SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
Small
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2025
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IF 12.1
Yangzi Shangguan,Ranhao Wang,Huan Tang,Shimao Deng,Qiushi Hu,Jiaxin Liang,Huiling Zhou,Xihan Chen,Hong Chen
Photocatalytic antibiotic degradation is an energy-efficient and environmentally friendly approach with the potential for large-scale application but is severely constrained by the lack of efficient and stable catalysts to produce reactive oxygen species (ROS). This research introduces a charge-ordered 3D Fe 3 S 4 -PUF composite integrated into a custom-built photocatalytic tandem continuous-flow cylinder reactor (TCCR) for antibiotic degradation. The system consistently achieves 100% tetracycline (TC) degradation efficiency with Fe 3 S 4 -PUF during 130 h of continuous operation, benefiting from the charge-ordered 3D Fe 3 S 4 -PUF framework and the TCCR design. Mechanism investigations reveal that the abundant Lewis basic ≡SH site and light-induced sustainable Fe 2+ /Fe 3+ redox cycling within Fe 3 S 4 facilitates the production of H 2 O 2 and ROS. Density functional theory (DFT) calculations indicate that Fe 2+ acts as an active site for capturing and activating O 2 , leading to either one-electron (O 2 →O 2 •− →H 2 O 2 →•OH) or two-electron transfer (O 2 →H 2 O 2 ) pathways. Meanwhile, photogenerated electron and the oxygen atoms in H 2 O 2 provide electrons to Fe 3+ , facilitating the reduction of Fe 3+ to Fe 2+ , thus elucidating the Fe 2+ /Fe 3+ redox cycling mechanism. Moreover, the 3D PUF structure enhances the mass transfer and pollutant-ROS interactions. The continuous-flow photocatalytic reaction validate the efficient antibiotic degradation of Fe 3 S 4 -PUF composite, suggesting its potential for implementation in large-scale antibiotic wastewater treatment systems.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2022
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IF 9.988
Yao Tang,Jibo Dou,Zhijiang Lu,Jianming Xu,Yan He
The sluggish Fe 3+ /Fe 2+ cycle was the rate-limiting step in the Fenton-like reaction, and metal-free carbonaceous materials are considered as emerging alternatives to solve this problem. However, the effect of carbon material properties on the distribution of reactive species remains poorly understood. This study investigated the possibility and mechanism of using biochar to accelerate the Fe 3+ /Fe 2+ cycle to overcome the low efficiency of Fe 3+ /persulfate (PS) catalytic oxidation of phenanthrene . More importantly, the contribution of reactive species in the reaction systems with the variation of biochar pyrolysis temperatures was quantitatively studied. The results showed that medium-temperature derived biochar (BC500) had the greatest ability to enhance the Fenton-like system compared to the low- and high-temperature (BC350/700), and the first-order rate constant achieved 5.2 and 35.7-fold increase against the biochar/PS and Fe 3+ /PS systems, respectively. Using electrochemical evidence, sulfoxide probe tests, and steady-state concentration calculations, radicals yields were found to rise and then reduce with decreasing pyrolysis temperature, while the nonradical contribution of Fe(IV) increased to 56.3%. Electron paramagnetic resonance, Boehm titration, and Raman spectroscopy unraveled that the enhanced effect of biochar resulted from itself persistent free radicals, phenolic-OH, and edge defects, which enabled electron transfer between Fe 3+ and biochar. Fe 2+ was thus continuously generated and effectively activated the PS. This work enables a better understanding of the Fe 3+ -mediated Fenton-like reaction in the presence of biochar and provides a sustainable green strategy for Fenton chemistry with potential applications.
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
PubMed
高影响因子
Engineering
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2023
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IF 12.8
Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao
Realizing fast and continuous generation of reactive oxygen species (ROSs) via iron-based advanced oxidation processes (AOPs) is significant in the environmental and biological fields. However, current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect, giving rise to the sluggish Fe 2+ /Fe 3+ cycle and low dynamic concentration of Fe 2+ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with MoS 2 to achieve ultra-efficient Fe 2+ regeneration (equilibrium Fe 2+ ratio of 82.4%) and remarkable stability (more than 20 cycles) via a circulating flow-through process. Unlike the conventional batch-type reactor, experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode, initiated by the convection-enhanced mass/charge transfer for Fe 2+ reduction and then strengthened by MoS 2 -induced flow rotation for sufficient reactant mixing, is crucial for oxidant activation and subsequent ROS generation. Strikingly, the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency. Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology, especially in large-scale complex wastewater treatment.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Bo Xue,Chuanruo Yang,Pengtao Guo,Ting Wang,Gan Li,Dahuan Liu
The low efficiency of photogenerated carriers separation and slow cycling of Fe 2+ /Fe 3+ in Fe-based metal–organic frameworks (MOFs) have limited the improvement of their photo-Fenton activity. Therefore, in this work, MIL-100/BiOBr heterogeneous photo-Fenton catalyst was constructed by compositing MIL-100 with BiOBr nanosheets through a simple solvent evaporation method. In this system, the type II heterojunctions formed by the close contact of MIL-100 and BiOBr can promote the separation of photogenerated carriers and accelerate the redox cyclic of Fe 2+ /Fe 3+ , thereby significantly enhancing the photo-Fenton activity. Under visible light irradiation for 60 min, the best removal rate of tetracycline hydrochloride (TCH) by MIL-100/BiOBr is 94.3 %. Remarkably, the MIL-100/BiOBr exhibits a nearly fourfold increase in degradation rate constant compared to MIL-100 at photo-Fenton system. In addition, the catalysts can maintain high degradation performance over a wide pH range (3–9) and the co-existence of different anions. An in-depth investigation of the degradation mechanism reveals that superoxide radicals ( · O 2 – ) and hydroxyl radicals (·OH) play major roles in the photo-Fenton system. Based on this, the possible degradation pathways were proposed. Therefore, this study provides a new strategy for Fe-based MOFs to remove emerging pollutants from wastewater by photo-Fenton reaction.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Heliyon
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2023
·Vol. 10
·期 1
·e23371
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IF 4
Mingming Zheng,Yinghao Li,Menghua Cao,Yuxin Guo,Guohong Qiu,Shuxin Tu,Shuanglian Xiong,Dun Fang
In the present study, we demonstrated that the presence of cysteine could remarkably enhance the degradation of atrazine by Fe 3 O 4 /persulfate system. The results of electron paramagnetic resonance (EPR) spectra confirmed the combination of cysteine and Fe 3 O 4 exhibited much higher activity on activation of persulfate to generate more SO 4 •- and •OH than Fe 3 O 4 alone. At pH of 3.0, SO 4 •- and •OH contributed to about 58.2 % and 41.8 % of atrazine removal respectively, while •OH gradually dominated the oxidation of atrazine from neutral condition to alkaline condition. The co-existing Cl - and HCO 3 - could quench SO 4 •- , resulting in the inhibition of atrazine degradation. The presence of low natural organic matters (NOM) concentration (0-2 mg L -1 ) could enhance the atrazine removal, and high concentration (>5 mg L -1 ) of NOM restrained the atrazine degradation. During the Cysteine/Fe 3 O 4 /Persulfate process, cysteine served as a complexing reagent and reductant. Through acidolysis and complexation, Fe 3 O 4 could release dissolved and surface bound Fe 2+ , both of which contributed to the activation of persulfate together. Meanwhile, cysteine was not rapidly consumed due to a regeneration process, which was beneficial for maintaining Fe 2+ /Fe 3+ cycle and constantly accelerating the activation of persulfate for atrazine degradation. The reused Fe 3 O 4 and cysteine in the Cysteine/Fe 3 O 4 /Persulfate process exhibited high stability for the atrazine degradation after three cycles. The degradation pathway of atrazine included alkylic-oxidation, dealkylation, dechlorination-hydroxylation processes. The present study indicates the novel Cysteine/Fe 3 O 4 /Persulfate process might be a high potential for treatment of organic polluted water.
研究领域:
环境科学
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化学工程
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水处理
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污染物降解
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DOI
PubMed
高影响因子
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