COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2017
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IF 2.714
Xiaoqin Huang,Yanli Niu,Weihua Hu
Heterogeneous Fenton catalyst with high activity and excellent durability is highly demanded for efficient removal of organic pollutants via well-known Fenton reaction. In this work Fe/Fe 3 C nanoparticles loaded on iron/nitrogen-doped graphene (Fe/Fe 3 C @ Fe/N-Graphene) were synthesized via spontaneous oxidative polymerization of dopamine (DA) on graphene oxide (GO) surface in the presence of iron (III) chloride, followed by thermal annealing. The Fenton catalytic performance of as-prepared Fe/Fe 3 C @ Fe/N-Graphene was evaluated by degrading rhodamine 6G (Rh 6G) as a model organic pollutant. It is found that as-prepared catalyst demonstrates good activity with a rate constant of 0.080 min −1 under optimal hydrogen peroxide (H 2 O 2 ) concentration and catalyst dosage. Moreover, its catalytic activity shows negligible decrease even after 13 successive cycles, exhibiting excellent catalytic durability. The possible mechanism behind the improved Fenton catalytic activity and durability was further discussed.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Xiaolin Shi,Guo Yang,Bo Xing,Caiyi Jiang,Hangdao Qin,Min Li,Fuping Zhang,Yi Wang,Dongzheng Wang,Xingyong Liu
Fluorine-containing wastewater seriously threatens human health due to the wide application of sodium p -perfluorous nonenoxybenzenesulfonate (OBS). Herein, a novel Fe-Co bimetallic biochar (Fe-Co@BC) with abundant pore structure, functional groups and quickly electron transfer capability was prepared using hydrothermal method. Meanwhile, Fe-Co@BC-Ⅰ exhibited a superior catalytic capacity for degradation of OBS in PMS system, and the removal efficiency of OBS reached to 94.1 % within 60 min. After three cycles, the removal efficiency of OBS still up to 80 % and the Fe-Co had almost no leaching (Fe: 0.006 mg/L; Co: 0.023 mg/L). Further mechanistic insights were verified that high catalytic capacity and stability ascribed to the synergistic effects of Fe and Co, where Fe-Co mutual interaction promoted the formation of Fe 2+ and Co 2+ and accelerated electron transfer of catalyst. In addition, the quenching experiments and electron paramagnetic resonance (EPR) proved that the degradation of OBS can be mainly ascribed to indirect oxidation of SO 4 −• , O 2 −• and •OH, and the possible degradation pathway of OBS was proposed in the Fe-Co@BC/PMS system. This study provides an insight into bimetallic prepared and activation PMS degradation fluorinated wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yanyu Song,Xianbo Sun,Long D. Nghiem,Jun Duan,Wen Liu,Yongdi Liu,Zhengqing Cai
Building a heterojunction is a fascinating option to guarantee sufficient carrier separation and transfer efficiency, but the mechanism of charge migration at the heterojunction interface has not been thoroughly studied. Herein, MIL-53(Fe)/Bi 4 O 5 I 2 photocatalyst with a Z-scheme heterojunction structure is constructed, which achieves efficient photocatalytic decontamination under solar light. Driven by the newly-built internal electric field (IEF), the formation of Fe-O-Bi electron migration channel allows for rapid separation and transfer of charge carriers at the heterojunction interface, confirmed by the material characterization and density functional theory (DFT) calculation. The narrower band gap and improved visible light response also contribute to the enhanced photocatalytic activity of composite materials. With levofloxacin as the target pollutant, the optimal MIL-53(Fe)/Bi 4 O 5 I 2 achieves complete removal of pollutant within 150 min, the photocatalysis rate of which is ca. 4.4 and 26.0 times that of pure Bi 4 O 5 I 2 and MIL-53(Fe), respectively. Simultaneously, the optimal composite material exhibits satisfactory photodegradation of seven fluoroquinolones, and the photocatalysis rates are as follows: lomefloxacin > ciprofloxacin > enrofloxacin > norfloxacin > pefloxacin > levofloxacin > marbofloxacin. DFT calculations reveal a positive relationship between degradation rate and Fukui index (ƒ 0 ) of main carbon atoms in seven fluoroquinolones. This study sheds light on the existence of electron migration channels at Z-scheme heterojunction interface to ensure sufficient photoinduced carrier transfer, and reveals the influence of pollutant structure on photolysis rate.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Tao Zhao,Dazhong Zhong,Qiang Fang,Xin Zhao,Runxin Du,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
The rational design of metal-organic frameworks (MOFs) provides potential opportunities for improving energy conversion efficiency. However, developing efficient MOF-based electrocatalysts remains highly challenging. Herein, a strategy involving strain engineering is developed to promote the electrocatalytic performance of MOFs by optimizing electronic configuration and improving the active site. As expected, the optimized CoFe–BDC NO 2 exhibits a low overpotential of 292 mV at 10 mA cm –2 and a small Tafel slope of 31.6 mV dec –1 as oxygen evolution reaction (OER) electrocatalyst. Notably, when CoFe–BDC NO 2 is prepared on Nickel foam (NF), the overpotential is only 345 mV at 1 A cm –2 , which ensures efficient water oxidation properties. Integrating CoFe–BDC NO 2 /NF anode in membrane electrode assembly (MEA) for overall water splitting and CO 2 reduction reaction (CO 2 RR) tests, the results show that the cell voltages of CoFe–BDC NO 2 /NF are 3.14 and 3.09 V at 300 mA cm –2 (25 °C), respectively, indicating that MOFs have various practical application prospects. The research of the structure-performance relationship reveals the lattice oxygen oxidation mechanism (LOM) where the Co-O-Fe bond is formed during the OER process by changing the electronic environment and coordination structure of CoFe–BDC NO 2 , and with high valence Co as active center, which provides a deep understanding of the structure design of MOFs and their structural transformation during OER.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Qingfei Zhao,Zhenpeng Guo,Zhuohan Wu,Shuyuan Dong,Ronghao Kang,Bingdian Jiang,Shuhui Guan,Ting Zhang,Zhenfeng Bian
The advanced oxidation process (AOP) based on hydroxyl radical ( • OH) has garnered increasing attention in water purification and wastewater treatment. However, producing • OH by activating hydrogen peroxide (H 2 O 2 ) encounters the challenges associated with the sluggish kinetics of Fe(II) regeneration. Herein, we developed a carambola-like catalyst of boron (B)-doped TiO 2 mesocrystals-based iron catalyst (Fe-B-MST), which served as a photocatalyst to modulate the regeneration of Fe(II) in photo Fenton-like systems. We successfully used the electrospinning method to gain membrane and realised the remediation of different industrial wastewater. The Fe-B-MST catalyst exhibits excellent efficiencies in the oxidative degradation of 4-chlorophenol (4-CP) pollutants, effectively facilitating the production of • OH while minimising the formation of toxic byproducts, with the first-order kinetic constant ( k = 2.372 min −1 ) being approximately 6.1 times greater than that without B doping, and 19.8 times greater than that observed with commercial TiO 2 . Theoretical calculations and related physicochemical characterisation reveal that B occupies an interstitial site in titania, conferring a sufficiently high valence band potential, making it thermodynamically favourable for H 2 O 2 oxidation and weakening its interaction with • OH, consequently increasing higher reactivity toward the targeted organic pollutant. The B doping facilitates electron transfer, promotes rapid reduction of Fe(III) to Fe(II), and further enhances • OH production via a photo Fenton-like reaction. The oxidation reaction stoichiometry efficiencies were quantified for different organics and calculated to be in the range of 7.70–24.20 % in Fe-B-MST/H 2 O 2 vis. system, representing an enhancement of 1.18–1.54 times compared to Fe-MST/H 2 O 2 vis. , alongside the utilisation efficiency of H 2 O 2 ( η ) of Fe-B-MST/H 2 O 2 vis. is 1.37–1.67 fold greater than that of Fe-MST/H 2 O 2 vis. after 30 min of reaction. This study expands our understanding and provides valuable insights into applying photocatalysis for enhanced wastewater treatment.
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CHEMICAL GEOLOGY
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2024
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IF 3.6
Kuan Cheng,Zesheng Yang,Guojun Chen,Shiwen Hu,Chao Guo,Yang Yang,Shan Wang,Ying Wang,Haibo Dong,Milan Wang,Pengfei Cheng,Tongxu Liu
The nitrate-reducing Fe(II)-oxidizing (NRFO) process plays a crucial role in geochemical Fe N coupled cycling under anoxic conditions. Both nitrate and nitrite can act as electron acceptors for NRFO bacteria, resulting in the formation of Fe(III) minerals. Nevertheless, the stability of Fe(III) minerals generated during the NRFO process remains unclear. In this study, the Fe(III) minerals were obtained using the model NRFO bacteria strain Acidovorax sp. BoFeN1 in the presence of nitrate or nitrite. The stability of the Fe(III) minerals was examined in the presence of the model Fe(III) reduction bacteria Shewanella oneidensis MR-1 (strain MR-1), the chemical reducing reagent sodium dithionite (Na 2 S 2 O 4 ), and hydrochloric acid (HCl), respectively. The main Fe(III) minerals were goethite in the nitrate treatments (named M nitrate ) and tightly attached to the surface of cells. Meanwhile, the main Fe(III) minerals were lepidocrocite in the nitrite treatments (named M nitrite ), showing slight adherence to the cell surface. The reductive dissolution kinetics of M nitrate by strain MR-1 revealed a gradual increase in Fe(II). Little Fe(II) was formed when reduced M nitrite , which was attributed to the residual nitrite acted as a competitive electron acceptor to Fe(III), inhibiting the microbial Fe(III) reduction processes. Furthermore, the Fe(III) minerals were harvested by centrifugation and then reacted with sodium dithionite and hydrochloric acid (HCl), respectively. The incorporation of sodium dithionite and hydrochloric acid facilitated the dissolution of Fe(III) minerals. In the M nitrite treatments, the Fe(III) minerals exhibit enhanced stability due to their inherent higher crystallinity and the protective influence of cell surface and microbial carbon. This study broadens our understanding of the formation and transformation of microbial Fe(III) minerals, thereby improving our knowledge of biogeochemical iron cycling under anoxic conditions.
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Environmental Science-Processes & Impacts
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2025
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IF 3.9
Rong Peng,Qi Zhu,Shuang Li,Hui Liu
The bacterium Comamonas terrigena strain HJ-2 has been reported as a nitrate-dependent iron-oxidizing bacterium, surprisingly with Fe(III) reduction ability. The control of iron redox cycling by the strain HJ-2 in the Fe(II)-Fe(III) co-existing system is mysterious and worthy of exploration. The present study demonstrates that HJ-2 utilizes nitrate as an electron acceptor to rapidly oxidize Fe(II), with negligible Fe(III) reduction, under neutral anaerobic conditions in a co-existing Fe2+ and ferrihydrite system. Nitrate significantly influences the iron transformation mediated by HJ-2. The final conversion ratio of Fe(II) increased from 27.94% to 96.67%, and the bio-oxidation rate of Fe(II) escalated from 0.000143 to 0.013 h⁻¹ as nitrate concentrations rose from 0.1 to 10 mM. X-ray diffraction results indicated that in the absence of HJ-2, goethite was the sole product, regardless of the nitrate concentration. While in the presence of HJ-2, the minerals formed transitioned from crystalline goethite and lepidocrocite to amorphous or weakly crystalline minerals with increasing nitrate concentration. Scanning electron microscopy and energy-dispersive X-ray spectroscopy showed that the morphology of the final mineral formed under high nitrate conditions resembled ferrihydrite, with higher carbon content on the mineral surface at elevated nitrate concentrations, suggesting enhanced production of bio-iron oxides and increased adsorption capacity for aqueous Fe(II). X-ray photoelectron spectroscopy results confirmed higher Fe(II) content on the amorphous minerals surface than goethite. This work provides new insights into microbial-mediated Fe-N cycling in natural environments, highlighting the significance of nitrate in driving iron redox processes and the iron mineral transformation by strain HJ-2.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Ting Zhou,Wenyi Dong,Xuechuan Li,Weigang Liu,Mengke Qiang,Hongjie Wang
High-valent ferric oxide species (HV-Fe(IV)) has been increasingly explored to selectively and efficiently remove pollutants from wastewater owing to its high reduction potential, long lifetime, and valuable resistance to anions. However, the directional production of HV-Fe(IV) and its mechanism remain challenging. Herein, a biochar-based catalyst with monoatomic Fe-trans-N 2 O 2 configuration and rich COOH group (SAFe-NKBC) was rationally constructed via KOH and supramolecular organic framework co-pyrolysis. As a result, the SAFe-NKBC/PMS system exhibited exceptional catalytic performance, achieving rapid sulfamethoxazole degradation (97.4% within 10 min) and TOC removal (73.1%). Mechanistic investigations revealed the cooperative catalytic role of single-atom Fe-trans-N 2 O 2 and COOH in biochar support via surface-confinement effect in boosting peroxymonosulfate activation and directional HV-Fe(IV) generation, mediating spatially coupled electron transfer and promoting selective oxidation pathways. Furthermore, a structure–activity relationship for various para-substituted anilines was systematically established via quantitative structure–activity relationship modeling based on different adsorption and oxidation descriptors. The valid descriptors were confirmed to predict reactivity, offering a molecular-level framework for water purification. Meanwhile, the catalyst demonstrated excellent resistance to matrix interference, long-term stability in flow-through systems, and significantly reduced toxicity of degradation byproducts, underscoring its potential in sustainable and precision-oriented water remediation. This work offered new insights into rational SAC design and reactivity prediction for sustainable water remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xianfa Zhang,Mingzhao Huang,Zuoming Zhou,Xiaodan Zhao,Guohua Jing
Sulfite activation with iron-based heterogeneous activators is a promising technology for the removal of organic contaminants from water. However, the slow valence transformation of >Fe(II)/>Fe(III) compromises sulfite activation efficiency. Regarding that the oxygen vacancy (Vo) can modulate the charge distribution and thus enhance >Fe(II)/>Fe(III) valence transformation via rapid electron transfer, Vo-enriched γ-Fe 2 O 3 is constructed for sulfite activation (simplified as the γ-Fe 2 O 3 -Vo/sulfite system). The γ-Fe 2 O 3 -Vo/sulfite system exhibits excellent abatement performance for iohexol (IOX) with the efficiency as high as 90.2 % within 1 h of reaction at pH 8.5, in which sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) are the major species. Electrochemical and DFT calculations reveal that Vo-enriched γ-Fe 2 O 3 possesses lower electrical impedance and the concomitant higher electron transfer efficiency. According to a series of characterizations, the enhance >Fe(II)/>Fe(III) valence transformation is confirmed to contribute to sulfite activation via the regulation of the electronic structure by the Vo. In addition, the degradation pathways of IOX are proposed by analyzing the degradation products of IOX by UPLC-QTOF-MS. Finally, the effects of different influencing factors on the degradation of IOX and the cyclic performance suggest the system shows strong resistance to interference and reusability, exhibiting superior application potential.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Zixuan Zhang,Chenying Zhou,Yiming Sun,Peng Zhou,Yang Liu,Heng Zhang,Ye Du,Chuanshu He,Zhaokun Xiong,Bo Lai
Fenton oxidation technology is a widely-used advanced oxidation technology. However, the generation of hydroxyl radicals is restrained by the sluggish recovery of Fe(II), thus affecting its long-lasting performance for water decontamination. Here, a novel niobium carbide (Nb 2 C) MXene material was applied as a green co-catalyst. Nb 2 C MXene can significantly promote Fenton reactions to produce hydroxyl radicals for degrading dimethyl phthalate (DMP) with high efficiency and high stability for long-term operation, which outperforms than various reported co-catalysts. Meanwhile, the Nb 2 C/Fe(III)/H 2 O 2 system is capable of non-selectively degrading a wide spectrum of refractory pollutants. Mechanism investigation reveals that Nb 2 C MXene as an electron donor can straight reduce Fe(III), meanwhile mediate electron shuttle from Fe(II) to H 2 O 2 to strongly expedite the generation of hydroxyl radicals. In addition, four main degradation routes of DMP were proposed. Therefore, this study offers an updated and valid strategy for the refractory organic pollutants elimination by coupling Nb 2 C MXene and Fenton oxidation.
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Journal of Environmental Sciences
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2024
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IF 5.9
Zheng Qi,Zaihui Huang,Chunguang Liu
Advanced oxidation processes (AOPs) exhibit significant potential for water disinfection due to their generation of large quantities of highly oxidizing free radicals. However, the neglect of viable but nonculturable (VBNC) cells obscures their true disinfection efficacy and potential environmental health risks. Therefore, the study evaluated the disinfection effectiveness and mechanisms of typical AOPs, including Fe/H 2 O 2 , Fe/persulfate (PS), and O 3 , from the perspective of the production of VBNC bacteria. The results indicate that Fe/PS exhibits the strongest bacterial inactivation rate (99.94%), and the cells lose their ability to reactivate. Fe/H 2 O 2 and O 3 induce more cells to enter the VBNC state compared to Fe/PS. Moreover, different AOPs result in varying levels of free radical production and utilization efficiency, with SO 4 •− and O 3 exhibiting greater selectivity in deactivating bacteria compared to HO • . The inhibition of VBNC bacteria production by Fe/PS treatment may be attributed to the combined action of HO • and SO 4 •− on microorganisms, leading to oxidative stress and metabolic disruption in bacteria through the inhibition of biofilm formation and aminoacyl-tRNA biosynthesis ( p < 0.05), thereby causing direct bacterial death rather than entry into the VBNC state. In contrast, Fe/H 2 O 2 and O 3 result in the upregulation of the metabolism of alanine, aspartate, and glutamate, as well as styrene degradation capacity by the bacteria, leading to the production of more VBNC bacteria. Overall, the study offers insights into mitigating potential biological risks in water disinfection and developing environmentally friendly and efficient disinfection technologies.
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FOOD CHEMISTRY
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2020
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IF 6.306
Xiamin Lv,Huasheng Man,Lijuan Dong,Jianying Huang,Xiangyang Wang
Carbon dots (CDs) have been a new class of fascinating carbon-based fluorescent nanomaterials. In the present work, new N -doped CDs with highly crystalline graphite structures are prepared from renewable precursors, chitosan and tartaric acid, and are well characterized. The prepared CDs are applied as a biocompatible fluorescent sensor for the sequential detection of Fe 3+ and AA. Among various transition metal ions, Fe 3+ can selectively quench the fluorescence of CDs. Upon the further addition of AA, the quenched fluorescence of CDs is then restored as Fe 3+ is reduced to Fe 2+ by AA, which can be utilized for the fluorescent determination of AA. A good linear relationship in the range of 0–150 μM of AA concentration is established with a low detection limit of 0.02 µM. Moreover, the practical applications of this fluorescent sensing method in measurement of AA in food samples are successfully realized with satisfactory results.
研究领域:
材料科学
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分析化学
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生物医学
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