phase receptor (ESS) of MP and 5-aminofluorescein derivatives as the fluorescent (FL)-labeled receptor (N-5-AF) of MP, which can selectively bind the MP and form a sandwich-type supramolecule. Under the optimum conditions, the detection limit was 0.4 μM, the linear range was 1.3–7.0 μM, the correlation coefficient R2 = 0.9983, and the recovery rate range was 96.6–101.1%. Interaction properties between the sensor and MP were investigated by UV-vis, FT-IR, and XRD. Both sensors were successfully applied to the determination of MP content in tap water and camellia.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tong Zhang,Yuan Chen,Yurong Zhang,Bin Liu,Yuanyuan Liu,Jianwei Zhao
Cr(VI) and catechol are common pollutants in wastewaters of tannery industry. Cr(VI) reduction by catechol results in accumulation of Cr(V)-complex and toxic o -benzoquinone. Cr(VI) reduction can be enhanced by accelerating the electron transfer from catechol to Cr(VI) using Fe(III). This electron transfer allows the continuous production of reactive oxygen species (ROS) in advanced oxidation processes, which further degrades catechol. However, the effects of catechol on Fe(III)-based Cr(VI) reduction and ROS production are not clear. In this study, the electron transfer pathway between catechol, Fe(III) and Cr(VI) was investigated along with the catechol degradation by ROS. Results show that the process of Cr(VI) reduction follows well a pseudo-second-order kinetic model, and the activation energy decreases by 4189 J/mol after electrons are transferred by Fe(III). Aqueous chromium (50 mg/L) was completely precipitated as Cr(OH) 3 , Fe x Cr 1-x (OH) 3 or Fe(OH) 3 -Cr(OH) 3 at Fe(III) concentration of 10 mmol/L. Residual catechol and Fe(II) in wastewater activated percarbonate, thereby producing OH for over 480 min at pH 3.0 and generating OH and CO 3 − for over 5 min at pH 10.0. Catechol was degraded by these ROS to butenedioic, oxalic, and formic acids, which were then mineralized to H 2 O and CO 2 . Catechol (2 mmo/L) was fully removed from wastewater with TOC removal of 37%, and the degradation was not affected by SO 4 2− and Cl − . This study provides new insights into the removal of pollutants from wastewaters via electron transfer mediated by Fe(III), and may aid in controlling the toxic effects of Cr(VI) and catechol-like organics in natural and engineered aquatic systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chengcheng Xu,Jing Deng,Shijun Zhu,Xiao Ling,Songtu Shen,Hongguang Guo,Qiongfang Wang,Xueyan Li
The introduction of ascorbic acid (AA) into Fe(III)/PS system exhibited extremely high activity on the removal of N,N-diethyl- meta -toluamide (DEET) and other pollutants. The removal efficiency of DEET within 30 min reached 90.13%, its dynamic curve obeyed second-order kinetic model and the k obs was calculated to be 0.150 L·mg −1 ·min −1 . Compared with other reducing agents, AA was tested to be the most suitable. The optimal dosages of Fe(III), PS and AA were tested to be 0.1, 1.0 and 0.5 mM, respectively. Furthermore, the introduction of AA extended the working pH to 2.5–9.3. Common anions posed different degrees of inhibition on DEET degradation at relatively high concentration, while a small dosage of HCO 3 − (<1 mM) abnormally exerted a positive role. In terms of reaction mechanism, scavenger experiment and EPR observation illustrated that ·OH and ·SO 4 − dominated DEET degradation, yet slight Fe(Ⅳ) was also found during the reaction, which indicated that Fe(Ⅳ) may also contribute to DEET removal. Different from the rapid consumption of Fe(II) in Fe(II)/PS system, Fe(II) in Fe(III)/PS/AA system entered a dynamic equilibrium state in the later stage of the reaction, which can decompose PS to form ·SO 4 − continuously. Furthermore, the reduction and chelation ability of AA both functioned a key role. According to the degradation intermediates identified by LC-MS analysis, the degradation pathways of DEET could be divided into two directions, which covered opening benzene ring and removing side chain.
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