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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Simultaneous removal of catechol and Cr(VI) from tannery wastewaters through Fe(III)-mediating electron transfer

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.

CAS / MDL: 120-80-9 15630-89-4
研究领域: 环境科学 · 化学工程
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FUEL · 2021 · IF 6.609

Silica improved formation of Fe(III)-S and electron-deficient effect in Fe-based catalysts to improve hydrodesulfurization

Xinyue Zhang,Bo Zhang,Yanjun Chen,Lei Li,Houxiang Sun,Xuandong Liu,Rong Guo,Bo Meng,Peng Liu,Weiyu Song,Qiaoxia Guo,Baojian Shen

Electronic structure tuning is an effective strategy to activate transition metals. In this study, silica-promoted γ-Al 2 O 3 -supported Fe-based hydrodesulfurization catalysts of Fe species with electron loss were successfully prepared by transferring electrons from Fe to Si. The characterization results showed that the Fe-based hydrodesulfurization catalyst with the addition of silica modulated the structure and properties of the active metal, which not only improved the degree of sulfidation of the active metal but also promoted the generation of Fe(III)-S. The hydrodesulfurization rate of dibenzothiophene showed a remarkable rise from 38.4 to 83.2% at 673 K. Importantly, the formation of Fe(III)-S greatly stretched the bond length of Fe-S bonds, exhibiting an increase of approximately 21%, this facilitating the generation of coordinatively unsaturated active site. Finally, the HDS reaction performance of the Fe-based hydrodesulfurization catalysts was mainly influenced by the Fe(III)-S/Fe(II)-S ratio, with the most significant enhancement in the direct desulfurization reaction path. The results of this study provide a promising approach for the design and development of environmentally friendly and economical Fe-based catalysts in the field of clean fuels.

研究领域: 催化 · 化学工程 · 材料科学 · 环境化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Enhancement of bisphenol A degradation by accelerating the Fe(III)/Fe(II) cycle in graphene oxide modified Fe(III)/peroxymonosulfate system under visible light irradiation

Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang

The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.

CAS / MDL: 3317-61-1
研究领域: 环境科学 · 材料科学
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JOURNAL OF ENVIRONMENTAL MANAGEMENT · 2018 · IF 4.005

EDTA-Fe(III) Fenton-like oxidation for the degradation of malachite green

Yi Hu,Yulian Li,Junyong He,Tao Liu,Kaisheng Zhang,Xingjiu Huang,Lingtao Kong,Jinhuai Liu

Industrial waste, urban sewage and aquaculture have led to severely increased grades of environment pollutants such as dyes, pesticides and fertilizer. The use of technologies for purifying contaminated waters can be difficult and toxic due to the anti-photolysis, anti-oxidation and anti-bio-oxidation characteristics of organic pollutants, and there is therefore a significant need for new approaches. Here, we report methods of Fenton oxidation and EDTA-Fe(III) Fenton-like oxidation which can be used to degrade malachite green (MG: a dye and antibiotic-like substance) from contaminated water. Compared with the degradation rate (59.34%) of the Fe(III)/H 2 O 2 Fenton process, the EDTA-Fe(III) Fenton-like oxidation got a better degradation rate (92.7%) at neutral pH conditions . By conducting a series of parallel controlled experiments (changing parameters such as the reactant concentration , temperature, and pH), we report the relationships between the degradation effect and different parameters, and we fitted their pseudo first order kinetic curves. Furthermore, we repeated to adjustment of the concentrations of MG in solutions to test the cycle performance and catalytic activities of EDTA-Fe(III)/H 2 O 2 system and it showed good repeatability in the first five rounds and all of them keep the degradation efficiencies greater than 80%. By conducting comparative spin-trapping electron paramagnetic resonance (EPR) experiments, we showed indirectly that the OH contributes to the degradation of MG. Additionally, the results of the EPR experiments showed that EDTA contributes to the generation of OH in the EDTA-Fe(III)/H 2 O 2 Fenton-like system. By conducting total organic carbon (TOC) analysis experiments, we found that EDTA was also oxidized to some extent during the degradation of MG. In all, the findings of this work widen the range of the optimal pH values up to neutral condition for degradation of MG by use of EDTA-Fe(III) Fenton-like system. And this system could be used as one approach for the degradation of organic pollutants at neutral conditions and provide some initial information regarding EDTA-Fe(III) Fenton-like oxidations. It's significant for the expansion of the homogenous Fenton-like family and its application in the field of water treatment .

CAS / MDL: 10025-77-1 569-64-2
研究领域: 环境科学 · 化学工程 · 水处理技术
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS · 2025 · IF 4.6

Fe(III)-controlled dual-channel ratiometric colorimetric sensing of Pb(II)

Xueyi Ren,Honglei Tian,Jianke Li,Yuhuan Zhang

Colorimetric detection methods are prosperous in the monitoring of contaminants in food and environmental matrices. However, the traditional single-channel color changes seriously restrict the enhancement of their sensitivity and facile applications. Herein, a Fe 3+ concentration-controlled dual-channel ratiometric colorimetric sensing platform for the sensitive detection of Pb 2+ was established. Generally, the low concentrations of Fe 3+ can trigger a typical absorption peak at 652   nm of the oxidized TMB (oxTMB). While high concentrations of Fe 3+ induce colorless-to-orange change due to the generation of biphenyl quinone with strong absorption peaks at 450   nm. Interestingly, the presence of Pb 2+ could convert Fe 3+ to Fe (3+x)+ by a displacement reaction, causing a blue-to-colorless change at low Fe 3+ concentrations or an orange-to-blue color change at high Fe 3+ concentrations. The latter dual-channel color variances corresponded to a more distinguished visual quantification of Pb 2+ compared to the former one-channel changes. As such, the Pb 2+ was detected over a range of 0.625-25   µM, with a low detection limit (LOD) of 70   nM. Additionally, by integrating smartphone optical equipment and color recognition software, an intelligent platform for the instant detection of Pb 2+ was established, with a LOD of 0.30   µM. In real samples detection, the developed smartphone sensing platform demonstrated excellent recovery rates (89.0±4.6% to 111.1±7.4%), comparable to the conventional UV-Vis spectroscopy. This work sheds light on fabrication dual-channel colorimetric detection methods for enhanced sensing performance and provides a rapid, sensitive, and intelligent platform for detecting small molecular hazards in the environment.

研究领域: 分析化学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Surface reconstruction of Fe(III)/NiS nanotubes for generating high-performance oxygen-evolution catalyst

Mengxiao Zhong,Weimo Li,Junjie Chen,Siyu Ren,Ruikai Qi,Ce Wang,Xiaofeng Lu

Designing high-performance and cost-effective oxygen-evolution electrocatalysts is highly required toward sustainable water electrolysis. Surface reconstruction is a promising strategy to realize the improvement of the oxygen-evolution reaction (OER) performance of transition metal-based electrocatalysts. Herein, we present a simple electrospinning-post treatment route to construct a novel Fe(III)/NiS electrocatalyst and investigate the key role of the surface reconstruction to significantly promote the OER performance. Owing to the unique tubular morphology and the formation of the highly efficient electrochemical active species of Ni(Fe)OOH during OER process, the prepared Fe(III)/NiS nanotubular catalyst exhibits a low overpotential of 264 mV at 10 mA cm −2 , superior to the benchmark RuO 2 and many other metal sulfide electrocatalysts. Furthermore, the catalyst also presents an excellent durability with no distinct activity reduction for over 70 h. This study offers a reliable surface reconstruction way to fabricate high-efficiency and outstanding durable OER electrocatalyst, enabling it promising prospect for water electrolysis with a reduced energy consumption.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 电化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2017 · IF 2.843

Fe(III)-Modified BiOBr Hierarchitectures for Improved Photocatalytic Benzyl Alcohol Oxidation and Organic Pollutants Degradation

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.

研究领域: 材料科学 · 环境科学 · 化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Fe(III) greatly promotes peroxymonosulfate activation by WS2 for efficient carbamazepine degradation and Escherichia coli disinfection

Hongwei Luo,Chenyang Liu,Ying Cheng,Yifeng Zeng,Dongqin He,Xiangliang Pan

The biggest problem with Fe/PMS (peroxymonosulfate) system is the slow generation rate of SO 4 − due to inefficient Fe 3+ /Fe 2+ cycle and the low decomposition efficiency of PMS . Here, we report the Fe 3+ -enhanced decomposition of PMS by a two-dimensional transition metal dichalcogenide WS 2 for pollutant degradation and E. coli disinfection. Experimental results showed that the removal rates of six representative pollutants were all above 90% under various pH conditions. Over a wide range of pH values (2–9), the removal rate of carbamazepine (CBZ) in PMS/WS 2 /Fe 3+ system almost reached 100% within 10 min, and E. coli could be inactivated by 97.3% within 1 min. WS 2 in the system accelerated the Fe 3+ /Fe 2+ cycle and participated in the activation of PMS. Electron paramagnetic resonance (EPR) measurements and scavenging experiments demonstrated that the SO 4 − and HO radicals were the main active oxidative species. The degradation pathway of CBZ was revealed based on its intermediates as determined by liquid chromatograph-mass spectrometer (LC-MS). The presence of common anions such as Cl − and HCO 3 − in PMS/WS 2 /Fe 3+ system noticeably affected the CBZ degradation. The characterization results verified the structural stability and the reusability of WS 2 . These research findings suggest that the combination of Fe 3+ and WS 2 is a promising method for PMS activation to remove organic pollutants and inactivate pathogenic bacteria during the process of wastewater treatment .

研究领域: 环境科学 · 水处理技术
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Scientific Reports · 2016 ·Vol. 6 ·期 1 ·1-11 · IF 5.228

A novel Fe(III) dependent bioflocculant from Klebsiella oxytoca GS-4-08: culture conditions optimization and flocculation mechanism

Yu Lei,Tang Qing-wen,Zhang Yu-jia,Chen Rong-ping,Liu Xin,Qiao Wei-chuan,Li Wen-wei,Ruan Hong-hua,Song Xin

In this work, the effect of cultivation factors on the flocculation efficiency (FE) of bioflocculant P-GS408 from Klebsiella oxytoca was optimized by the response surface methodology. The most significant factor, i.e . culture time, was determined by gray relational analysis. A total of 240 mg of purified P-GS408 was prepared from 1 liter of culture solution under the optimal conditions. GC-MS analysis results indicated that the polysaccharide of P-GS408 mainly contains Rhamnose and Galactose, and the existence of abundant hydroxyl, carboxyl and amino groups was evidenced by FTIR and XPS analyses. With the aid of Fe 3+ , the FE of kaolin solution by P-GS408 could achieve 99.48% in ten minutes. Functional groups of polysaccharide were involved in the first adsorption step and the zeta potential of kaolin solution changed from −39.0 mV to 43.4 mV in the presence of Fe 3+ and P-GS408. Three-dimensional excitation-emission (EEM) fluorescence spectra demonstrates that the trivalent Fe 3+ and Al 3+ can bind efficiently with P-GS408, while those univalent and divalent cations cannot. With the help of SEM images, FTIR, zeta potential and EEM spectra, we proposed the P-GS408 flocculation mechanism, which consists of coordination bond combination, charge neutrality, adsorption and bridging, and net catching.

研究领域: 微生物学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Atomically disperse Fe(III) species on the MoS2 basal plane as an efficient peracetic acid activator for water decontamination

Jingwen Wang,Yu Yang,Lei Chen,Yanping Ding,Linli Tan,Qiulin Shi,Yong Liu,Pengchao Xie

Molybdenum disulfide (MoS 2 ) is viewed as a promising two-dimensional Fenton-like catalyst, but the basal plane could not be well applied in peroxides activation. In this study, Fe(III) species were atomically impregnated on the MoS 2 basal plane to enhance peracetic acid (PAA) activation. The surface Fe(III) up shifted the d-band centre of MoS 2 and acted as electron shuttles in breaking the O-O bonds of PAA. HO • , CH 3 COO • and Fe(V) were generated in the Fe(III)-MoS 2 /PAA system, whereas the 1 O 2 production was inhibited on the Fe(III)-MoS 2 surface. Sulfamethazine (SMT) was efficiently degraded by Fe(III)-MoS 2 /PAA during 15 min reaction, with the observed removal efficiencies of SMT by Fe(III)-MoS 2 ( k obs ) being 25-fold higher than that by MoS 2 . Increasing the dosages of PAA and Fe(III)-MoS 2 facilitated SMT degradation, and high removal rate of SMT was achieved in the pH range of 3–5. HO • and Fe(V) were identified as critical reactive species responsible for the SMT degradation. Nitrification and Smiles rearrangement were proposed as the degradation pathways of SMT based on the identified oxidation products. This study demonstrates that impregnating Fe species would be an effective strategy for strengthening the Fenton-like reactivity of MoS 2 .

研究领域: 环境科学 · 化学
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FOOD CHEMISTRY · 2023 · IF 8.8

Solvothermal synthesis of bifunctional carbon dots for tartrazine and Fe(III) detection from chamomile residue by ternary DES pretreatment

Zheng Guo,Han-Yi Zheng,Zhong-Ying Huang,Yue-Zhen Liu,Yao-Hua Liu,Yun Chen,Jing Gao,Yong Hu,Chao Huang

A ternary deep eutectic solvent (DES) consisting of choline chloride, lactic acid, and urea in a molar ratio of 1:2:2 was used to pretreat chamomile residue, followed by carbon dots (CDs) preparation using a one-pot solvothermal method . The CDs prepared under the suitable conditions had a high quantum yield of 47.34% and could be used as a bifunctional fluorescent probe for the detection of tartrazine and Fe(III). The concentration of tartrazine or Fe(III) had a good linear relationship with the fluorescence intensity of CDs that the determination coefficient ( R 2 ) was 0.9957 and 0.9943, and the limit of detection (LOD) was 40 nM and 119 nM, respectively. After verifying the different fluorescence quenching mechanisms of CDs by these two substances, a quantitative analysis was performed on real samples with recoveries of 90.70%∼104.29%. Overall, this study provided a promising technology for chemical conversion from low-cost chamomile residue to attractive bifunctional fluorescent probe.

研究领域: 材料科学 · 环境科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Degradation of ethylbenzene in aqueous solution by sodium percarbonate activated with EDDS–Fe(III) complex

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.

研究领域: 环境科学 · 化学工程
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