SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Haonan Chen,Shiqi Tian,Zheng-Qian Liu,Jun Ma,Gang Wen
Iron oxides are widely utilized in catalytic ozonation, but their effectiveness is often limited by the slow Fe(II)/Fe(III) redox cycle. In this study, a series of metal sulfide–iron oxide composites were synthesized, all of which exhibited enhanced catalytic performance, with MoS 2 @Fe 3 O 4 showing outstanding efficiency. The catalytic system decomposes ozone (O 3 ) into hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ), with ·OH predominantly contributing to the oxidation process. The catalytic process was significantly enhanced through three key pathways: (i) metal sulfides themselves demonstrate superior ozonation catalytic performance compared to iron oxides; (ii) the presence of Mo(IV) effectively promotes the Fe(II)/Fe(III) redox cycle; and (iii) the transient superoxide radical (·O 2 − ), a crucial intermediate in ozone chain decomposition, rapidly reduces high-valence Mo(VI) to Mo(IV), thereby reinforcing the Mo redox cycle, further strengthening the Fe redox cycle, and leading to the accumulation of 1 O 2 . Notably, the efficient utilization of ·O 2 − represents a unique mechanism in the catalytic ozonation system. These findings emphasize the critical role of the Mo redox cycle in enhancing Fe redox activity to promote catalytic ozonation, providing valuable insights for the development of advanced metal sulfide–iron oxide catalysts for environmental applications.
研究领域:
环境科学
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催化材料
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Haiyuan Chi,Chengjun Li,Mei Huang,Jinquan Wan,Xiaoxia Zhou,Bing Yan
Sulfate radicals-based advanced oxidation processes are regarded as effective methods for removing organic contaminants. However, current removal technologies are often unable to achieve satisfactory results due to the low concentrations and high stability that are frequently characteristics for many types of organic contaminants. To improve the efficacy of using sulfate radicals to remove organic contaminants, we designed metal–organic frameworks (Fe(II)-MOFs) modified with enrichment and specific recognition of molecular imprinting layer (Fe(II)-MOFs@MIP). Using dibutyl phthalate (DBP) as the model target contaminant, the selectivity coefficient towards DBP was 7.28 for adsorption and 4.46 for catalytic degradation of Fe(II)-MOFs@MIP, which is excellent for most of the imprinted material. Additionally, we achieved the accurate recognition (169.25 μg × g −1 ) and efficient degradation (0.071 min −1 ) of DBP reducing levels to 100 μg × L -1 . UV–vis analysis confirmed that specific recognition of DBP was mainly through hydrogen bonding and π-π interaction, while in-situ Raman and radical quenching experiments showed that the imprinting layer could accurately adsorb and produce the spatial confinement effects on target contaminants, thereby reducing the transfer distance of free radicals. As a result, we show that Fe(II)-MOFs@MIP can achieve efficient targeted degradation of DBP, opening up a new avenue for the removal of this and other highly stable organic contaminants present at low concentrations in environmental systems.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Journal of Cleaner Production
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2024
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IF 9.7
Jiaxing Wu,Jianqun Bao,Xuya Zhang,Zhuang Yang,Yiqi Liu,Mingxia Zhou,Yajun Wang,Guiyuan Jiang,Wenqing Yao
The efficient activation of peroxymonosulfate (PMS) in advanced oxidation technology is hindered by the low Fe(II)→Fe(III)→Fe(II) cycle efficiency. Herein, we report a Fe(II)/decahedral monoclinic BiVO 4 composite photocatalyst with a highly exposed (010) facet prepared by a hydrothermal method combined with a wet impregnation strategy. The numerous photogenerated electrons on the (010) facet promote the cycling of Fe(II)→Fe(III)→Fe(II) process, thereby significantly enhancing the PMS activation rate. The charge transfer mode of 1% Fe(II)/BiVO 4 was inferred from in situ X-ray photoelectron spectra. The composite catalyst exhibits significantly higher activity (96.7%) than the pristine BiVO 4 without facet regulation (56%). Controlling the crystal facets can effectively separate the photogenerated carriers of BiVO 4 ; the photogenerated electrons catalyze the cyclic transformation of Fe(III)/Fe(II) to efficiently activate PMS and degrade antibiotics. This work confirms the synergistic effect of facet engineering and the photocatalytic PMS activation system and provides a new perspective for the degradation of antibiotics.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Ying Liu,Yi Liu,Yingying Xu,Qingshen He,Rongyang Yin,Pengfei Sun,Xiaoping Dong
Nitrophenols (NPs) are widely used in industries and highly toxic to ecological environment and human health. Because aminophenols (APs) are important chemicals, catalytic reduction of NPs via efficient and environment-friendly strategies is of great importance. Herein, we developed a green photocatalysis route to efficiently convert NPs to APs using a Fe (II) modified graphitic carbon nitride (g-C 3 N 4 ) photocatalyst, where phenanthroline units were employed to bridge Fe (II) and carbon nitride framework. The optimized sample P-CN-8-Fe presented significantly improved absorption of visible light, separation of photogenerated charges and carrier transportation in comparison with the pristine g-C 3 N 4 and the modified samples of CN-Fe and P-CN-8. Accordingly, the P-CN-8-Fe showed a high conversion (97%) of p -nitrophenol ( p -NP) to p -aminophenol ( p -AP) under 2 h visible light irradiation, and meanwhile possessed high photocatalytic durability. Its high activity was also demonstrated through photocatalytic reduction of other NPs and nitrobenzene compounds. Finally, a possible mechanism was proposed for the photocatalytic reduction of p -NP by P-CN-8-Fe. This work provides an effective approach to prepare Fe (II) modified g-C 3 N 4 through the bridging effect of phenanthroline group, which is a potential visible light driven photocatalyst for reduction of nitrobenzene derivatives.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Haishuo Wang,Jie Zhang,Zhichun Li,Bin Shi,Shiyin Li,Heyong Huang
Microcystin-LR (MCLR) is a highly toxic pollutant widely distributed in eutrophic waters. The interplay between dissolved organic matter (DOM) and metal ions has been extensively reported; however, the impact of DOM-metal complexes on MCLR remains to be thoroughly studied. In this research, equilibrium dialysis was employed to study the kinetics and isotherms of MCLR adsorption by DOM, meanwhile the Density functional theory (DFT) calculations provided insights into the theoretical mechanisms of Fe(II)/Mn(II) involvement in the adsorption process. The adsorption kinetics revealed that the process is physicochemical, with chemisorption being the critical factor controlling the adsorption rate. The adsorption isotherms confirmed that Fe(II) alters the spatial arrangement of adsorption sites on the superficies of DOM, with the complexes of Fe(II) and DOM from the macrophyte-dominated regions of Lake Taihu (MDR-Fe(II)) showing the uppermost adsorption capacity of 6193.965 µg/g among all combinations. The influence of different cations (K + , Ca 2+ , Na + , Mg 2+ ) on the adsorption of MCLR to DOM is divergent, with metals either reducing MCLR adsorption through competition for adsorption sites or increasing it by forming ternary complexes. The pH decrease reduced the affinity of DOM to metal ions while simultaneously enhancing MCLR adsorption through changes in its ionization state. DFT calculations demonstrated that Fe(II)/Mn(II) reduces the resistance to interaction between functional groups on DOM and MCLR, with carboxyl-Fe(II)-carboxyl interactions showing the highest binding energy (ΔG = −7.253 eV). Overall, Fe(II)/Mn(II) enhances the adsorption of MCLR via altering the structure and surface electrostatic potential distribution of DOM. This research indicates that the ultimate fate of MCLR in aquatic ecosystems is affected by DOM and metal ions.
研究领域:
环境科学
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毒理学
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理论化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Qizhan Zhang,Minghua Zhou,Xuedong Du,Pei Su,Wenyang Fu,Ge Song
To simultaneously improve the H 2 O 2 electrosynthesis, Fe(II) regeneration and pH application range in EF process, a highly efficient dual-cathode electro-Fenton (EF) process using easily available Fe(III) as catalysts for the treatment of organic wastewater at a wide pH range was first proposed, in which natural air diffusion electrode (NADE) was designed as one cathode for H 2 O 2 production without aeration and the modified carbon felt (MCF) was acted as the other cathode mainly for Fe(II) regeneration. Nitric acid modification significantly enhanced the electrochemical properties of CF and introduced more oxygen-containing functional groups. The Fe(II) regeneration rate of MCF with higher electroactive surface area was 4.7 times that of CF cathode at pH 7. It was found that as the homogeneous Fe(III) was hydrolyzed into solid hydroxides, the accompanying H + decreased the solution pH and MCF not only accelerated the dissolved Fe(III)/Fe(II) cycle but also reduced the adsorbed solid iron to ≡Fe(II) on the cathode surface. This simultaneously promoted the homogeneous and heterogeneous Fenton reactions and enhanced the efficiency of EF degradation process. For bronopol, 2,4-dichlorophenoxyacetic acid, sulfamethazine and phenol (100 mg L −1 ), the process had TOC removal of 48%−72% within 60 min with the corresponding mineralization current efficiency of 16.5%−56.2%, and the electrical energy consumption <0.225 kWh (gTOC) −1 , which all greatly advantaged over that of the conventional EF. Therefore, this process is efficient and low-cost, being very promising for the treatment of organic wastewater.
研究领域:
环境科学
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污水处理
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电化学技术
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DOI
高影响因子
CHEMOSPHERE
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2017
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IF 4.208
Zilong Zhao,Wenyi Dong,Hongjie Wang,Guanhan Chen,Wei Wang,Zekun Liu,Yaguang Gao,Beili Zhou
Elimination of hypophosphite (HP) was studied as an example of nickel plating effluents treatment by O 3 /H 2 O 2 and sequential Fe(II) catalytic oxidation process. Performance assessment performed with artificial HP solution by varying initial pH and employing various oxidation processes clearly showed that the O 3 /H 2 O 2 ─Fe(II) two-step oxidation process possessed the highest removal efficiency when operating under the same conditions. The effects of O 3 dosing, H 2 O 2 concentration, Fe(II) addition and Fe(II) feeding time on the removal efficiency of HP were further evaluated in terms of apparent kinetic rate constant. Under improved conditions (initial HP concentration of 50 mg L −1 , 75 mg L −1 O 3 , 1 mL L −1 H 2 O 2 , 150 mg L −1 Fe(II) and pH 7.0), standard discharge (<0.5 mg L −1 in China) could be achieved, and the Fe(II) feeding time was found to be the limiting factor for the evolution of apparent kinetic rate constant in the second stage. Characterization studies showed that neutralization process after oxidation treatment favored the improvement of phosphorus removal due to the formation of more metal hydroxides. Moreover, as a comparison with lab-scale Fenton approach, the O 3 /H 2 O 2 ─Fe(II) oxidation process had more competitive advantages with respect to applicable pH range, removal efficiency, sludge production as well as economic costs.
研究领域:
环境工程
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废水处理
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化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Linke Jiang,Ruiqi Wang,Shuiqin Shi,Junmei Yan,Mingbao Feng,Lianbao Chi
With the aging of the global population and continued economic development, the use of sartan-type antihypertensive drugs (e.g., losartan (LOS), telmisartan (TEL), and valsartan (VAL)) has increased with widespread contamination issues. However, the effect of advanced oxidation processes (AOPs) on the degradation of sartans remains unknown. Therefore, AOPs such as the Fe(II)/peroxymonosulfate (PMS) system and ozonation were used to treat the typical sartans, which led to the formation of various transformation products (TPs). This research involves the formation mechanisms of these TPs following AOPs including aldolization, hydroxylation, ring cleavage, carbonylation and cyclization. The risk evaluation focused on the biodegradability and toxicity of the drugs and their TPs, assessed using computerized toxicity prediction software. The findings indicated that the biodegradability of most TPs was generally poor and most TPs exhibited acute/chronic toxicity. This underscores the need for caution when applying AOPs in water treatment to prevent secondary contamination and suggests the potential necessity of integrating AOPs with complementary purification technologies. This research provides novel insights into the degradation pathways and environmental risks of sartans, emphasizing the importance of a holistic approach to water treatment.
研究领域:
环境科学
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水处理
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药物化学
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毒理学
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
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2016
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IF 4.712
Qiong Hu,Baojing Zhou,Pengyun Dang,Lianzhi Li,Jinming Kong,Xueji Zhang
We report a versatile approach for the colorimetric assay of alkaline phosphatase (ALP) activity based on the distinctive metal-to-ligand charge-transfer (MLCT) absorption properties of Fe(II)-phenanthroline reporter. In the presence of ALP, the applied substrate ascorbic acid 2-phosphate is enzymatically hydrolyzed to produce ascorbic acid, which then reduces Fe 3+ to Fe 2+ . The complexation of Fe 2+ with the bathophenanthroline disulfonate (BPS) ligand generates a blood-red Fe(BPS) 3 4− reporter, which is characterized by an intense MLCT absorption band at 535 nm in the visible range. Under optimal conditions, the spectral output exhibits a good quantitative relationship with ALP activity over the range of 0–220 mU mL −1 with a detection limit of 0.94 mU mL −1 . Moreover, the activity of ALP can also be conveniently judged through naked-eye observations. Results indicate that it is highly selective and can be applied to the screening of ALP inhibitors. In addition, it has been successfully employed to detect the endogenous ALP level of undiluted human serum samples, with a detection limit of 1.05 mU mL −1 being achieved. This approach avoids any elaborately designed substrates and holds considerable simplicity and flexibility for reporter design. This study broadens the horizon of the applications of phenanthroline-based transition metal complexes. Furthermore, an efficient and practical method like this has the potential to be widely used in clinical applications and in the point-of-care testing.
研究领域:
分析化学
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生物化学
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临床诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Theranostics
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2020
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IF 8.579
Qingqing Tian,Lu An,Qiwei Tian,Jiaomin Lin,Shiping Yang
Rationale : Chemodynamic therapy (CDT) based on the Fe(II)-mediated Fenton reaction is an emerging tumor treatment strategy. However, the catalytic efficiency in tumors is crucially limited by Fe(II). Herein, an endogenous hydrogen sulfide (H 2 S) accelerated Fe(III)/Fe(II) transformation and photothermal synergistically enhanced CDT strategy based on ellagic acid-Fe-bovine serum albumin (EA-Fe@BSA) nanoparticles (NPs) was developed for colon tumor inhibition. On the one hand, the Fe(III) with low catalytic activity in the EA-Fe@BSA NPs could be rapidly reduced to the highly active Fe(II) by the abundant H 2 S in colon cancer tissues. Thus, a rapid Fe(III)/Fe(II) conversion system was established, wherein highly active Fe(II) ions were continuously regenerated to improve the CDT efficiency. On the other hand, the photothermal effect of EA-Fe@BSA NPs also accelerated the production of hydroxyl radicals (•OH), thereby synergistically enhancing the CDT performance and improving the therapeutic efficacy. Methods : The endogenous H 2 S accelerated Fe(III)/Fe(II) conversion and PTT enhanced CDT were investigated by characterization of the Fe valence state and detection of •OH. T 1 -weighted magnetic resonance imaging (MRI) was tested both in vitro and in vivo . The biocompatibility of NPs were examined via MTT assay, hemolysis analysis and routine blood measurements. The enhanced CDT was investigated in HCT116 colon cancer cells by Calcein-AM/PI staining and MTT assay, and tumor inhibition was demonstrated in HCT116 tumor bearing mice. Results : In this work, EA-Fe@BSA NPs were constructed as a CDT theranostic reagent. The H 2 S accelerated Fe(III)/Fe(II) conversion was confirmed, more degradation of MB and generation of •OH demonstrated the enhanced CDT in vitro . EA-Fe@BSA NPs exhibited good T 1 -weighted MRI performance. More importantly, it displayed strong near-infrared (NIR) absorption and excellent photothermal efficiency, further promotes the production of •OH. Hence, the efficacy of CDT was enhanced, and the tumor growth was inhibited efficiently. Conclusion : All results demonstrate that this strategy based on endogenous H 2 S promoted Fe(III)/Fe(II) transformation together with PTT acceleration permits efficient Fenton-reaction- mediated CDT both in vitro and in vivo , which holds great potential for effective colon cancer theranostics.
研究领域:
生物医学工程
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肿瘤治疗
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纳米医学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）