JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
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IF 8.4
Zhiquan Xiang,Yijie Zhang,Lei Bo,Zhuowei Shen,Dan Wang,Zhiqiang Shen,Yaoyu Tang
Aniline in landfill leachate was used as a target pollutant and treated by a catalytic ozonation process (COP). The catalyst was based on waste iron shavings, which were oxidatively modified to form an iron-based ozonation catalyst (FOC), and subsequently compressed into an iron-based packing for catalyzing the ozonolysis of aniline (FCOP). The special porous structure of the compressed packing material enhanced the decomposition of O 3 . FCOP achieved 93% removal of aniline from the simulated wastewater, which was significantly better than the ozonation alone process (OOP). At low pH (<3), the removal of aniline relied on the endo-Fenton mechanism due to the presence of Fe 2+ and H 2 O 2 . At high pH (>5), aniline was removed by the COP mechanism. At the FOC surface, electron transfer facilitated ozonolysis to produce •OH radicals, which simultaneously produced Fe 2+ oxidation and Fe 3+ reduction, establishing a redox cycle. The main role of -OH in the FCOP system and the aniline degradation pathway were determined using EPR and related techniques. FCOP is a cost-effective and environmentally friendly process that can be used to treat aniline in the future.
研究领域:
环境科学
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化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Lifeng Hao,Junhuan Zhao,Kangyuan Li,Weiping Zheng,Yanfei Yang,Chenyang Qiu,Zewen Jiang,Wenjun Xia
We report a hydrothermal engineering strategy to synergistically regulate structural barriers, oxygen vacancy-driven redox cycling, and surface functionalization in Ce-NiCo-LDH coatings for ultralong corrosion protection. Vertically aligned LDH nanosheets constructed a tortuous labyrinth barrier to physically impede corrosive species penetration. Oxygen vacancies acted as electron reservoirs to drive Ce 3+ /Ce 4+ redox cycling, enabling dynamic passivation repair via preferential Ce 4+ → Ce 3+ reduction at vacancy sites. Surface functionalization further enhanced protection through two independent pathways: CTAB induced interlocked fibrous nanostructures for mechanical reinforcement, while PFDT grafting formed a fluorine-rich hydrophobic barrier through C-F dipole interactions. EIS characterization demonstrated a 3.6-fold enhancement in charge transfer resistance (Rct = 5.1 × 10 5 Ω·cm 2 ) for the sequentially hydrothermally processed Ce-NiCo-LDHs compared to their single-step counterparts (1.4 × 10 5 Ω·cm 2 ). The CTAB-modified coating achieved 99.0 % inhibition efficiency, while PFDT modification provided long-term hydrophobicity. This triple-scale synergy-structural obstruction, redox-mediated self-healing, and surface engineering-provides a universal framework for designing advanced protective coatings.
研究领域:
材料科学
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腐蚀工程
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表面工程
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Hui Xu,Jia Ye,Longyuan Lin,Minmin Lian,Jicheng Chen
A novel technique for generating tetramethylpyrazine (TTMP) was proposed, carried out on a phenolics-Fenton coupled redox cycling system in an acetoin-ammonium acetate (AA-ACT) pattern reaction. The TTMP generation employing the Fenton system is a first-order reaction that significantly increased the reaction rate, especially in the early stages, distinguishing it from the original zero-order kinetics reaction pattern. Further, the Fenton reaction effectively promotes the TTMP generation at lower temperature, and epigallocatechin gallate (EGCG) could reset the Fenton reaction, accomplishing the redox cycle. We have discovered a novel class of intermediate products, N-substituted amides, which act as a “reservoir” and transform into amino acid, then undergo aromatization to generate TTMP. The results provide a useful supplement for intelligent synthesis route design, and a new approach for understanding the transformation pathways of pyrazines.
研究领域:
生物化学
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合成生物学
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高影响因子
ELECTROCHIMICA ACTA
·
2021
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IF 6.901
Fei Miao,Zehao Liu,Xin Kang,Cheng Cheng,Xiaoyu Mao,Ruimeng Li,Heng Lin,Hui Zhang
Heterogeneous catalytic oxidation based on iron species for peroxymonosulfate (PMS) activation is considered as one of the most attractive strategies for wastewater treatment. However, the rate-limiting regeneration of Fe(II) from Fe(III) heavily hampers the efficient activation of PMS. In this study, the introduction of electric field to the Fe-supported bentonite (Fe-B) activated PMS process was proposed to enhance the Fe(III)/Fe(II) redox cycle. The Fe-B catalyst performed well in the removal of Acid Orange 7 (AO7) through the synergistic effect of electrolysis and the continuous redox cycle of Fe(III)/Fe(II) for PMS activation. The use of 0.5 g L −1 Fe-B catalyst and 10 mM PMS yielded nearly complete removal of the AO7 (50 mg L −1 ) in 60 min at 2 mA cm −2 of current density. Based on the results of electron paramagnetic resonance (EPR) spectroscopy, chemical quenching tests, X-ray photoelectron spectroscopy (XPS) analysis, and electrochemical measurements, the decolorization of AO7 was dominantly attributed to surface-bound radicals (SO 4 •− ads and • OH ads ) and also the direct electron transfer at DSA anode. Moreover, the electro/Fe-B/PMS system showed an effective pH range from 2.6 to 9.0 and the abatement of AO7 was slightly affected in the presence of natural background anions. This work provides a feasible strategy of PMS activation by cost-effective Fe-B catalyst coupling with electric field and gives an insight into the accelerated oxidation of recalcitrant pollutants.
研究领域:
环境科学
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化学工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Hanzi Liu,Changfu You,Haiming Wang
Transient in-situ IR spectroscopy was performed to analyze the molecular behavior of selective catalytic reduction of NO with NH 3 on V 2 O 5 -WO 3 /TiO 2 catalyst. During NH 3 adsorption, an unexpected growth in the intensity of Lewis acid sites was observed due to the hydrogen migration, which was verified by the DFT calculation and the existence of intermediate species. The comparison between the isolated atmosphere experiments and the simultaneous exposure of NH 3 -NO-O 2 on catalytic monolayer demonstrated that: (i) there exists a pathway for Lewis to Brønsted acid sites transformation at T > 300 °C, (ii) the rate determining step of the SCR cycle involves in the re-oxidation of acid sites by O 2 at 200–300 °C. Generally, the Lewis acids are crucial at high temperatures, while Brønsted acids dominate the overall reaction at lower temperatures. Based on the experimental data and the DFT calculation, a mechanism for ammonia adsorption, acidity conversion and re-oxidation for the redox loop of the de-NOx reaction was proposed. The findings shed light on the understanding of relative strength of NO reduction and acid re-oxidation at different temperatures.
研究领域:
环境科学
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催化化学
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高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Jingchun Yan,Yudong Chen,Weiguo Gao,Yun Chen,Linbo Qian,Lu Han,Mengfang Chen
A high catalytic system using Cu layered double hydrotalcite (Cu(II)-Mg(II)-Fe(III)LDHs) and hydrogen peroxide (H 2 O 2 ) was developed for the degradation of ethylbenzene. It was identified that the degradation efficiency of ethylbenzene (0.08 mmol L −1 ) and TOC removal were 96.1% and 39.7% respectively in the presence of 0.1 g L −1 Cu(II)-Mg(II)-Fe(III)LDHs with (Cu 2+ + Mg 2+ )/Fe 3+ molar ratio of 5.0 and 0.16 mmol L −1 H 2 O 2 in 6.0 h. Based on ESR and XPS data, hydroxyl radicals (•OH) were the predominant free radical specials generated from the catalytic decomposition of H 2 O 2 for the degradation of ethylbenzene. The redox of Cu(II)/Cu(III) on the layered Cu(II)-Mg(II)-Fe(III)LDHs surface active sites accounted for the formation of •OH radicals and the cycle of Cu(II) in the Cu(II)-Mg(II)-Fe(III)LDHs/H 2 O 2 system were proposed.
研究领域:
环境科学
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催化化学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 99
·期 12
·2665-2676
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IF 2.8
Yongming Wang,Qiang Chen,Yuezong Su,Yuxuan He,Jin Qian,Kailin Xu
BACKGROUND The increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe 2 /MoSe 2 (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX. RESULTS Over 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of 1 O 2 , SO 4 •– and • OH in the degradation system, with SO 4 •- predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen-containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non-toxic. CONCLUSION This work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real-world water treatment applications. © 2024 Society of Chemical Industry (SCI).
研究领域:
环境科学
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化学工程
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高影响因子
CHEMOSPHERE
·
2022
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IF 8.943
Jiaojiao Yang,Binyu Guo,Lei Li,Quanyuan Chen,Chensi Shen,Juan Zhou
The limited regeneration of Fe 2+ in the Fe-catalyzed advanced oxidation processes (AOPs) constrained its application for the removal of organic pollutants. Herein, MoSe 2 was introduced to promote the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in the Fe 2+ /PMS system. Compared with Fe 2+ /PMS processes, the 2,4-D degradation efficiency and PMS decomposition rate respectively increased by 73.8% and 84.2% in the MoSe 2 /Fe 2+ /PMS system. DFT simulation results suggested that Se atoms acted smoothly as the bridge supporting the charge transfer from Mo to adjacent Fe atoms, which led to the reduction of Fe 3+ . The rapid regeneration of Fe 2+ boosted the activation of PMS and the degradation of pollutants. Additionally, the electron paramagnetic resonance (EPR) and quenching experiments results indicated that SO 4 ∙ − , ∙OH, and 1 O 2 accounted for 2,4-D degradation, and SO 4 ∙ − and 1 O 2 predominated the reaction. The Mo based co-catalysts showed better co-catalytic effect than the W counterparts, and the moderate adsorption for PMS and lower electron transfer electron transfer resistance accounted for the more excellent co-catalytic performance of MoSe 2 than that of WSe 2 . In addition, the degradation efficiency of 2,4-D was up to 95.5% after five cycles of MoSe 2 in the co-catalytic system. The coexistent humic acid (HA) and Cl − showed ignorant negative effect on the degradation, while HCO 3 − would depress the oxidation reaction. The acidic etching wastewater can be applied as the Fe ions source in this co-catalytic process to remove 2,4-D effectively.
研究领域:
环境科学
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化学工程
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高影响因子
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