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CHEMOSPHERE · 2024 · IF 8.1

Enhanced uranium removal from aqueous solution by core–shell Fe0@Fe3O4: Insight into the synergistic effect of Fe0 and Fe3O4

Shizong Wang,Jun Hu,Jianlong Wang

In this study, Fe 0 @Fe 3 O 4 was synthesized and used to remove U(VI) from groundwater. Different experimental conditions and cycling experiments were used to investigate the performance of Fe 0 @Fe 3 O 4 in the U(VI) removal, and the XRD, TEM, XPS and XANES techniques were employed to characterize the Fe 0 @Fe 3 O 4 . The results showed that the U(VI) removal efficiency of Fe 0 @Fe 3 O 4 was 48.5 mg/g that was higher than the sum of removal efficiency of Fe 0 and Fe 3 O 4 . The uranium on the surface of Fe 0 @Fe 3 O 4 mainly existed as U(IV), followed by U(VI) and U(V). The Fe 0 content decreased after reaction, while the Fe 3 O 4 content increased. Based on the results of experiments and characterization, the enhanced removal efficiency of Fe 0 @Fe 3 O 4 was attributed to the synergistic effect of Fe 0 and Fe 3 O 4 in which Fe 3 O 4 accelerated the Fe 0 corrosion that promoted the progressively formation of Fe(II) that promoted the reduction of adsorbed U(VI) to U(IV) and incorporated U(VI) to U(V). The performance of Fe 0 @Fe 3 O 4 at near-neutrality condition was better than at acidic and alkalic conditions. The chloride ions, sulfate ions and nitrate ions showed minor effect on the Fe 0 @Fe 3 O 4 performance, while carbonate ions exhibited significant inhibition. The metal cations showed different effect on the Fe 0 @Fe 3 O 4 performance. The removal efficiency of Fe 0 @Fe 3 O 4 decreased with the number of cycling experiment. Ionizing radiation could regenerate the used Fe 0 @Fe 3 O 4 . This study provides insight into the U(VI) removal by Fe 0 @Fe 3 O 4 in aqueous solution.

研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2021 · IF 7.086

Synergistic chromium(VI) reduction and phenol oxidative degradation by FeS2/Fe0 and persulfate

Weichun Yang,Xiaomin Li,Dongdong Xi,Qi Li,Zhihui Yang,Xiaobo Min,Zhang Lin,Qi Liao

It is a challenge to simultaneously treat the combined pollutants of chromium(VI) (Cr(VI)) and organics (such as phenol) in wastewater. Here, a stable and efficient redox system based on FeS 2 sulfidated zero valent iron (FeS 2 /Fe 0 ) and persulfate (PS) was developed to synchronously remove Cr(VI) and phenol. 100% of phenol (10 mg/L) was oxidized in 10 min and Cr(VI) (20 mg/L) was completely reduced to Cr(III) in 90 min in the FeS 2 /Fe 0 +PS system with a pH range of 3.0–9.0, respectively. phenol was selectively oxidized without re-oxidizing Cr(III) in such system. The surface-bound Fe 2+ was the major reactive species to synchronously reduce Cr(VI) and oxidize phenol. The mechanisms were elucidated that the phenol degradation was accelerated by the generated Cr(III) complexing with its products, and that SO 4 2− , whose production speed was accelerated by the PS activation to oxidize phenol and FeS 2 , was conductive to corrode Fe 0 to regenerate the surface-bound Fe 2+ for reducing Cr(VI) and oxidizing phenol. It is potential to develop a high-performance and large-scaled FeS 2 /Fe 0 -based redox platform to remediate the complex pollution of Cr(VI) and organics.

CAS / MDL: 7439-89-6
研究领域: 环境科学 · 化学工程
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WATER RESEARCH · 2014 · IF 5.323

Activating persulfate by Fe0 coupling with weak magnetic field: Performance and mechanism

Xinmei Xiong,Bo Sun,Jing Zhang,Naiyun Gao,Jimin Shen,Jialing Li,Xiaohong Guan

Weak magnetic field (WMF) and Fe 0 were proposed to activate PS synergistically (WMF-Fe 0 /PS) to degrade dyes and aromatic contaminants. The removal rates of orange G (OG) by WMF-Fe 0 /PS generally decreased with increasing initial pH (3.0–10.0) and increased with increasing Fe 0 (0.5–3.0 mM) or PS dosages (0.5–3.0 mM). Compared to its counterpart without WMF, the WMF-Fe 0 /PS process could induce a 5.4–28.2 fold enhancement in the removal rate of OG under different conditions. Moreover, the application of WMF significantly enhanced the decolorization rate and the mineralization of OG. The degradation rates of caffeine, 4-nitrophenol, benzotriazole and diuron by Fe 0 /PS were improved by 2.1–11.1 fold due to the superimposed WMF. Compared to many other sulfate radical-based advanced oxidation technologies under similar reaction conditions, WMF-Fe 0 /PS technology could degrade selected organic contaminants with much greater rates. Sulfate radical was identified to be the primary radical species responsible for the OG degradation at pH 7.0 in WMF-Fe 0 /PS process. This study unraveled that the presence of WMF accelerated the corrosion rate of Fe 0 and thus promoted the release of Fe 2+ , which induced the increased production of sulfate radicals from PS and promoted the degradation of organic contaminants . Employing WMF to enhance oxidation capacity of Fe 0 /PS is a novel, efficient, promising and environmental-friendly method since it does not need extra energy and costly reagents.

CAS / MDL: 5680-61-5
研究领域: 环境科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Highly efficient persulfate oxidation process activated with pre-magnetization Fe0

Yuwei Pan,Minghua Zhou,Xiang Li,Liting Xu,Zhuoxuan Tang,Xuejie Sheng,Bing Li

Highly efficient persulfate oxidation process activated with pre-magnetization Fe 0 (pre-magnetization Fe 0 /PS) was employed to degrade Orange anthraquinone dye at different Fe 0 dosages (1–8   mmol/L), initial pH levels (3–10) and PS dosages (2–8   mmol/L). Pre-magnetization Fe 0 /PS possessed 8.4–119.6 folds enhancement in degradation rate and could widen pH range and save 90% Fe 0 and PS dosage when compared with conventional Fe 0 /PS process. And this effect was ascribed to the change of Fe 0 characteristics after pre-magnetization. This significant improvement was also observed on the degradation of many refractory contaminants of tartrazine, phenol, 2,4-dichlorophenol (2,4-DCP), p -chlorophenol, chlorobenzene, nitrobenzene, p -nitrophenol and p -nitrchlorobenzene, which were 2.8–11.4 folds of those by Fe 0 /PS process. Pre-magnetization Fe 0 /PS is a more promising process since it does not require any change of the present water and wastewater treatment process, and does not need an extra energy source, costly materials, and complex equipment.

研究领域: 环境科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

Highly efficient advanced oxidation processes (AOPs) based on pre-magnetization Fe0 for wastewater treatment

Xiang Li,Minghua Zhou,Yuwei Pan,Liting Xu,Zhuoxuan Tang

Advanced oxidation processes (AOPs) has great potential for wastewater treatment, but still limited in application due to their high cost for extensive reagent and energy demand, and restricted working conditions (e.g. narrow pH range). Here, AOPs based on pre-magnetization Fe 0 (Pre-Fe 0 ) were found to be highly efficient at wider pH conditions, partly solved the above problems. After pre-magnetization, Fe 0 was supposed to be easier to be corroded, which remarkably improved processes (e.g., Pre-Fe 0 /H 2 O 2 , Pre-Fe 0 /K 2 S 2 O 8 ) efficiency several to >100 folds and valid for many refractory contaminants (e.g. dyes, phenols, organic acids), compared with that conventional processes without pre-magnetization. Moreover, the process efficiency could be sustained by the recovery of magnetism of Pre-Fe 0 . Thus AOPs based on pre-Fe 0 is more promising to take place of conventional Fe 0 based AOPs since it is more efficient but does not require any change of the present water and wastewater treatment process, and does not need an extra energy source, costly materials, and complex equipment.

研究领域: 环境科学 · 化学工程
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International Journal of Environmental Science and Technology · 2013 ·Vol. 11 ·期 4 ·881-890 · IF 1.844

Zero-valent iron/persulfate(Fe0/PS) oxidation acetaminophen in water

Deng J.,Shao Y.,Gao N.,Deng Y.,Tan C.,Zhou S.

Zero-valent iron (Fe 0 ), as an alternative iron source, was evaluated to activate persulfate (PS) to degrade acetaminophen (APAP), a representative pharmaceutically active compound in water. Effects of key factors in the so-called Fe 0 /PS process, including Fe 0 dosage, initial pH, temperatures and chelating agents, were studied. Under all the conditions tested, the APAP degradation followed a pseudo-first-order kinetics pattern. The degradation efficiency of APAP was highest when the Fe 0 to PS molar ratio increased to 1:1, and the degradation rate constant and removal were 23.19 × 10 −3 min −1 and 93.19 %, respectively. Comparing with Fe 2+ , Fe 0 served as an alternative iron source that can gradually release Fe 2+ into water, thereby consistently activating PS to produce sulfate radicals. The Fe 0 /PS system was effective in a broader pH range from 3 to 8.5. Heat could facilitate production of sulfate radicals and enhance the APAP degradation in the Fe 0 /PS system. High reaction temperature also improved the Fe 2+ /PS oxidation of APAP. Finally, sodium citrate (a chelating agent) at an appropriate concentration could improve the APAP degradation rate in the Fe 2+ /PS and Fe 0 /PS system. The optimal molar ratio of Fe 0 to citrate depended on solution pH. Our results demonstrated that Fe 0 was an alternative iron source to activate PS to degrade APAP in water.

CAS / MDL: 103-90-2
研究领域: 环境科学 · 化学工程 · 水处理
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SEPARATION AND PURIFICATION TECHNOLOGY · 2016 · IF 3.299

Novel Fenton-like process (pre-magnetized Fe0/H2O2) for efficient degradation of organic pollutants

Yuwei Pan,Minghua Zhou,Xiang Li,Liting Xu,Zhuoxuan Tang,Mengmeng Liu

A new modified Fenton-like process (pre-magnetization Fe 0 /H 2 O 2 ) was employed to enhance the degradation of organic pollutants and reduce reagents dosage, using azo dye of tartrazine as the model. Compared with Fe 0 /H 2 O 2 process, pre-magnetization Fe 0 /H 2 O 2 process could have 1.3–11.2 folds enhancement in the degradation rate of tartrazine at different Fe 0 dosages (0.5–4   mmol), initial pH levels (2–6.5) and H 2 O 2 dosages (0.25–2   mmol) owing to the change of Fe 0 characteristics after pre-magnetization. The contact angle of pre-magnetization Fe 0 decreased from 58.4° to 19.8° enhancing the hydrophilicity and BET increased from 0.15   m 2 /g to 1.94   m 2 /g, which improved the corrosion of Fe 0 and accelerated the generation of Fe 2+ . Similar to the case of tartrazine, pre-magnetization Fe 0 /H 2 O 2 process had remarkable improvement on many refractory contaminants. The degradation rate constant of methyl orange, orange, methylene blue, 2,4-dichlorophenol (2,4-DCP), acetylsalicylic acid, phenol and tetracycline by pre-magnetization Fe 0 /H 2 O 2 process was 5.2, 21.3, 9.2, 5.6, 12.3, 9.5 and 3 folds of that by Fe 0 /H 2 O 2 process, respectively. The “magnetic memory” of pre-magnetization Fe 0 could last 24   h which was suitable for off-site application, and the lost some or all “magnetic memory” could be recovered after second pre-magnetization. Pre-magnetization Fe 0 /H 2 O 2 is a more promising and highly efficient Fenton process since it does not require any change of the present water and wastewater treatment process , and does not need an extra energy source and complex equipment but can widen pH range and save more than 75% Fe 0 and H 2 O 2 dosages.

研究领域: 环境科学 · 化学工程 · 废水处理
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CHEMOSPHERE · 2019 · IF 5.108

Pre-magnetized Fe0 as heterogeneous electro-Fenton catalyst for the degradation of p-nitrophenol at neutral pH

Yusi Tian,Minghua Zhou,Yuwei Pan,Jingju Cai,Gengbo Ren

Pre-magnetized Fe 0 (Pre-Fe 0 ) was for the first time applied as heterogeneous catalyst to enhance the oxidation efficiency of electro-Fenton (EF) for the degradation of p -nitrophenol (PNP). The parameters including current, initial pH and pre-Fe 0 dosage of Pre-Fe 0 /EF process were optimized and compared with other two processes (conventional Fe 0 /EF and electro-oxidation) to confirm its advantage. The rate constants of PNP removal were 1.40–3.82 folds of those by Fe 0 /EF process under various experimental conditions. The application of pre-Fe 0 as catalyst could extend the working pH range from 3.0 to neutral conditions for PNP removal and reduce the Fe 0 dosage from 2 to 0.5 mM corresponding to Fe 0 /EF, avoiding the second pollution of iron sludge . The superiority of Pre-Fe 0 /EF process was also verified to improve the degradation and mineralization of other phenols and antibiotics. Furthermore, a possible pathway of PNP degradation was revealed by the identification of intermediates and organic acids, and the possible mechanism of pre-Fe 0 efficiently enhanced the EF efficiency was proposed. This work demonstrated that such a novel heterogeneous EF process using pre-Fe 0 catalyst was clean and promising for the degradation of refractory organic pollutants .

研究领域: 环境科学 · 化学工程
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Journal of the Taiwan Institute of Chemical Engineers · 2017 · IF 4.217

Preparation of bifunctional hollow mesoporous Fe0@C@MnFe2O4 as Fenton-like catalyst for degradation of Tetrabromobisphenol A

Fu He,Yong Ji,Yang Wang,Yun Zhang

Nanoscale zerovalent iron (nZVI) loaded magnetic hollow mesoporous bimetallic Fenton-like catalyst, Fe 0 @C@MnFe 2 O 4 , was prepared by a one-pot solvothermal method. Carbon shell of polydopamine (PDA) was formed through self-oxidation of dopamine by adding MnFe 2 O 4 hollow spheres into dopamine solutions. Then Fe 2+ ions were adsorbed on the surface of PDA@MnFe 2 O 4 to obtain active nZVI in-situ through subsequent calcinations. Thus, the mesoporous carbon shell of Fe 0 @C@MnFe 2 O 4 had a great contribution to high adsorption capacity for concentrating TBBPA around the catalyst. The high concentration of TBBPA outside would further facilitate the transportation to the inside of the hollow catalyst to achieve a high catalytic efficiency. Fe 0 @C@MnFe 2 O 4 , as an integrated adsorbent-catalyst, was used to remove Tetrabromobisphenol A (TBBPA) in aqueous solution with the presence of H 2 O 2 and NH 2 OH. Over 90% of TBBPA can be removed within 120 min. According to the result of ESI–MS, β -scission and debromination were involved in the degradation of TBBPA. The reused catalyst could be easily separated by using an external magnetic field in seconds. After ten cycles, the catalyst was still of good activity. The excellent removal efficiency of TBBPA might be attributed to the synergistic effect from high adsorption capacity and efficient Fenton-like catalytic reaction of Fe 0 @C@MnFe 2 O 4 .

CAS / MDL: 79-94-7
研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2018 · IF 4.427

Degradation of diclofenac by H2O2 activated with pre-magnetization Fe0: Influencing factors and degradation pathways

Xiang Li,Minghua Zhou,Yuwei Pan

Diclofenac sodium (DCF) is frequently detected as a non-steroidal pharmaceutical in the aquatic environment. In this study, the degradation of DCF in two heterogeneous systems, pre-magnetization Fe 0 /H 2 O 2 (Pre-Fe 0 /H 2 O 2 ) and Fe 0 /H 2 O 2 system, was comparably studied. Our findings proved that Pre-Fe 0 could significantly improve the degradation and dechlorination of DCF due to the change of Fe 0 characteristics after pre-magnetization. Compared with Fe 0 /H 2 O 2 process, Pre-Fe 0 /H 2 O 2 process has 2.1–7.0 times higher rate constant for DCF degradation at different H 2 O 2 dosages (0.25–2.0 mM), initial pH (3.0–6.0) and Fe 0 dosages (0.25–1.5 mM). The characterizations by X-ray Photoelectron Spectroscopy and Electron Paramagnetic Resonance confirmed that the enhancement attributed to the increase of Fe 0 corrosion and fast generation of OH . In addition, preliminary degradation mechanism was elucidated by major products identification using UPLC-MS, through which the degradation intermediates, such as 4-hydroxy-diclofenac or 5-hydroxydiclofenac, 2,6-dichloroaniline, phenylacetic acid, 1,3-dichlorobenzene and 2-aminophenylacetic acid were identified. Hydroxylation, decarboxylation , C N bond cleavage and ring-opening involving the attack of OH or other substances, were the main degradation mechanism. Therefore, Pre-Fe 0 /H 2 O 2 process, which does not need extra energy and costly reagents, is an efficient and environmental-friendly process to degrade DCF.

研究领域: 环境科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

A MOF-derived Fe3O4/Fe0/Fe3C-2-600 dual-cathode electro-Fenton system construction: Revealing the mechanism for active centers linked by Fe0 as an electronic transfer station for enhancing Fenton reaction

Chuan Cao,Yanjun Guo,Dadi Chen,Jun Cui,Xiang Hu

Conventional heterogeneous iron-based catalysts face challenges such as insufficient catalytic activity, sluggish Fe(Ⅲ)/Fe(Ⅱ) cycle, and hindered electron transfer during Fenton catalytic reactions. Herein, Fe 3 O 4 /Fe 0 /Fe 3 C-2-600, obtained by calcining MIL-88B (Fe) in-situ growth on stainless-steel mesh at varying temperatures, was served as a catalytic electrode in a dual-cathode electro-Fenton system. The catalytic mechanism was elucidated by density functional theory (DFT) calculations. Based on the calculations, the presence of Fe 0 could induce electron transfer to Fe(Ⅲ), accelerating the Fe(Ⅲ)/Fe(Ⅱ) cycle. Simultaneously, Fe 0 was functioned as an electron transfer station, rapidly exporting electrons from the internal Fe 3 O 4 core to the surface graphite layer, further activating H 2 O 2 . Due to the rapid electron transfer, the Fe 3 O 4 /Fe 0 /Fe 3 C-2-600 cathodes demonstrated remarkable catalytic activity, achieving a 97.7 % degradation of tetracycline (TC) within 12 min. According to electron spin resonance tests and quenching experiments, hydroxyl radicals (·OH) was identified as the main active species. In addition, the possible degradation pathways of TC were proposed, according to the results of high-performance liquid chromatography-mass spectrometry (HPLC-MS). The Fe 3 O 4 /Fe 0 /Fe 3 C-2-600 cathode presented a promising strategy for developing an efficient and straightforward method to construct internal electric fields that could accelerate electron transfer in Fenton reactions. Moreover, the integration with the double-cathode electro-Fenton system, realizes the concept of reagent-free and sustainable catalysis, enhancing its practical application value.

研究领域: 环境科学 · 材料科学
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WATER RESEARCH · 2024 · IF 11.4

Electric syntrophy-driven modulation of Fe0-dependent microbial denitrification

Tianyu Gao,Ying Li,Ke Dai,Fangang Meng

In natural or engineered anaerobic environments, iron oxidation-driven microbial denitrification plays a critical role in the water or wastewater treatment. Herein, we report a previously unidentified metallic iron (Fe 0 )-dependent denitrification mode driven by the electro-syntrophic interaction between electroactive microorganism and denitrifier. In a model denitrifying consortium of Shewanella oneidensis and Pseudomonas aeruginosa , we find that P. aeruginosa can accept electrons for nitrate reduction via the constructed electron transfer system of Fe 0 – S. oneidensis – P. aeruginosa . In the electro-syntrophic consortium, the membrane-bound CymA–OmcA–MtrC protein complexes of S. oneidensis drive the generation, transfer and consumption of electrons, thus enabling modulation of microbial metabolic activity. Specially, using Fe 0 as the sole electron donor, S. oneidensis can act as a bio-engine to harvest electrons and conserve energy from Fe 0 biocorrosion. Electrons released by S. oneidensis are utilized by P. aeruginosa for accomplishing microbial denitrification. Metatranscriptomics analysis demonstrated that the direct electron cross-feeding process facilitates the expression of genes encoding for denitrification enzymes, intracellular electron transfer proteins, and quorum sensing of P. aeruginosa . The Fe 0 -dependent electronic syntrophy in this work could provide a metabolic window for the growth of denitrifiers that is a new insight into nitrate removal or global nitrogen cycle.

研究领域: 环境微生物学 · 生物地球化学 · 废水处理 · 微生物生态学
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